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# Contents

### Preface

This dissertation describes work undertaken at the Cavendish Laboratory between October 1998 and October 2001, under the supervision of Professor Peter Littlewood.

Some of the work presented in this thesis has been published, has been submitted for publication, or is in preparation for publication, in the papers:

* M. H. Szymanska, P. B. Littlewood, R. J. Needs, “Excitons in T-shaped quantum wires”, Phys. Rev. B, 63, 205317 (2001).
* J. Rubio, L. N. Pfeiffer, M. H. Szymanska, A. Pinczuk, S. He, H. U. Baranger, P. B. Littlewood, K. W. West, B. S. Dennis, “Coexistence of Excitonic Lasing with Electron-Hole Plasma, Spontaneous Emission in One-Dimensional Semiconductor Structures ”, accepted for publication in Solid State Commun..
* M. H. Szymanska, P. B. Littlewood, “Bose Einstein Condensation of cavity polaritons and lasing - crossover between the two regimes”, in preparation for Phys. Rev. Letters.
* J. Rubio, L. N. Pfeiffer, M. H. Szymanska, A. Pinczuk, S. He, H. U. Baranger, P. B. Littlewood, K. W. West, B. S. Dennis, “Two-mode lasing in a quantum wire” in preparation for Phys. Rev. B

Except where stated otherwise, this dissertation is the result of my own work and contains nothing which is the outcome of work done in collaboration. This dissertation has not been submitted, in whole or in part, for any degree or diploma other than that of Doctor of Philosophy at the University of Cambridge.

Marzena Hanna Szymanska

Trinity College

October 2001

### Summary

There are two distinct phenomena where quantum coherence has been observed on the macroscopic scale: the laser and Bose Einstein condensation. Although the physics underlying these processes is fundamentally different, they both could potentially be observed in the same microcavities, and both would be a source of a coherent light.

In the first part of this thesis I study the intermediate regime between ordinary lasing and a BEC of exciton polaritons. I take into account the fermionic structure of polaritons, treating the excitons as two-level systems coupled to a single mode in a microcavity. I introduce decoherence and dissipation processes to this system. Employing many-body Green function techniques, similar to those used by Abrikosov and Gor’kov in their theory of gapless superconductivity, I provide a mathematical structure that unifies models of lasers with models of condensates. This allows me to study the stability of the polariton condensate with respect to decoherence processes and the crossover between the polariton condensate and the laser. I give detailed indications of a regime in which the condensate should be observed to guide experimental work and show how to distinguish the Bose condensate from a laser.

The second part of this thesis is concerned with properties of excitons and modelling of excitonic lasing in quasi-one-dimensional quantum wires. I develop a very general numerical method of calculating the properties of wires with different shapes and materials. Using this method I study the properties of very wide range of T-shaped quantum wires. I also develop an analytical model for the two-mode laser. Using my theory I explain the detailed issues raised by experiments. The method is being used in designing a high performance 1D wire laser in collaboration with Bell Laboratories.

### Acknowledgements

I am deeply indebted to my supervisor, Peter Littlewood for his guidance, support and encouragement, for his constant optimism over the last three years and for his advice in many matters of my academic life.

I owe particular thanks to Paul Eastham for many exciting discussions and his stimulating criticism. I am very grateful to Richard Needs, Peter Haynes, Andrew Porter and Greg McMullan for their help and advice concerning the computational techniques. I am pleased to thank Hidefumi Akiyama, Loren Pfeiffer and Aron Pinczuk for numerous interesting discussions during my visits at Bell-Laboratories. I would like to record my gratitude to Ben Simons and David Khmeltnitskii for their helpful opinions and suggestions, and Robert Moir, Chris Pickard, Mike Towler and Jem Pearson for proofreading parts of this thesis.

Special mentions are due to Tracey Ingham, our group secretary, for being so helpful in solving numerous problems of everyday life in TCM. I also owe particular thanks to Yong Mao, Mercedes Hinton and Francesca Marchetti for their support during the ups and downs of my life in Cambridge. Finally and most importantly I would like to thank my family for their love, help and encouragement throughout my PhD.

I acknowledge financial support from Lucent Technologies, Trinity College Cambridge, Cambridge Overseas Trust and an ORS award.

### Introduction

Coherence is a property of waves which describes how much they resemble a smooth sine wave. In a quantum theory matter, similarly to light, has a wave-like character and can exhibit coherence. However, neither the wave nature of matter nor coherent states are generally observed in everyday life. This is because, usually, only a tiny fraction of particles occupy the same quantum state leading to an incoherent, classical world.

It is, however, possible to produce systems in which a large number of particles occupy the same coherent state observable on a macroscopic scale. One of the most common and widely used for practical applications is the laser - a coherent state of light. Observation of a coherent state of massive, interacting and number conserved bosons, known as a Bose Einstein condensate (BEC), is very difficult due to large decoherence effects, and requires very low temperatures. Liquid Helium and trapped atomic gases remain the only systems where BEC is experimentally observed and controlled. Superconductivity \- a coherent state of paired electrons - closes the list of current experimental realisations of macroscopic quantum coherent states. These few experimental realisations have had a large impact on an understanding of quantum physics.

Another candidate for BEC, which would be very interesting for practical applications, is excitons - bound states of electrons and holes which occur in semiconductors. Together with the decoherence effects the major difficulty in obtaining the coherent state of excitons is their non-equilibrium nature. They decay into light. Excitons can, however, be placed in an optical cavity, where photons are prevented from escaping. If the exciton-photon interaction is sufficiently strong they form new particles: cavity exciton-polaritons which are bosons and so can Bose condense.

Miniaturisation and improvements in the quality of optical cavities in recent years bring new possibilities for the observation of coherent effects. In cavities the size of a wavelength of light, called microcavities, the exciton-photon interaction is particularly strong and the decoherence is reduced. The experimental observation of Bose condensation of cavity polaritons might become possible. Such a polariton condensate could also be a new source of coherent light where, in contrast to lasers, no population inversion would be required.

Although the first laser action was observed long ago, extensive research is still being done in the search for miniaturised, low-threshold lasers. Recent achievements in manufacturing good quality low-dimensional microstructures provide the possibility for much better performance of optical devices.

My thesis addresses two aspects of this subject. In the first part we develop a theory which connects Bose-Einstein condensation of microcavity polaritons and lasing. The second part is devoted to modelling excitonic lasing in quasi-one-dimensional, T-shaped quantum wires.

#### Bose Einstein condensation of microcavity polaritons and lasing crossover between the two regimes

There are two distinct phenomena where quantum coherence has been observed on the macroscopic scale: the laser and Bose Einstein condensation. Although the physics underlying both processes is fundamentally different, they both could potentially be observed in the same microcavities, and both would be a source of a coherent light.

The BEC of excitons or exciton-polaritons is still an open issue, undergoing extensive experimental research. Indications of some excitonic coherence effects in semiconductor microcavities were reported but whether BEC of exciton-polaritons took place remains unresolved.

As the BEC of polaritons could be a source of a coherent light the issue arises how the condensation can be distinguished from an ordinary lasing. The development of a theory which connects these two regimes in microcavity, predicts the major signs of a condensate, and checks its stability with respect to decoherence processes is of both fundamental interest and will help experimentalists in the search for condensation.

Generalisation of existing laser theories to include the media coherence effects seems very promising as a polariton condensate could be a source of a coherent light without the population inversion.

We study the intermediate regime between ordinary lasing and a BEC of exciton polaritons. We take into account the fermionic structure of polaritons, treating the excitons as two-level systems coupled to a single mode in a microcavity. We introduce decoherence and dissipation processes to this system.

In the limit of very large decoherence we obtain a conventional laser. In the opposite regime we can examine the stability of the BEC of polaritons.

The work, although motivated by the experiments on semiconductor excitons, is much more general, and can be applied to any two-level systems interacting via photons confined in a cavity.

#### Excitons in T-shaped quantum wires

Optical properties of electrons and holes confined to few dimensions are of particular interest for optical and electronic devices. As the dimensionality of the structure is reduced, the density of states tends to bunch together leading to a singularity in the 1D case. At the same time the excitonic interaction in 1D is enhanced. For the ideal 1D quantum wire, the excitonic binding energy and oscillator strength diverge suggesting that they can be greatly increased in practice for quasi-1D wires. Both effects provide possibilities for improving the performance of optical devices such as semiconductor lasers.

A much studied quasi-1D experimental system is the T-shaped quantum wire formed at the intersection of two quantum wells. Laser emission from the lowest exciton state in T-shaped quantum wires has been experimentally observed, and an interesting observation of two-mode lasing in such wires has been recently reported.

We develop a rate equation model to understand this two-mode lasing phenomena. The model gives very good agreement with experimental data, which suggests that we have lasing from two different excitonic states in the structure. Thus excited states seem to be very important for the operation of excitonic lasers.

Motivated by the growing experimental realisation of these structures, as well as the interesting report of lasing phenomena, we have developed a numerical method to calculate energies, oscillator strengths for radiative recombinations, and two-particle wave functions for the ground state exciton and the excited states in a T-shaped quantum wire. These calculations are being used to design improved excitonic lasers which will operate at room temperature.

## Part I Bose Condensation of Cavity Polaritons and Lasing <br>Crossover Between the Two Regimes

### Chapter 1 Introduction

In this Chapter we introduce basic concepts of Bose-Einstein condensation and briefly review the main theoretical and experimental work which has been done up to date in the area of BEC of excitons and polaritons which is relevant for our work. We also give a short description of the quantum theory of the laser and a general account of the relationship between a Bose condensate and a laser.

#### 1.1 Bose-Einstein Condensation

Bose-Einstein condensation is a phase transition in which a macroscopic number of particles all go into the same quantum state . This property place the Bose condensate as a separate state of matter, distinct from all other states in which the occupation of any single-particle eigenstate is negligible in comparison to the total particle number. This macroscopically occupied state has remarkable properties. In an extended system macroscopic occupation of one state implies that the wave function of a single particle can extend over macroscopic distances throughout the system and thus there is a long-range order in the phase of the condensate. Long-range phase coherence means that the local phase at every point in the condensate has a well define value. Since the Hamiltonian does not depend on the phase of the wavefunctions such phase locking implies broken gauge symmetry. A well defined phase, according to the Heisenberg uncertainty principle, causes the number of particles not to have a definite value and thus the condensate has to be a coherent state and not a number state.

The only experimental realisations of BEC are liquid Helium and trapped atomic gases. A superconductor is yet another example of a macroscopic coherent state. However the fermionic structure of Cooper pairs in a superconductor affects some of its properties, and thus this state is sometimes distinguished from the BEC in a strict sense. It would be of a great fundamental interest to add a few more experimental realisations to this short list. Liquid Helium and trapped atomic gases are probably not the most suitable systems for practical applications and a realisation of a BEC in a solid - state system would be more practical.

Neutral electronic excitations in a solid can have a bosonic nature, and thus could be candidates for Bose condensation. In semiconductors the electron in the conduction band and the hole in the valence band interact via an attractive Coulomb interaction, and can form a bound state called exciton. An exciton, as a particle build up from two fermions, is a boson and thus has the properties which result from Bose statistics.

There are, however, some practical difficulties concerning BEC of excitons. In semiconductors the Coulomb interaction between the electron and the hole within exciton is screened by other carriers and thus the binding energy of exciton is much weaker than that of the analogous hydrogen atom. Therefore excitons can only exist at low temperatures or in low-dimensional structures, where their binding energy is enhanced. Another fundamental difficulty is that the large population of an externally excited excitons is not a real ground state of semiconductor. Excitons are not conserved particles and can recombine emitting photons. However, if the lifetime of the exciton is long in comparison with the thermalisation time a quasi-equilibrium Bose condensate could be observed. Thus materials with very weak light-matter coupling would be good candidates for such condensates. We will give a brief review of experimental advances in this area in Section 1.2.

The strong light-matter interaction does not always have to be disadvantageous for the formation of the condensate. At certain conditions it is the strong dipole coupling which would favour the condensation. One of the examples is a coherently excited semiconductor. In experiments where electrons and holes are created by an external coherent light the non-equilibrium driven condensate would form. Coherence in such systems does not appear spontaneously but is inherited from an external coherent pump. Another example would be to prevent the coherent excitations from escaping by placing the sample in an optical cavity. If the interaction between atoms or excitons in semiconductors and light is strong the new quasiparticles, called cavity polaritons, would form. Polaritons as a coupled states of photons and electronic excitations are bosons and thus similarly as pure excitons could Bose condense. Bose condensation of excitons and polaritons has been a subject of extensive experimental investigations in recent years which we will briefly review in Section 1.4 and Chapter 4.

BEC was first described for a non-interacting, ideal gas of free bosons. This description still remains a standard textbook theory despite that it does not explain all basic properties of real Bose condensates stated in the first paragraph of this Section. However, the instability of the normal state is present even in the non-interacting Bose-gas and thus this model gives the first insight into the phenomena of Bose condensation.

For an ideal gas of bosons with mass $`m`$ and particle number $`N`$, the occupation of a single eigenstate with energy $`ϵ_k`$ is given by a Bose distribution

$$n_𝐤=\frac{1}{e^{\beta (ϵ_k\mu )}1},$$

where $`ϵ_k=\mathrm{}^2𝐤^2/2m`$, $`\mu 0`$ is a chemical potential and $`\beta =1/kT`$. The total number of particles in the system is

$$\underset{𝐤}{}n_𝐤=N,$$
(1.1)
and thus the density of particles is

$$n=\frac{N}{V}=\frac{1}{(2\pi )^3}\frac{1}{e^{\beta (ϵ_k\mu )}1}𝑑𝐤.$$
(1.2)
It can be noticed that the integral (1.2) cannot account for all the particles in a system at all $`T`$ and $`n`$, since $`\mu `$ must have an upper bound of zero for the distribution function to be defined at all energies. At a given temperature the density of particles which corresponds to $`\mu =0`$ is a critical density which can not be exceeded within the equation (1.2). This implies that for densities higher that this critical density the summation in equation (1.1) can not be simply replaced by an integral and the only way to accommodate all the particles in the system is by placing the macroscopic number of bosons into a small, non-macroscopic number of states.

