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# Metal induced gap states and Schottky barrier heights at non–reactive GaN/noble metal interfaces

## I Introduction

GaN has certainly been one of the most studied compounds in the last few years, mainly because of both interesting optical properties and remarkable thermal stability, which render this semiconductor particularly suitable for important technological applications. As is well known, however, device performances depend on good metallic contacts and so the study of Schottky barrier heights (SBH) in GaN/metal systems is of great relevance: as an example, the performance of GaN–based laser diodes is still limited by the difficulty in making low resistance ohmic contacts. In this regard, surface reactivity and the presence of interface states are also seen to play a relevant role in Schottky barrier formation.

In a previous work, we investigated the GaN/Al system, which is considered to be a reactive interface due to the Ga–Al exchange reaction driven by AlN formation at the immediate interface; we studied the ideal interface , as well as the effects on the interface properties of some defects (such as atomic swap and GaxAl1-xN intralayers ) at the initial stages of the SBH formation .

In the present work, we report results of ab-initio calculations for GaN/M interfaces (with M = Ag, Au) which are considered to be non–reactive and compare the results (such as metal induced gap states (MIGS) and SBH) with those obtained for GaN/Al, in order to understand the dependence of the relevant electronic properties on the deposited metal. The interest in studying noble metal contacts resides in understanding the effect of the $`d`$ states on the Fermi level position, which has been thought to be relevant in the case of GaAs interfaces . Moreover, we investigate the role of the atomic positions in the interface region in determining the final SBH values: starting from GaN/Al, line–ups differing by as much as 0.80 eV can be produced by changing the interface N-metal interplanar distance from its equilibrium value to that corresponding to the GaN–Ag interface; as a result, the Schottky barrier height is brought to a value very close to that obtained for GaN/Ag. This leads to the conclusion that strain effects, mainly affecting the magnitude of the interface dipole, play a major role in determining the final SBH at the GaN/metal interface.

## II Technical details

The calculations were performed using the all–electron full-potential linearized augmented plane wave (FLAPW)  method within density functional theory in the local density approximation (LDA). We used a basis set of plane waves with wave vector up to $`K_{max}`$ = 3.9 a.u., leading to about 2200 basis functions and for the potential and the charge density we used an angular momentum expansion up to $`l_{max}`$ = 6; tests performed by increasing $`l_{max}`$ up to 8 showed changes in the Schottky barrier height of less than 0.03 eV. The Brillouin zone sampling was performed using 10 special $`k`$–points according to the Monkhorst-Pack scheme . The muffin tin radii, $`R_{MT}`$, for Au and Ag were chosen equal to 2.1 a.u., while for Ga and N we used $`R_{MT}`$ = 1.96 and 1.65 a.u., respectively. We have considered supercells containing 15 GaN layers (8 N and 7 Ga atoms) and 9 metal layers; tests performed on the cell dimensions have shown that bulk conditions are well recovered far from the interface using this 15+9 layer cell size (see discussion below).

## III Structural properties

GaN is well known to show polytypism between the zincblende and the wurtzite phase, so that either one can be easily stabilized; we therefore concentrate on  ordered N–terminated zincblende interfaces in order to avoid the contribution of spontaneous polarization effects inside GaN that might contribute to the Schottky barrier height. Our goal is in fact to investigate the role played by the different metals in determining the position of the Fermi level within the semiconductor band gap. We considered the metal as grown epitaxially on a GaN substrate ($`a_{subs}`$ = $`a_{GaN}=4.482`$ Å). Given the bulk lattice constants of the three metals, $`a_{\mathrm{Al}}=4.05`$ Å, $`a_{\mathrm{Ag}}=4.09`$ Å and $`a_{\mathrm{Au}}=4.08`$ Å, all the metals considered show a quite large mismatch with the GaN substrate, ranging from 8.8 % in the case of fcc–Ag up to 9.6 % in the case of fcc–Al. In all cases, their lattice constants are smaller than that of the substrate, which implies that appreciable bond length relaxations are expected for the metal overlayers. We calculated the most stable structures, assuming pseudomorphic growth conditions and a geometry in which the metal atoms simply replace the Ga atoms on their fcc-sites, using total energy minimization and the ab initio forces calculated on each atomic site to find the equilibrium values of the interface Ga-N, N-M and M-M interplanar distances. In–plane relaxations, as well as the possibility of in-plane reconstruction of the GaN surface, before or during metal deposition, were neglected. In this work, in fact, we are interested mostly in studying the effect of the metal overlayer on the interface GaN/M electronic properties rather than determining the structural configurations that may occur experimentally.

Our structural data are reported in Table I. Due to a refinement  of our previous calculations on the GaN/Al system, the data listed in Table I for this system differ from those already published; the largest change occurs for the Al–Al bulk interplanar distance. For clarity, we report our previous results in parenthesis in this same Table. Let us focus on the structural rearrangement of Al, Ag and Au on the GaN substrate and consider some relevant interplanar distances (i.e. distances between atomic planes along the  growth direction). A comparison between the free-electron-like case of Al and the behavior of noble metals shows that none of the metals considered seems to alter appreciably the bond length at the interface semiconductor layer so that the interplanar distance remains close to its bulk value (1.12 Å); the larger deviation, found in the case of Ag, still gives a reduction of the Ga–N interface distance by less than 5%. A larger difference is found for the interface nitrogen–metal interplanar distance: the N–Al distance is smaller than those corresponding to the Ag and Au structures by about 20 $`\%`$. This can be related to the different bonding at the interface in the different cases - as will be further discussed later on. For both Al and Au we find that the interplanar metal–metal distance, $`d_{int}^{MM}`$, increases compared to the bulk, leading to a bond–length larger than equilibrium just at the interface layer. This effect is far more evident in the case of Al and can be related to a weakening of the $`s`$–type metallic Al–Al bond due to a partial $`sp`$ hybridization of the interface aluminum in the Al–N covalent bond. We find that already in the sub–interface layers the forces are very small, thereby indicating that the metals recover quickly their strained bulk–tetragonal bond–lengths.

In the last column of Table I, we report the interplanar distances calculated according to the macroscopic theory of elasticity (MTE) for the tetragonal metal strained to match the GaN substrate, using the bulk elastic constants  and the equilibrium bond lengths  as input parameters. We recall that in all cases considered, the mismatch is pretty large (about 9%) so that we might be probably out of the range of validity of the MTE. In fact, the discrepancies between the optimized interplanar distances within the bulk regions (namely, $`d_{bulk}^{MM}`$) and those predicted by MTE range between 1% in the case of Au to up to 8% in the Al case. As expected, the bond length distances in the metal bulk side are very similar for all the metals considered, seeing that their equilibrium lattice constants are very close.

## IV MIGS: the noble metal case and comparison with the GaN/Al system

We compare in Fig.1 the atomic site–projected partial density of states (PDOS) for the GaN/Au and GaN/Al interfaces and inner N and M atoms, taking the valence band maximum (VBM) of the inner N PDOS as the zero of the energy scale (vertical arrows denote the position of $`E_F`$). The GaN/Ag PDOS is very similar to that of GaN/Au, and are therefore not shown. In order to demonstrate the presence of the MIGS and the strong effect of the metal deposition on the interface semiconducting atoms, we show as reference the PDOS of the same atoms (N and metal) in the corresponding bulk compounds (i.e. zincblende GaN and bulk metal). The PDOS for the interface N and Au atoms - essentially due to $`p`$ and $`d`$ states, respectively \- (Fig. 1 (c) and (d)) show peaks with a quite high density of states in the GaN band gap energy region (i.e., between 0 and 1.8 eV). We recall here that LDA strongly underestimates the GaN band gap whose experimental value is $`E_{gap}^{expt}`$ = 3.39 eV ); these states are seen to disappear in the inner bulk atom (Fig. 1 (a) and (b)). Therefore, the presence of the metal affects only the semiconductor layers closer to the interface; already in the second layer (not shown) the MIGS decrease appreciably and the DOS gets very close to their bulk shape. Bulk conditions are perfectly recovered in the inner layers (see the practically overlapping lines in Fig. 1 (a) and (e)), showing that the supercell dimensions are sufficient for our purposes. In particular, we notice that the LDA GaN gap is recovered in the PDOS of the inner N atoms.

Apart from the presence of MIGS, the PDOS for both the N and Au interface atoms shows strong differences relative to the bulk, much larger than in the GaN/Al case, where the most relevant difference consists in the general modulation which brings the Al PDOS from the free–electron square–root–like behavior closer to the PDOS of bulk AlN. The reason for this behavior is that in GaN/Au, the Au $`3d`$ states are occupied and interact strongly with the N p states, which are also filled. As a result, the antibonding states rise in energy above the semiconductor VBM and form the peaks at around 1.5 eV, just in proximity to $`E_F`$. Such features are absent in the GaN/Al case (Fig. 1 (g)) and are present in the PDOS of the interface N and Au atoms (Fig. 1 (c)), completely disappearing on atoms far from the junction inside GaN. The presence of a peak at $`E_F`$ might indicate a tendency to an instability, probably leading to in–plane reconstruction with the possible introduction of defects. The spatial location of the charge density corresponding to the peak around $`E_F`$ is shown in Fig.2: these states, which have a clear anti–bonding character between N and Au, are mainly localized in the interface region with a resonant behavior inside the Au region (not shown) and a negligible charge density in the GaN region. A similar situation occurs in the GaN/Ag system (not shown) and was also reported for a  GaAs/Ag interface, whereas it is completely absent in GaN/Al-type structures due to the lack of $`d`$–states in this system.

The overall shape of the interface N PDOS shows a depletion of states in the region from $`4`$ to $`1`$ eV, and a peak around $`5`$ eV, presumably representing the bonding partners of the structures around $`E_F`$ and around the GaN VBM. This corresponds to a degradation of the $`sp^3`$ bonding environment around the interface N. On the basis of this discussion, we can try to give an explanation for the much larger distances $`d_{int}^{NAu}`$ and $`d_{int}^{NAg}`$, compared with the Al case. In fact, the N-Al interface bond is similar to the one in bulk AlN which provides its stability. The N-Au bond, on the other hand, mixes together filled states and pushes towards higher energies the antibonding combinations (with a large anion (N) contribution) around $`E_F`$ (but mostly below it). This is consistent with the smaller amount of charge present inside the interface N atom, to be discussed later. In this scenario, decreasing the N-Au (Ag) distances, would not further stabilize the structure.

In order to investigate the spatial dispersion of the occupied gap states, we show in Fig. 3 the macroscopic  average of the MIGS charge density in GaN/Al (solid line), GaN/Au (dotted line) and GaN/Ag (dot-dashed line). As already pointed out for GaN/Al , the presence of the metal affects almost exclusively the interface semiconductor layer; the MIGS decay exponentially, approaching zero inside the semiconductor. Due to the different density of states distribution of Al and Au (or Ag) for energies close to $`E_F`$ and the consequent different positions of $`E_F`$ with respect to the GaN VBM, the total integrated MIGS charge in the whole cell (metal side included) is larger in the free–electron metal–like case; however, the behavior of these states as a function of the distance from the junction in the three interfaces is overall very similar. Actually, we find from Fig. 3 a very similar behavior, which can be extrapolated with an exponential, leading to the same decay length (see Ref.  for details) for both GaN/Au and GaN/Ag estimated to be $`\lambda `$ = 2.0 $`\pm `$ 0.1 Å., which is close to the value obtained for the GaN/Al system ($`\lambda `$ 1.9 Å ). Therefore, even though the energy dispersion of the MIGS is somewhat different in the free–electron–like and noble metal interfaces (see Fig. 1), they are equally screened in the semiconductor side within 1–2 layers, thus showing that, within a good approximation, $`\lambda `$ is a GaN bulk property.

