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# Cluster growing process and a sequence of magic numbers.

Permanent address:\]A. F. Ioffe Physical-Technical Institute of the Russian Academy of Sciences, Polytechnicheskaya 26, St. Petersburg, Russia 194021 Permanent address:\]A. F. Ioffe Physical-Technical Institute of the Russian Academy of Sciences, Polytechnicheskaya 26, St. Petersburg, Russia 194021

## Abstract

We present a new theoretical framework for modelling the cluster growing process. Starting from the initial tetrahedral cluster configuration, adding new atoms to the system and absorbing its energy at each step, we find cluster growing paths up to the cluster sizes of more than 100 atoms. We demonstrate that in this way all known global minimum structures of the Lennard-Jonnes (LJ) clusters can be found. Our method provides an efficient tool for the calculation and analysis of atomic cluster structure. With its use we justify the magic numbers sequence for the clusters of noble gases atoms and compare it with experimental observations. We report the striking correspondence of the peaks in the dependence on cluster size of the second derivative of the binding energy per atom calculated for the chain of LJ-clusters based on the icosahedral symmetry with the peaks in the abundance mass spectra experimentally measured for the clusters of noble gases atoms. Our method serves an efficient alternative to the global optimization techniques based on the Monte-Carlo simulations and it can be applied for the solution of a broad variety of problems in which atomic cluster structure is important.

It is well known that the sequence of cluster magic numbers carries essential information about the electronic and ionic structure of the cluster LesHouches . Understanding of the the cluster magic numbers is often equivalent or nearly equivalent to the understanding of cluster electronic and ionic structure. A good example of this kind is the observation of the magic numbers in the mass spectrum of sodium clusters Knight84 . In this case, the magic numbers were explained by the delocalised electron shell closings (see MetCl99  and references therein). Another example is the the discovery of fullerenes, and in particular the $`C_{60}`$ molecule Kroto85 , which was made by means of the carbon clusters mass spectroscopy.

The formation of a sequence of cluster magic numbers should be closely connected to the mechanisms of cluster formation and growing. It is natural to expect that one can explain the magic numbers sequence and find the most stable cluster isomers by modelling mechanisms of cluster assembling and growing. On the other hand, these mechanisms are of interest on their own and the correct sequence of the magic numbers found in such a simulation can be considered as a proof of validity of the cluster formation model.

The problem of magic clusters is closely connected to the problem of searching for global minima on the cluster multidimentional potential energy surface. The number of local minima on the potential energy surface increases exponentially with the growth cluster size and is estimated to be of the order of $`10^{43}`$ for $`N=100`$ LesHouches . Thus, searching for global minima becomes increasingly difficult problem for large clusters. There are different algorithms and methods of the global minimisation, which have been employed for the global minimisation of atomic cluster systems (see LesHouches  and references therein). These techniques are often based on the Monte-Carlo simulations.

The algorithm which we describe in this work is based on the dynamic searching for the most stable cluster isomers in the cluster growing process. Our calculations demonstrate that our approach is an efficient alternative to the known techniques of the cluster global minimisation. The big advantage of our approach consists in the fact that it allows to study not just the optimized cluster geometries, but also their formation mechanisms.

In the present work we approach the formulated problem in a most simple, but general form. In our most simple scenario, we assume that atoms in a cluster are bound by Lennard-Jones potentials and the cluster growing takes place atom by atom. In this process, new atoms are placed on the cluster surface in the middle of the cluster faces. Then, all atoms in the system are allowed to move, while the energy of the system is decreased. The motion of the atoms is stopped, when the energy minimum is reached. The geometries and energies of all cluster isomers found in this way are stored and analysed. The most stable cluster configuration (cluster isomer) is then used as a starting configuration for the next step of the cluster growing process.

Starting from the initial tetrahedral cluster configuration and using the strategy described above, we have analysed cluster growing paths up to the cluster sizes of more than $`100`$ atoms. We have found that in this way practically all known global minimum structures of the Lennard-Jonnes clusters (see LesHouches  and references therein) can be determined, which proves that our method is indeed an efficient alternative to other cluster global optimization techniques such as basin hoping algorithm LesHouches .

In our model we consider an atomic cluster as a group of atoms that interact with each other by pairing forces. The interaction potential between two atoms in the cluster can, in principle, be arbitrary. In this work, we use the Lennard-Jones (LJ) potential:

$$U(r)=4\epsilon \{(\sigma /r)^{12}(\sigma /r)^6\},$$
(1)
where $`r`$ is the interatomic distance, $`\epsilon `$ is the depth of the potential well ($`\epsilon >0`$), $`2^{1/6}\sigma `$ is the pair bonding length.

The constants in the potentials allow one to model various types of clusters for which LJ paring force approximation is reasonable. The most natural systems of this kind are the clusters consisting of noble gases atoms Ne, Ar, Kr, Xe. The magic numbers for this type of clusters have been experimentally determined in Echt81 ; Haberland94 . In our modelling of the cluster growing process we focus on this example and consider it below in detail. The constants in the LJ potential appropriate for the noble gases atoms one can find in RS . The LJ forces are also appropriate for modelling nuclear clusters consisting of alpha particles BM . Note that for the LJ clusters it is always possible to chose the coordinate scale so that $`\sigma =1`$. It makes all LJ cluster systems scalable. They differ only by the choice of the energy parameter $`\epsilon `$ and the mass of a single constituent (atom).

