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PHYSICAL REVIEW B 79, 125311 ͑2009͒

Probing the excitation spectrum of condensates

Michiel Wouters1 and Iacopo Carusotto2,3 1Institute of , Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland 2CNR-INFM BEC Center and Dipartimento di Fisica, Università di Trento, I-38050 Povo, Italy 3Institute of Quantum Electronics, ETH Zürich, 8093 Zürich, Switzerland ͑Received 29 September 2008; revised manuscript received 27 November 2008; published 13 March 2009͒ We propose a four-wave mixing experiment to probe the elementary excitation spectrum of a nonequilibrium Bose-Einstein condensate of - under nonresonant pumping. Analytical calculations based on mean-field theory show that this method is able to reveal the characteristic negative feature of the Bogoliubov dispersion. Numerical simulations including the finite spatial profile of the excitation laser spot and a weak disorder confirm the practical utility of the method for realistic condensates.

DOI: 10.1103/PhysRevB.79.125311 PACS number͑s͒: 03.75.Kk, 71.36.ϩc, 78.47.nj

I. INTRODUCTION either at the absorption17 and resonant Rayleigh scattering18 spectra or at the density response to an external pertur- A series of remarkable experiments have recently demon- bation.19 strated the occurrence of Bose-Einstein condensation in sys- In the present work, we push these ideas forward and we tems of exciton-polaritons in semiconductor microcavities.1–5 propose a simple four-wave mixing ͑FWM͒ spectroscopy These observations, together with parallel ones on scheme to measure the dispersion of all elementary excita- condensation in magnetic solids,6 are opening the way to the tions branches of a nonresonantly pumped polariton conden- investigation of the Bose-Einstein condensation phase tran- sate: of the three incident beams needed in a FWM experi- sition and of Bose-condensed quantum fluids in completely ment, two are provided by the condensate and one by an new regimes far from thermal equilibrium where the state of external laser field. The dispersion of excitations is inferred the condensate is no longer determined by a thermal equilib- by scanning the energy and wave vector of this latter beam rium condition but by a dynamical balance between driving and by recording the transmitted, reflected, and/or four-wave and dissipation.7 mixed beams. A first application of related FWM techniques A key quantity in the theory of quantum fluids is the dis- to polariton systems across the parametric oscillation thresh- persion of the elementary excitations, which determines the old was reported in Ref. 20, but no specific interest was paid dynamics of the system in response to external perturbations to the excitation modes of the condensate itself. and, in particular, plays a central role in determining its su- The mean-field Gross-Pitaevskii formalism to describe the perfluidity properties.8 While detailed knowledge is nowa- polariton condensate dynamics that was introduced in Ref. days available of the and roton branches of liquid 16 is briefly reviewed in Sec. I and then applied in Sec. II to helium and of the Bogoliubov modes of dilute atomic gases,9 describe the FWM response of polariton condensates. Closed not much experimental work has been performed yet on po- formulas are extracted for the transmission, reflection, and lariton condensates. On one hand, pioneering luminescence10 FWM signals in the spatially homogeneous case and then and pump-and-probe experiments11,12 have addressed the ex- used to discuss the main features of the spectra. Generaliza- citations of resonantly pumped condensates in an optical tion to the experimentally relevant case of finite-size conden- parametric oscillator ͑OPO͒ configuration; on the other hand, sate is investigated in Sec. III: the efficiency of the FWM luminescence experiments suggesting a linear dispersion of method for realistic condensates is confirmed by means of a the elementary excitations in nonresonantly excited polariton numerical solution of the polariton Gross-Pitaevskii equation condensates have been recently reported.13 Still, none of ͑GPE͒ in nonuniform geometries. Conclusions are finally these works has provided complete evidence of the peculiar drawn in Sec. IV. features that were predicted to appear because of the non- 14–16 equilibrium nature of polariton condensates. II. ELEMENTARY EXCITATION SPECTRUM From a different standpoint, while quite some evidence is available for “off-branch” scattering processes in OPO As a consequence of the short lifetime of polaritons in configurations,10,11 no observation of the related negative en- state-of-the-art microcavities, the polariton condensate can ergy “” branch that is expected to appear under non- hardly be considered as a thermal equilibrium object: con- resonant pumping as a consequence of polariton-polariton tinuous external pumping is necessary to keep the conden- interactions has been reported yet. Most likely, this stems sate in a stationary state, and the state of the condensate is from the fact that experiments were based on luminescence determined by a dynamical balance between pumping and spectroscopy13 so that the emission from the ghost branch dissipation. While the distribution of large sys- was easily masked by the much stronger background of the tems still appears to follow at large the typical ex- condensate emission. A few recent theoretical works have ponential law of equilibrium statistical mechanics,1–3 clear proposed more refined schemes that appear suited to over- evidence of the nonequilibrium nature of the polariton con- come this difficulty and detect this elusive branch by looking densate has been observed in the ballistic outward polariton