We plot in Fig. 4 the binding energies of $`1s`$ core levels, with respect to the $`E_F`$ of Ga and N (panels (a) and (b) respectively) and the difference between MT charges in the GaN/M superlattices (SL) and in GaN bulk (Fig.4 (c) and (d) for the Ga and N atoms, respectively) as a function of the distance from the interface. As already discussed in Ref. , it is clear that in the Al case the charge rearrangement at the interface causes a small effect (about 0.15 eV) on the interface N core level and negligible effects on the other semiconductor atoms. On the other hand, in the noble metals case, the interface effect is much stronger: the GaN interface layer shows core level binding energies differing by about 0.4 (0.5) eV for Ag (Au), from the values of the inner bulk-like atoms. Moreover, the core levels bending in going from the bulk towards the interface follows an opposite trend in the noble and free-electron–like metals. This behaviour is consistent with the trend of the valence charge inside atomic spheres: the interface nitrogen atom shows a charge depletion (enhancement) with respect to the bulk atoms in the noble metal (Al) case. As discussed above, the presence of a peak (see Fig.1) in the GaN gap energy region, with antibonding N $`p`$Au $`d`$ character, might be the cause of this charge rearrangement and the resulting chemical shift observed on the core level profiles.

## V Schottky barrier heights

To calculate the values of the SBH, we adopt the usual procedure  which takes core levels as reference energies. In particular, the potential discontinuity can be expressed as the sum of two terms: $`\mathrm{\Phi }_B=\mathrm{\Delta }b+\mathrm{\Delta }E_b`$, where $`\mathrm{\Delta }b`$ and $`\mathrm{\Delta }E_b`$ denote an interface and bulk contribution, respectively. We evaluate $`\mathrm{\Delta }b`$ taking the difference of Ga $`1s`$ and the noble–metal $`1s`$ core levels energies in the superlattice: $`\mathrm{\Delta }b=E_{1s}^{Ga}E_{1s}^{NM}`$. On the other hand, the bulk contribution can be evaluated from separate calculations for bulk GaN and noble–metal and calculating the difference between the binding energies of the same $`1s`$ levels considered above: $`\mathrm{\Delta }E_b=(E_{VBM}^{GaN}E_{1s}^{Ga})(E_F^{NM}E_{1s}^{NM})`$.

The $`p`$ type SBH values obtained, shown in Table II, include a spin–orbit perturbation $`\mathrm{\Delta }_{SO}^{GaN}`$ 0.1 eV, but do not include quasi–particle corrections. Note that, as already pointed out, this refinement in the calculation of the GaN/Al system  gives a $`4\%`$ difference in the N-Al interface distance (which changes the core level alignment at the interface) and a large difference in the tetragonal bulk Al interplanar distance. This last quantity affects the Al core level binding energies used in the evaluation of the final SBH, changing considerably the bulk contribution, essentially related to the absolute deformation potential of the Fermi level in bulk Al. As a result, we obtain a SBH value different from the one previously published  ($`\mathrm{\Phi }_B`$ = 1.12 eV). The values shown in Table II are in good agreement (within 0.1-0.2 eV) with those calculated from the density of states, obtained by considering the SBH as the energy distance between $`E_F`$ (see vertical arrows in Fig. 1) and the top of the valence band of the PDOS corresponding to the inner semiconductor layer inside the bulk region of the superlattice (the energy zero in Fig.1).

We note that the SBH values in the noble–metal case are lower than the SBH in the GaN/Al interface ($`\mathrm{\Phi }_{B_p}(GaN/Al)`$ = 1.51 eV). To better understand this result, we should consider that the Al and noble metal interfaces differ in two main aspects: (i) different chemical species of the metal overlayer and (ii) different structural properties, $`i.e.`$ different bond lengths at the interface that comprise, in all respects, an interfacial strain contribution. In particular, from inspection of Table I it is evident that the Ag and Au structures show very similar $`d_{int}^{NM}`$ and $`d_{int}^{MM}`$ interplanar distances, which are at variance with those with Al. In order to separate the chemical from the strain contribution, we evaluate the SBH for three different structures that can be regarded as intermediate steps necessary to bring the GaN/Al structure to match perfectly the GaN/Ag one. We show in Table III the interface interplanar distances and final SBH values for the equilibrium GaN/Al and GaN/Ag systems and for the three intermediate interfaces. In the first structure (Step I), the interplanar $`d_{int}^{NM}`$ distance of the GaN/Al SL is taken equal to that minimized for the GaN/Ag SL ($`d_{int}^{NM}`$ = 1.32 Å) : the SBH is reduced from 1.5 eV to 0.76 eV (this surprising result will be discussed in detail later on).

As a second step (Step II), we change $`d_{int}^{MM}`$ to recover that calculated for the GaN/Ag structure: $`d_{int}^{MM}`$ = 1.60 Å. The SBH is remarkably less sensitive to this parameter, giving only a 0.04 eV change in the potential barrier which brings the SBH to about 0.80 eV. This is expected since the metal efficiently screens out the perturbation generated by atomic displacements: actually, the dynamical effective charge, related to the dipole induced by a unit displacement of atoms, is zero inside a metal.

In the third structure (Step III), the Ga-N interface distance is brought to its value in the GaN/Ag superlattice, $`d_{int}^{GaN}`$ = 1.07 Å, and we have a system where Al atoms perfectly replace Ag in GaN/Ag. Although this last structural change is very small (about 4 $`\%`$), this interplanar distance turns out to be very important for the final potential line–up, due to the incomplete screening in the semiconductor side and the large N effective charge. As a result, the SBH changes appreciably ($`\mathrm{\Phi }_B`$ = 0.71 eV). This final result is quite close (within 0.2 eV) to the value found for the real GaN/Ag interface, showing that apparently the interface strain plays a more important role than the bare chemical contribution.

Perhaps the most surprising result of our tests is the very strong dependence of the SBH on the interface N–Al distance, whose variation represents the larger contribution to the difference between GaN/Al and GaN/Ag (Au) SBHs. Test calculations have shown an almost perfect linear behaviour of $`\mathrm{\Phi }_B`$ against $`d_{int}^{NAl}`$, leading to an Al effective charge $`Z_L^{}=0.08`$, ($`Z_L^{}=Z_T^{}/ϵ_{\mathrm{}}`$, where $`Z_T^{}`$ is the Born dynamical charge and $`ϵ_{\mathrm{}}`$ is the electronic static dielectric constant). This result is in sharp contrast with the case of GaAs/Al , where no significant changes were found for small elongations of the As-metal interface distance, therefore resulting in $`Z_L^{}`$ 0 - an almost perfect metallic behavior. As a further test, we performed calculations on GaAs/Al, similar to those of Ruini et al., confirming their results both in terms of the SBH values, and of their behavior as a function of $`d_{int}^{AsAl}`$.

A possible explanation of the striking difference between the GaN/Al and GaAs/Al systems can be provided by an analysis of the relevant physical parameters involved. The MIGS decay length is larger for GaAs/Al ($`\lambda _{GaN}`$ 2 Å and $`\lambda _{GaAs}`$ 3 Å), therefore providing a more extended region with metallic behavior inside the semiconductor; in addition, the density of states at the Fermi level, $`N(E_F)`$, is larger for GaAs/Al (see Fig 5), giving rise to a smaller (by a factor of $`1.5`$) Thomas-Fermi screening length $`\lambda _{TF}`$ in this system. Still, the values of the MIGS decay length and of $`N(E_F)`$ are not very different between GaAs and GaN, so that it is not at all obvious to expect such a behavior of the SBH in the two compounds.

To understand these results, we can use elementary electrostatics arguments. If we make a few rough assumptions such as a simple Yukawa–like screened potential and consider a metallic behavior inside the semiconductor up to distances of the order of $`\lambda `$, the MIGS decay length, we find that the potential difference across the metal/semiconductor junction induced by displacements of the Al interface atom scales with the factor $`e^{k_{TF}\lambda }`$. If we now estimate the values of the Thomas–Fermi screening lengths, $`k_{TF}`$, using the GaN/Al and GaAs/Al superlattice value of $`N(E_F)`$, we are led to the conclusion that a unit displacement of the interface Al atoms produces a potential change across the interface which is roughly 7 times larger in GaN/Al than in GaAs/Al. Considering the crudeness of this model, such an estimate is in satisfactory agreement with the first–principles results, which indicate a factor of $`10`$ for the same ratio. In other words, GaAs screens out almost perfectly all the structural changes in the interface region (namely, displacements of the interface Al atoms), while the same is not true for GaN.

In order to further investigate the effects of the $`d_{int}^{NM}`$ change, we compare the core levels and MT charges for the equilibrium GaN/Al interface and the Step I system. Recall that these systems are exactly equal, except for the difference in the interface nitrogen–metal distance: $`d_{int}^{NM}`$ = 1.11 Å and $`d_{int}^{NM}`$ = 1.32 Å, for the equilibrium and Step I structures, respectively. As in Fig. 4, we show in Fig. 6 the trends for the core level binding energies (panels (a) and (b) for Ga and N atoms, respectively) and the difference between the MT charges compared to their values in the bulk compounds (panels (c) and (d) for Ga and N atoms, respectively), as a function of the atomic distance from the interface. In terms of core levels and charge transfer within the MT, a comparison with Fig. 4 shows that the Step I system behaves very closely the GaN/Ag structure but very differently from the equilibrium GaN/Al interface. Therefore, the electronic charge distribution around the interface N and Al atoms has a strong dependence on the interplanar distance and is able to reduce the SBH by as much as 0.75 eV, bringing a GaN/Al Step I SBH within only 0.16 eV from the GaN/Ag SBH.

The dispersion of the SBH values seems to exclude a Fermi level pinning in the GaN case, as experimentally confirmed by the large spread of values reported in the literature for the SBH between GaN and different metals. In particular, let us recall those obtained for $`n`$-GaN/Ag and $`n`$-GaN/Au: $`\mathrm{\Phi }_{B_p}^{expt}(nGaN/Ag)`$ = 2.7 eV  and $`\mathrm{\Phi }_{B_p}^{expt}(nGaN/Au)`$ 2.4 eV  and 2.2 eV . On the other hand, recent photoemission measurements  performed for Au deposited on $`p`$-type GaN show that the Fermi level is stabilized around 1 eV above the $`p`$-GaN VBM, in apparent good agreement with our calculated value ($`\mathrm{\Phi }_B`$ = 1.08 eV). The disagreement between some of these values and our calculated ones are certainly related to the different conditions of the GaN surface (which is ideal in our calculations and subject to different preparations in the experimental case); moreover, we considered the GaN zincblende structure and  oriented interfaces, whereas all the experimental samples are grown on  wurtzite GaN.