In our approach the atomic motion in the cluster is described by the Newton equations with the LJ pairing forces. The system of coupled equations for all atoms in the cluster are solved numerically using the 4-th order Runge-Kutta method. The primary goal in this simulation was to find the solutions of the equations that lead to the stable cluster configurations and then to chose energetically the most favourable one. The choice of initial conditions for the simulation and the algorithm for the solution of this problem are described below.

Our cluster searching algorithm is constructed on the idea that each minimum on the cluster potential energy surface corresponds to the situation, when all the atoms are located in their equilibrium positions. A minimum can be found by allowing atoms to move, starting from a certain initial cluster configuration, and by absorbing all their kinetic energy in the most efficient way. If the starting cluster configuration for $`N+1`$ atoms has been chosen on the basis of the global minimum structure for $`N`$ atoms, then it is natural to assume, and we prove this in the present work, that the global minimum structure for $`N+1`$ atoms can be easily found. The success of this procedure reflects the fact that in nature clusters in their global minima often emerge namely in the cluster growing process, which we simulate in such calculation.

We have employed the following algorithm for the kinetic energy absorption. At each step of the calculation we consider the motion of one atom only, which undergoes the action of the maximum force. At the point, in which the kinetic energy of the selected atom is maximum, we set the absolute value of its velocity to zero. This point corresponds to the minimum of the potential well at which the selected atom moves. When the selected atom is brought to the equilibrium position, the next atom is selected to move and the procedure of the kinetic energy absorption repeats. The calculation stops when all the atoms are in equilibrium.

We have considered a number of scenario of the cluster growing on the basis of the developed algorithm for finding the stable cluster configurations.

In the most simple scenario clusters of $`N+1`$ atoms are generated from the N-atomic clusters by adding one atom to the system. In this case the initial conditions for the simulation of N+1-atomic clusters are obtained on the basis of the chosen N-atomic cluster configuration by calculating the coordinates of an extra atom added to the system on a certain rule. We have probed the following paths: the new atom can be added either (A1) to the center of mass of the cluster, or (A2) randomly outside the cluster, but near its surface, or (A3) to the centers of mass of all the faces of the cluster (here, the cluster is considered as a polyhedron), or (A4) to the points that are close to the centers of all the faces of the cluster, located from both sides of the face on the perpendicular to it, (A5) to the centers of mass of the faces laying on the cluster surface.

The choice of the method how to add atoms to the system depends on the problem to be solved. For example, with A1 and A2 methods large clusters consisting of many particles can be generated rather quickly. The A2 method is especially fast, because adding one atom to the boundary of the cluster usually does not lead to the recalculation of its central part. The A3 and A4 methods can be used for searching the most stable, i.e. energetically favourable, cluster configurations or for finding cluster isomers with some other specific properties. The A4 method leads to finding more cluster isomers than the A3 one, but it takes more CPU time. The A5 method is especially convenient for modelling the cluster growing process which we focus on in this paper. Using this method one can generate the cluster growing paths for the most stable cluster isomers.

When considering the cluster growing process, new atoms should be added to the system starting from the initially chosen cluster configuration step by step until the desired cluster size is reached. Each new step of the cluster growing should be made with the use of the methods A1-A5. The criteria for the cluster selection in this process can be as follows: at every step (SE1) one of the clusters with the minimum number of atoms is selected, or (SE2) the cluster with the minimum energy among the already found stable clusters of the maximum size is selected, or (SE3) the cluster with the maximum energy among the already found stable clusters of the maximum size is selected.

The SE1 criterion is relevant in the situation, when the full search of cluster isomers is needed. It is applicable to the systems with relatively small number of particles. The SE2 criterion is relevant for modelling the cluster growing process. It turns out to be very efficient and leads to finding the most stable cluster configurations for a given number of particles. The SE3 criterion might be useful for the redirection of the cluster growing process towards the lower energy cluster isomers branches.

Calculations performed with the use of the methods described above show that often clusters of higher symmetry group possess relatively low energy. Thus, the symmetric cluster configurations are often of particular interest. The process of searching the symmetric cluster configurations can be speed up significantly, if one performs the cluster growing process with the imposed symmetry constraints. This means that for obtaining a symmetric $`N`$ atomic cluster isomer from the initially chosen symmetric $`(NM)`$-atomic configuration one should add $`M`$ atoms to the surface of this isomer symmetrically.

Using our algorithms we have examined various paths of the cluster growing process and determined the most stable isomers up to the cluster sizes of more than 100 atoms. The binding energies per atom as a function of cluster size for the calculated cluster chains are shown in figure 1. In the insertion to figure 1 we present the experimentally measured abundance mass spectrum for the Ar clusters at 77K Echt81 ; Haberland94 .

We have generated the chains of clusters based on the icosahedral, octahedral, tetrahedral and decahedral symmetries with the use of the A3-A5 and SE2-SE3 methods. In a few particular cases for $`N>70`$, we have also used manual modifications of the starting cluster geometries. In all our calculations we have used the dimensionless form of the LJ-potential, i.e. put $`\sigma =1`$. The potential constant has been chosen as $`\epsilon =1/4`$. Such a choice of constants is the most universal. It allows one to rescale easily all the results to any concrete choice of $`\sigma `$ and $`\epsilon `$.