The theory of a non-interacting Bose gas explains the macroscopic occupation of a small number of quantum states and gives the density and the temperature of a transition. However, this theory does not explain why all the excess particles should occupy only one single-particle state and not a few states close to the ground state . Another problem is that for the non-interacting boson model the condensate would be a number state of the form

$$(\psi ^{})^N|vac.$$
(1.3)
The wavefunction (1.3) does not contain the phase coherence characteristic of real condensates.

Interactions between particles would resolve both problems discussed in the previous paragraph. Even arbitrarily weak interactions can create a macroscopic energy difference between different macroscopically occupied eigenstates, whose energies would be very close to the ground state in the absence of interactions. Interactions thus favour the occupation of the single lowest energy eigenstate only. In the presence of interactions the condensate wavefunction will no longer be a number state but will become a coherent state of the form

$$e^{\lambda \psi ^{}}|vac.$$
(1.4)
The interaction mixes the single particle states and thus the total energy of the system can be lowered with respect to the energy in a number state by taking into account the interference terms between different single-particle eigenstates within the coherent state wavefunction. Coherent state has a fixed phase but allows for the fluctuation of the condensate population. Only the average particle number in the condensate is well defined and equal to $`\lambda `$ (eqn 1.4).

The Bogoliubov theory of the weakly interacting Bose gas is used to describe atomic condensates. Other condensates mentioned at the beginning of this section have additional complications which can not be accounted for by this theory. The interactions in liquid Helium are far too strong to be described by the weakly interacting gas model. In the case of superconductors the internal fermionic structure of the Cooper pairs cannot be neglected. Excitons and polaritons could be treated as structureless bosons only at very low densities, probably to low to acquire phase coherence. For higher densities, similarly as in superconductors, the internal fermionic structure has to be included.

In the next few sections we will review the existing theories and experiments concerning quasi-equilibrium exciton condensation, coherently driven condensates, polariton stimulated scattering and equilibrium isolated polariton condensation.

#### 1.2 Condensation of Excitons

In materials where the light-matter interaction is very weak, for example $`Cu_2O`$ or $`CuCl`$, the electronic excitations have long life-time. This time might be long enough to achieve a thermal equilibrium and to acquire a phase coherence due to the mutual interactions. Thus we might expect a quasi-equilibrium condensate.

Bosons on an atomic energy scale, apart from photons, are always composite, build up from an even number of fermions. In the case of $`{}_{}{}^{4}He`$ or any other atomic or molecular system it is very difficult experimentally to compress them to such high densities that the underlying fermionic degrees of freedom would play an important role. In the case of electronic excitations, such as for example excitons in semiconductors, due to their large radii and the possibilities of creating them by external excitations, the high densities can be easily realised and the underlying fermionic nature can play an important role.

The major nonlinearities arising with increasing density are screening and the saturation of the underlying fermionic states, the so called “phase-space filling” effect. At low densities, when the exciton radius is small compared with the distance between excitons, the condensate would resemble a BEC of point-like bosons, while in the opposite limit, where excitons overlap and the fermionic states saturate, the system would form a BCS-like coherent pair-state, called an excitonic insulator in semiconductor physics. In other words we have a transition from a real-space pairing of tightly bound excitons to a momentum-space pairing of weakly correlated and overlapping electron-hole pairs.

By analogy to superconductivity Keldysh, Kozlov and Kopaev developed a theory  which smoothly connects these two regimes of densities. Excitons are treated not as structureless bosons but as electrons and holes interacting via the attractive Coulomb potential. Introducing $`b_𝐤`$ and $`a_𝐤`$ as annihilation operators for an electron with momentum k in the conduction and valence bands respectively, the creation operator for an exciton is

$$D^{}=\underset{𝐤}{}\varphi _𝐤b_𝐤^{}a_𝐤.$$

$`\varphi _𝐤`$ is the internal orbital wavefunction and remains close to the single exciton form at low densities, where exciton-exciton interactions do not affect the internal structure of the exciton. As we discussed in the Section 1.1, the Bose condensate is a macroscopically occupied state with long-range phase coherence. Thus we expect the wavefunction of an exciton condensate to be a coherent state of the form

$$|\mathrm{\Phi }_\lambda =e^{\lambda D^{}}|vac=\underset{𝐤}{}e^{\lambda \varphi _𝐤b_𝐤^{}a_𝐤}|vac.$$
(1.5)
Expanding the exponential in the equation (1.5) and taking into account the exclusion principle for fermionic operators $`b^{}`$ and $`a`$, the condensate wavefunctions would have the form

$$|\mathrm{\Phi }_\lambda =\underset{𝐤}{}(1+\lambda \varphi _𝐤b_𝐤^{}a_𝐤)|vac.$$
(1.6)
Equation (1.6) is a special case of the BCS wavefunction for the coherent state of Cooper pairs in the superconductors

$$|u,v=\underset{𝐤}{}(u_𝐤+v_𝐤b_𝐤^{}a_𝐤)|vac,$$
(1.7)
where

$$|u_𝐤|^2+|v_𝐤|^2=1.$$
(1.8)
The wavefunction (1.7) provides a smooth transition between Bose-condensed excitons at low densities and BCS-like collective state of electron and holes (so called excitonic insulator) at high densities; at very high densities it approaches an uncondensed electron-hole plasma. This form of the wavefuncion was widely used to describe BEC of excitons, particularly by Comte and Nozières .

The evolution of the state (1.7) as the density grows can be seen in Figure 1.1 .

The behaviour of $`|v_𝐤|`$ is shown as a function of the energy $`ϵ_𝐤`$ for different densities. $`\lambda `$ is an average number of particles in the state, fixed by the density, while the shape of the $`v_𝐤`$ shows the internal structure of the electron-hole pair. At low densities where $`u_𝐤1`$ and $`v_𝐤\lambda \varphi _𝐤1`$, $`|v_k|`$ scales with a constant shape as a function of density (curves a and b in Fig. 1.1) and describes essentially the single exciton wavefunction.

With increase in the density the $`|v_𝐤|`$ finally approaches 1 (curve c in Fig. 1.1) and due to the exclusion principle, expressed by the equation (1.8), cannot increase any further. In order to accumulate more particles it is necessary to occupy more energetic states in k-space (curves d and e in Fig. 1.1). This saturation occurs when excitons start overlapping, and the resulting ground state becomes BCS-like collective state, characterised by a small energy gap in the excitation spectrum which decreases with density. In the regime of very high densities $`v_𝐤`$ becomes a step function, $`|v_𝐤|=1`$ if $`𝐤<𝐤_𝐅`$, $`0`$ if $`𝐤>𝐤_F`$, characteristic for electron-hole plasma. Thus, the saturation of the fermionic states together with screening would eventually suppress the condensation at high densities.

Another enemy of the excitonic condensation are impurities present in semiconductor. The influence of impurities on the excitonic insulator was discussed by Zittartz . He studied randomly distributed normal impurities which, in the case of oppositely charged electrons and holes, have the same effect as magnetic impurities in superconductors. He applied the Abrikosov and Gor’kov theory  to the excitonic insulator case and showed that beyond a critical impurity concentration the excitonic phase cannot exist. Close to the critical concentration there is a gapless excitonic insulator analogous to a gapless superconductor.

Experimental work on Bose condensation of excitons rely on looking at systems with a long lifetime for recombination such as $`Cu_2O`$ and $`CuCl`$ or dipole excitons in coupled quantum wells. A very good review of the recent advances in this area, both the experimental and the theoretical, can be found in references .

The evidences for the existence of Bose condensates in $`Cu_2O`$ are based on spectral analysis or detecting superfluidity of excitons. Lin and Wolfe  observed lineshapes in photoemission that were consistent with strong degeneracy and possibly consistent with BEC of excitons. Experiments by Mysyrowicz and co-workers - reported an anomalous ballistic transport of excitons over large distances which was argued to be a sign of superfluidity; these have been criticised as possibly being due to phonon-wind transport -, a purely classical effect. Most recently , Wolfe retracted the earlier experiments because the absolute measurements of the exciton density showed they were too low to give BEC.

A coupled quantum wells system consists of two different, adjacent planes with electrons in one layer and holes in the other. Applied electric field keep both kinds of carriers in separate two-dimensional planes. This arrangement reduces the overlap of the wavefunctions of the electron and the hole and thus increases the lifetime of excitons. While the first set of experiments claiming to see Bose statistics in these systems were retracted, the most recent work by Butov et al. - concludes that there is evidence of stimulated scattering, and therefore densities reaching the quantum regime; but there is no evidence for BEC.

One problem with an interpretation of the experimental data, and also with the control of the condensate, comes from the fact that excitons decay emitting light, and thus the condensate is only a quasi-equilibrium phenomena, which can survive only up to the time scale for recombination. One way to go would be to look for materials where light-matter interaction is very weak and so consequently excitons have relatively long lifetime. But the strong exciton-photon interaction does not necessarily preclude the existence of a condensate if the coherence is maintained in the photons. This could be realised in two fundamentally different situations.

The first one is the coherently driven system. In the presence of an external strong, coherent laser field the non-equilibrium condensate of electronic excitation can form. Instead of spontaneous symmetry breaking leading to a condensation the exciton system inherit its coherence from the external coherent photon field.

The second case is a spontaneous condensation of cavity polaritons achieved by placing the system in an optical cavity, where photons and thus the coherence is prevented from escaping.

#### 1.3 Coherently driven systems

The properties of the media in the strong coherent electromagnetic field were first studied by Galitskii, Goreslavskii and Elesin  then broth into the context of exciton condensation by Elesin and Kopaev  and further developed by Schmitt-Rink, Chemla and Haug .

In the presence of electromagnetic field with very high intensity the interaction between electronic excitations and light is particularly strong. It cannot be tackled by a perturbation theory but as a major interaction in the system must be treated exactly. The Hamiltonian for the electronic excitations and their interaction with the external electromagnetic wave $`A`$ cos $`\omega t`$ is the following

$$H=\underset{𝐤}{}ϵ_𝐤(b_𝐤^{}b_𝐤a_𝐤^{}a_𝐤)+\mathrm{\Delta }_k(b_𝐤^{}a_𝐤e^{i\omega t}+a_𝐤^{}b_𝐤e^{i\omega t})+H_{Coul},$$
(1.9)
where $`\mathrm{\Delta }_k=g_kA`$ and $`g_k`$ is a coupling strength between matter and light. The $`H_{Coul}`$ is the Coulomb interaction between carriers. In the absence of the Coulomb interaction it is possible to diagonalise this Hamiltonian by means of first a unitary transformation to change to a representation in which the Hamiltonian does not depend on time and then a canonical transformation to make it diagonal:

$$H_0=\underset{𝐤}{}E_𝐤(\beta _𝐤^{}\beta _𝐤\alpha _𝐤^{}\alpha _𝐤).$$
(1.10)
The new quasiparticles $`\beta _k`$ and $`\alpha _k`$ are linear combinations of $`a_k`$ and $`b_k`$ with the dispersion law

$$E_k=\sqrt{(ϵ_k\omega )^2+\mathrm{\Delta }_k^2}.$$
(1.11)
In the presence of a strong electromagnetic field the electronic levels get mixed and the relevant description is in terms of new quasiparticles $`\beta _k`$ and $`\alpha _k`$, which are coherent superpositions of the upper and the lower electronic states. Since the electron is in a coherent superposition of both levels, the polarisation of the particles is finite. Thus a macroscopic coherent polarisation of the media appears, inherited from the coherent pump field.

The new quasiparticles $`\beta _k`$ and $`\alpha _k`$ are subject to other interactions of a different origin (Coulomb interactions, collisions with phonons or impurities). These additional interactions can be treated perturbatievly if they are weak in comparison with electron - photon coupling, and the kinetic equations for the quasiparticles can be obtained. If the other interactions become comparable with light-matter coupling, the quasiparticle picture breaks down and we are back to the usual weak regime of light-matter interactions.

Schmitt-Rink et al  studied the behaviour of a coherently driven system for a wide range of pump intensity (i.e the density of electronic excitations) for two cases with and without the Coulomb interaction using more rigorous Keldysh non-equilibrium Green function techniques. They obtained all regimes of real-space and momentum space pairing discussed in the Section 1.2. At high pump intensities the Coulomb interaction gives only a small correction to the dominant processes induced by the coherent pump filed. In contrast at small pump intensities the Coulomb interactions play an important role and leads the electrons and holes to form bound excitons which are then coherently driven by the field.

Due to the external source of a coherence the coherently driven condensate is much more robust than the equilibrium excitonic insulator and thus exist for all temperatures and densities. Screening and phase-filling effects, which suppress the equilibrium excitonic condensate at high densities, are also present in the case of coherently driven systems. However, high densities in this case correspond to a strong pump field which dominates the physics, and the gapped condensate is present.

Schmitt-Rink et al  also point out that their results, in the case without the Coulomb interaction, are equivalent to those obtained for an ensemble of independent two-level atoms as the optical transition with different k decouple. We will come back to this point in Section 3.1 when we introduce the two-level oscillators model for the electronic excitations.

#### 1.4 Polariton Condensation

Another way to prevent the exciton condensate from decaying is to place the media in the cavity, where photons are confined and thus prevented from escaping. Similarly as in Section 1.3 strong light-matter interaction mixes the photon and exciton states and causes the formation of the new quasiparticle cavity-polariton. Polariton can be seen as a superposition of a plane wave of the electromagnetic field and a plane wave of polarisation. It was first introduced by Hopfield  to describe the light in a bulk material. Cavity polaritons have been experimentally observed for atoms , quantum wells  and bulk excitons , excitons in organic semiconductors  and exciton complexes .