We note finally that the spread of experimental values for GaN/metal interfaces has not been found for the GaAs/metal systems, where a Fermi level pinning was experimentally observed . This can be understood in terms of the much more efficient screening provided by GaAs with respect to GaN, as discussed above. In fact, the main difference between the noble metal and Al systems is the length of the anion–metal bond which gives rise to large variations of the interface dipole: this electrostatic contribution is poorly screened in GaN and therefore contributes considerably to the final SBH value. In addition, it has to be observed that GaAs matches better (within 2$`\%`$) the Au, Ag and Al lattice constants so that the interface strain does not play a crucial role in this case.

## VI Conclusions

We have performed FLAPW calculations for  ordered GaN/Ag and GaN/Au interfaces, mainly focusing on the electronic properties and comparing our results with those obtained from previous calculations for the GaN/Al interface. Our calculations show that there is an appreciable density of MIGS in the noble metal interfaces considered (even higher than in the GaN/Al case); however, the presence of the gap states is relevant in the interface layer only, being strongly reduced already in the sub–interface layer. We estimate the MIGS decay length to be $`\lambda `$ 2.0 Å, for all the metals considered (Al, Ag and Au). The SBH values ($`\mathrm{\Phi }_{B_p}(GaN/Ag)`$ = 0.87 eV and $`\mathrm{\Phi }_{B_p}(GaN/Au)`$ = 1.08 eV) are significantly smaller than the value obtained in the GaN/Al case ($`\mathrm{\Phi }_{B_p}(GaN/Al)`$ = 1.51 eV); we demonstrated that the appreciable SBH reduction in going from the free–electron to the noble–metal case is mostly due to structural effects. In particular, the distance between the last N and the first metal layer plays a critical role in dictating the final SBH value, in contrast with that found in GaAs/Al, where previous , as well as our present, calculations showed negligible effects of this same structural parameter. We found that the largest structural differences between the various GaN/M interfaces considered are related to this distance, mainly determined by the different bonding nature between N and free–electron–like or noble metals. Finally, we were able to show, at least for our perfectly ordered abrupt interfaces, that the lack of Fermi level pinning in GaN can be understood in terms of electrostatic effects related to variations of the interface anion–metal dipole: these effects are not properly screened in GaN, so that they contribute considerably to the final potential line–up at the interface.

## VII ACKNOWLEDGEMENTS

We gratefully acknowledge useful discussions with Prof. R. Resta and Dr. A. Ruini. Work in L’Aquila and Cagliari supported by grants of computer time at the CINECA supercomputing center (Bologna, Italy) through the Istituto Nazionale di Fisica della Materia (INFM). Work at Northwestern University was supported by the U.S. National Science Foundation through the Northwestern Materials Research Center.


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# The Polytropic Equation of State of Interstellar Gas Clouds

## 1 Introduction

A fundamental problem in the theory of star formation is the physical structure of molecular gas clouds, such as dense cores and Bok globules, from which (low-mass) stars are formed. Early work on the thermal and chemical balance of interstellar clouds has been performed by de Jong, Dalgarno & Boland (1980) and Falgarone & Puget (1985). A framework for active regions such as Orion has been developed by Tielens & Hollenbach (1985). The above work has been extended and refined by many authors (see Hollenbach & Tielens 1999 for a review), driven to a large extent by recent advances in observational techniques.

Examples of such observational progress include the catalog of 248 optically selected Bok globules of Clemens & Barvainis (1988), the NH3 survey of isolated cores in Taurus by Benson & Myers (1989, and references therein), the measurement of non-thermal line widths in regions surrounding ammonia cores (Fuller & Myers 1992, Goodman et al. 1998), and the use of spectroscopy of various atoms and molecules as temperature and density diagnostics of different types of interstellar clouds as summarized in van Dishoeck (1997).

Despite this wealth of observational data, the nature of their equation of state (EOS) remains a major theoretical problem that concerns the stability and collapse of these molecular clouds The stiffness of the EOS can be largely responsible for the resulting density probability function of interstellar gas in the turbulent ISM (Scalo et al. (1998) and Passot & Vazquez-Semadeni 1998). In particular, the value of gamma affects the densities that can be attained behind shocks (Vazquez-Semadeni, Passot & Pouquet 1996), the fraction of gas driven to high densities by turbulent interactions (c.f. Scalo et al. 1998), and the stability of clouds being overrun by shocks (e.g. Tohline, Bodenheimer & Christodoulou 1987; Foster & Boss 1996). In the present paper we concentrate on the effects of the EOS for the fragmentation of individual collapsing clouds. Before embarking on an analysis of the EOS of interstellar gas clouds, say of the form $`P=P(\rho ,T_\mathrm{g},T_\mathrm{d},V,B,I,C)`$ for pressure $`P`$, density $`\rho `$, gas temperatures $`T_\mathrm{g}`$, dust temperature $`T_\mathrm{d}`$, velocity $`V`$, magnetic field $`B`$, radiation intensity $`I`$, and chemical composition $`C`$, one should assess which of the possible physical quantities entering the EOS dominates in the parameter ranges under study.

The importance of $`\rho `$ and $`T_\mathrm{g}`$ is self-explanatory. The presence of warm dust can play a role since it can heat the gas through gas-grain coupling and radiatively through optically thick molecular lines (Takahashi, Hollenbach & Silk 1983). The velocity field, even when it does not contribute to the turbulent pressure, strongly influences the optical depth of atomic and molecular cooling lines, and hence the thermal balance of the medium. The magnetic field plays an important role in the support of interstellar gas (McKee 1999). The presence of ultraviolet or other hard radiation sources strongly influences the chemical, thermal and ionization balance of the ambient medium, and hence the overall EOS. Finally, the chemical composition of the gas also depends on the metallicity since it is the abundance of atoms and molecules which influences the local cooling rate.

In the present work, a polytropic equation of state, $`P=K\rho ^\gamma `$, is assumed to describe the physical state of the gas. The exponent $`\gamma `$ is considered to be a function $`\gamma (T_\mathrm{g},T_\mathrm{d},V,I,C)`$. That is, the magnetic pressure is assumed to be not dominant in the support of the model cloud. The radiation field $`I`$, in addition to the radiation emitted by the dust grains, is assumed to be given by the cosmic ray ionization rate. In other words, the visual extinction of the model cloud is assumed to be sufficient to shield the gas from any ultraviolet (stellar) sources.

We note that $`\gamma `$ is the logarithmic derivative of $`P`$ with respect to $`\rho `$. That is, since $`P\rho T`$ it follows that $`\gamma =1+\frac{d\mathrm{log}T}{d\mathrm{log}\rho }`$. Through implicit differentiation the above derivative is related to the logarithmic derivatives of the heating and cooling functions, which can be quite complex. It is this dependence of $`\gamma `$ on the details of heating and cooling that is the main topic of the present paper.

In the remainder of the paper, a useful guide is the density dependence of the heating and cooling rate. If the density dependence of the heating rate is steeper (shallower) than that of the cooling rate, then $`\gamma `$ is larger (smaller) than unity. A similar result holds for the kinetic temperature. Here, the cosmic ray ionization rate is always linear in the density and independent of temperature, whereas gas-grain heating and cooling is quadratic in the density and proportional to $`T_\mathrm{g}^{1/2}(T_\mathrm{g}T_\mathrm{d})`$. Optically thin, subthermally excited cooling lines have a quadratic density dependence which becomes linear in the thermalized (high density) limit and even effectively sub-linear when radiative trapping (optical depth effects) becomes important. Finally, collisional de-excitation rates are characterized by powers of the temperature on the order of $`0.51.5`$, whereas excitation rates are modified by an exponential factor which is of the order of unity for kinetic temperatures larger than the pertaining excitation temperatures.

In general, our results are applicable mostly to dense and/or well shielded molecular clouds/cores where the pressure appears to be close to thermal, with only a small additional contribution to the line-widths from turbulent motions, and the ionization fraction is small (Goodman et al. 1998, and references therein). That is, we assume that the clouds are outside the regime where the so-called Larson (1981) laws apply, which indicate an increase in the non-thermal line width with length scale.

One should note that polytropic models can also be extended into the regime where there is a significant contribution to the pressure from turbulence and magnetic fields. The polytropic temperature $`T`$ should then be interpreted as representing the total velocity dispersion $`\sigma `$, i.e., $`T\sigma ^2`$ (Maloney 1988). A complete description of polytropic models, including composite ones for non-thermal pressure effects and bulk properties like mass, radius and density contrast, is presented in Curry & McKee (1999). The aim here is to study the thermal regime and to investigate the specific effects of metallicity, radiative transfer and internal sources on the stiffness of the resulting local EOS.

## 2 Model Description

The results presented here were obtained by application of the numerical code of Spaans (1996), described in detail in Spaans & Norman (1997); Spaans & van Dishoeck (1997); and Spaans & Carollo (1998). The interested reader is referred to these papers for a description of the underlying algorithm. The code has been specifically designed to solve large chemical networks with a self-consistent treatment of the thermal balance for all heating and cooling processes known to be of importance, and to be computable with some sense of rigor, in the interstellar medium (Spaans & Ehrenfreund 1999). Care has to be taken in the treatment of line trapping for the atomic and molecular cooling lines which dominate the thermal balance. Collisional de-excitation and radiative trapping is most prominent in the density range $`10^310^4`$ cm-3 (Scalo et al. 1998). Our result were found to be in good agreement with those of Neufeld et al. (1995) for their, and our, adopted linear velocity gradient model (see further details below).

The adopted chemical network is based on the UMIST compillation (Millar, Farquhar & Willacy 1997) and is well suited for low temperature dense molecular clouds, with the latest rates for the important neutral-neutral reactions. The radiative transfer is solved by means of a Monte Carlo approach (Spaans & van Langevelde 1992) with checks provided by an escape probability method for large line optical depths. The thermal balance includes heating by cosmic rays, absorption of infrared photons by H2O molecules and their subsequent collisional de-excitation, and gas-grain heating. The cooling includes the coupling between gas and dust grains (Hollenbach & McKee 1989), atomic lines of all metals, molecular lines, and all major isotopes, as described in Spaans & Norman (1997) and Spaans et al. (1994), and also in Neufeld, Lepp & Melnick (1995) for the regime of very large line optical depth. All level populations are computed in statistical equilibrium at a relative accuracy, also imposed on the ambient line radiation field, of no less than $`10^3`$. The combined chemical and thermal balance is required to obey a convergence criterion between successive iterations of 0.5%.

For the low metallicity computations, the relative contributions to the total cooling by H2 and HD can become significant. Since the value of $`\gamma `$ depends on the logarithmic derivative of the cooling rate with respect to temperature and density, the end result could become quite sensitive to the (quantum mechanical) treatment of H-H2, H2-H2 and He-H2 collional processes.

The main differences between calculations of H-H2 and H2-H2 collisions are due to different potentials (surfaces) and whether reactive collisions, i.e., the exchange of an H atom, are included (important above 1000 K). The shape of the potential surface is quite important for the lower temperatures, where rotational quantum effects dominate. This situation has improved greatly over recent years (c.f. Forrey et al. 1997). Nevertheless, we have restricted our calculations to $`Z0.01`$ Z. In this regime, there are other atomic and molecular coolants which still contribute, at the 30% level, diminishing the relative importance of the aforementioned sensitivities.