Figure 1 shows that the most stable clusters are obtained on the basis of the icosahedral symmetry configurations with exceptions for $`N=38`$, $`75N77`$ and $`N=98`$. In these cases the octahedral cluster symmetry becomes more favourable. The cluster chains based on the tetrahedral and decahedral symmetries have no intersections with the icosahedral chain of clusters although there is interplay between these two curves and the octahedral one.

The main trend of the energy curves plotted in figure 1 can be understood on the basis of the liquid drop model, according to which the cluster energy is the sum of the volume and the surface energy contributions:

$$E_N=\lambda _VN+\lambda _SN^{2/3}\lambda _RN^{1/3}$$
(2)
Here the first and the second terms describe the volume, and the surface cluster energy correspondingly. The third term is the cluster energy arising due to the curvature of the cluster surface. Choosing constants in (2) as $`\lambda _V=0.71703`$, $`\lambda _S=1.29302`$ and $`\lambda _R=0.56757`$, one can fit the global energy minimum curve plotted in figure 1 with the accuracy less than one per cent. The deviations of the energy curves calculated for various chains of cluster isomers from the liquid drop model (2) are plotted in figure 2. The curves for the icosahedral and the global energy minimum cluster chains go very close with each other and the peaks on these dependences indicate the increased stability of the corresponding magic clusters. The ratio between the volume and surface energies in (2) can be characterised by the dimensionless parameter $`\delta =\lambda _V/\lambda _S`$, being equal in our case to $`\delta =0.5545`$.

The dependence of the binding energies per atom for the most stable cluster configurations on $`N`$ allows one to generate the sequence of the cluster magic numbers. In the insertion to figure 2 we plot the second derivatives $`\mathrm{\Delta }E_n^2`$ for the chain of icosahedral isomers. We compare the obtained dependence with the experimentally measured abundance mass spectrum for the Ar clusters at 77K Echt81 ; Haberland94  (see insertion to figure 1) and establish the striking correspondence of the peaks in the measured mass spectrum with those in the $`\mathrm{\Delta }E_n^2`$ dependence. Indeed, the magic numbers determined from $`\mathrm{\Delta }^2E_N`$ are in a very good agreement with the numbers experimentally measured for the Ar and Xe clusters: 13, 19, 23, 26, 29, 32, 34, 43, 46, 49, 55, 61, 64, 71, 74, 81, 87, 91, 101, 109, 116, 119, 124, 131, 136, 147 Echt81 ; Haberland94 . The most prominent peaks in this sequence 13, 55 and 147 correspond to the closed icosahedral shells, while other numbers correspond to the filling of various parts of the isosahedral shell.

The connection between the second derivatives $`\mathrm{\Delta }^2E_N`$ and the peaks in the abundance mass spectrum of clusters one can understand using the following simple model. Let us assume that the mass spectrum of clusters is formed in the evaporation process. This means that changing the number of clusters, $`n_N`$, of the size $`N`$ in the cluster ensemble takes place due to the evaporation of an atom by the clusters of the size $`N`$ and $`N+1`$, i.e. $`\mathrm{\Delta }n_Nn_{N+1}W_{N+1N}n_NW_{NN1}`$, where the evaporation probabilities are proportional to $`W_{N+1N}e^{\frac{E_N+E_1E_{N+1}}{kT}}`$ and $`W_{NN1}e^{\frac{E_{N1}+E_1E_N}{kT}}`$. Here $`T`$ is the cluster temperature, $`k`$ is the Bolzmann constant. In the limit $`\mathrm{\Delta }E_N/kT1`$, one derives $`\mathrm{\Delta }n_Nn_N(E_{N+1}+E_{N1}2E_N)/kT\mathrm{\Delta }^2E_N`$. These estimates demonstrate that the positive second derivative $`\mathrm{\Delta }^2E_N`$ should lead to the enhanced abundance of the corresponding clusters.

In figure 3, we plot images of the magic clusters up to $`N=71`$. For $`N=32`$ and $`N=34`$, we present the icosahedral isomer and the one possessing the global energy minimum. We also plot the image of the octahedral $`N=38`$ cluster, which is found to be more stable than the clusters from the icosahedral chain. Experimentally $`N=38`$ is not found to be the magic cluster, although it is the global minimum cluster, being magic for the octahedral cluster chain (see figures 1 and 2). This fact can be understood if one takes into account that different symmetry cluster chains are formed independently and the transition of clusters from one chain to another at certain $`N`$ is not possible. It is clear from the binding energy analysis that the icosahedral chain of clusters should be dominating. In experiments, clusters of the icosahedral chain mask clusters of other symmetry chains even in the situations when these other clusters are energetically more favourable, like it occurs for $`N=38`$.

In this paper we have discussed the classical models for the cluster growing process, but our ideas can be easily generalized on the quantum case and be applied to the cluster systems with different than LJ type of the inter-atomic interaction. It would be interesting to see to which extent the parameters of inter-atomic interaction can influence the cluster growing process and the corresponding sequence of magic numbers or whether the crystallization in the nuclear matter consisting of alpha particles and/or nucleons is possible. Studying cluster thermodynamic characteristics with the use of the developed technique is another interesting problem which is left opened for future considerations.

The authors acknowledge support from the the Alexander von Humboldt Foundation and DAAD.