Quantum wells confined in a planar microcavity is a particularly good system to observe the coherence effects. The binding energy of ideal quantum well exciton is four times that of the bulk exciton and the photon-matter interaction in a microcavity is particularly strong, as the decoherence effects are reduced, allowing to study the so called strong-coupling regime.

Microcavity polaritons are subject of intensive experimental research in recent years. A strong-coupling polariton effect for excitons coupled to photons was first observed in microcavity GaAs/AlGaAs quantum well by Weisbuch et al  in 1992. Since then there were many experiments studying the properties of cavity polaritons in various systems out of which the most interesting is the observation of stimulating scattering for polaritons  \- .

Stimulating scattering, similarly as BEC, is an effect of quantum statistics of indistinguishable Bose particles. The scattering rate into a particular final state is proportional to a factor $`(1+N_f)`$, where $`N_f`$ is the occupation number of the final state. Thus, particles already present in the particular eigenstate enhance the transitions of other particles into this eigenstate. This process for photons leads to a lasing action while for polaritons it can give an increase by orders of magnitude of the total scattering rate even in the normal state. This effect can be observed by measuring the photoluminescence from an optically excited semiconductors and indeed in recent experiments  \-  authors observe a nonlinear build-up of a lower polariton population as a pumping intensity is increased. There is a clear threshold in the pump intensity where the stimulated scattering starts. Above this threshold a large occupation of the lower polariton states is observed. This population is usually far from thermal equilibrium with few exceptions where the thermalised emission is claimed .

Stimulated scattering of polaritons causes macroscopic occupation of a single quantum state and in this way is similar to Bose condensate. However BEC is characterised by a phase coherence which is unlikely to be present in these experiments. The experiments are performed in the very low density limit and thus a considerably long time is required for the interactions to produce a phase coherence. This time is most likely to be longer that the lifetime of the cavity mode. In addition there are also other pair-breaking decoherence processes, which we will show in this work to be more destructive at low densities. In present experiments the attempt to increase the density of polaritons results not in the formation of the condensate but in a switching into the weak-coupling regime and lasing. Thus definite evidence for BEC of polaritons has not been given.

However, the observation of the stimulating scattering for polaritons suggests that another effect of bosonic statistic, BEC should be in principle possible in these systems. The issue is not whether or not excitons are bound or ionised into a plasma, but whether the decoherence suppresses the excitonic polarisation. We will show in this work that indeed the regime of BEC exists for sufficiently large densities and low decoherence. Thus the problem is to experimentally achieve the right regime. We will come back to this issue in more details in the Chapter 4.

Now we will present the existing theory of isolated polaritons in which the decoherence and dissipations processes are ignored. First we discuss the low density regime and then the generalised model for all densities.

##### 1.4.1 Low Density Regime

The first approximation usually made is to treat the excitons as structureless bosons and thus the interacting exciton-photon system is nothing more than two coupled harmonic oscillators. The Hamiltonian for structureless excitons dipole coupled to photons after the rotating-wave approximation is

$$H=\underset{𝐤}{}ϵ_𝐤D_𝐤^{}D_𝐤+\omega _𝐤\psi _𝐤^{}\psi _𝐤+g_𝐤(D_𝐤^{}\psi _𝐤+\psi _𝐤^{}D_𝐤).$$
(1.12)
The Hamiltonian (1.12) can be diagonalised using the canonical transformation

$$\left(\begin{array}{c}P_𝐤^1\\ P_𝐤^2\end{array}\right)=\left(\begin{array}{cc}\mathrm{cos}\theta _𝐤& \mathrm{sin}\theta _𝐤\\ \mathrm{sin}\theta _𝐤& \mathrm{cos}\theta _𝐤\end{array}\right)\left(\begin{array}{c}D_𝐤\\ \psi _𝐤\end{array}\right)$$

to the following form

$$H=E_𝐤^1P_𝐤^1P_𝐤^1+E_𝐤^2P_𝐤^2P_𝐤^2,$$

where $`P_𝐤^1`$ and $`P_𝐤^2`$ are the two polariton levels and are linear combinations of exciton and photon $`P_𝐤^{1,2}=u_𝐤^{1,2}D_𝐤+v_𝐤^{1,2}\psi _𝐤`$ with the dispersion relation

$$E_𝐤^{1,2}=\frac{1}{2}\left[ϵ_𝐤+\omega \pm \sqrt{(ϵ_𝐤\omega )^2+4g_𝐤^2}\right].$$
(1.13)
The two-dimensional polariton energies are illustrated in Fig. 1.2.

The first estimate in studying the BEC of polaritons is to treat them as weakly interacting, structureless bosons and to use the theory of atomic condensates to predict the transition temperature and density. However one can easily notice that this picture is far from being complete. There are several effects which are important for the formation of the condensate and are not included within the above treatment.

1) Phase space filling effect. With the increase in the excitonic density saturation of the underlying fermionic states becomes important. This saturation takes place for densities at which excitons start overlapping. Phase space filling effect is not included in the model of polaritons described at the beginning of this Section.

2) Disorder. All theories for exciton and polariton condensation as well as driven condensates discussed so far consider ideal and infinite structures, where bare electronic excitations are propagating states with a well defined momentum. However, the real structures are far from being perfect and contain a high level of disorder caused by fluctuations in thickness of quantum well and alloying concentration or presence of impurities. The disorder potential is usually weak with respect to the binding energy of excitons and thus does not destroy them. However, the exciton centre of mass wavefunction would be localised in the minima of the disorder potential rather then propagating through the sample. The correlation length of the disorder potential and thus the spatial extend of the exciton centre of mass wavefunction vary typically from a few to about ten exciton Bohr radius . Thus a localised exciton picture might be more relevant for these structures.

3) Screening. The Coulomb interaction between electron and hole in the exciton is screened by other excitations. This screening increases with the increase in density leading to a complete dissociation of excitons at very high densities and thus the decrease in the strength of the exciton-photon interaction.

4)Decoherence effects. Apart from the exciton-photon interaction there are other processes present in the cavity. Excitons interact with phonons and impurities, they are subject to collisions and pumping processes. Despite the advances in the fabrication of microcavities the mirrors are not perfect and the photons can escape. These processes could cause the suppression of the condensate and the strong coupling regime altogether.

##### 1.4.2 Generalisation of Polariton Condensation to Include Phase Space Filling Effect

The first two of the effects described at the end of the Section 1.4.1: the phase space filling effect and the disorder were studied by Eastham and Littlewood . In contrast to the propagated excitons model they use the generalised Dicke model widely applied in quantum optics to study the radiative decay of atomic gases and lasers. The electronic excitations are treated as an ensemble of two-level oscillators dipole coupled to one mode of the electromagnetic filed. The upper level corresponds to the excited state of an atom or the presence of a localised exciton at a given site in the material, while the lower state corresponds to the ground state of the atom or the lack of an exciton. The two-level oscillators interact through the common photon mode and all other direct interactions are neglected. The Dicke model is generalised to include the distribution of excitonic energies and coupling strength and the constrain in the number of excitations is imposed. The Hamiltonian for this model is

$$H=\underset{j=1}{\overset{N}{}}ϵ_j(b_j^{}b_ja_j^{}a_j)+\omega _c\psi ^{}\psi +\underset{j=1}{\overset{N}{}}\frac{g_j}{\sqrt{N}}(b_j^{}a_j\psi +\psi ^{}a_j^{}b_j),$$
(1.14)
where $`b`$ and $`a`$ are fermionic annihilation operators for an electron in an upper and lower states respectively and $`\psi `$ is a photon bosonic annihilation operator. The sum here is over the possible sites where an exciton can be present (different molecules or localised states in the disorder potential) and not over the momentum like in the case of propagating excitons. The fermionic structure is included through the single occupancy constrain for both levels of the two-level oscillator expressed in the commutation relations for the $`a`$ and $`b`$ fermionic operators. Thus this model includes a phase space filling type effect and the disorder, and does not include screening and decoherence effects.

In real structures different types of excitons could be present. The exciton could be localised in a minimum of the disorder potential, some traps could be big enough so that a few excitons can be present on one side, some excitons could extend for large distances and finally some propagate in the sample. Depending on the material and the growth condition of the sample certain types would be dominant. The model discussed in this Section gives very good description of the tightly bound, Frenkel excitons which can be treated as a point-like compared with a wavelength of light, localised by the disorder or bound on impurities or molecular excitons in organic materials. This model describes the opposite limit to the ideal structures with propagating exciton centre-of mass wavefunctions but recent experiments in quantum wells  \-  suggest that it might be more relevant, at least at low densities.

Eastham and Littlewood consider a thermal equilibrium of this model at fixed number of excitations (excitation density) in the cavity equal to $`n_{ex}`$ ($`\rho _{ex}`$), where

$$n_{ex}=\frac{1}{2}\underset{j=1}{\overset{N}{}}(b_j^{}b_ja_j^{}a_j)+\psi ^{}\psi =N\rho _{ex}.$$
(1.15)
This corresponds to the situation, where system is initially excited with an external pump and then isolated so that the excitations can not decay out of the cavity, and the thermal equilibrium can be achieved.

They use functional path integral techniques and show that the mean-field solution is well controlled by the number of sites available, N, with fluctuations of order of 1/N and thus exact in the limit where $`N\mathrm{}`$. They show that the wavefunction

$$|u,v=\underset{j}{}e^{\lambda \psi ^{}}(u_j+v_jb_j^{}a_j)|vac$$

is an exact ground state for $`N\mathrm{}`$.

Eastham and Littlewood study the ground state and the excitation spectrum of this model for a range of temperature, excitation densities, photon-exciton detuning and exciton energy distribution. They recover the crossover from the structureless polariton condensate to the BCS-like coherent state, where saturation effects are important. In contrast to the excitonic insulator the BEC of generalised polaritons is present even at very high excitation densities due to the presence of highly occupied photon mode. At low densities the condensate is more exciton-like, while at high densities it has more photon-like character. At zero temperature the system is always condensed as the decoherence processes are not included in the model. The condensate has a gap in the excitation spectrum of magnitude $`4g|\lambda |`$, where $`\lambda `$ is an amplitude of the coherent photon field and $`g`$, as usual, is the coupling constant between photon and exciton (see Figure 1.3).

Their work shows that although the phase space filling effect causes the collapse of the splitting between the two polariton peaks in the normal state with increasing density, it does not destroy condensation even at very high excitation densities. Due to this saturation effect in the fermionic space the condensate is becoming more photon like as the excitation density is increased, but nevertheless the coherence in the media and the gap in the excitation spectrum are present (see Figure 1.3).

Polariton condensate as a coherent state of photons and electronic excitations would be a source of a coherent light. The issue arises how it is different and how it can be distinguished from the ordinary laser. Two major conclusions can be derived from their theory. Firstly, in contrast to lasers the coherent light in polariton condensate would be present even without population inversion. Secondly, the polariton condensate, unlike the laser, would have a gap in the excitation spectrum.

Both processes, the polariton condensate and laser, are fundamentally different and appear in different regimes of the light-matter interaction. Polariton condensate is a condensate of strongly coupled modes of light and electronic excitations. Laser is a weak-coupling phenomenon and is essentially a coherent state of photons created by stimulated emission from an inverted electronic population due to the strong pumping. Both processes can be present in the same microcavity systems and the essential light-matter interaction would be described by the same Hamiltonian (1.14). Thus the laser and the polariton condensate can be viewed as two different regimes in microcavity. In the Section 1.2 we discussed the crossover between the regime of BEC and BCS-like states with a change in the density of the electronic excitations. Now, the crossover between the strong coupling regime of a polariton condensate and a weak coupling regime of a laser is caused by a different phenomena. We will show in the Chapter 3 that the decoherence processes drive this crossover.

The model studied by Eastham and Littlewood is a closed system model with the dipole interaction between excitons and photons only. However, in real microcavities other interactions are also present. There are elastic collisions between excitons, exciton interactions with phonons and impurities and radiative decay to modes different that the cavity mode. Excitons are also subject to pumping and the photon field decay from the cavity. All these processes would cause the decoherence of the coherent state favoured by the major exciton-photon interaction. The relative strength of these processes with respect to the light-matter interaction will determine the regime in the cavity. In a strong coupling regime all other interactions are very small in comparison to the dipole interaction, while in the opposite, weak-coupling regime the other interactions are comparable to the exciton-photon coupling.

In this work we would like to address the problem of the influence of the decoherence processes on the polariton condensate. Decoherence can drive this system through phase transitions. Thus, we would like to study different regimes as the decoherence is changed for a range of excitation densities. This will firstly allow us to study the stability of the polariton condensate to various decoherence processes, and then to establish a crossover between an ideal polariton condensate and a laser.

In order to establish the connection between the polariton condensate and the laser we will first review the basic properties and a quantum theory of the laser.

#### 1.5 Laser

Photon laser is a weak-coupling regime phenomenon in which, according to the Fermi golden rule, the rate of transition is determined by the squared matrix element of the perturbation between the initial and final states. In a laser an ensemble of atoms (excitons, electron and holes) interacts with a photon field confined in the cavity. This interaction causes transitions between two electronic levels in the media stimulated by the photon field and thus proportional to the number of photons in the cavity. Stimulated emission, proportional also to the number of atoms in an upper state, results in emission of a photon with the same phase as the photon which causes the transition and is thus coherent with the cavity mode. Stimulated absorption results in an absorption of the cavity mode photon and is proportional to the number of atoms in the lower state. The transition from the upper to the lower level can also be caused by vacuum fluctuations and is called spontaneous emission. It causes the emission of the photon with a random phase and is thus incoherent with the photon mode in the cavity. Spontaneous emission is small in comparison to the stimulated emission if many photons are present in the cavity with a ratio 1:n, where n is the number of photons in the cavity mode. In order to build up a macroscopic coherent population of photons stimulated emission has to overcome absorption and thus an inverted ensemble of atoms is necessary for a laser action. In order to overcome the cavity losses, spontaneous emission and all other decay processes and to keep the population of atoms inverted, a sufficiently strong pumping mechanism has to be applied.