As an additional check, we have performed runs with the recent le Bourlot et al. (1999) H2 rates. We have found no significant changes in $`\gamma `$ for our adopted metallicities. Finally, for zero metallicity gas, and in the absence of HD cooling, we found (albeit tentatively given the above caveats) that $`\gamma `$ is always less than unity. The inclusion of HD restricts this result to densities less than $`10^5`$ cm-3.

## 3 The Initial Mass Function

Before discussing the results of our computations, we want to outline how the value of $`\gamma `$ could related to the process of star formation, i.e., how a large value of $`\gamma `$ might suppress the formation of stars.

The polytropic equation of state of interstellar gas clouds may be relevant to determinations of stellar masses. Our starting point is to pose the question: is there a characteristic stellar mass? Observationally, the answer appears to be positive. The IMF, $`dN/dMm^{1x}`$, for the number $`N`$ of stars per unit of mass $`M`$, has $`x>1`$ above $`1\mathrm{M}_{}.`$ Below $`0.3\mathrm{M}_{}`$, virtually all data suggests a flattening to $`1\stackrel{<}{}x\stackrel{<}{}0.`$ The critical value that defines a characteristic mass is $`x1`$ for a logarithmic divergence in total mass toward decreasing mass, and there is no doubt that there is a transition from $`x>1`$ to $`x<1`$ in the range $`0.21\mathrm{M}_{}`$. Hence there is a characteristic stellar mass. Whether this varies with environment is uncertain, but $`m_{\mathrm{char}}0.3\mathrm{M}_{}`$ fits most data (cf. Scalo 1998).

The status of theoretical discussions of a critical mass often centers on the thermal Jeans mass, $`m_\mathrm{J}T^{3/2}\rho ^{1/2}`$, generalized to include external pressure, $`m_{\mathrm{J},\mathrm{P}}T^2P^{1/2}`$, turbulence $`m_{\mathrm{J},\mathrm{t}}\mathrm{\Delta }V^4P^{1/2}`$, or magnetic flux support $`m_{\mathrm{J},\mathrm{B}}B^3\rho ^1`$ (c.f. Elmegreen 1999, Larson 1998). The generalized Jeans scale most likely applies to the masses of atomic and molecular clouds or to self-gravitating clumps. However, the fact that in the interstellar medium, the Jeans mass in diffuse atomic or molecular clouds generally exceeds stellar masses by a large factor, apart from the very coldest clumps, argues that the physics of the IMF is more complicated than Jeans instability. The Jeans mass is a fragmentation scale according to linear theory, and three-dimensional simulations indeed find that clump masses are described by the Jeans scale. Nevertheless, simulations cannot currently resolve the scales of individual protostars on solar mass scales. Analytic arguments, on the contrary, of opacity-limited fragmentation find scales of $`0.01\mathrm{M}_{}`$, or far less than the characteristic stellar mass scale.

All of this seems to suggest that the Jeans mass is not very relevant to the IMF, not withstanding the Elmegreen (1999) and Larson (1998) results. If it were, of course, the critical polytropic index for fragmentation to occur is 4/3. This has the following significance: one can write $`m_\mathrm{J}\rho ^{(3/2)(\gamma 4/3)}`$. As collapse occurs, smaller and smaller masses fragment, and one plausibly ends up with a powerlaw IMF only if $`\gamma <4/3`$. This argument could apply to the clump mass function within molecular clouds. The physics of nonlinear fragmentation is complicated, and this is at least a necessary condition for a power law IMF to continue to very small mass scales (compared to the initial Jeans mass).

But what really determines stellar masses? Physical processes that must play a role in determining the characteristic stellar mass scale include clump coagulation (Allen & Bastien 1995), clump interactions (Klessen, Burkert & Bate 1998) and protostellar outflows (Nakano, Hasegawa & Norman 1995; Silk 1995) that halt accretion. One conjecture is that feedback from protostars plays a crucial role in limiting accretion. The latter depends crucially on the accretion rate to protostellar cores (various authors relate inflow to outflow rates on energetic grounds), which in turn depends sensitively on the turbulent velocity. The maximum embedded young stellar object luminosity correlates with NH3 core line width $`\mathrm{\Delta }V`$ (Myers & Fuller 1993) and clump mass (Kawamura et al. 1998) over a wide range. Myers & Fuller (1993) concluded that variations in the initial velocity dispersion from core to core is a key determinant of the stellar mass formed from such a core. Also, Fuller & Myers (1992) concluded that the physical basis of line width-size relations (the so-called Larson laws) is part of the initial conditions for star formation. The theoretical justification incorporates disk physics and, at least conceptually, magnetic fields (Adams & Fatuzzo 1996; Silk 1995). So if the above holds (theoretically and observationally, both aspects are relevant), then one might argue that the characteristic mass of a young stellar object depends primarily on $`\mathrm{\Delta }V`$. The latter is determined by the kinetic temperature if the thermal line width dominates in a prestellar core. This situation holds for low mass star formation but less so for the high mass cores, where the nonthermal contribution to the line width (i.e. turbulent or magnetic) can be as large as 50-80% (c.f. Myers & Fuller 1993). In any case, $`\gamma =1`$ appears the most natural critical value of interest.

If $`\gamma =1`$ is indeed a critical value in this sense, there is the possibility that the primordial EOS with a stiffer polytropic index, $`\gamma >1`$, leads to a peaked IMF, i.e. one biased toward massive stars, whereas current star formation, where the molecular gas is characterised by an EOS with $`\gamma <1`$, results in runaway fragmentation and hence a power law IMF.

## 4 Results

The model results333Extensive tables can be obtained from MS. are obtained for self-gravitating, quiescent spherical clouds with total column densities per unit of velocity given by

$$N^{\mathrm{SIS}}(\mathrm{H}_2)=5.1\times 10^{19}n(\mathrm{H}_2)^{1/2}\mathrm{cm}^2\mathrm{per}\mathrm{km}\mathrm{s}^1,$$
$`(1)`$
(the singular isothermal sphere value; Neufeld et al. 1995) to set the optical depth parameter for any species, total hydrogen densities $`n_\mathrm{H}=10^210^6`$ cm-3, metallicities $`Z=10.01Z_{}`$ in solar units, and a possible homogeneous background infrared radiation (IR) field given by 100 K dust grains. The total visual extinction through the region containing the model cloud is fixed at $`A_\mathrm{V}=100`$ mag, although this is only important for determining the dust emission optical depth in the IR background case. Models are also constructed for a constant velocity gradient field of 3 km s-1 pc-1, which is a factor of three larger than the value adopted in Goldsmith & Langer (1978), corresponding to an optical depth parameter of

$$N^{\mathrm{VG}}(\mathrm{H}_2)=1.0\times 10^{18}n(\mathrm{H}_2)\mathrm{cm}^2\mathrm{per}\mathrm{km}\mathrm{s}^1.$$
$`(2)`$
It has been shown by Neufeld & Kaufman (1993) that this choice violates the virial theorem in the limit of high density. Therefore, (1) is interpreted to apply to a (statistically) static cloud supported by thermal pressure, whereas (2) should be seen as representative of a dynamic medium in a state of infall or outflow. The cosmic ray ionization rate is taken equal to $`\zeta _{\mathrm{CR}}=3\times 10^{17}`$ s-1.

### 4.1 Variations in $`\gamma `$: Competition between Heating and Cooling Processes

Figures 1 and 2 present results which do not include an IR background radiation field, e.g. little or no ongoing star formation, or a warm CMB. Figure 1 displays the results for a quiescent velocity field with a velocity dispersion of $`\mathrm{\Delta }V=0.3`$ km s-1 for H2. Figure 2 is for the corresponding case of a velocity gradient of 3 km s-1 pc-1. The value of $`\gamma `$ becomes of the order of unity for low metallicities, $`Z<0.03Z_{}`$, and densities $`n_\mathrm{H}<10^5`$ cm-3. The reason is that the cooling of the ambient medium becomes dominated by H2 and HD (Norman & Spaans 1997), which emit optically thin line radiation. At low densities, the level populations are not thermalized and the cooling rate has a density dependence which is steeper than linear and typically quadratic, whereas the cosmic ray heating rate is linear in the density.

At higher densities gas-grain cooling becomes important. This has a quadratic density dependence, and the equation of state softens in the absence of any embedded sources (Scalo et al. 1998), but to a lesser extent due to the lower dust abundance, for small metallicities. Even though no computations were performed beyond densities of $`3\times 10^6`$ cm-3, the gas-grain coupling at very large densities is so strong that the gas temperature follows the grain temperature and the value of $`\gamma `$ will increase again and attain a value of unity if embedded protostars are present and the ambient radiation field is not coupled to the local gas density (see below).

The high $`\gamma `$ region between $`10^3`$ and $`10^4`$ cm-3 is the result of line trapping and collisional de-excitation. Line trapping causes the cooling rate to depend on the density with an effective power less than unity due to absorption and subsequent collisional de-excitation, while the cosmic ray heating rate is always linear in the density, independent of the kinetic temperature. It should be emphasized that the effect of radiative trapping is stronger for the quiescent velocity field, but also depends crucially on the specific implementation that we have chosen. A truly turbulent velocity field (Kegel, Piehler & Albrecht 1993), i.e. one with a finite correlation length, may lead to a quite different value of $`\gamma `$ in the density range $`10^310^4`$ cm-3.

### 4.2 High Redshift Star formation

As can be seen in Figure 3, the inclusion of an IR background leads to a much stiffer polytropic equation of state for high, $`Z>0.1Z_{}`$, metallicities. The reason is that the abundant presence of water leads to heating through absorption of IR radiation and subsequent collisional de-excitation (Takahashi et al. 1983) for densities between $`3\times 10^3`$ and $`3\times 10^4`$ cm-3. Temperature effects play a role here in the determination of the line opacities, but this is essentially a heating term that is between linear and quadratic in the ambient density. Since this heating rate is roughly proportional to the abundance of H2O, it is negligible for metallicities $`Z<0.1Z_{}`$. At very high densities, $`n_\mathrm{H}>3\times 10^6`$ cm-3, the gas and dust become completely coupled, and $`\gamma `$ approaches unity since the gas temperature will simply follow the dust temperature. This only follows provided that the strength of the IR radiation field is independent of the ambient density. This point will re-addressed in the next subsection on starburst galaxies.

Note also that $`\gamma `$ decreases to unity from above for densities larger than $`10^5`$ cm-3 because of the high temperature of the FIR background. This causes the dust to heat the gas and results in a relatively stiff EOS, even for low metallicities where H2 and HD dominate. This is because at these high densities the overall cooling rates are at their thermodynamic limit, roughly linear in the density, while the dust-gas heating rate goes like the square of the density. Note that for $`T<200`$ K, HD quickly becomes the dominant coolant of pristine gas. The lower equilibrium temperature of the gas facilitates the thermalization of the level populations. Finally, for densities larger than $`3\times 10^5`$ cm-3 radiative trapping becomes important for HD, leading to a density dependence of its cooling rate of less than unity.