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# Observation of sub-Fourier resonances in a quantum-chaotic system

## Abstract

We experimentally show that the response of a quantum-chaotic system can display resonance lines sharper than the inverse of the excitation duration. This allows us to discriminate two neighboring frequencies with a resolution nearly 40 times better than the limit set by the Fourier inequality. Furthermore, numerical studies indicate that there is no limit, but the loss of signal, to this resolution, opening ways for the development of sub-Fourier quantum-chaotic signal processing.

preprint: v 1.03

Any time-dependent signal can be characterized by its frequency spectrum, obtained by a Fourier transform. The Fourier inequality implies that getting a narrow frequency spectrum requires that the corresponding temporal signal lasts a long time. This inequality links the width $`\mathrm{\Delta }f`$ of the frequency spectrum and the temporal width $`\mathrm{\Delta }t`$ of the signal note:Fourier  : $`\mathrm{\Delta }f\mathrm{\Delta }t1/2`$. A rule that is usually deduced from the above one states that two frequencies cannot be distinguished before a time proportional to the inverse of their difference. Of course, if the signal/noise ratio is infinite, two unresolved frequencies can still be distinguished using a good fit. This is not the problem we are here interested in. We rather concentrate on the raw width of a resonance signal, before any fit is performed. Physically, the Fourier inequality sets a limit to the minimum width of a resonance line to the inverse of the time duration of the experiment, a rule that applies also to quantum systems. For instance, the width of Ramsey fringes ref:Ramsey  is limited by the time interval between the crossing times corresponding to the two Ramsey zones, and the frequency width of an atomic or molecular resonance absorption line is generally given by the inverse of the lifetime of the excited state. However, these conclusions rely on the linear relation between the system’s response to the excitation, and this limit can in principle be overcome provided a suitable non-linearity is introduced. The simplest example is to use a multiphoton resonance. Indeed, the frequency width of a $`n`$-photon excitation line is divided by a factor up to $`n`$ compared to a single photon excitation, as recently observed with multiphoton Raman transitions on atomic rubidium ref:Multiphoton . In this case, the sub-Fourier character originates from the fact that it is $`n^{th}`$ harmonic of the external driving frequency that has to be compared to the atomic frequency, and not the driving frequency itself. As a consequence, such a device is not very flexible, as it allows sub-Fourier lines only at subharmonics of the intrinsic atomic frequency. In the present paper, we show that, for a quantum system displaying chaos (which implies the presence of an intrinsic nonlinearity), sub-Fourier resonances can be widely observed, without the need of a resonance with some internal frequency of the system. They rely on a different process: the high sensitivity of a quantum chaotic device to periodicity breaking.

The system we studied is an atomic version of the quasiperiodically driven quantum kicked rotor described in ref:Bicolor . The periodic quantum kicked rotor ref:aQKR  is a paradigmatic model for studies of time-dependent quantum-chaotic systems. Its atomic version has been implemented in recent experiments by many groups ref:Bicolor ; ref:eQKR ; ref:Raizen98 , and consists in placing a laser-cooled atomic cloud in a periodically pulsed, far-detuned ($`\mathrm{\Delta }_L`$ 9.2 GHz $`1.7\times 10^3\mathrm{\Gamma }`$ in the present case), standing laser wave (SW). The atoms and the electromagnetic field then interact via the so-called “dipole” force ref:Dipole , which is conservative; the high laser-atom detuning insuring that dissipative effects due to spontaneous emission are negligible. The corresponding hamiltonian for a single atom is then, in convenient dimensionless units ref:Raizen98 :

$$H_1=\frac{P^2}{2}+K\mathrm{cos}\theta \underset{n=1}{\overset{N_1}{}}\delta _\tau (tn)$$
(1)
where time is measured in units of the kick period $`T_1=1/f_1`$, $`P`$ is the reduced momentum in units of $`M/(2k_LT_1)`$ ($`k_L`$ is the laser wavenumber and $`M`$ the mass of the atom), $`\theta =2k_Lz`$ the reduced position of the atom along the SW axis, $`K=\mathrm{\Omega }^2T_1\tau \mathrm{}k_L^2/(2M\mathrm{\Delta }_L)`$ the normalized kick intensity ($`\mathrm{\Omega }`$ is the resonant Rabi frequency of the SW beams), $`N_1`$ the number of kicks, and $`\delta _\tau (t)`$ a Dirac-like square function of width $`\tau `$ with $`\tau T_1`$ \[$`\delta _\tau (t)=1/\tau `$ for $`|t|\tau /2`$ and $`\delta _\tau (t)=0`$ elsewhere\]. In the limit $`\tau 0`$, the dynamics of the system is entirely determined by two parameters: the kick intensity (or stochasticity parameter) $`K`$ and the effective Planck constant $`\mathrm{}_{\mathrm{eff}}=4k_L^2T_1\mathrm{}/M`$. For $`K1`$, the classical dynamics associated with the hamiltonian Eq. (1) is a chaotic, although perfectly deterministic, ergodic diffusion in phase space, and the mean kinetic energy $`P^2/2`$ roughly grows linearly with time. Its quantum dynamics is however completely different, and displays a phenomenon known as “dynamical localization” (DL), which is a signature of quantum chaos ref:DL . DL consists in the suppression of the classical momentum diffusion (or a freezing of the wave packet evolution) after some localization time $`t_L`$, due to quantum destructive interferences among the various chaotic classical trajectories. For $`t>t_L`$, the average momentum distribution of the atom presents a characteristic time-independent exponential shape $`p(P,t>t_L)\mathrm{exp}(|P|/L)`$, with a localization length in the momentum space given by $`L`$. DL is intimately related to the periodic character of the kick sequence, and bears a close analogy with Anderson’s localization in disordered solids ref:AndersonLoc .