The pumping mechanism and other decoherence processes acting on atoms are strong, comparable to the interaction with light. Thus lasers operate in the regime, where the coherent polarisation of the media is very heavily damped and the atomic coherence is very much reduced. A coherent photon field, oscillating at bare cavity mode frequency, is the only order parameter in the system. The above properties define the regime considered by all laser theories.

The quantum theory of a laser was developed in the sixties using the quantum Langevin equations, equations of motion for the density matrix or master equations . We will present the quantum Langevin equations’ formulation developed by Haken  as it can be easily connected to the formulation of polariton condensate developed by Eastham and Littlewood.

A laser is described as an open system interacting with an environment. The system consists of an ensemble of two-level oscillators dipole interacting with a cavity mode. The Hamiltonian for the system is given by the equation (1.14). All other processes are treated as an environment which cause decoherence, dissipation and pumping of the energy. These processes are of a different physical nature, depending on the material, and their exact details are not important for the general laser theory. They can be modelled as baths of harmonic oscillators, interacting with the system in a way that would give the same effect as the original interactions. These baths are assumed to be very large in comparison with the system and thus not changed by the system. The laser Hamiltonian can be written in a general form as

$$H=H_S+H_{SB}+H_B,$$
(1.16)
where $`H_S`$ is a system Hamiltonian given by equation (1.14). $`H_{SB}`$ describes the interactions between the system and its baths

$$\begin{array}{c}H_{SB}=\underset{k}{}g_\kappa (k)(\psi ^{}d_k+d_k^{}\psi )+\underset{j,k}{}g_\gamma _{}(j,k)(b_j^{}a_jc_{j,k}^\alpha +c_{j,k}^\alpha a_j^{}b_j)+\hfill \\ \hfill \underset{j,k}{}g_\gamma _{}(j,k)(b_j^{}a_jc_{j,k}^\beta +c_{j,k}^\beta a_j^{}b_j)+\underset{j,k}{}g_\eta (j,k)(b_j^{}b_ja_j^{}a_j)(c_{j,k}^\delta +c_{j,k}^\delta ),\end{array}$$
(1.17)
while $`H_B`$ is a Hamiltonian for the baths

$$\begin{array}{c}H_B=\underset{k}{}\omega _\kappa (k)d_k^{}d_k+\underset{j,k}{}\omega _\gamma _{}(j,k)c_{j,k}^\alpha c_{j,k}^\alpha +\hfill \\ \hfill \underset{j,k}{}\omega _\gamma _{}(j,k)c_{j,k}^\beta c_{j,k}^\beta +\underset{j,k}{}\omega _\eta (j,k)c_{j,k}^\delta c_{j,k}^\delta ,\end{array}$$
(1.18)
where $`c_{j,k}^{}`$ and $`c_{j,k}`$ are the bosonic creation and annihilation operators, respectively, for the baths. The first term in equation (1.17) gives the decay of the photon field from the cavity. The second term describes incoherent pumping of atoms, while the third term describes nonradiative recombinations or spontaneous emission to the modes other than the cavity mode. The fourth term gives rise to all the decoherence processes which do not destroy excitations like collisions, phonons or impurity scattering. The first three terms in equation (1.17), apart from fluctuations, give rise to the flow of an energy through the system. In order to obtain a dissipation of the energy from the system the baths need to be kept at a positive temperature whereas to model the pumping process the bath must be at negative temperature which correspond to the ensemble of inverted harmonic oscillators.

From the Hamiltonian (1.16), using some approximations, it is possible to derive the quantum Langevin equations for the system operators or density matrix, where the influence of the baths would be simplified. We will present this procedure for the field operator only, as the derivation for the atomic operators would follow in a similar manner.

The Heisenberg equations of motion for the field and its bath annihilation operators are

$`{\displaystyle \frac{d\psi }{dt}}`$ $`=i\omega _c\psi i{\displaystyle \underset{j}{}}g_ja_j^{}b_ji{\displaystyle \underset{k}{}}g_\kappa (k)d_k`$ (1.19)
$`{\displaystyle \frac{dd_k}{dt}}`$ $`=i\omega _\kappa (k)d_kig_\kappa (k)\psi .,`$ (1.20)
Integrating the equation (1.20) we obtain the following equation for the bath operator

$$d_k(t)=d_k(t_0)e^{i\omega _\kappa (k)(tt_0)}ig_\kappa (k)_{t_0}^t𝑑t^{^{}}\psi (t^{})e^{i\omega _\kappa (k)(tt^{})}.$$
(1.21)
Substituting equation (1.21) into equation (1.19) we obtain the following integro-differential equation for the field operator

$$\begin{array}{c}\frac{d\psi }{dt}=i\omega _c\psi i\underset{j}{}g_ja_j^{}b_ji\underset{k}{}d_k(t_0)e^{i\omega _\kappa (k)(tt_0)}\hfill \\ \hfill \underset{k}{}g_\kappa (k)^2_{t_0}^t𝑑t^{^{}}\psi (t^{})e^{i\omega _\kappa (k)(tt^{})}.\end{array}$$
(1.22)
The third term in equation (1.22) does not depend on the field operators and acts as a random fluctuating force. The forth term is in general quite complicated and connects the behaviour of the field operator at time $`t`$ with its past. In laser theory this term is simplified using the following approximations:

* There is a smooth dense spectrum of oscillator frequencies.
* The coupling constant of the system to the bath and the density of states for the bath are smooth, slowly varying functions of the frequency of the oscillators.
* The time scales for the bath degrees of freedom are much shorter than for the system degrees of freedom, so that there is no memory in the system, and the state of the system does not depend on its past. It is the so-called Markov approximation.

Transforming $`_k𝑑\omega _\kappa D_\kappa (\omega _\kappa )`$ and using the above approximations, the last term in equation (1.22) can be simplified:

$$\underset{k}{}g_\kappa (k)^2_{t_0}^t𝑑t^{^{}}\psi (t^{})e^{i\omega _\kappa (k)(tt^{})}=\kappa \psi (t),$$
(1.23)
where $`\kappa =\pi g_\kappa ^2(0)D_\kappa (0)`$ and $`D_\kappa `$ is a density of states for the bath. Introducing the following abbreviation for the fluctuating force

$$i\underset{k}{}d_k(t_0)e^{i\omega _\kappa (k)(tt_0)}=F(t),$$

the final equation for the field operator is

$$\frac{d\psi }{dt}=(i\omega _c\kappa )\psi i\underset{j}{}g_ja_j^{}b_j+F(t).$$
(1.24)
Following the same procedure it is possible to derive similar equations of motion for the atomic operators. The equation for the atomic polarisation is

$$\frac{da_j^{}b_j}{dt}=(i2ϵ_j\gamma _{})a_j^{}b_j+ig_j\psi (b_j^{}b_ja_j^{}a_j)+\mathrm{\Gamma }_j,$$
(1.25)
and for the atomic population inversion

$$\frac{d(b_j^{}b_ja_j^{}a_j)}{dt}=\gamma _{}(d_0b_j^{}b_j+a_j^{}a_j)+2ig_j(\psi ^{}a_j^{}b_jb_j^{}a_j\psi )+\mathrm{\Gamma }_{j,d},$$
(1.26)
where

$`\gamma _{}`$ $`=2(\gamma _{}+\gamma _{})`$ $`\gamma _{}`$ $`=\gamma _{}+\gamma _{}+\eta `$ $`d_0`$ $`={\displaystyle \frac{\gamma _{}\gamma _{}}{\gamma _{}+\gamma _{}}}.`$
and

$`\gamma _{}`$ $`=\pi g_\gamma _{}^2(0)D_\gamma _{}(0)`$ $`\gamma _{}`$ $`=\pi g_\gamma _{}^2(0)D_\gamma _{}(0)`$ $`\eta `$ $`=\pi g_\eta ^2(0)D_\eta (0).`$
$`D_\gamma _{}`$, $`D_\gamma _{}`$ and $`D_\eta `$ are the densities of states for the appropriate baths.

All the interactions with an environment together with the distribution of energies $`ϵ_j`$ due to disorder, give additional broadening to the natural linewidth of the system. This broadening can be homogeneous or inhomogeneous depending on its physical origin.

Inhomogeneous broadening takes place when the optical transition energies are split (in the case of degeneracies) or shifted in a different way for different sites. This broadening has a Gaussian distribution and can be included into the model by setting the two-level oscillators energies $`ϵ_j`$ to be Gaussian distributed around some mean value. The physical origin of this broadening depends on the material used for a laser medium. It can be caused by the fluctuations in thickness of a quantum well and alloying concentration or presence of impurities inserted at non-equivalent lattice sites.

The homogeneous broadening corresponds to the situation, where all sites are broadened in the same way. It can be caused by collisions with phonons or impurities, or lattice vibrations which are fast in comparison to the laser process. This broadening can only be modelled by the means of appropriate dynamic baths.

The influence of baths in the Heisenberg equations of motion, after the approximations described in this section, manifests itself as decay constants for the photon field and the polarisation independent of time and frequency, a pump constant for inversion, and the random fluctuating forces (noise). The mean values of the noise terms are zero. Thus in the mean-field approximation equations (1.24) - (1.26) would have only appropriate decay constants and the random forces would disappear. The atomic equations could be summed to obtain the equation for the total inversion $`D=_j(b_j^{}b_ja_j^{}a_j)`$, and a total polarisation $`P=_ja_j^{}b_j`$. If we then rescale these equations by the number of atoms in the cavity N, introducing a rescaled photon field $`\psi /\sqrt{N}`$, polarisation $`P/\sqrt{N}`$ and inversion $`D/N`$ it will become apparent that the deterministic terms are of order $`N^0`$, while the noise terms are all of order $`1/\sqrt{N}`$. In realistic systems the number of atoms is very large and thus the noise terms are small compared with the deterministic terms. In a limit where $`N\mathrm{}`$ the noise terms become zero and the mean-field approach is exact.

In order to study a regime below the lasing threshold, where the macroscopic coherent fields are absent, and also to determine the linewidth of the laser light, fluctuations above mean-field have to be included. Most of the other properties of lasers above threshold can be derived using the mean-field approximation, since the number of atoms is always very large.

#### 1.6 BEC and Lasing

The properties of a laser can be derived from the Hamiltonian (1.16) with large interactions with an environment. If in the same Hamiltonian we set the coupling constants between the system and the environment to zero, we obtain Hamiltonian (1.14) of which the ground state was shown by Eastham and Littlewood to be a polariton condensate. Thus by varying the magnitude of the coupling constants between the system and the baths in the Hamiltonian (1.16) we should be able to study all different phases driven by the decoherence. This should allow us to check the stability of the polariton condensation to the interactions with the outside world at a small coupling strength, and to establish the connection between polariton condensation and lasers as the decoherence is increased.

In Chapter 2 we will show that the Langevin equations (1.24) - (1.26), widely used in laser theories, cannot be used to establish this connection. We will show that the time(frequency) independent decay constants are critical in these equations and even at arbitrarily small decoherence strength lead to completely different solutions from those in the absence of the environment. We will give physical insight why the approximate treatment of the baths, in the manner of equations (1.24) \- (1.26), gives non-physical answers in some regimes. In Chapter 3 we use Green’s function techniques, similar to Abrikosov and Gor’kov theory of gapless superconductivity, to treat the influence of the environment in the self-consistent way and to study different regimes as the decoherence is changed. Finally, in Chapter 4 we summarise the conclusions and give an account of the work still in progress as well as possible future developments.

### Chapter 2 BEC and Lasing - Langevin Equations

In this Chapter we consider the Langevin equations derived for the laser system in Section 1.5. These equations become the equations of motions for the isolated system studied by Eastham and Littlewood when the coupling to the environment is zero. Firstly we show that these equations in a steady state lead to the same solutions obtained by Eastham and Littlewood using path-integral methods. Thus the equation of motion is yet another method of studying the polariton condensate but more importantly it brings a connection to the laser equations. We then consider the Langevin equations with a finite coupling to the environment and show that the fact the decay constants are independent of time (frequency) is critical in these equations and even at arbitrarily small decoherence strength lead to completely different solutions than in the absence of an environment. This criticality is however non-physical and arises only due to the approximations used in deriving the Langevin equations.

#### 2.1 Mean-Field Langevin Equations

The Langevin equations for the laser system (1.24) - (1.26) after the mean-field approximation take the following form:

$`{\displaystyle \frac{d\psi }{dt}}`$ $`=(i\omega _c\kappa )\psi i{\displaystyle \underset{j}{}}g_jp_j`$ (2.1)
$`{\displaystyle \frac{dp_j}{dt}}`$ $`=(i2ϵ_j\gamma _{})p_j+ig_j\psi d_j,`$ (2.2)
$`{\displaystyle \frac{dd_j}{dt}}`$ $`=\gamma _{}(d_0d_j)+2ig_j(\psi ^{}p_jp_j^{}\psi ),`$ (2.3)
where $`\psi `$, $`p_j`$ and $`d_j`$ are the photon field, the polarisation and the inversion of a two-level oscillator. At zero temperature $`<>`$ means the quantum-mechanical average in the ground state of the system. By definition the coherent state is an eigenstate of a bosonic annihilation operator and thus the average of this operator in the coherent state is equal to the corresponding eigenvalue which is non-zero for an occupied state. The average of an annihilation operator in an normal state is however zero. Thus the mean-field equations (2.1) - (2.3) describe the behaviour of the coherent part of the photon field and polarisation. As we discussed in Section 1.5 they are exact in the limit $`N\mathrm{}`$ for an isolated condensate and laser system above the laser threshold.