Even though no results are shown for intermediate (30-60 K) temperature dust backgrounds, $`\gamma `$ first decreases to somewhat below unity around $`10^5`$ cm-3 in these cases, if the metallicity is less than 0.1 Z. It then approaches unity from below for the reasons given above. Finally, in the limit of a large velocity gradient, H2O plays a minor role and its heating (or cooling) does not strongly influence the thermal balance of the gas (Takahashi et al. 1983).

Since an IR background is naturally present in the form of the CMB for redshifts larger than $`z1030`$, one can speculate on the nature of very early star formation. That is, any dense shielded region which has been enriched by metals through the first supernova explosions, viewed here as the product of the very first population III stars, will become more stable in the presence of an intense CMB background. Conversely, metal-poor regions will retain a polytropic exponent of $`1`$. Therefore, high redshift star formation may exhibit the counter-intuitive property that metal enrichment and a warm CMB together “halt” the process of star formation for a metallicity $`Z_\mathrm{c}>0.1Z_{}`$, even though the gas is intrinsically capable of cooling efficiently (Spaans & Norman 1997).

Once the CMB temperature drops below $`40`$ K, at $`z15`$, any dense, $`n_\mathrm{H}>10^4`$ cm-3, cloud of high or even modest metallicity rapidly develops a $`\gamma `$-value smaller than unity and is prone to collapse. In effect, although more detailed calculations are required to substantiate this, the CMB may play an integral part in determing the epoch of efficient early star formation. One also sees that the primordial IMF can change strongly as one goes from a $`\gamma >1`$ to a $`\gamma <1`$ EOS. In the former regime one expects only large density excursions to collapse, leading to an IMF biased toward massive stars.

### 4.3 Starburst Galaxies

A similar phenomenon can occur in luminous (IR) starburst galaxies in that warm, $`50200`$ K, opaque dust hardens the polytropic equation of state of a nuclear starburst region. The system Arp 220 is a possible example, being optically thick at 100 $`\mu `$m. From the results presented here, one concludes that such IR luminous opaque systems have an IMF which is quite shallow, favoring high mass star formation. This may in fact be desirable to maintain the required power of such galaxies through supernova explosions (c.f. Doane & Mathews 1993).

Note though that in these extreme systems there is a strong coupling between the ambient radiation field and the star formation rate $`R`$, and hence with the gas density. Typical Schmidt star formation laws adopt an observationally motivated value of $`12`$ for the dependence of $`R`$ on gas density (Kennicutt 1998) in star-forming spiral galaxies, with a best fit value of $`r=1.4`$. Since the resulting dust temperature depends on the $`1/5`$ power of the ultraviolet energy density (Tielens & Hollenbach 1985), the effective $`\gamma `$ for $`r=2`$ ($`r=1`$) is 1.4 (1.2), consistent with the above results.

## 5 Discussion

The polytropic equation of state of interstellar gas clouds has been computed for a range of physical parameters, and its relation to the IMF, high redshift star formation, and starburst galaxies has been investigated. A much needed extension of the results presented here lies in MHD, and particularly turbulence. The magnetic and velocity fields are important for pressure support away from the most centrally condensed part of a molecular cloud core, and radiative transfer effects in a turbulent medium are non-trivial. More to the point, the polytropic EOS indices computed here, with their relevance to the IMF as discussed in Section 4, are to be applied to a medium with a given cloud density probability distribution, as investigated in Scalo et al. (1998). Such a cloud density probability distribution can only be derived from detailed hydrodynamic simulations which include magnetic pressure and Coriolis forces. Furthermore, $`\gamma `$ can also affect, in a way still to be investigated, star formation and the underlying IMF in other scenarios like turbulence-induced condensation or shocked-cloud induced star formation. We would like to mention as well the work by Ogino, Tomisaka & Nakamura (1999) that shows that the mass accretion rate in their polytropic simulations of collapsing clouds depends a lot on whether gamma is taken as 0.8 or 1.2.

Extensions in terms of multiple polytropic models for the core and envelope of a molecular cloud, such as discussed in Curry & McKee (1999), are another avenue to explore for the bulk properties of interstellar clouds. Caveats in the approach presented here are grain mantle evaporation which can influence the abundance of H2O and hence the heating rate in the presence of an IR background, uncertainties in the chemical reaction rates of neutral-neutral reactions at low temperatures, and details of the freeze-out onto grains of molecular species. We hope that through a synthesis of the approach adopted here and those of others mentioned above, one can address the question of cloud stability and collapse in a more general (cosmological) framework.

We are grateful to the referee, John Scalo, for his constructive comments, which improved the presentation of this paper, and his emphasis on the computation of the zero metallicity case. Discussions with Ewine van Dishoeck and John Black on the collisional cross sections of H2 are also gratefully acknowledged. MS is supported by NASA through grant HF-01101.01-97A, awarded by the Space Telescope Institute, which is operated by the Association of Universities for Research in Astronomy, Inc., for NASA under contract NAS 5-26555. J.S. has been supported in part by grants from NSF and NASA at UC Berkeley.


text:
# Prospects for photon blockade in four level systems in the N configuration with more than one atom.

## I Introduction

Recent work by Imamoğlu et al suggested a promising scheme for observing photon blockade in a highly non-linear cavity, where the change in the Kerr nonlinearity due to single photon effects was enough to make the cavity non-resonant with modes of more than one photon. As described in their work, such a device could work as a single-photon turnstile, similar to that realised recently by Kim et al  in a semiconductor junction, which might be useful for quantum computation and the generation of non-classical light fields. The work by Imamoğlu et al was based on the use of the adiabatic elimination procedure and later studies showed that the breakdown of the procedure in the high dispersion limit leads to prohibitive restrictions on the parameter space where photon blockade could be observed in a multi-atom system. Further to this, Werner and Imamoğlu and Rebić et al suggested that these problems could be overcome by using a system with a single atom. The question of observing photon blockade in multi-atom systems is of more than just theoretical interest. Possible schemes for observing photon blockade depend on directing a low flux atomic beam through a high finesse cavity and this implies that there will be an uncertainty in the number of atoms present in the cavity at any given time. We show that the photon blockade, in certain circumstances, remains strong even for a fluctuation in the atom number. Recent work has highlighted the importance of employing a mutual detuning between the cavity and the semiclassical coupling field to shift the many atom degenerate state out of resonance. Our work builds on this idea and presents a detailed atom-cavity dressed state calculation showing the parameter regimes which offer the best prospects for the observations of photon blockade in one, two and three atom systems. We show that current technology should allow the construction of a system exhibiting photon blockade. We suggest that photon blockade can be best realised, not in a MOT as originally envisaged by Imamoğlu et al, but by sending a low atom current beam through a cavity of the style realised by Hood et al  and Münstermann et al.

Photon blockade in a cavity can be explained quite simply. An external field drives a cavity that is resonant when there are zero or one photon in the cavity and non-resonant for two (or more) photons. This can be achieved by introducing a medium into the cavity, exhibiting a large Kerr non-linearity which alters the refractive index as a function of the intensity. In general, one would expect to find large non-linearities in systems exhibiting electromagnetically induced transparency .

## II Dressed states of the atom-cavity system

Consider a four level atom as depicted in figure 1. The energy levels are labeled in order of increasing energy as $`|a`$, $`|b`$, $`|c`$ and $`|d`$ with associated energies of $`\mathrm{}\omega _a`$, $`\mathrm{}\omega _b`$, $`\mathrm{}\omega _c`$ and $`\mathrm{}\omega _d`$ respectively and transition frequencies $`\omega _{\alpha \beta }=\omega _\alpha \omega _\beta `$ where $`\alpha ,\beta =a,b,c,d`$. The $`|b|c`$ transition is driven by a strong classical coupling field, with frequency $`\omega _{\text{class}}`$, Rabi frequency $`\mathrm{\Omega }`$ , detuned from the $`|b|c`$ transition by an amount $`\delta _{cb}=\omega _{\text{class}}\omega _{cb}`$. The atoms are in a cavity with resonance frequency $`\omega _{\text{cav}}`$ which is detuned from the $`|a|c`$ transition by an amount $`\delta _{ca}=\omega _{\text{cav}}\omega _{ca}`$, detuned from the $`|b|d`$ transition by an amount $`\mathrm{\Delta }=\omega _{\text{cav}}\omega _{db}`$ and not interacting with the $`|b|c`$ transition. The detunings $`\delta _{cb}`$ and $`\delta _{ca}`$ are set equal to ensure that the $`|a|b`$ transition is driven by a two photon resonance. We therefore define the mutual detuning, $`\delta =\delta _{cb}=\delta _{ca}`$. The cavity is driven by an additional classical field with frequency $`\omega _e=\omega _{\text{cav}}`$ and power, $`P`$. We analyse the effect of this field by examining the dressed states of the atom-cavity system. This configuration of fields and atomic levels is called the N configuration and has been considered previously . The cavity linewidth is $`\mathrm{\Gamma }_{\text{cav}}`$. The atom-cavity mode coupling is $`g_{\alpha _1\alpha _2}=\left(\omega _{\alpha _1\alpha _2}/2\mathrm{}ϵ_0V_{\text{cav}}\right)^{1/2}\mu _{\alpha _1\alpha _2}`$ where $`\alpha _1`$ and $`\alpha _2`$ correspond to atomic levels, $`\mu _{\alpha _1\alpha _2}`$ is the electric dipole moment of the transition, $`V_{\text{cav}}`$ is the cavity volume and $`ϵ_0`$ is the permittivity of free space. The Hamiltonian for the system with $`N`$ atoms in the frame rotating at the cavity resonance frequency in the rotating-wave approximation is

$`{\displaystyle \frac{\widehat{}}{\mathrm{}}}`$ $`=`$ $`i\stackrel{~}{\mathrm{\Gamma }}_c{\displaystyle \underset{j=1}{\overset{N}{}}}\widehat{\sigma }_{cc}^ji\stackrel{~}{\mathrm{\Gamma }}_d{\displaystyle \underset{j=1}{\overset{N}{}}}\widehat{\sigma }_{dd}^j+{\displaystyle \underset{j=1}{\overset{N}{}}}\mathrm{\Omega }\left(\widehat{\sigma }_{cb}^j+\widehat{\sigma }_{bc}^j\right)`$ (2)
$`+{\displaystyle \underset{j=1}{\overset{N}{}}}g_{ac}\left(\widehat{a}\widehat{\sigma }_{ca}^j+\widehat{a}^{}\widehat{\sigma }_{ac}^j\right)+{\displaystyle \underset{j=1}{\overset{N}{}}}g_{bd}\left(\widehat{a}\widehat{\sigma }_{db}^j+\widehat{a}^{}\widehat{\sigma }_{bd}^j\right)i\mathrm{\Gamma }_{\text{cav}}\widehat{a}^{}\widehat{a}.`$
where $`\stackrel{~}{\mathrm{\Gamma }}_c=\mathrm{\Gamma }_c+i\delta `$, $`\stackrel{~}{\mathrm{\Gamma }}_d=\mathrm{\Gamma }_d+i\mathrm{\Delta }`$, $`\mathrm{\Gamma }_\alpha `$ is the decay rate from atomic state $`|\alpha `$, $`\widehat{a}`$ $`\left(\widehat{a}^{}\right)`$ is the cavity photon annihilation (creation) operator and $`\widehat{\sigma }_{\alpha _1\alpha _2}^j`$ is the atomic operator $`|\alpha _1\alpha _2|`$ acting on atom $`j`$.