The sensitivity of DL to deviations from exact periodicity is at the heart of the present experiment. Consider the following hamiltonian, consisting in two series of pulses of frequencies $`f_1`$ and $`f_2`$, with a ratio $`r=f_2/f_11`$, and relative phase $`\phi `$:

$$H_2=H_1+K\mathrm{cos}\theta \underset{n=1}{\overset{N_2<rN_1}{}}\delta _\tau \left(t\frac{n+\phi /2\pi }{r}\right)$$
(2)
with the same normalizations as in Eq. (1). If $`r=1`$ (or, more generally, equal to any rational number), the perturbation is periodic and $`H_2`$ leads to dynamical localization. If the value of $`r`$ is slightly shifted from 1 and turns irrational, the kick series loses its temporal periodicity, DL disappears and the quantum evolution is on the average a continuous chaotic diffusion leading to arbitrarily large momenta. The dependence of the DL on the rational or irrational character of $`r`$ was recently observed experimentally ref:Bicolor . A fundamental question is: how fast can the quantum system distinguish between a true simple rational value of $`r`$ and a neighboring irrational value? The present experiment gives an unexpected response to this question.

In the experiment, a sample of cold cesium atoms issued from a standard magneto-optical trap is kicked by a far-detuned stationary wave (SW) with two series of kicks of frequencies $`f_1`$ and $`f_2`$ for a duration $`T=N_1T_1`$, according to the hamiltonian Eq. (2). The SW pulses are assumed to be short enough that the atomic motion during a pulse can be neglected, and the SW acts, with respect to atomic center of mass dynamics, as an instantaneous kick. Just after the end of the kick sequence, the number of zero momentum atoms $`p(P=0)`$ is probed with a Raman velocity selective excitation ref:Raman . Since the atom-number is conserved during the kick sequence, $`p(0)`$ is proportional to the inverse of the typical momentum at the end of the pulse sequence, i.e. $`1/\sqrt{P^2}`$, and thus measures the degree of localization: the wider the momentum distribution, the smaller the value of $`p(0)`$. Whereas $`f_1`$ is kept constant, this procedure is repeated for various values of $`f_2=rf_1`$, leading to the resonance line shown in Fig. 1. As expected, this line has a maximum at $`r=1`$ where DL is present. A remarkable feature is that its width is extremely narrow and easily beats the standard Fourier limitation, with a $`\mathrm{\Delta }r_{\mathrm{exp}}=0.0026`$, ($`\mathrm{\Delta }`$ is the full width at half maximum, FWHM) and thus $`\mathrm{\Delta }f_2=f_1\mathrm{\Delta }r_{\mathrm{exp}}47`$ Hz, yielding:

$$\mathrm{\Delta }f_2T\frac{1}{38}1$$
(3)
Indeed, in a first approach, one would consider the frequency spectrum of the excitation formed by the two series of pulses. The Fourier spectrum of an infinite sequence of pulses of frequency $`f_1`$ is a comb of peaks separated by $`f_1`$. Since the sequence has a finite duration $`T`$, each peak in the Fourier transform has a width $`1/T`$. Furthermore, since the pulse duration $`\tau `$ is also finite, the whole spectrum is multiplied by the factor:

$$\left(\frac{\mathrm{sin}(\pi f_1\tau )}{\pi f_1\tau }\right)^2\text{ .}$$
(4)
When two sequences with slightly different frequencies are combined, the resulting Fourier spectrum has two series of peaks that may overlap. This is visible in Fig. 2, which shows, for different values of $`r`$, the squared modulus of the Fourier transform of the double kick sequence (with $`\phi =0`$), in the neighborhood of the fundamental frequency $`f_1`$. Consider the function $`F_{1/2}(r)`$, defined as the squared modulus of the Fourier transform at frequency $`f_{1/2}=(f_1+f_2)/2=f_1(1+r)/2`$. This function is large when the two peaks overlap and goes to zero when the two frequencies are completely resolved, giving a quantitative measure of the Fourier resolution. In order to make a comparison with the experimental data, $`F_{1/2}(r)`$ is also plotted in Fig. 1. Its width $`\mathrm{\Delta }F_{1/2}(r)`$ is 0.091, and $`\mathrm{\Delta }F_{1/2}(r)/\mathrm{\Delta }r_{\mathrm{exp}}35`$, clearly showing that Fourier limit has been overcome.