Equation (2.2) can be rearranged to obtain

$$\psi =\frac{(\frac{d}{dt}+i2ϵ+\gamma _{})p_j}{igd_j}.$$
(2.4)
Substituting this expression into equation (2.3) yields

$$\frac{d(d_j^2+4|p_j|^2)}{dt}=4\gamma _{}(\frac{\gamma _{}}{\gamma _{}}d(d_0d_j)2|p_j|^2).$$
(2.5)
This equation is a differential equation which connects the coherent polarisation and the inversion of the two-level oscillator. By setting $`\gamma _{}`$, $`\gamma _{}`$ and $`\kappa `$ to zero in the equations (2.1) - (2.3) we can obtain the Heisenberg equations of motion for the isolated system studied by Eastham and Littlewood. Let us first consider the isolated case.

#### 2.2 Isolated System

The equation (2.5) for the isolated system becomes

$`{\displaystyle \frac{d(d_j^2+4|p_j|^2)}{dt}}`$ $`=0`$ $``$ $`d_j^2+4|p_j|^2`$ $`=Cons.`$ (2.6)
The polarisation of the medium is connected with the transitions between levels and is equal to the off-diagonal terms of the system density matrix or the Green function. For the coherent polarisation to have a non-zero value, the system must be in a mixture of lower and upper states. When the inversion is exactly 1 (or -1), all atoms are in the upper (or lower state) and thus the coherent polarisation must disappear. This condition would be satisfied by constant in equation (2.6) equalling unity and thus the relation between the coherent polarisation and inversion would become

$$|p_j|^2=\frac{1}{4}(d_j1)(d_j+1).$$
(2.7)
The dependence of the coherent polarisation on the inversion is shown in Figure 2.1 (blue curve). In the isolated condensate, unlike in lasers, the coherent polarisation is present even without the population inversion in the system (even for $`d<0`$). We are interested in the steady state solutions to these equations in which the coherent fields oscillate at the constant frequency:

$`\psi (t)`$ $`=\psi e^{\mu t}`$ $`p(t)`$ $`=pe^{\mu t}.`$ (2.8)
Substituting both the Ansatz (2.8) and equation (2.7) into equations (2.1) and (2.2) we obtain

$`\psi `$ $`={\displaystyle \frac{1}{\omega _c\mu }}{\displaystyle \underset{j}{}}g_jp_j`$ (2.9)
$`p_j`$ $`=sign(ϵ_j\mu ){\displaystyle \frac{g_j\psi }{2\sqrt{g_j^2|\psi |^2+(ϵ_j\mu )^2}}}`$ (2.10)
$`d_j`$ $`={\displaystyle \frac{|ϵ_j\mu |}{\sqrt{g_j^2|\psi |^2+(ϵ_j\mu )^2}}}.`$ (2.11)
From equations (2.9) and (2.10) after rescaling the coherent field by $`\sqrt{N}`$ ($`\psi \psi \sqrt{N}`$) we obtain the following equation for the coherent field

$$(\omega _c\mu )\psi =\frac{\psi }{2N}\underset{j}{}\frac{g_j^2}{E_j}$$
(2.12)
where we define

$$E_j=sign(ϵ_j\mu )\sqrt{g_j^2|\psi |^2+(ϵ_j\mu )^2}.$$

Equations (2.9) - (2.12) are exactly the same as the zero temperature equations obtained by Eastham and Littlewood  using path-integral methods and describe the polariton condensate for a wide range of densities. The structure of the equation (2.12) is similar to the BCS gap equation.

#### 2.3 System with Decoherence

In this Section we will examine the case when interactions with the environment are present. We are again interested in the steady state solutions of the equation (2.5). It can be shown that the only steady state solution to this equation occurs when

$`{\displaystyle \frac{\gamma _{}}{\gamma _{}}}d_j(d_0d_j)2|p_j|^2`$ $`=0`$ $``$ $`|p_j|^2={\displaystyle \frac{\gamma _{}}{2\gamma _{}}}d_j(d_0d_j).`$ (2.13)
In the most ideal case when we have neither spontaneous emission nor any other decoherence process in the system and the only interactions with the environment are pumping and the decay of the cavity field we obtain

$$|p_j|^2=\frac{1}{2}d_j(1d_j).$$
(2.14)
We can see from equations (2.13) and (2.14) that for an arbitrarily small strength of the interaction with the environment we obtain completely different solutions to that given by equation (2.7) for an isolated system. It can be shown that the solutions for an isolated condensate would decay out when interactions with the outside world are present. Even for an arbitrary small interaction with the environment in order to obtain a non-zero coherent polarisation, the inversion $`d`$ must be grater than zero which means the system must be inverted. Figure 2.1 shows the comparison between the isolated condensate (blue curve) and one interacting with an environment (red curves). The solid red curve shows the most ideal case when the only interactions are pumping and the decay of the cavity field. Even in this situation for an arbitrarily small pumping the system goes from the blue to the solid red curve. The dashed red curve shows the example when other decoherence processes are present for the case where $`d_0=0.8`$ and $`\gamma _{}/\gamma _{}=0.4`$. This is still a very small decoherence. In a usual operating regime for a laser $`\gamma _{}\gamma _{}`$ and thus the coherent polarisation would be very small for all values of the inversion.

The frequency at which the coherent fields oscillate for an isolated condensate can be obtained from the density equation (1.15). In general this frequency has a very complicated form but at low densities approaches the polariton energy given by equation (1.13) and is dependent on the coupling strength between matter and light, $`g`$ for all densities. In the case where the interactions with the environment are included within the Langevin equations (1.24) - (1.26) this frequency can be calculated by comparing the real and the imaginary parts of equations (2.1) and (2.2). In the case of uniform energies $`ϵ_j=ϵ`$ and coupling constant $`g_j=g`$ it takes a simple form

$$\mu =\frac{\gamma _{}\omega _c+\kappa 2ϵ}{\gamma _{}+\kappa },$$

which in the case of the usual laser operating condition $`\gamma _{}\kappa `$ leads to $`\mu \omega _c`$. Again it can be seen that even for an arbitrarily small coupling to the environment this frequency is completely different to the one obtained for an isolated condensate. Most importantly it does not depend on $`g`$. Thus we can conclude that within the Langevin equation approach with constant decay rates even for arbitrary small coupling to the environment the system goes to the weak light-matter coupling regime. This surely cannot be physical.

#### 2.4 Conclusions

We have shown that the Langevin equations with constant decay rates even for an arbitrary small decoherence strength lead to completely different, essentially laser-type, solutions than for the isolated system.

In this work we would like to stress that this criticality is not a physical one and results purely from the approximations applied in deriving the Langevin equations for this system. This conclusion seems not to be widely appreciated and even in a relatively recent publication  similar decay constants in the equations of motion for the coherently driven excitonic insulator have been used, leading to the conclusion that the excitonic insulator phase cannot exist for an arbitrary small decoherence.

Let us get some physical insight into this problem. In order to obtain the Langevin equations (1.24) - (1.26) all the baths were averaged out before the essential dipole interaction was taken into account. The ideal condensate has a gap in the density of states which would still be present for small decoherence. It is clear that the coherent fields in this regime cannot be damped just by constant decay rates independent of frequency as there are no available states to decay to. As the decoherence is increased this gap gets smaller and finally is completely suppressed causing the coherent fields to be strongly damped. In order to describe this behaviour the decoherence processes have to be treated self-consistently. The baths have to be averaged out in such a way that the essential interactions and thus the gap in the density of states is taken into account.

The equations of motion with decay constants independent of time and frequency, although perfectly correct in describing the laser where the decoherence processes are very large, cannot be used to study the regime with a small decoherence when the gap in the density of states is present nor to establish a connection between an isolated condensate and a laser.

In the next chapter we present an alternative method which takes all this essential physics into account. By analogy with superconductivity we use Green function methods similar to the Abrikosov and Gor’kov theory of gapless superconductivity and treat the decoherence in a self-consistent way which allow us to move smoothly between an isolated condensate and other regimes driven by the decoherence.

### Chapter 3 Self-consistent Green’s-Function Approach

We study the behaviour of a system which consists of a photon mode dipole coupled to a medium of two-level oscillators in a microcavity in the presence of the decoherence. We consider two types of decoherence processes which are analogous to magnetic and non-magnetic impurities in superconductors. We study different phases of this system as the decoherence strength and the excitation density is changed. For a low decoherence we obtain a polariton condensate with comparable excitonic and photonic parts at low densities and a BCS-like state with bigger photon component due to the fermionic phase space filling effect at high densities. In both cases there is a large gap in the density of states. As the decoherence is increased the gap is broadened and suppressed, resulting in a gapless condensate and finally a suppression of the coherence in a low density regime and a laser at high density limit. A crossover between these regimes is studied in a self-consistent way similar to the Abrikosov and Gor’kov theory of gapless superconductivity .

#### 3.1 Model

The model we consider in this work is schematically shown in Figure 3.1.

It consists of a system of two-level oscillators dipole coupled to one confined cavity mode as described in the Section 1.4.2. This system is then subject to various decoherence, pumping and damping processes described, as in laser theory (Section 1.5), as baths of harmonic oscillators coupled to the system in a way that gives the same effect as the original interactions.

This model includes:

* major Coulomb interaction between the electron and hole within exciton,
* phase space filling effect,
* disorder in the material (inhomogeneous broadening of excitonic energies),
* various types of decoherence effects,

and does not include:

* screening,
* Coulomb interactions between excitons.

Thus this model:

* gives a very good description of tightly bound, Frenkel - type of excitons localised by disorder or bound on impurities, molecular excitons in organic materials or atoms in the solid state,
* gives a qualitative description within a mean-field approximation for other types of excitons like Wannier excitons or excitons propagating in a sample.

The second application follows from the fact that the dipole interaction between excitons and photons is a dominant interaction at high excitation densities (large photon fields). In the case of a driven excitonic system Schmitt-Rink at al  pointed out that for a very large pumping, and thus high excitation densities, the Coulomb interaction is just a very minor correction to the dominant dipole coupling. They also state that in the absence of the Coulomb interaction their results for propagating electrons and holes are equivalent to those obtained for an ensemble of independent two-level oscillators as optical transitions with different k decouple. In the case of low densities the dominant Coulomb interaction, that between an electron and hole within the same exciton, is taken into account in our model. All other Coulomb interactions are much weaker and in any case are found within the mean-field techniques of Keldysh  \-  for exciton condensation to give rise to a formation of a coherent excitonic insulator phase and thus would only enhance the dipole coupling. Therefore the localised two-level oscillator model can be applied to obtain a qualitative description of the physical behaviour even for the propagated or weekly bound excitons. It would give similar predictions to the model based on propagating electrons and holes with Coulomb interactions treated within mean-field approximations. It does not include screening and other non mean-fields effects.

We would like to stress that in this work we intend to study a very general model of the media and consider in details the influence of various types of decoherence processes in microcavity and different phases induced by the decoherence and the excitation density. At this stage we do not want to model any particular media with its complex interactions which would only make the general picture less clear. The specific details of the particular media could however be easily included into our model, we will discuss this possibility in the Sections 4.1.3 and 4.1.4.

We consider the following Hamiltonian:

$$H=H_0+H_{SB}+H_B$$
(3.1)
where

$$H_0=\underset{j=1}{\overset{N}{}}ϵ_j(b_j^{}b_ja_j^{}a_j)+\omega _c\psi ^{}\psi +\underset{j=1}{\overset{N}{}}\frac{g_j}{\sqrt{N}}(b_j^{}a_j\psi +\psi ^{}a_j^{}b_j).$$
(3.2)
$`H_0`$ describes an ensemble of two-level oscillators dipole coupled to one cavity mode and is exactly the same as the Hamiltonian (1.14) studied for an isolated condensate by Eastham and Littlewood . For the detailed description of this Hamiltonian see Section 1.4.2. $`H_{SB}`$, similarly as in the laser theory described in the Section 1.5 (equation (1.17)), contains all interactions with an environment. In our work we include a more general coupling to the environment than in the laser theory, allowing the interactions with an upper level to be different that with a lower level (the fourth and the fifth terms in the equation (3.3) instead of the fourth term in the equation (1.17)):

$$\begin{array}{c}H_{SB}=\underset{j,k}{}g_\kappa (k)(\psi ^{}d_k+d_k^{}\psi )+\hfill \\ \hfill \underset{j,k}{}g_\gamma _{}(j,k)(b_j^{}a_jc_{j,k}^\alpha +c_{j,k}^\alpha a_j^{}b_j)+\underset{j,k}{}g_\gamma _{}(j,k)(b_j^{}a_jc_{j,k}^\beta +c_{j,k}^\beta a_j^{}b_j)\\ \hfill +\underset{j,k}{}g_{\gamma _b}(j,k)b_j^{}b_j(c_{j,k}^b+c_{j,k}^b)\underset{j,k}{}g_{\gamma _a}(j,k)a_j^{}a_j(c_{j,k}^a+c_{j,k}^a).\end{array}$$
(3.3)
The total number of excitations

$$n_{ex}=\frac{1}{2}\underset{j=1}{\overset{N}{}}(b_j^{}b_ja_j^{}a_j)+\psi ^{}\psi ,$$
(3.4)
which is the sum of photons and excited two-level oscillators, is conserved in a steady state. The $`H_B`$ is a Hamiltonian for the baths as in the equation (1.18). In the Hamiltonian (3.1) we have not included terms that couple different sites (i.e. $`a_jb_k^{}`$ with $`kj`$) as their influence would be small in comparison to the coupling within the same site.