We find the dressed states by diagonalizing $`\widehat{}`$. Fortunately, $`\widehat{}`$ is block diagonal in the bare state basis. The $`n`$th block can be identified by starting with the state $`|a,a,\mathrm{},n`$, representing all the atoms in state $`|a`$ and the cavity field in the $`n`$ photon state $`|n`$, and finding the closed set of states coupled to $`|a,a,\mathrm{},n`$ by $`\widehat{}`$. Diagonalizing this block gives the $`n`$ quanta manifold of dressed states.

We first consider the case of a single atom in the cavity. The zero quanta manifold consists solely of the state $`|a,0`$. The one quantum manifold is spanned by the states $`|a,1`$, $`|b,0`$ and $`|c,0.`$ The corresponding block of $`\widehat{}/\mathrm{}`$ can be written in matrix form in this basis as

$$\frac{_1^{\left(1\right)}}{\mathrm{}}=\left[\begin{array}{ccc}i\mathrm{\Gamma }_{\text{cav}}& 0& g_{ac}\\ 0& 0& \mathrm{\Omega }\\ g_{ac}& \mathrm{\Omega }& i\stackrel{~}{\mathrm{\Gamma }}_c\end{array}\right]$$
(3)
where the superscript on $``$ refers to the number of atoms and the subscript to the number of quanta in the system. In order to simplify the expressions for eigenvalues and eigenvectors, we assume $`\mathrm{\Gamma }_{\text{cav}}=0`$. The figures which follow, however, have been generated using non-zero values of $`\mathrm{\Gamma }_{\text{cav}}`$. Diagonalising the matrix $`_1^{\left(1\right)}/\mathrm{}`$ with $`\mathrm{\Gamma }_{\text{cav}}=0`$ gives the dressed state energies

$`_+`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c+\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\left(\mathrm{\Omega }^2+g_{ac}^2\right)}\right)/2`$
$`_0`$ $`=`$ $`0`$
$`_{}`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\left(\mathrm{\Omega }^2+g_{ac}^2\right)}\right)/2`$
and corresponding dressed states $`|D_+`$, $`|D_0`$ and $`|D_{}`$ respectively. In this form, the real part of the eigenstate corresponds to the state energy and the imaginary part to the width of the state. These eigenstates form the well known Mollow triplet  and are presented in figure 2(a) as a function of the scaled mutual detuning, $`\delta /\mathrm{\Omega }`$, with $`\mathrm{\Gamma }_c/\mathrm{\Omega }=0.1`$, $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=0.01`$ and $`g_{ac}/\mathrm{\Omega }=1`$. It is important to express the form of the central dressed state, $`|D_0`$ which is

$`|D_0={\displaystyle \frac{\mathrm{\Omega }}{\sqrt{\mathrm{\Omega }^2+g_{ac}^2}}}|a,1{\displaystyle \frac{g_{ac}}{\sqrt{\mathrm{\Omega }^2+g_{ac}^2}}}|b,0.`$

Photon blockade will occur in this dressed-state picture when the cavity driving field resonantly couples the zero to one quantum manifolds, and only weakly couples the one and two quanta manifolds. We can gauge the extent of these couplings by treating each transition driven by the cavity driving field as a separate, closed two-state system. This approach will break down when multiple states are excited simultaneously. However, in situtations where the photon blockade effect occurs, the number of dressed states that are significantly occupied will be minimal and our two-state model should give a reasonably accurate picture of the degree of excitation of each transition.

The effect of the cavity driving field on the cavity-atom system can be treated by including the additional term on the right hand side of equation 2

$`\mathrm{}\beta (\widehat{a}+\widehat{a}^{})`$where $`\beta =\sqrt{P\mathrm{\Gamma }_{\text{cav}}T^2/\left(4\mathrm{}\omega _{\text{cav}}\right)}`$ is the external field-cavity mode coupling strength for a cavity mirror transmittance of $`T`$. In our two state model the cavity driving field drives transitions between lower and upper states, $`|L`$ and $`|U`$, in the $`n`$ and $`n+1`$ quanta manifolds respectively. The effective Rabi frequency of the transition is given by

$`\mathrm{\Omega }_e=\left|\beta L\left|\widehat{a}\right|U\right|.`$Under these conditions, the steady state population of $`|U`$ is given by

$`\rho _{\text{exc}}={\displaystyle \frac{\mathrm{\Omega }_e^2}{2\mathrm{\Omega }_e^2+\mathrm{\Delta }_e^2+\mathrm{\Gamma }_U^2}}`$where $`\mathrm{\Delta }_e`$ is the detuning of the external cavity driving field from the $`|L|U`$ transition and $`\mathrm{\Gamma }_U`$ the decay rate of state $`|U`$, assumed to take population from $`|U`$ to $`|L`$. Note that we have ignored the decay rate from $`|L`$. We denote the maximum value of $`\rho _{\text{exc}}`$ over all transitions from a given lower state to all possible upper states in the $`n`$ quantum manifold as $`\rho _{\text{exc}}^{\left(n\right)}`$. For ideal photon blockade, we require $`\rho _{\text{exc}}^{\left(1\right)}0.5`$ for the transition from the ground state, $`|L=|a,a,\mathrm{},0=|G_0`$ to the maximally coupled one quantum dressed state $`|G_1`$. For the case that $`|G_1=|D_0`$, we note that $`\mathrm{\Gamma }_U`$ will be small, because $`|D_0`$ contains no proportion of atomic state $`|c`$. Thus it is possible to inject a single quantum of energy into the atom-cavity system for modest values of $`\beta `$. Ideal blockade also requires that $`\rho _{\text{exc}}^{\left(2\right)}`$ be negligible for transitions between $`|L=|G_1`$ and states $`|U`$ of the two quantum manifold.

We next consider the two atom, one quantum manifold of states. In this case, the basis states are $`|a,a,1`$, $`|a,b,0`$, $`|a,c,0`$, $`|b,a,0`$ and $`|c,a,0`$ and the corresponding block of $`\widehat{}/\mathrm{}`$ can be written in matrix form as

$$\frac{_1^{\left(2\right)}}{\mathrm{}}=\left[\begin{array}{ccccc}i\mathrm{\Gamma }_{\text{cav}}& 0& g_{ac}& 0& g_{ac}\\ 0& 0& \mathrm{\Omega }& 0& 0\\ g_{ac}& \mathrm{\Omega }& i\stackrel{~}{\mathrm{\Gamma }}_c& 0& 0\\ 0& 0& 0& 0& \mathrm{\Omega }\\ g_{ac}& 0& 0& \mathrm{\Omega }& i\stackrel{~}{\mathrm{\Gamma }}_c\end{array}\right]$$
(4)
Diagonalising $`_1^{\left(2\right)}/\mathrm{}`$ yields the eigenvalues

$`_{+2}`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c+\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\left(\mathrm{\Omega }^2+2g_{ac}^2\right)}\right)/2`$
$`_{+1}`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c+\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\mathrm{\Omega }^2}\right)/2`$
$`_0`$ $`=`$ $`0`$
$`_1`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\mathrm{\Omega }^2}\right)/2`$
$`_2`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\left(\mathrm{\Omega }^2+2g_{ac}^2\right)}\right)/2`$
with associated dressed states $`|D_{+2}`$, $`|D_{+1}`$, $`|D_0`$, $`|D_1`$ and $`|D_2`$. The dressed state energies are plotted in figure 2(b) for the same conditions as in figure 2(a). There are some important similarities between the spectrum of eigenstates for the one atom and two atom cases. In each case there is a state with zero energy, indicating that transitions from the zero to the one quantum manifold are possible for a cavity driving field tuned to the cavity resonance $`\omega _{\text{cav}}`$. The states which are anti-crossing in each manifold are asymptotic to the lines$`/\mathrm{\Omega }=0`$ and $`/\mathrm{\Omega }=\delta /\mathrm{\Omega }`$ with the point of closest approach being at $`\delta /\mathrm{\Omega }=0`$. It is also important to realise that although there are five distinct eigenstates only three of these eigenvalues will couple to the ground state of the atom cavity system, i.e. the matrix element $`a,0\left|\widehat{a}\right|D_N`$ is non-zero only for $`N=0`$, $`\pm 2`$. For this reason only the optically active states $`|D_{+2}`$, $`|D_0`$ and $`|D_2`$ are plotted in figure 2(b).

We have also solved the analogous three and four atom Hamiltonians and we summarise our results for the eigenstates in each case as

$`_{+2}`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c+\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\left(\mathrm{\Omega }^2+Ng_{ac}^2\right)}\right)/2`$ (5)
$`_{+1}`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c+\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\mathrm{\Omega }^2}\right)/2`$ (6)
$`_0`$ $`=`$ $`0`$ (7)
$`_1`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\mathrm{\Omega }^2}\right)/2`$ (8)
$`_2`$ $`=`$ $`\left(i\stackrel{~}{\mathrm{\Gamma }}_c\sqrt{\stackrel{~}{\mathrm{\Gamma }}_c^2+4\left(\mathrm{\Omega }^2+Ng_{ac}^2\right)}\right)/2`$ (9)
where $`N=1,2,3,4`$ indicates the number of atoms in the cavity. The degeneracies of the eigenvalues presented in equations 9 are interesting to observe, namely the $`_{+2}`$, $`_0`$ and $`_2`$ values are all non-degenerate, whilst the $`_{+1}`$ and $`_1`$ values are $`\left(N1\right)`$ fold degenerate. (The latter values, $`_{+1}`$ and $`_1`$ do not occur for $`N=1`$). The presence of the zero eigenvalue, $`_0`$, indicates that it is possible to inject one photon into the atom-cavity system with a cavity driving field tuned to $`\omega _{\text{cav}}`$.