If the width of the resonance line is not Fourier-limited, what is the origin of the process giving such a resolution? A first idea coming to mind is that each atom is not excited just by the fundamental frequencies $`f_1`$ and $`f_2`$, but also by their harmonics. The $`j^{th}`$ harmonic of each fundamental frequency has the same width $`1/T`$, but their frequency separation $`j(f_1f_2)`$ is increased by a factor $`j`$. One would thus attribute the high resolution of the system to the presence of the high harmonics in the excitation spectrum itself. In fact, this interpretation is invalid for several reasons. Firstly, the experimental kicks are not real $`\delta `$-peaks, but have a finite duration $`\tau `$ which implies that the weights of the high harmonics are small. For instance, with $`\tau =3`$ $`\mu `$s, as for the curve shown in Fig. 1, only harmonics up to $`j=18`$ lie in the central lobe of function (4). The harmonic $`j=35`$, whose frequency separation would corresponds to the experimental resolution observed in Fig. 1, lies beyond the first lobe with a very small intensity (less than 2% of the intensity of the first harmonic). Secondly, when $`\tau `$ is increased, with a constant pulse height (which implies that $`K`$ is increased, as it is proportional to $`\tau `$), the relative weight of the high harmonics decreases, because of the factor Eq. (4). But we verified both experimentally and numerically that the system’s resolution increases: the resonance lines becomes narrower (see Fig. 3). Finally, we also performed numerical simulations using a slightly different hamiltonian, in which the two-frequency excitation is given by:

$$\left[1+A\mathrm{cos}(2\pi rt)\right]\underset{n=1}{\overset{N}{}}\delta _\tau (tn)\text{ .}$$
(5)
In this case, the second frequency is introduced as a modulation of the intensity of the pulses. The spectrum of this excitation can be calculated straightforwardly, and is composed of series of peaks at frequencies $`\omega _j/2\pi =j`$ ($`j`$ is an integer) with related sidebands at $`\omega /2\pi =j\pm (r1)`$. The frequency separation between the two series of peaks in the spectrum is $`r1`$, independent of $`j`$: the high harmonics do not provide higher resolution. Despite that, the numerical simulation shown in Fig. 3 is clearly below the Fourier limit. The above arguments thus neatly rule out the effect of high harmonics as a dominant process at work in our experiment. The observed ultra-narrow resonance line is in fact due to the highly sensitive response of the quantum chaotic system itself to the excitation, as we will no explain with semi-heuristic elements.

In the experiment, the atomic wave packet undergoes a series of kicks separated by a free evolution. In momentum representation, a free evolution during a time $`t`$ amounts in multiplying the wave function by a phase factor $`\mathrm{exp}(i\mathrm{\Phi })`$ with $`\mathrm{\Phi }=P^2t/(2\mathrm{}_{\mathrm{eff}})`$. For simplicity, consider the particular case $`\phi =0`$, without loss of generality. In this case, the time interval between the last kick ($`N^{th}`$ kick) of the first series and the corresponding kick of the second the series is $`N(r1)/r`$. The system can resolve the two frequencies if the phase evolution $`\mathrm{\Phi }`$ during this interval, is of the order of one:

$$\mathrm{\Phi }(N)=\frac{P^2}{2\mathrm{}_{\mathrm{eff}}}N\frac{r1}{r}1\text{ .}$$
(6)
Before applying Eq. (6), it is important to distinguish two different regimes: (a) before the localization time, $`N<N_L`$ (where $`N_L=t_L/T_1`$), the dynamics is a classical diffusion, and $`P^2N`$; (b) for $`N>N_L`$ the momentum distribution is localized and $`P^2`$ is roughly constant. Thus, according to Eq. (6), the resolution $`(r1)`$ has a fast, unusual, decrease as $`N^2`$ as long as $`N<N_L`$, and a slower decrease as $`N^1`$ for $`N>N_L`$. Otherwise stated, for times $`t<t_L`$ the system takes an advance over the Fourier limit that it preserves when $`t>t_L`$. Effectively, the numerical simulations in Fig. 3 indicate that the linewidth decreases faster than the standard Fourier decrease, as $`N^1`$. The higher resolution results, on the one hand, from the sensitivity of the quantum interference process to frequency differences, and, on the other hand, from the amplification of such sensitivity by a chaotic diffusion. The underlying physical process relies on long-range correlations in the momentum space. Breaking exact time periodicity of the excitation destroys those correlations and, as a consequence, the localization. This also suggests that the frequency resolution improves as the dynamics becomes more chaotic, as $`K`$ increases. Numerically, no lower limit has been found to the resolution, which can reach several orders of magnitude below the Fourier limit. There are nevertheless limits for real applications since the signal $`p(P=0)`$ decreases with increasing $`K`$, roughly like $`1/K`$. In our experiment, the signal/noise ratio is of the order of 100, which in principle allows widths below 1/100 of the Fourier limit. There is however an experimental imperfection: the SW waist is only about 1.6 times the size of the atomic cloud: depending on their position in the laser beam, the atoms experience different values of $`K`$. This leads to an inhomogeneous broadening of the resonance line, which explains the discrepancies between experimental data and the numerical simulation in Fig. 3. Improvements towards narrower sub-Fourier lines are currently under study.

A few additional remarks might be done. Firstly, sub-Fourier behavior is allowed because the resonance lines are not the direct Fourier transform of a temporal signal. Secondly, the observation of sub-Fourier lines is not limited to a specific choice of parameters. The curve displayed in Fig. 1 is the most sub-Fourier one (by a factor 35) that we have observed, but sub-Fourier widths are a standard behavior. Thirdly, since the process described here involves two frequencies, it is quite analogous to a frequency measurement by the heterodyning technique. This might be exploited for realizing ultra-fast frequency locking to a standard frequency, using $`p(0)`$ as an error signal, that would thus respond in a sub-Fourier time. In a completely different field, an analogy can be made between the present experiment and near field optical microscopy where details of size far below the diffraction limit can be resolved. In both cases, the resolution is obtained at the price of a signal loss.