The second term in equation (3.3) describes an incoherent pumping of two-level oscillators. The third term contains all the processes which cause the transition from the upper to the lower level and thus destroy the electronic excitations such as the decay to photon modes different to the cavity mode. Finally, the fourth and the fifth terms describe all the decoherence processes which act on upper and lower levels respectively but do not change the total number of excitations in the cavity, for example collisions and interactions with phonons and impurities. Thus these four terms contain all the essential groups of decoherence processes in the media. The first term gives rise to the decay of the photon field from the cavity.

The fourth and the fifth term in equation (3.3) can be expressed as

$$\underset{j,k}{}g_{\gamma _1}(j,k)(b_j^{}b_j+a_j^{}a_j)(c_{j,k}^\zeta +c_{j,k}^\zeta )+\underset{j,k}{}g_{\gamma _2}(j,k)(b_j^{}b_ja_j^{}a_j)(c_{j,k}^\theta +c_{j,k}^\theta ).$$
(3.5)
The first term in expression (3.5) with the second and the third terms in the equation (3.3) describe the part of a total interaction which acts on the upper and lower levels with opposite sign. It can be shown that these processes are analogous to the pair-breaking, magnetic impurities in superconductors. We will refer to them later as the type 1 decoherence processes. The exact origin of these interactions depends on the details of the media. Physically these processes correspond to potentials which vary rapidly in space (on the lengthscale of excitons) or in time. They can be high energy phonons, collisions or impurities. In the case of electrons and holes even the normal impurities could be pair-breaking processes as the electric charge of the impurity acts with the opposite sign on the electron and the hole .

The second term in expression (3.5) contains interactions which are the same for both levels and are analogous to normal, non-magnetic, impurities in superconductors. We will call them type 2 processes. This processes correspond to potentials which vary very slowly in space in comparison to the size of excitons or in time. They do not have any pair-breaking effects and lead only to a broadening of energies.

Since the upper and the lower level are different and contain fermions with an opposite charge both kinds of interactions would always be present. In addition to these two types of processes the energies of the two-level oscillators, $`ϵ_j`$, can be inhomogeneously broadened due to fluctuations in the thickness of quantum well and alloying concentration or presence of impurities inserted at non-equivalent lattice sites.

The second and the third terms in equation (3.3), describing the incoherent pumping and dumping respectively can, in addition to having the pair-breaking effect, change the number of electronic excitations in the cavity and together with the decay of the cavity photon mode cause the flow of energy through the system. In the steady state, despite this energy flow, the total number of excitations is constant in time and proportional to the ratio between the pumping and the damping processes while the absolute magnitude of all the processes gives the decoherence strength. For very big pumping and photon decay rates the system would be out of equilibrium.

In this work we present only the influence of the decoherence on the system. The implications of a non-equilibrium system is work in progress. The equilibrium assumption can be completely justified if the system is pumped slowly, with a rate slower than the thermalisation rate. This does not put any restrictions on the strength of the decoherence nor the density of excitations. The pair-breaking processes described by the first term in expression (3.5) give exactly the same decoherence effects as the pumping and damping of two-level systems preserving equilibrium for any strength of the interaction. The ratio between the pumping and all the damping processes which can be arbitrary big even for small absolute values of both will be expressed in terms of the excitation density $`\rho _{ex}`$. For rapidly pumped systems, where the thermal distribution of quasiparticles cannot be assumed, we study only the influence of the decoherence. Non-equilibrium techniques would have to be applied to describe all the physics. We will address this problem later.

The analogy between superconductivity and an excitonic insulator was noticed and used in a pioneering work of Keldysh  and explored later on by others. This analogy was also stressed by Eastham and Littlewood  in their work on polariton condensation. The analogy to superconductivity appears to be useful also in our study of the influence of the decoherence on the polariton condensate. We can easily show that the type 1 decoherence processes acting on the microcavity condensate are analogous to the magnetic impurities in superconductors while the type 2 processes to the non-magnetic ones. Thus we can use similar methods to that used by Abrikosov and Gor’kov in their theory of gapless superconductivity .

#### 3.2 Green’s-Function Formulation

We use the self-consistent Green’s function techniques similar to the Abrikosov and Gor’kov theory of gapless superconductivity . Introducing the Nambu notation

$$\eta _j=\left(\begin{array}{c}b_j\\ a_j\end{array}\right),$$

all the Green functions are 2 x 2 matrices

$$G=\left(\begin{array}{cc}G_{bb}& G_{ba}\\ G_{aa}& G_{ab}\end{array}\right)$$

as in the BCS theory. $`G_{bb}(j,tt^{^{}})=Tb_j(t)b_j^{}(t^{^{}})`$ and $`G_{aa}(j)=Ta_j(t)a_j^{}(t^{^{}})`$ are the normal, diagonal Green’s functions which give the population distribution of the two-level oscillators while $`G_{ab}(j,tt^{^{}})=Tb_j(t)a^{}(t^{^{}})`$ and $`G_{ba}(j,tt^{^{}})=Ta_j(t)b^{}(t^{^{}})`$ are the anomalous, off-diagonal, ones which give the coherent polarisation of the media and are non-zero only in a coherent state.

Since the overall phase of a coherent state is arbitrary, we can choose the $`\psi `$ to be real and thus the Fourier transform of the zero order Green’s function, which is the Green’s function for the Hamiltonian $`H_0`$ (equation (3.2)) is

$$G_0^1(j,i\omega _n)=i\omega _n(ϵ_j\mu )\tau _3+g\psi \tau _1,$$

where $`\tau _{1,3}`$ are the usual Pauli spin matrices. We can introduce the self-energy $`\mathrm{\Sigma }`$ through the Dyson equation

$$G^1(j,i\omega _n)=G_0^1(j,i\omega _n)\mathrm{\Sigma }(j,i\omega _n),$$
(3.6)
where $`G`$ is a Green’s function for the whole Hamiltonian $`H`$, equation (3.1). Now we can write the total Green’s function $`G`$ in the same form as the zero-order Green’s function $`G_0`$

$$G^1(j,i\omega _n)=i\stackrel{~}{\omega _n}(\stackrel{~}{ϵ_j}\mu )\tau _3+g\stackrel{~}{\psi }\tau _1,$$
(3.7)
using the frequency dependent, renormalised $`\stackrel{~}{\omega _n}`$, $`\stackrel{~}{ϵ_j}`$ and $`\stackrel{~}{\psi }`$.

In this work we consider the decoherence processes given by the expression (3.5). The self-energy for the type 1 processes (the first term in the expression (3.5)) in a Born approximation is

$$\mathrm{\Sigma }_1(j,i\omega _n)=\underset{k}{}g_{\gamma _1}(k)(c_{j,k}+c_{j,k}^{})G(j,i\omega _n)\underset{k^{^{}}}{}g_{\gamma _1}(k)(c_{j,k^{^{}}}+c_{j,k^{^{}}}^{}),$$
(3.8)
while for the type 2 processes (the second term in the expression (3.5)) is

$$\mathrm{\Sigma }_2(j,i\omega _n)=\underset{k}{}g_{\gamma _2}(k)(c_{j,k}+c_{j,k}^{})\tau _1G(j,i\omega _n)\tau _1\underset{k^{^{}}}{}g_{\gamma _1}(k)(c_{j,k^{^{}}}+c_{j,k^{^{}}}^{}).$$
(3.9)
Using the Markov approximation and assuming that all coupling constants of the system to the baths, as well as the baths density of states, are very broad slowly varying functions of frequency we obtain

$$\mathrm{\Sigma }_1(j,i\omega _n)=\gamma _1G(j,i\omega _n),$$
(3.10)
and

$$\mathrm{\Sigma }_2(j,i\omega _n)=\gamma _2\tau _1G(j,i\omega _n)\tau _1,$$
(3.11)
where $`\gamma _1=g_{\gamma _1}(0)^2N_1(0)`$ and $`\gamma _2=g_{\gamma _2}(0)^2N_2(0)`$. $`N_{1,2}`$ are densities of states for the respective baths.

Substituting equations (3.10) or (3.11) into equation (3.6) and then comparing with the equation (3.7) we can obtain for both cases three equations determining the renormalised frequency, energy and coherent photon field

$`\stackrel{~}{\omega _n}`$ $`=\omega _n+\gamma _{1,2}{\displaystyle \frac{g\stackrel{~}{\omega _n}}{\stackrel{~}{\omega _n}^2+(\stackrel{~}{ϵ_j}\mu )^2+g^2\stackrel{~}{\psi }^2}},`$ (3.12)
$`\stackrel{~}{ϵ_j}`$ $`=ϵ_j\gamma _{1,2}{\displaystyle \frac{g\stackrel{~}{ϵ}}{\stackrel{~}{\omega _n}^2+(\stackrel{~}{ϵ_j}\mu )^2+g^2\stackrel{~}{\psi }^2}},`$ (3.13)
$`\stackrel{~}{\psi }`$ $`=\psi \gamma _{1,2}{\displaystyle \frac{g\stackrel{~}{\psi }}{\stackrel{~}{\omega _n}^2+(\stackrel{~}{ϵ_j}\mu )^2+g^2\stackrel{~}{\psi }^2}}.`$ (3.14)
We then have a self-consistency equation for the off-diagonal part of the Green’s function $`G`$ which is equal to the average coherent polarisation of the media

$$\frac{1}{N}\underset{j}{}a_j^{}b_j=P=\beta ^1\underset{\omega _n,j}{}\frac{g\stackrel{~}{\psi }}{\stackrel{~}{\omega _n}^2+(\stackrel{~}{ϵ_j}\mu )^2+g^2\stackrel{~}{\psi }^2}.$$
(3.15)
Both order parameters, the coherent polarisation and the coherent photon field, are connected through equation

$$\psi =\frac{g}{\omega _c\mu }P.$$
(3.16)
From equation (3.16) we can see that the ratio between the two order parameters is essentially determined by the chemical potential, which in the steady state can be calculated from the equation (3.4). A number of electronic excitations refered to later as inversion can be obtained from the diagonal elements of the Green’s function and is equal to

$$\frac{1}{2}\underset{j}{}(b_j^{}b_ja_j^{}a_j)=\beta ^1\underset{\omega _n,j}{}\frac{2(\stackrel{~}{ϵ}_j\mu )}{\stackrel{~}{\omega _n}^2+(\stackrel{~}{ϵ_j}\mu )^2+g^2\stackrel{~}{\psi }^2}.$$
(3.17)
Using the equations (3.12) - (3.14) we can determine the renormalised $`\stackrel{~}{\omega _n}`$, $`\stackrel{~}{ϵ_j}`$ and $`\stackrel{~}{\psi }`$ as a functions of bare $`\omega _n`$, $`ϵ_j`$, $`\psi `$ and $`\gamma `$. In the case of the type 1 decoherence processes we obtain for $`\stackrel{~}{\psi }`$

$$\stackrel{~}{\psi }=\frac{\psi }{2}+\frac{\sqrt{2}\psi }{4E_j}\sqrt{E_j^24\gamma _1^2\omega _n^2+\sqrt{16\gamma _1^2E_j^2+(E_j^2+4\gamma _1^2+\omega _n^2)^2}},$$
(3.18)
and for $`\stackrel{~}{ϵ_j}`$ and $`\stackrel{~}{\omega _n}`$

$`\stackrel{~}{\omega _n}`$ $`={\displaystyle \frac{\omega _n\stackrel{~}{\psi }}{2\stackrel{~}{\psi }\psi }},`$ (3.19)
$`\stackrel{~}{ϵ_j}`$ $`={\displaystyle \frac{ϵ_j\stackrel{~}{\psi }}{\psi }},`$ (3.20)
while for the type 2 decoherence processes we have

$$\begin{array}{c}\stackrel{~}{\psi }=\frac{\psi }{2}+\hfill \\ \hfill \frac{\sqrt{2}\psi }{4(\omega _n^2+g^2\psi ^2)}\sqrt{E_j^22(ϵ\mu )^2+4\gamma _1^2\omega _n^2+\sqrt{16\gamma _2^2(\omega _n^2+g^2\psi ^2)+(E_j^24\gamma _1^2+\omega _n^2)^2}},\end{array}$$
(3.21)
and

$`\stackrel{~}{\omega _n}`$ $`={\displaystyle \frac{\omega _n\stackrel{~}{\psi }}{\psi }},`$ (3.22)
$`\stackrel{~}{ϵ_j}`$ $`={\displaystyle \frac{ϵ_j\stackrel{~}{\psi }}{2\stackrel{~}{\psi }\psi }},`$ (3.23)
where for both cases

$$E_j=\sqrt{(ϵ_j\mu )^2+g^2\psi ^2}.$$
(3.24)
Substituting the equations (3.18) - (3.20) or (3.21) - (3.23) into equation (3.15), summing over the Matsubara frequencies and using equation (3.16) we can determine the coherent polarisation $`P`$ and the coherent photon field $`\psi `$ as functions of the system parameters $`ϵ`$, $`\omega _c`$, decoherence parameter $`\gamma _{1,2}`$ and chemical potential $`\mu `$. The chemical potential can be then obtained from the equation for the number of excitations (3.4). The integrals over the Matsubara frequencies at zero temperature in the equations (3.15) and (3.15) as well as the determination of the chemical potential from the equation (3.4) have to be performed numerically.