Now we consider the two quanta manifold for a cavity containing one atom. This manifold is spanned by the states $`|a,2`$, $`|b,1`$, $`|c,1`$ and $`|d,0`$ and the corresponding block of $`\widehat{}/\mathrm{}`$ in matrix form is

$`{\displaystyle \frac{_2^{\left(1\right)}}{\mathrm{}}}=\left[\begin{array}{cccc}2i\mathrm{\Gamma }_{\text{cav}}& 0& \sqrt{2}g_{ac}& 0\\ 0& i\mathrm{\Gamma }_{\text{cav}}& \mathrm{\Omega }& g_{bd}\\ \sqrt{2}g_{ac}& \mathrm{\Omega }& i\left(\mathrm{\Gamma }_{\text{cav}}+\stackrel{~}{\mathrm{\Gamma }}_c\right)& 0\\ 0& g_{bd}& 0& i\stackrel{~}{\mathrm{\Gamma }}_d\end{array}\right]`$In order to observe photon blockade in such a system, it is essential that none of the eigenstates of $`_2^{\left(1\right)}/\mathrm{}`$ are resonantly coupled by the cavity driving field to the occupied states of the one quantum manifold. To achieve this, we require $`\rho _{\text{exc}}^{\left(2\right)}0.5`$, the smaller $`\rho _{\text{exc}}^{\left(2\right)}`$ the greater the degree of photon blockade. A plot showing the eigenenergies of this system with associated linewidths, $`\mathrm{\Gamma }_x`$ where $`x`$ is the dressed state under consideration, is presented in figures 3(a) and 3(b). In each case $`\mathrm{\Delta }/\mathrm{\Omega }=2`$, $`\mathrm{\Gamma }_c/\mathrm{\Omega }=\mathrm{\Gamma }_d/\mathrm{\Omega }=0.1`$, $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=0.01,`$ $`g_{ac}/\mathrm{\Omega }=1`$ and in figure 3(a) $`g_{bd}/\mathrm{\Omega }=1`$ and the energies are plotted as a function of $`\delta /\mathrm{\Omega },`$ whereas in figure 3(b) $`\delta /\mathrm{\Omega }=0`$ and the energies are plotted as a function of $`g_{bd}/\mathrm{\Omega }`$. The important features to recognise from these two traces is the shift of the smallest magnitude energy state from zero, indicating (as highlighted in  and ) that photon blockade will indeed be possible in the one atom case.

Similarly, for the two atom case, the basis states of the two quanta manifold are $`|a,a,2,`$ $`|a,b,1`$, $`|a,c,1`$, $`|b,a,1`$, $`|c,a,1`$, $`|a,d,0`$, $`|b,b,0`$, $`|b,c,0`$, $`|c,b,0`$, $`|c,c,0`$,and $`|d,a,0`$ where the notation is $`|\text{atom 1, atom 2, cavity field}`$. In matrix form, the corresponding block of the Hamiltonian is

$`{\displaystyle \frac{_2^{\left(2\right)}}{\mathrm{}}}=\left[\begin{array}{ccccccccccc}2i\mathrm{\Gamma }_{\text{cav}}& 0& \sqrt{2}g_{ac}& 0& \sqrt{2}g_{ac}& 0& 0& 0& 0& 0& 0\\ 0& i\mathrm{\Gamma }_{\text{cav}}& \mathrm{\Omega }& 0& 0& g_{bd}& 0& 0& g_{ac}& 0& 0\\ \sqrt{2}g_{ac}& \mathrm{\Omega }& i\mathrm{\Gamma }_t& 0& 0& 0& 0& 0& 0& g_{ac}& 0\\ 0& 0& 0& i\mathrm{\Gamma }_{\text{cav}}& \mathrm{\Omega }& 0& 0& g_{ac}& 0& 0& g_{bd}\\ \sqrt{2}g_{ac}& 0& 0& \mathrm{\Omega }& i\mathrm{\Gamma }_t& 0& 0& 0& 0& g_{ac}& 0\\ 0& g_{bd}& 0& 0& 0& i\stackrel{~}{\mathrm{\Gamma }}_d& 0& 0& 0& 0& 0\\ 0& 0& 0& 0& 0& 0& 0& \mathrm{\Omega }& \mathrm{\Omega }& 0& 0\\ 0& 0& 0& g_{ac}& 0& 0& \mathrm{\Omega }& i\stackrel{~}{\mathrm{\Gamma }}_c& 0& \mathrm{\Omega }& 0\\ 0& g_{ac}& 0& 0& 0& 0& \mathrm{\Omega }& 0& i\stackrel{~}{\mathrm{\Gamma }}_c& \mathrm{\Omega }& 0\\ 0& 0& g_{ac}& 0& g_{ac}& 0& 0& \mathrm{\Omega }& \mathrm{\Omega }& i\mathrm{\Gamma }_t& 0\\ 0& 0& 0& g_{bd}& 0& 0& 0& 0& 0& 0& i\stackrel{~}{\mathrm{\Gamma }}_d\end{array}\right]`$where $`\mathrm{\Gamma }_t=\mathrm{\Gamma }_{\text{cav}}+\stackrel{~}{\mathrm{\Gamma }}_c`$.

The energy eigenvalues of $`_2^{\left(2\right)}/\mathrm{}`$ are presented in figures 4(a) and 4(b). As in the two atom, single quantum case there are optically inactive states, and these have been removed from the figures. Figure 4(a) was generated for $`\mathrm{\Delta }/\mathrm{\Omega }=2`$, $`\delta /\mathrm{\Omega }=0`$, $`\mathrm{\Gamma }_c/\mathrm{\Omega }=\mathrm{\Gamma }_d/\mathrm{\Omega }=0.1`$, $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=0.01`$ and $`g_{ac}/\mathrm{\Omega }=1`$. As can be seen, for this case there is a zero eigenvalue so we would expect that there would be resonant coupling from the single quantum manifold to the two quantum manifold by a cavity driving field tuned to $`\omega _{\text{cav}}`$ and hence, photon blockade would not be observed in this case. However in figure 4(b) we illustrate the effect of introducing a small mutual detuning, $`\delta ,`$ from state $`|c`$. The parameters used were $`\mathrm{\Delta }/\mathrm{\Omega }=2`$, $`\delta /\mathrm{\Omega }=0.5`$, $`\mathrm{\Gamma }_c/\mathrm{\Omega }=\mathrm{\Gamma }_d/\mathrm{\Omega }=0.1`$, $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=0.01`$ and $`g_{ac}/\mathrm{\Omega }=1`$. It is important to observe the shift of the smallest magnitude eigenvalue from zero. Although this shift is less than for the corresponding single atom case, it is still feasible to consider building a cavity to observe this photon blockade. This point will be elaborated on in the conclusions.

## III Photon blockade in a realistic system

Of critical importance to the experimental observation of photon blockade in atomic systems, is the question of how to trap single or small numbers of atoms within a small, high finesse optical cavity. We know of no demonstration of continuous trapping, however recent experiments conducted by Hood et al and Münstermann et al have shown that it is possible to have a cavity with extremely low atom fluxes passing through it. This was achieved in  by allowing atoms to fall from a leaky MOT into the cavity and in  by directing atoms out of a MOT and into the cavity. One would expect such atomic ejections to be stochastic in nature and as a consequence, the probability of having a certain number of atoms in the cavity should follow Poissonian statistics. In order to build a device which uses photon blockade, it will therefore be necessary to ensure that significant photon blockade will be observed over as wide a range of atomic numbers as possible, otherwise the photon blockade could be lost and the performance of the device degraded.

A complication in the experimental realisation of photon blockade is that the parameters chosen in the theoretical plots shown above were assumed to be independent variables. In general this will not be the case unless great care is taken in the preparation of an experiment. Specifically, for transitions in an alkali vapour which might realise the N configuration, one would expect the dipole moments of all relevant transitions to be of the same order, with the atom-cavity coupling set solely by the cavity volume, a parameter shared by both the $`|a|c`$ and $`|b|d`$ transitions. One would therefore expect $`g_{ac}g_{bd}=g`$. Also, because of the shared cavity, the detuning parameters are not independent, so if we assume that $`\omega _{ca}\omega _{db}=\delta _\omega `$ then we find that $`\mathrm{\Delta }=\delta +\delta _\omega `$. These extra considerations will be included in the analysis to follow, which concentrates on experimentally realisable effects rather than the general theoretical demonstration presented above. We start by investigating photon blockade using the parameters $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=0.01`$, $`\mathrm{\Gamma }_c/\mathrm{\Omega }=\mathrm{\Gamma }_d/\mathrm{\Omega }=0.1`$, $`\delta _w/\mathrm{\Omega }=0`$ and $`\beta /\mathrm{\Omega }=1`$. For these values $`\rho _{\text{exc}}^{\left(1\right)}0.5`$, as is expected due to the presence of the strongly absorbing state at the cavity resonance.

In figure 5 (a) we show a pseudo-colour plot of $`\rho _{\text{exc}}^{\left(2\right)}`$ as a function of $`\delta /\mathrm{\Omega }`$ and $`g/\mathrm{\Omega }`$ for the one atom two quanta case, where colour is indicative of the value of $`\rho _{\text{exc}}^{\left(2\right)}`$, blue being 0 and red being 0.5. The graph clearly shows $`\rho _{\text{exc}}^{\left(2\right)}`$ decreasing monotonically with $`g/\mathrm{\Omega }`$, indicating the effectiveness of photon blockade correspondingly increasing. This is expected, as a large $`g`$ will give rise to a highly nonlinear system. Also note that $`\rho _{\text{exc}}^{\left(2\right)}`$ increases as $`\left|\delta /\mathrm{\Omega }\right|`$ increases, indicating that the photon blockade is a resonance phenomenon.

In figure 5(b) we show the analogous $`\rho _{\text{exc}}^{\left(2\right)}`$ plot for two atoms. In accord with the preliminary results which suggested that photon blockade was not possible in the multi-atom system we find $`\rho _{\text{exc}}^{\left(2\right)}0.5`$ in the vicinity of $`\delta /\mathrm{\Omega }=0`$, implying that photon blockade will not be observable for these choices of parameters. However, by increasing the mutual detuning and employing a modest atom-cavity coupling, regions of strong photon blockade are observable, typified by the minimum recorded value on figure 5(b) of $`\rho _{\text{exc}}^{\left(2\right)}=0.0087`$.

The three atom case is shown in figure 5(c) for the same parameter regime as the one and two atom cases. The form of $`\rho _{\text{exc}}^{\left(2\right)}`$ is similar to that of the two atom case, with the same overall structure, but narrower regions where photon blockade should be observable, this is shown by the smaller blue region of figure 5(c) than figure 5(b). Again very low values of $`\rho _{\text{exc}}^{\left(2\right)}`$ were obtained, with a minimum recorded value of $`\rho _{\text{exc}}^{\left(2\right)}=0.0070`$.

To use photon blockade as a tool for new quantum devices it is necessary to identify real systems in which these effects may be observed. As an example of what may be achieved with the current state of the art, we take parameters from a recent experimental paper  and make some minor assumptions about how they might apply to atoms falling through a high finesse cavity. It should certainly be possible to achieve a coupling field Rabi frequency of $`\mathrm{\Omega }=10`$ MHz, external field-cavity coupling strength of $`\beta =1`$MHz and Hood et al achieve $`g=120`$ MHz and $`\mathrm{\Gamma }_{\text{cav}}=40`$ MHz. For a system based on transitions in the <sup>87</sup>Rb D<sub>2</sub> line  we may assume $`\delta _\omega =6600`$MHz and $`\mathrm{\Gamma }_c=\mathrm{\Gamma }_d=17.8`$ MHz. We ignore the Zeeman magnetic sublevels since these form a simple, effective three level $`\mathrm{\Lambda }`$ system (for states $`|a`$, $`|b`$ and $`|c`$) for the situation under consideration . Assuming equal rates of radiative decay, these translate into our system as $`g/\mathrm{\Omega }=12`$, $`\mathrm{\Gamma }_c/\mathrm{\Omega }=\mathrm{\Gamma }_d/\mathrm{\Omega }=1.78`$, $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=4`$, $`\delta _\omega /\mathrm{\Omega }=660`$ and $`\beta /\mathrm{\Omega }=0.3`$. In figure 6(a) we present a plot of $`\rho _{\text{exc}}^{\left(1\right)}`$ as a function of $`g/\mathrm{\Omega }`$ and $`\delta /\mathrm{\Omega }`$ for one atom in the cavity, with the plots showing $`\rho _{\text{exc}}^{\left(2\right)}`$ in (b) and (c) for one and two atoms respectively.