In conclusion, we have experimentally demonstrated the possibility of using of a quantum-chaotic device to discriminate two frequencies, far below the Fourier limit. The principle relies on the sensitivity of quantum interferences to periodicity breaking, amplified by a chaotic diffusive process. No physical law has been broken, but the very widely used “rule of thumb” stating that the minimum width of a quantum resonance should be limited by the excitation time is here not valid, opening the way to a new field of quantum-chaotic signal processing.

###### Acknowledgements.

Laboratoire de Physique des Lasers, Atomes et Molécules (PhLAM) is Unité Mixte de Recherche UMR 8523 du CNRS et de l’Université des Sciences et Technologies de Lille. Centre d’Etudes et de Recherches Laser et Applications (CERLA) is supported by Ministère de la Recherche, Région Nord-Pas de Calais and Fonds Européen de Développement Economique des Régions (FEDER). Laboratoire Kastler-Brossel de l’Université Pierre et Marie Curie et de l’Ecole Normale Supérieure is UMR 8552 du CNRS. CPU time on a NEC SX5 computer has been provided by IDRIS.


text:
# Models of Irradiated Extrasolar Giant Planets

## 1. Introduction

Since the discovery of 51 Pegasi b (Mayor and Queloz 1995) and the nearly one hundred extrasolar giant planets (EGPs) that have been detected subsequently by radial velocity techniques (see this proceedings and references in Burrows et al. 2001), an increasing fraction of the world’s astronomers has been engaged in determining the best means to detect such planets directly. While the orbital elements of substellar-mass objects with Mpsin(i)s that range from $``$0.2 to $``$10 MJ can constrain formation mechanisms and dynamical evolution, they are no substitute for direct spectral measurements. It is by imaging the planet and obtaining optical, near-infrared, and mid-infrared spectra that an EGP’s atmospheric structure, composition, gravity, radius, and mass can be determined. Such physical characteristics are essential data if the study of EGPs is to mature in the next decade into a major astronomical field. They are also essential if the distinctions between brown dwarfs and giant planets of the same mass are to be determined. It may be that, for a given primary star, different origins and histories at birth translate into different compositions and rotation rates. Spectra will be essential in determining this.

From space, SIM will provide accurate astrometric masses (not merely Mpsin(i)s) for the known EGPs. However, from the ground spectral deconvolution techniques, adaptive optics, interferometry (e.g., using the LBT, VLTI, KIA) and a host of promising and novel methods summarized during this conference encourage one to believe that light from an EGP will soon be detected. From space, optical coronagraphs with ultrasmooth mirrors (e.g., Eclipse, ESPI, JPF), infrared interferometers, and precision transit missions (e.g., MOST, Eddington, Kepler, COROT) are in various stages of planning or preparation. The space-based transit missions will be preceded by a host of ground-based transit searches (e.g., STARE, BEST, WASP, STEPSS, TeMPEST). Transit data married with precise stellar and Doppler wobble measurements can provide mass-radius relations for the close-in EGPs (“roasters”) from which one can extract structural and evolutionary information (Guillot et al. 1996; Burrows et al. 2000). The first discovered transiting extrasolar planet, HD209458b, for which a large radius of $``$1.4 RJ and a mass of 0.69 MJ were obtained (Cody and Sasselov 2002; Brown et al. 2001; Charbonneau et al. 2000; Henry et al. 2000) has jump-started the scramble to understand EGPs under severe irradiation regimes. The demonstration that the depth of HD209458b’s transit is wavelength-dependent (Hubbard et al. 2001) and that neutral sodium resides in its atmosphere (Charbonneau et al. 2002) is an indication of the vast potential of transit studies. The discovery of a collection of transiting planets, not just one, will be a milestone in the study of EGPs.

This tempo of activity focussed on obtaining direct measurements of EGP properties demands a corresponding effort by the theoretical community to calculate the spectra of EGPs around a variety of stars, at a variety of orbital distances, and with a variety of masses and ages. We have undertaken such a project and in this short contribution present some of our preliminary results. A more comprehensive treatment can be found in Sudarsky, Burrows, and Hubeny (2002, in preparation). We have calculated EGP spectra for 51 Peg b, $`\tau `$ Boo b, HD209458 b, $`\upsilon `$ And b,c,d, GJ 876 b,c, $`ϵ`$ Eridani b, 55 Cnc b,c,d, HD114762 b, HD1237 b, and a host of other radial-velocity EGPs, as well as for theoretical objects at the full potential range of orbital distances, around a collection of stellar subtypes, and employing a variety of cloud models. The fluxes at the Earth, as well as the planet/star contrasts as a function of wavelength from 0.4 $`\mu `$m to 30 $`\mu `$m have been determined.

## 2. A Potpourri of Irradiated EGP Spectra

Figure 1 depicts the run with orbital distance from 0.05 to 1.0 A.U. of self-consistent EGP reflection spectra (including heating by stellar irradiation) around a G0 V star. What is actually shown in Fig. 1 is the planet/star flux ratio, a quantity that in some ways is more useful to potential observers. Rayleigh scattering at short wavelengths, methane features for the more distant (hence, cooler) objects, Na-D and K I features at 0.589 $`\mu `$m and 0.77 $`\mu `$m , respectively, and water (steam) features are in evidence. Without Rayleigh scattering, the flux shortward of 0.6 $`\mu `$m would be 3-6 orders of magnitude lower. This set of models does not include clouds (Sudarsky, Burrows, and Hubeny 2002), but the characteristic increase in the trough/peak contrasts with increasing distance, the relative strength of the planet at 3-5 $`\mu `$m , and the wide range of flux ratios from $`10^3`$ to $`10^{10}`$ serve to emphasize that the choice of spectral range is crucial if the direct light of the planet is to be measured. In addition, though for roasters the planet flux at 10 parsecs in the near infrared can reach $``$10 milliJanskys (a rather large number), the glare of the star is still a challenge to direct detection. Figure 2 portrays the corresponding temperature/pressure profiles. A signature of irradiation, the bump near one bar pressure, is in evidence.