Using the above method we could determine the ground state properties of the system such as the ground state average of the coherent field, of the coherent polarisation and of the inversion as well as the chemical potential. Also the excitation spectrum, i.e the density of states, can be obtained from the diagonal part of the Green function of a real frequency. Considering the analytical continuation of $`G(j,i\omega _n)\overline{G}(j,\omega )`$, where $`\omega _n`$ and $`\omega `$ are the Matsubara and the real frequencies respectively, and thus using the usual substitution $`i\omega _n\omega i\delta `$, we obtain the relationship between the Green function $`G(j,i\omega _n)`$ and the density of states $`A(\omega )`$

$$A(\omega )=\underset{j}{}\underset{\delta 0^+}{lim}ImG_{bb}(j,\omega +i\delta +\mu ),$$
(3.25)
which in our case would take the form

$$A(\omega )=\underset{j}{}Im\frac{\stackrel{~}{\omega }+(\stackrel{~}{ϵ}_j\mu )}{\stackrel{~}{\omega }^2+(\stackrel{~}{ϵ_j}\mu )^2+g^2\stackrel{~}{\psi }^2}.$$
(3.26)
$`\stackrel{~}{\omega }`$, $`\stackrel{~}{ϵ_j}`$ and $`\stackrel{~}{\psi }`$ are functions of $`\omega `$, $`ϵ_j`$, $`\psi `$ and $`\gamma `$ which can be obtained from the equations (3.18) - (3.20) or (3.21) - (3.23) by the following substitution $`i\omega _n\omega i\delta `$. It can be shown by analysing equation (3.26) that the system of two-level oscillators with uniform energies, $`ϵ_j=ϵ`$, in the presence of the type 1 processes has a gap, $`\mathrm{\Delta }`$, in the density of states of magnitude

$$\mathrm{\Delta }=2\sqrt{(ϵ\mu )^2+g^2\psi ^2)}4\gamma _1.$$
(3.27)
The major difference between our calculations and the Abrikosov and Gor’kov theory  is that we have two order parameters connected through the chemical potential which needs to be determined. We use a different form of the density of states for the two-level oscillators than in their theory. Instead of a flat distribution of energies from $`\mathrm{}`$ to $`+\mathrm{}`$ used in the Abrikosov and Gor’kov method we first perform the calculations for the degenerate case where all two-level oscillators have the same energy $`ϵ`$ and then we use a realistic Gaussian distribution of energies, present in the real microcavities. To account for these differences we need to include the additional, third equation for renormalised $`\stackrel{~}{ϵ}`$ not present in the original Abrikosov and Gor’kov method and the constraint equation for $`n_{ex}`$. In the Abrikosov and Gor’kov theory they consider free propagating electrons with momentum k over which all the summations are performed and the external impurities mix these k states. In our model of the localised two-level systems the summations are performed over the sides where the two-level oscillators can be present and it is assumed that the interactions with the environment do not mix these sides.

To perform the calculations we rescale the coherent fields by $`\sqrt{N}`$ and consequently the inversion and the number of excitations by $`N`$ introducing the excitation density $`\rho _{ex}=n_{ex}/N`$. In this terminology the minimum $`\rho _{ex}=0.5`$ corresponds to no photons and no electronic excitations in the system. The condition $`\rho _{ex}=0.5`$ in the absence of photons would correspond to all two-level oscillators in excited states, thus to the maximum inversion.

#### 3.3 Results

We calculate first the ground state coherent field $`\psi `$, the coherent polarisation $`P`$, the inversion and the chemical potential as functions of the decoherence strength $`\gamma `$ and the excitation density $`\rho _{ex}`$. Then we study the excitation spectrum of the system for different regimes. The ground state properties and the excitation spectrum allow us to obtain a phase diagram for different excitation densities and decoherence strengths. We consider the influence of the type 1 and the type 2 decoherence processes and the inhomogeneous broadening of exciton energies.

##### 3.3.1 Type 1 (Pair-Breaking) Decoherence Processes

We first consider in detail the influence of the type 1 decoherence processes on the system of two-level oscillators with uniform energies $`ϵ_j=ϵ`$.

###### The Ground State - Coherent Fields

To examine the ground state properties of the system we first study the mean value of the annihilation operator of the field and the polarisation. This mean is non-zero only in a coherent state. Figure 3.2 (upper panel) shows the behaviour of the coherent part of the photon field $`\psi `$ as the decoherence strength $`\gamma `$ is changed for different excitation densities $`\rho _{ex}`$.

For small values of $`\gamma /g`$, up to some critical value $`\gamma _{C1}`$, $`\psi `$ is practically unchanged while for $`\gamma /g>\gamma _{C1}`$ the coherent field is damped quite rapidly with the increasing decoherence strength. This critical value of the decoherence strength, $`\gamma _{C1}`$ is proportional to $`\rho _{ex}`$, suggesting that for higher excitation densities the system is more resistant to the decoherence processes. At low excitation densities, where $`\rho _{ex}<0`$, there is a second critical value of the decoherence strength, $`\gamma _{C2}`$, where both coherent fields are sharply damped to zero. As the excitation density is increased, precisely at $`\rho _{ex}=0`$, $`\gamma _{C2}`$ moves to infinity and it does not exist for $`\rho _{ex}>0`$ \- coherent fields although damped are never completely suppressed.

The behaviour of the electronic inversion, given by the equation (3.17), is presented in Fig. 3.2 (middle panel). In this region of the decoherence strength where $`\psi `$ is damped the inversion increases. At low excitation densities ($`\rho _{ex}<0`$) the inversion approaches $`\rho _{ex}`$ for $`\gamma /g=\gamma _{C2}`$ and stays constant as $`\gamma `$ is further increased. At high excitation densities ($`\rho _{ex}>0`$) the inversion asymptotically approaches zero with increasing decoherence strength.

The ratio of coherent polarisation to coherent field $`P/\psi `$ is presented in Fig. 3.2 (lower panel). For an isolated system, where $`\gamma =0`$, this ratio depends on the excitation density. The condensate becomes more photon like as $`\rho _{ex}`$ is increased due to the phase space filling effect. For finite $`\gamma `$, at a given excitation density, this ratio decreases with increasing $`\gamma `$ meaning that the coherent polarisation is more heavily damped than the coherent photon field by the type 1 decoherence processes. At $`\rho _{ex}<0`$ this ratio becomes undefined for $`\gamma /g>\gamma _{C2}`$ when both coherent fields vanish.

###### Excitation Spectrum and the Phase Diagram

Now we examine the density of states for the system in different regimes for different values of $`\rho _{ex}`$ and $`\gamma `$. In Fig. 3.3 we present the density of states for $`\rho _{ex}=0.2`$ and six different values of $`\gamma `$.

In the absence of decoherence (Fig. 3.3 a) we have two sharp peaks at two quasi-particle energies, $`\pm E`$, given by equation (3.24) for the uniform case ($`E_j=E`$). As $`\gamma `$ increases these two peaks broaden, which causes the decrease in the magnitude of the energy gap (Fig. 3.3 b and c). The magnitude of the energy gap in the uniform case is equal to $`2E4\gamma `$, which is given in more detail in equation (3.27). Finally, precisely at $`\gamma _{C1}`$ (shown in Fig. 3.2), these two broadened peaks join together and the gap closes (Fig. 3.3 d). When the decoherence strength is increased further (Fig. 3.3 e) these two peaks overlap more and the shape of the gapless density of states changes. For $`\gamma /g>\gamma _{C2}`$ the coherent fields are suppressed, thus Fig 3.3 f shows the normal state density of states in the absence of coherence.

There are clearly three different phases depending on the decoherence strength $`\gamma `$ and the excitations density $`\rho _{ex}`$. In the Fig. 3.4 we present a phase diagram for the system.

The phase boundaries are defined by $`\gamma _{C1}`$ and $`\gamma _{C2}`$ for different values of $`\rho _{ex}`$.

Below the solid line, for small decoherence, we have a phase in which both coherent fields and the energy gap in the density of states are present. In this region coherent fields are protected by the energy gap and remain practically unchanged while the energy gap narrows as the decoherence is increased. At low densities within this phase we have a BEC of polaritons with the electronic and photonic parts comparable in size. At high densities we have a BCS-type of condensate with photon component increasing with the excitation density. Despite the predominantly photon-like character of this phase at very high densities, the coherence of the media is still large and this phase can be distinguish from a laser by the presence of a gap in the density of states (Fig 3.5 \- right panel). The crossover between high and low densities is a smooth evolution and there are no rapid phase transitions.

Between the solid and dashed lines there is a phase where the coherent fields are present without the energy gap in the density of states. This phase exists for all values of the decoherence parameter at the excitation densities $`\rho _{ex}>0`$. The coherent fields are no longer protected by the gap and get damped as the decoherence is increased. The coherent polarisation is more heavily damped than the coherent field. Within this phase we have at low densities a gapless, light-matter condensate, analogous to gapless superconductivity whilst at very high densities we have essentially the laser system.

Finally, above the dashed line there is a phase where the coherent fields are completely suppressed.

###### Crossover to Laser

The features of the second phase (between the solid and the dashed lines) in Fig. 3.4 at high $`\rho _{ex}`$ are essentially the same as those of the laser system. The laser operates in the regime of a very strong decoherence, comparable with the light-matter interaction itself. For a sufficiently large ratio of pumping and damping processes, which sets the excitation density in the cavity, even in the presence of such a large decoherence the laser action can be observed. The coherent polarisation in a laser system is much more heavily damped than the photon field and the gap in the density of states is not observed. Thus the laser is a regime of our system for very large $`\rho _{ex}`$ and $`\gamma `$.

Laser theories, due to the approximations on which they are based, can only be valid in a regime where the gap in the density of states is suppressed and thus for a large decoherence. At the time when these theories were proposed they were deemed sufficient as most lasers operate in such a regime. Miniaturisation and improvements in the quality of optical cavities in recent years can lead to a large suppression of decoherence in a laser media. For small decoherence and very small pumping in comparison to decay processes, when $`\rho _{ex}`$ is much smaller then $`0`$, the laser theories would predict a lack of coherence while the real ground state of the system would be a more matter-like condensate. Thus an extension of laser theories to account for the gap in the excitation spectrum and coherence in a media is necessary.

When both the gap and the coherence in a media are taken into account, in contrast to a traditional laser, the coherent photon field can be present without the population inversion in the media. The polariton condensate is thus an example of a laser without inversion.

It has to be pointed out that the distinction between a laser and a Bose condensate of polaritons is not a particularly clear one. In the laser, coherence in the media (manifested by the coherent polarisation) although small, is not completely suppressed so the laser can be seen as a gapless condensate with a more photon-like character. One of the possible distinctions between BEC and laser could be an existence of an energy gap in the excitation spectrum.

##### 3.3.2 Type 2 (Non-Pair-Breaking) Decoherence Processes

We have also studied the type 2 decoherence processes, analogous to the non-magnetic impurities in superconductors, which act in an exactly the same way on the upper and the lower levels of the two-level oscillator (the second term in the expression 3.5). We found that these processes give rise to the broadening of energies of the two-level system and do not have any pair-breaking effects. In the Abrikosov and Gor’kov theory, due to the flat density of sates used in the calculations, the non-magnetic impurities do not influence the superconducting state at all. In the case of uniform or realistic, Gaussian distributed energies of the two level oscillators the type 2 processes have some quantitative influence on the coherent fields and the gap but cannot cause any phase transitions. We now perform the self-consistent method described in Section 3.2 for the type 2 decoherence processes. The results are shown as dotted lines in onset of Fig. 3.2 and in Fig. 3.3.

###### The Ground State - Coherent Fields

In the inset of Fig. 3.2 we present for comparison the coherent photon field (upper panel), the inversion (middle panel), and the ratio between the coherent polarisation and the coherent photon field (lower panel) in the presence of the type 1 (solid line) and the type 2 (dotted line) decoherence processes for two excitation densities $`\rho _{ex}=0.2`$ and $`\rho _{ex}=0.2`$. It can be noticed that the sharp phase transitions at $`\gamma _{C1}`$ and $`\gamma _{C2}`$ discussed for the type 1 decoherence processes are not present for the case of the type 2 processes. With the increase of the decoherence strength from zero the coherent fields are slightly damped and they slowly decrease, asymptotically approaching zero at low excitation densities ($`\rho _{ex}<0`$) or a constant value at high densities ($`\rho _{ex}>0`$). Although both coherent fields are damped the behaviour of their ratio strongly depends on the excitation density. Since the type 2 processes give rise to the broadening of energies, the behaviour of the ratio $`P/\psi `$ depends on the position of the chemical potential with respect to the energy distribution. Thus the type 2 processes can make the condensate more photon or more exciton like depending on the parameters of the system. The two different cases are presented in Fig. 3.2.

###### Excitation Spectrum

The density of states in the presence of type 2 processes is shown in Fig 3.3 (dotted lines) for the same parameters as were used in Section 3.3.1 for studying the influence of type 1 decoherence processes. It can be noticed that, although the two quasiparticle peaks get very broad, the gap is only slightly affected by the type 2 processes and is always present. Even for much larger values of $`\gamma `$ than presented in Fig 3.3 the gap is not suppressed. The gap in the density of states is present until the coherent fields get completely suppressed. At high excitation densities ($`\rho _{ex}>0`$) coherent fields are always present and thus the density of states will have a gap for all values of the decoherence strength.

Despite a different physical origin the type 2 processes give similar effect as the inhomogeneous broadening of energy levels in the case of an isolated system (see ).

##### 3.3.3 Inhomogeneous Broadening of Energies

Finally, we study the influence of the type 1, pair-breaking processes on the system of realistic, inhomogeneously broadened two-level oscillators. We replace the summations over sites with integrals over the energy distribution. We assume this distribution to be a Gaussian with mean $`ϵ_0`$ and variance $`\sigma `$.

Our results show that the Gaussian broadening of energies does not add any qualitative difference to the uniform case. The coherent fields are, as expected, slightly smaller than in the degenerate case but all the regimes and transitions described in the Section 3.3.1 are also present here. The critical values of decoherence strength, $`\gamma _{C1}`$ and $`\gamma _{C2}`$ are slightly smaller and the energy gap narrower than in system without energy broadening for the same parameters. Fig 3.5 shows the density of states for the system of the inhomogeneously broadened two-level oscillators with standard deviation $`\sigma =0.5g`$ for different values of the type 1 decoherence strength at two different excitation densities.