There are some important features to note in figures 6. In 6(a) $`\rho _{\text{exc}}^{\left(1\right)}`$ increases monotonically with $`g/\mathrm{\Omega }`$ and, for the scale used, is independant of $`\delta /\mathrm{\Omega }`$. The value of $`\rho _{\text{exc}}^{\left(1\right)}`$ is qualitatively very similar for one, two and three atoms, with the values of $`\rho _{\text{exc}}^{\left(1\right)}`$ slightly increasing as the number of atoms increases. As an example, for $`g/\mathrm{\Omega }=12`$, $`\rho _{\text{exc}}^{\left(1\right)}=0.3099`$, $`0.3824`$ and $`0.4148`$ for one, two and three atoms respectively. Traces 6(b) and (c) show $`\rho _{\text{exc}}^{\left(2\right)}`$ for the one and two atom cases respectively. The value of $`\rho _{\text{exc}}^{\left(2\right)}`$ for the one atom case is very small across the entire parameter space, indicating that photon blockade should be easy to observe for a single atom. Of interest is the resonance in the vicinity of $`\delta =\delta _w`$ which will be discussed below. There is an extra resonance in the vicinity of $`\delta =0`$ for the one atom case, although this is not present to the same extent in the two and three atom cases. For two atoms, and also for three atoms (not shown), the overall values (away from the resonances) of $`\rho _{\text{exc}}^{\left(2\right)}`$ appear to increase with the number of atoms and are much larger than for the one atom case. Qualitatively, $`\rho _{\text{exc}}^{\left(2\right)}`$ for two and three atoms are extremely similar, with maximum values along the line $`g/\mathrm{\Omega }=12`$ of $`\rho _{\text{exc}}^{\left(2\right)}=0.2244`$ and $`0.3092`$ for two and three atoms respectively. These observations would appear to agree with the intuitive idea that photon blockade would be more difficult in multi-atom systems and that there is a qualitative difference between the single atom case and multi-atom cases.

The results for $`\rho _{\text{exc}}^{\left(2\right)}`$ in the vicinity of $`\delta /\mathrm{\Omega }=660`$ are shown in figure 7. The significance of this region is that we have $`\delta =\delta _w`$ so that the cavity is now resonant with the $`|b|d`$ transition. To our knowledge, this situation has not been previously explored and the consequences it has for photon blockade are significant. In figure 7 we present $`\rho _{\text{exc}}^{\left(2\right)}`$ for one, two and three atoms in plots (a), (b) and (c) respectively. The behaviour of $`\rho _{\text{exc}}^{\left(1\right)}`$ shows no resonance phenomena and is described above, it is only by considering $`\rho _{\text{exc}}^{\left(2\right)}`$ that the resonance is observed. In 7(a) we see generally small values for $`\rho _{\text{exc}}^{\left(2\right)}`$ indicating that photon blockade should be observable. With the exception of the ‘shelf’ for $`g/\mathrm{\Omega }1`$, $`\rho _{\text{exc}}^{\left(2\right)}`$ has the a similar chevron shape to that observed in the ideal case, shown in figure 5(a), although with very much smaller values. In figures 7(b) and (c), we observe a roughly triangular region of low $`\rho _{\text{exc}}^{\left(2\right)}`$, superimposed on the background of $`\rho _{\text{exc}}^{\left(2\right)}`$ noted earlier. Values of $`\rho _{\text{exc}}^{\left(2\right)}<0.01`$ are present where $`\rho _{\text{exc}}^{\left(1\right)}>0.35`$ for both the two and three atom cases. This suggests that the non-linearity of the system is very large about this resonance. Further investigations of this resonance will be done with increasing number of atoms to show how robust the photon blockade will be as any relaxation of the requirement for low number of atoms will enhance the prospects for experimental verification of this effect.

## IV Photon blockade with an off resonant cavity

The discussions above have used a system where the cavity is driven resonantly by the external field. This has a significant drawback in trying to realise a continuously operating device inasmuch as when there are no atoms in the cavity, the cavity will absorb photons from the external field. To overcome this using the on-resonance configuration, one must run the experiment in a pulsed mode to ensure that there are no photons in the cavity prior to atoms entering the cavity. There is, however, another alternative. This occurs when the cavity driving field is not tuned to the cavity resonance, but instead is tuned to a side resonance of the one atom dressed system. In this case there will be strong coupling between the external driving field and the cavity when there is one atom in the cavity and no coupling when there are zero atoms in the cavity. By studying the form of the dressed state eigenvalues given in equation 9 it is clear that there is a dependence of the eigenvalue with the number of atoms so that it should be possible to choose $`g_{ac}`$ such that the one-quantum manifold is only coupled into when there is only one atom in the cavity. These conditions are best met for the case that both $`\delta `$ and $`\mathrm{\Omega }`$ are small compared to $`g_{ac}`$ to ensure the maximum shift in eigenvalues with number of atoms.

## V Conclusions

We have presented detailed calculations which show the parameter space where photon blockade in one, two and three atom systems should be observable. By considering transitions on the <sup>87</sup>Rb D<sub>2</sub> line, we have suggested that photon blockade should be observable using current state of the art technology, such as has been recently demonstrated .

We have pointed out that strong photon blockade should be possible when the cavity resonance is tuned to the $`|b|d`$ transition, despite a large mutual detuning, $`\delta `$. This resonance may relax the requirements on the energy levels of the atomic species under consideration.

We gratefully acknowledge financial support from the EPSRC and useful discussions with Ole Steuernagel (University of Hertfordshire), Derek Richards (The Open University), Danny Segal and Almut Beige (Imperial College).

## VI Figures

Figure 1: Energy level diagram for the four level N system. The atoms are labelled in order of increasing energy as $`|a`$, $`|b`$, $`|c`$, and $`|d`$ with energies $`\mathrm{}\omega _a`$, $`\mathrm{}\omega _b`$, $`\mathrm{}\omega _c`$ and $`\mathrm{}\omega _d`$ respectively. A strong classical coupling field with frequency $`\omega _{\text{class}}`$ and Rabi frequency $`\mathrm{\Omega }`$ is applied to the $`|b|c`$ transition and detuned from it by an amount $`\delta =\omega _{cb}\omega _{\text{class}}`$. The atoms are placed in a cavity with resonance frequency $`\omega _{\text{cav}}`$ which is detuned from the $`|a|c`$ transition by $`\delta `$ and from the $`|b|d`$ transition by $`\mathrm{\Delta }=\omega _{db}\omega _{\text{cav}}`$. The cavity is driven resonantly by an external classical driving field with external field-cavity coupling strength $`\beta `$ and frequency $`\omega _{\text{cav}}`$.

Figure 2: Eigenvalues of the one quantum manifold as a function of the scaled mutual detuning $`\delta /\mathrm{\Omega }`$ for one and two atoms in the cavity. In each case the parameters used were $`g_{ac}/\mathrm{\Omega }=1`$, $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=0.01`$ and $`\mathrm{\Gamma }_c/\mathrm{\Omega }=0.1`$. In figure 2(a) the spectrum for a single atom interacting with a single cavity photon traces out the well known Mollow triplet. In figure 2(b) we present the analogous trace for two atoms instead of one where the optically inactive dressed states, $`|D_{+1}`$ and $`|D_1`$ have been removed.

Figure 3: Eigenvalues of the two quanta manifold for a single atom. Parameters used were the same as those in figure 2, but with the addition of $`\mathrm{\Gamma }_d/\mathrm{\Omega }=0.1`$ and $`\mathrm{\Delta }/\mathrm{\Omega }=2`$. Figure 3(a) has $`g_{bd}/\mathrm{\Omega }=1`$ and the energy eigenvalues are plotted as a function of scaled mutual detuning, whilst figure 3(b) has $`\delta /\mathrm{\Omega }=0`$ and the energy eigenvalues are plotted as a function of $`g_{bd}/\mathrm{\Omega }`$.

Figure 4: Eigenvalues of the two quanta manifold for two atoms in the cavity with the parameters $`\mathrm{\Delta }/\mathrm{\Omega }=2`$, $`\mathrm{\Gamma }_c/\mathrm{\Omega }=\mathrm{\Gamma }_d/\mathrm{\Omega }=0.1`$, $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=0.01`$ and $`g_{ac}/\mathrm{\Omega }=1`$, as a function of $`g_{bd}/\mathrm{\Omega }`$. In 4(a) the mutual detuning $`\delta /\mathrm{\Omega }=0`$ and no photon blockade is observed, in 4(b) a small mutual detuning of $`\delta /\mathrm{\Omega }=0.5`$ is applied and the photon blockade is restored for a cavity driving field tuned to $`\omega _{\text{cav}}`$. Note that the optically inactive states have been removed in these traces also.

Figure 5: $`\rho _{\text{exc}}^{\left(2\right)}`$ plotted as a function of scaled detuning $`\left(\delta /\mathrm{\Omega }\right)`$ and scaled coupling $`\left(g/\mathrm{\Omega }\right)`$ for one atom (a), two atoms (b) and three atoms (c). The colour of the plot shows the value of $`\rho _{\text{exc}}^{\left(2\right)}`$ with blue being zero, red 0.5. The parameters chosen for these figures were $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=0.01`$, $`\mathrm{\Gamma }_c/\mathrm{\Omega }=\mathrm{\Gamma }_d/\mathrm{\Omega }=0.1`$, $`\delta _w/\mathrm{\Omega }=0`$ and $`\beta /\mathrm{\Omega }=1`$. Note that over this paramter range, $`\rho _{\text{exc}}^{\left(1\right)}=0.5`$.

Figure 6: Pseudo-colour plots of $`\rho _{\text{exc}}^{\left(1\right)}`$ and $`\rho _{\text{exc}}^{\left(2\right)}`$. The parameters chosen were those which could be expected in a realistic experiment involving <sup>87</sup>Rb atoms. These parameters were $`\mathrm{\Gamma }_c/\mathrm{\Omega }=\mathrm{\Gamma }_d/\mathrm{\Omega }=1.78`$, $`\mathrm{\Gamma }_{\text{cav}}/\mathrm{\Omega }=4`$, $`\delta _\omega /\mathrm{\Omega }=660`$ and $`\beta /\mathrm{\Omega }=0.3`$. Figure (a) corresponds to $`\rho _{\text{exc}}^{\left(1\right)}`$ for one atom, whilst (b) and (c) correspond to $`\rho _{\text{exc}}^{\left(2\right)}`$ for one and two atoms respectively. Note that the colour scales for each figure vary according to the maximum values of $`\rho _{\text{exc}}`$.

Figure 7: Pseudo-colour plots of $`\rho _{\text{exc}}^{\left(2\right)}`$ in the vicinity of the resonance $`\delta =\delta _w`$ for one (a), two (b) and three (c) atoms. The parameters used were the same as in figure 6.