Figure 3 shows a representative theoretical spectrum at an average phase for a planet that may be orbiting $`ϵ`$ Eridani at 3.3 A.U. (Hatzes et al. 2000). This model spectrum incorporates water clouds with 5-micron ice particles. As can be seen in Fig. 3, the presence of clouds elevates the flux in the optical to a significant degree. The result is the classic “two–hump” spectrum (crudely, reflection at short wavelengths and emission at long wavelengths) (Saumon et al. 1996), but with important differences. In particular, there is a pronounced excess near 4–6 $`\mu `$m and the spectrum is peppered with CH4 and water absorption features.

For the close-in EGPs such as 51 Peg b, HD209458b, and $`\tau `$ Boo b, the planet/star flux ratios shortward of one micron are $``$10-5, but they climb to $`3\times 10^4`$ around 1.65 $`\mu `$m and 2.2 $`\mu `$m . At $``$4.0 $`\mu `$m , they can be near $`10^3`$, with a slight dependence on the presence of clouds. The $`\upsilon `$ And system, boasting three EGPs with orbital distances from 0.059 A.U. to 2.5 A.U., shows the entire range of potential behaviors for irradiated giant planets. The corresponding flux ratios can vary from three to twelve orders of magnitude, depending upon wavelength and cloud model. The planets around GJ 876 (M4 V) provide an example of irradiation by a dim star. A transit by an EGP of such a late star (with a small radius) would be spectacular in a way that the few nanoJansky fluxes in the near infrared from the wider of the pair of GJ 876’s planets is not.

## 3. On the Wavelength Dependence of EGP Transits

HD209458b, while not a Rosetta Stone for the subject of EGPs, does nevertheless show the presence of atmospheric sodium and has provided a mass-radius point. More such points are anticipated. The HST/STIS data for HD209458b (Brown et al. 2001; Charbonneau et al. 2002) cover the wavelength range from 0.58 $`\mu `$m to 0.64 $`\mu `$m , which includes the Na-D line at 0.589 $`\mu `$m . To $`4\sigma `$, a difference between the transit depth at Na-D and the average depth was detected. However, Na-D is not the only feature predicted in the transit depth spectrum. Figure 4 from Hubbard et al. (2001) shows that measurements of the transit depth as a function of wavelength can be used to reveal other atmospheric constituents such as potassium and, importantly, water. “Absorption” features appear upside-down on Fig. 4, where a large radius reflects a larger opacity. Therefore, a transit spectrum can be used as an erzatz for a direct reflection spectrum (that may be more difficult to obtain) to determine atmospheric abundances.

However, care must be exercised in the interpretation of such “spectra”; they are not the same as reflection spectra. In particular, the transit depth spectrum is a probe of the slant column near the terminator of the planet, the cord optical depth. The actual spectrum of the planet is related more to the normal column depth and to the radial temperature/pressure profile; it is an integral measure of whole-planet emissions. Fortney et al (2002, in preparation and presented at this conference) interpret the discrepancy between the STIS Na-D results and the Hubbard et al. (2002) predictions at 0.589 $`\mu `$m as being due to the neglect by the latter of photoionization and charge exchange in HD209458b’s upper atmosphere (down to $``$1–5 millibars). When Fortney et al. (2002) include the ionization of sodium in their transit spectrum calculation (which involves 2D Monte Carlo transport), they can reproduce the transit observations. But when we calculate the reflection spectra for the same object with and without ionization down to the level necessary to reproduce the HST/STIS results, we see very little difference. In short, a transiting planet’s reflection spectrum does not reveal much about its transit-depth spectrum and care must be taken not to confuse the two.

## 4. Summary Thoughts

NASA and ESA are poised to spend 100’s of millions of dollars in the next decade to detect and characterize extrasolar planets. The best data in the short term will be for EGPs, not terrestrial planets. Hence, for those most interested in discovering Earths, the natural and inevitable path is by way of the giant planets now being discovered in profusion in the solar neighborhood. For those for whom EGPs are not mere stepping stones, the next decade promises a rich harvest of new worlds and stimulating finds. Our calculations are designed to provide the necessary theoretical underpinnings for this quest at one of astronomy’s newest frontiers.

### Acknowledgments.

The authors thank Bill Hubbard, Jonathan Lunine, Jim Liebert, Ivan Hubeny, Christopher Sharp, Drew Milsom, Maxim Volobuyev, Curtis Cooper, and Jonathan Fortney for fruitful conversations and help during the course of the work summarized here, as well as NASA for its financial support via grants NAG5-10760 and NAG5-10629. They would also like to congratulate the organizers, Drake Deming and Sara Seager, for pulling off without a perceptible hitch such a useful and important meeting.

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