The broadening of the density of states and the suppression of the energy gap can be observed as $`\gamma `$ is increased. The last curve in the Fig 3.5 (left panel) shows the normal state density of states where the coherent fields are suppressed. In the Fig 3.5 (right panel) where the coherent fields are present for all the values of $`\gamma `$ the last curve has no signs of the gap.

As we have pointed out in Section 3.3.2 the type 2 decoherence processes give similar effects as the inhomogeneous broadening of energy levels. The difference is that the density of states in the presence of the type 2 processes has sharp boundaries. This is a result of the method which is used to perform the calculations. It can be noticed that if the bath operators for the type 2 processes, $`c^\theta `$’s in expression (3.5), were just numbers, the second term in expression (3.5) could had been included into the first term in equation (3.2) and would had just given a random $`ϵ_i`$. In our calculations the $`c^\theta `$’s are operators and we use a self-consistent Born approximation, which is not exact, and makes errors in the tail of the distribution. Thus, because of the way the calculations are done, the density of states produced always has sharp boundaries.

#### 3.4 Conclusions

In this work we have studied the influence of two kinds of decoherence processes and energy broadening on the system of interacting two-level oscillators (atoms or excitons) with the photon mode in the cavity. We have noticed that the widely used Langevin equations with the decay constants independent of frequency cannot be used for a small decoherence when gap in the density of states is present. We propose a self-consistent method similar to the Abrikosov and Gor’kov theory of gapless superconductivity  which allow us to study all regimes of the system as the decoherence is changed from zero to large values and for a wide range of excitation densities. At low excitations and small decoherence we obtain a coupled matter-light condensate with a gap in the density of states. As the decoherence is increased at low excitation densities we obtain a gapless condensate and finally a complete suppression of coherence. With an increase in the excitation density the condensate becomes more photon like, but a large gap in the density of states is present for a small decoherence strength. In the limit of a very large excitation density and a large decoherence we reach a gapless, laser-like regime in which the coherent polarisation is very small in comparison with the coherent photon field.

We have shown that the polariton condensate, even in the presence of the interactions with an environment, is protected by the energy gap and thus should be observable if the decoherence is not too large. This gap increases with an increase in the excitation density and thus, in contrast to excitonic insulator, polariton condensate should be present at high densities.

Our results suggest that, in contrast to lasers, a coherent light can be generated without a population inversion. This work generalised the existing laser theories to include the gap in the excitation spectrum caused by the coherence in a media in the low decoherence regime.

We have studied separately the two types of decoherence processes in order to understand their different influence on the system. Although in the real cavities both decoherence processes and inhomogeneous broadening of energies will be present, only the pair-breaking, type 1, processes are responsible for the phase transitions and the suppression of the gap in the density of states. The type 2 processes and the inhomogeneous broadening of energies cannot on its own lead to the phase transitions. However they would make the amplitude of the coherent fields smaller and thus, in the presence of the pair-breaking processes, would cause these transitions to be present at smaller decoherence strength. For the quantitative analysis and the comparison with experiments all the decoherence processes should be included.

We have treated all the decoherence processes in a phenomenological way to study their qualitative influence on the general system. In the case of a particular example, when the origin and the density of states for the environment is known, it would be possible to perform more detailed calculations. In general the bath propagators in the equations (3.8) and (3.9) would be frequency dependent and thus $`\psi `$ would depend on the frequency as well. This frequency dependence of the coherent field, as in an Eliashberg theory of superconductivity , would have to be included in the calculations.

In this work we have studied the influence of the decoherence on an equilibrium, incoherently pumped system. However, in the same way it would be possible to examine the influence of an environment on coherently driven condensates discussed in the Section 1.3. The coherent photon field in the driven system is an external, fixed, parameter and not a self-consistent field satisfying equation (3.15). In contrast the gap in the density of states, proportional to the coherent field amplitude, is present exactly as for an equilibrium condensate. Thus the decoherence processes in the coherently driven system should be treated in the same way as for an equilibrium condensate described in this Chapter. In a recent paper  authors have ignored this fact and performed the Langevin equation method with the constant decay rates to study the stability of the driven excitonic condensate concluding that the condensed phase will be destroyed due to an arbitrarily small decoherence. In our opinion this is not physical and results only from the performed approximations.

### Chapter 4 Conclusions and Future Directions

In this work we have developed a method to include general decoherence effects in the systems with an energy gap in the excitation spectrum. We have shown that the widely used Langevin equations with the constant, frequency independent decay rates are not valid in the regime where the gap is present. The decoherence has to be treated in a self-consistent way similar to the Abrikosov and Gor’kov theory of gapless superconductivity. We studied the general form of the interactions, introducing pair-breaking and non-pair-breaking processes and thus our theory is applicable to a wide range of systems. For more detailed results, the particular origin of the interactions and thus the particular density of states for the baths have to be taken into account.

This method allows us to study the stability of the polariton condensate. For low decoherence strength the condensate is protected by the gap in the density of states. This gap is proportional to the amplitude of the coherent photon field and thus is larger for higher densities. As the decoherence is increased the gap gets smaller and finally is completely suppressed.

Experiments on cavity polaritons which report the stimulated scattering into the lower polariton branch  \-  (see Section 1.4) are performed at low densities to avoid the fermionic phase space filling effect, so that two clear polariton peaks could be seen. For such densities the gap in the excitation spectrum would be very small and easily suppressed by the decoherence processes in the sample. Indeed such a gap is not observed in the photoluminescence spectrum. The attempt to increase the density of polaritons in these experiments results not in the formation of the condensate but in a switching into the weak-coupling regime and lasing.

This is not surprising since the increase in the density of polaritons in these experiments is obtained by increasing the pumping of excitons. As we discussed in Chapter 3, the incoherent pumping is a pair-breaking decoherence process and thus the increase in the pumping intensity results in the increase of not only the density of excitons but also the decoherence strength. As shown by Eastham and Littlewood , the fermionic structure of excitons does not prevent condensation, even at very high densities. Thus, in the current experiments it is not a phase-space filling effect which lead to a laser as the pump intensity is increased, but the increase in the decoherence strength. If the polariton condensate is ever to be observed an increase in density without an increase in decoherence is necessary.

The density of excitons is proportional to the ratio between the pumping and the cavity decay rates. This ratio can be large even for small values of both rates. Thus, in order to achieve high densities without large decoherence the cavity decay rate must be small, which suggests that experiments should concentrate on improving the quality of the mirrors in microcavity systems.

The localised and tightly bound excitons, like excitons in disordered quantum wells or Frenkel-type excitons in organic compands, seem to be better candidates for observing the polariton condensate than the high-quality GaAs quantum wells with weakly bound, delocalised excitons. Static disorder is not a pair-breaking effect and would have a weaker influence on the condensate than screening and ionisation in the case of delocalised or weakly bound excitons.

Our method allows us to study different regimes as the decoherence and the excitation density is changed and thus to examine the crossover from a polariton condensate to a laser. The laser emerges from the polariton condensate at high densities when the gap in the density of states closes for large decoherence and thus is analogous to a gapless superconductor. Our work generalises the existing laser theories to include coherence effects in the media. When this coherence is included the generation of a coherent photon field without population inversion becomes possible.

In the case of coherently driven systems, in which a gap in the density of states would be present, the decoherence processes have to be also treated in a self-consistent way, similar to that described in this work.

Our method is not limited to semiconductor excitons and can be applied to any bosonic excitations which can be described as two-level oscillators, like two electronic levels in atoms or molecules.

There are many directions in which our work could be further extended. In the next Section we will review this possible directions and indicate the work being undertaken at the moment.

#### 4.1 Future Work

##### 4.1.1 Finite Temperatures

The results presented in this work are performed at zero temperature for which the summations over the Matsubara frequencies in equations (3.15) and (3.17) become integrals and are performed numerically. The extension to finite temperatures is straightforward. At finite temperatures the summations over a discrete $`\omega _n`$, which in the case of fermions would be $`\omega _n=(2l+1)\pi /\beta `$ can be performed using the standard techniques  and thus finite temperatures could be easily studied.

##### 4.1.2 Non-Equilibrium

A much more important extension that the finite temperature case is the problem of non-equilibrium systems. For a system with very strong pumping and decay processes the thermal distribution of the relevant quasiparticles cannot be assumed. It would be of a great interest to examine the influence of non-equilibrium on the behaviour of this system. This would also allow us to directly compare our theory to experiments on stimulated scattering of polaritons which are mainly out of equilibrium. We would also be able to directly apply our theory to coherently driven systems which are also out of thermal equilibrium. This work is currently in progress.

In this work we included the pair-breaking effect of pumping by studying the processes described by the first term of expression (3.5), which has the same decoherence effect as pumping but do not cause the system to be in a non-equilibrium state. The ratio between the pump and the decay rates was introduced in terms of the excitation density $`\rho _{ex}`$. To study the influence of the system being out of equilibrium we fully include the decay of the cavity field and the pumping (the first, second and third terms in equation (3.3)) which would cause a flow of energy through the system. We do not need to consider the constraint (3.4) now, as the density of the system would get fixed in a steady state by the relative strength of the pumping and the decay processes. The photon field $`\psi `$ in this case becomes a function of frequency in a similar way to an Eliashberg theory of strong coupling superconductors . All the external decoherence processes need to be included in a similar way as presented in this work so that the gap in the density of states is taken into account. The non-equilibrium Keldysh techniques need to be applied to obtain the distribution of particles in the steady state. Thus, using the analogy to superconductivity, we need to include the decoherence processes as in the Abrikosov and Gor’kov theory of gapless superconductivity, the frequency dependent photon field as in an Eliashberg theory of strong coupling superconductor and the flow of the energy through the system in a non-equilibrium state in the same framework. It is not surprising that it is very difficult, if not impossible, to treat such a complex problem within the Green’s functions techniques presented in this work. We think that the more powerful field theoretical methods, like a non-linear sigma model, would be more suitable here. The implementation of this method for our model is still in progress.

##### 4.1.3 Microscopic Details of the Decoherence Processes

If the microscopic origins of the decoherence processes are known for a particular experimentally studied system, the theory could be extended to include this information. The detailed account of the coupling constants and the density of states for the environment can be easily included within this framework. In general the baths propagators in the equations (3.8) and (3.9) would be frequency dependent and thus $`\psi `$ would depend on frequency as in the Eliashberg theory of gapless superconductors . The phenomenological constants $`\gamma _1`$ and $`\gamma _2`$ can thus be, in principle, obtained from this microscopic calculation for a particular system.

##### 4.1.4 Generalisation of the Model

Finally, we can generalise the model itself to account for a different level of disorder and a binding energy of excitons in a material. As we discussed in the Section 1.4.2, the samples are characterised by a different level of fluctuations in the thickness of the quantum well, alloying concentration or presence of impurities. The spatial extent of the excitons also depends on the materials being used and vary from tightly bound, Frenkel-type excitons to weakly bound, extended Wannier excitons. Although in light of recent experiments  \- , the localised exciton picture seems the most relevant the theory could be extended to account for different situations.

In the absence of disorder, when the exciton centre of mass wavefunction would propagate through the sample, the direct Coulomb interactions could be incorporated at a mean-field level in a similar way as in the case of a coherently driven excitonic insulator . As we discussed in the Section 3.1, adding the direct Coulomb interactions between excitons within a mean-field would only give small corrections to the theory presented in this work. At high densities the Coulomb interaction is very small in comparison to the dominant dipole interaction while at low densities the dominant part of the Coulomb interaction is the one between an electron and a hole within the same exciton, which is included in our model. But for qualitative analysis of a particular media this correction could be included.

For materials with Frenkel excitons the theory could be extended to include several localised exciton states on each site rather that just the one assumed in this work. In the case of a narrow disorder quantum well such a generalisation would also be possible in principle but the electronic structure of these systems is not yet well studied and thus quantitative description would be difficult.

#### 4.2 Summary

We have studied the equilibrium Bose condensation of cavity polaritons in the presence of decoherence. We have shown

* That the widely used Langevin equations with the constant, frequency independent decay rates are not valid for systems in which the gap in the density of states is present.
* That in the regime of weak decoherence the decoherence processes have to be treated self-consistently, in a way that the gap in the density of states is taken into account.

We use self-consistent Green’s function techniques, similar to the Abrikosov and Gor’kov theory of gapless superconductivity , to study different regimes in microcavity as the decoherence strength and the excitation density is changed. We have shown

* That at small decoherence the polariton condensate is protected by the energy gap in the excitation spectrum. The gap is proportional to the coherent field amplitude and thus the excitation density, so the condensate is more robust at high densities.
* That this gap gets smaller and eventually is completely suppressed as the decoherence is increased.
* That there is a regime, analogous to the gapless superconductor, when the coherent fields are present without an energy gap. This regime, at very high excitation densities, have all the features of a photon laser.

We study the influence of the two different types of processes, a pair-breaking and a non-pair-breaking ones as well as the inhomogeneous broadening of the energies. We have shown

* That only the type 1, pair-breaking processes can lead to phase transitions.
* That the type 2, non-pair-breaking processes and the inhomogeneous broadening of energies can give only quantitative influence to the behaviour of the system and can not prevent the condensation.

We have

* Studied the phase diagram of the system given by the Hamiltonian (3.1) for different values of the decoherence strength and the excitation densities.
* Established the crossover between an isolated polariton condensate and a photon laser as the decoherence strength is increased.
* Generalised the existing laser theories to include coherence effects in the media and the energy gap in the excitation spectrum.
* Shown that, unlike in the traditional laser, the coherent photon field can be present without a population inversion when the coherence effects in the media are taken into account.