1098-0121/2009/79͑12͒/125311͑6͒ 125311-1 ©2009 The American Physical Society MICHIEL WOUTERS AND IACOPO CARUSOTTO PHYSICAL REVIEW B 79, 125311 ͑2009͒

␻ ͑ ͒ The condensate energy c central dot is blue shifted 5 with respect to the bottom of the lower polariton branch ͑dotted line͒ by the condensate-condensate and condensate- ␻ ␻ 4 reservoir interactions, c = 0 +gnc +gRnR. Here, nc and nR are the densities, respectively, of the condensate and of the FWM exciton reservoir, while the g and g coupling constants char- 3 R acterize the interactions, respectively, between a pair of con- densate polaritons and between the condensate polaritons μ

)/ 2

0 and reservoir . The Bogoliubov spectrum of equilib- ω

− ␻ ͑ ͒ ͓␧ ͑␧ rium condensates has the standard form Bog k = k k ω ( ͔͒1/2 1 +2gnc in terms of the bare polariton dispersion at linear regime. Within the parabolic approximation, this can be writ- probe ␧ ប 2 / ten as k = k 2mLP. As discussed in Ref. 16, the effective 0 width ⌫ is defined as ⌫=␣␤␥/͑1+␣␤͒, in terms of the ␣ / scaled pump intensity = P Pth−1 above the threshold value −1 ␤ ͑ ͒ Pth and the coefficient defined in terms of gain rate R nR of the condensate from the excitonic reservoir as ␤ 0 Ј͑ 0 ͒/ ͑ 0 ͒ ␣ӷ −2 =nRR nR R nR . Well above the threshold 1, the effec- −2.5 −2 −1.5 −1 −0.5 0 0.5 1 1.5 2 2.5 ⌫ k ξ tive width recovers the empty-cavity polariton decay rate ␥. FIG. 1. ͑Color online͒ Plot of the elementary excitation spec- Note how the dispersion of elementary excitations signifi- ␻ ␻ trum in a spatially homogeneous geometry and sketch of the pro- cantly differs from the naive Hartree prediction = 0 ប 2 / ͑ ͒ posed FWM experiment. The central dot indicates the wave vector +2gRnR +gnc + k 2m dashed line and rather recovers in ␻ ␻ k=0 and the energy ␻c of the condensate. The heavy solid line is the high-momentum region the value = 0 +2gRnR +2gnc the dispersion ͓Eq. ͑1͔͒ of the elementary excitations on top of the +បk2 /2m which correctly includes a factor of 2 due to condensate. The arrows show the parametric scattering process on bosonic exchange ͑solid line͒. Provided that the effect of which our proposed scheme is based: the condensate is probed at saturation24 on the polariton interactions is negligible, these the lower dot, and the response is probed via the emission at the simple arguments can be used to isolate the contribution of, upper dot. The dotted line is the dispersion of free polaritons at respectively, the condensate-reservoir and the condensate- linear regime. The solid and dashed lines include the blue shift due condensate interactions to the blue shift and possibly even to condensate-condensate and condensate-reservoir interactions as evaluate the fraction of condensed excitons with respect to ␥ ⌫ mentioned in the text. System parameters: = =gnc and gRnR the total number of excitons in the microcavity. =0.5gnc.

flow from small-sized condensates21,22 as well as in the spon- III. FOUR-WAVE MIXING SPECTROSCOPY SCHEME taneous appearance of vortices in the presence of a signifi- Even though a simple luminescence experiment should in 23 cant disorder potential. principle be able to reveal both the positive and the negative Several theoretical papers have recently investigated the ghost branches of the elementary excitation spectrum shown effect of the nonequilibrium condition on the elementary ex- in Fig. 1, experimental observations have not been able to 14,16 citation spectrum and, in particular, have pointed out the provide unambiguous evidence of the ghost branch yet.1,3,13 diffusive nature of the Goldstone mode at low wave vectors. Most likely the very weak luminescence coming from the In what follows, we shall adopt the point of view of our ghost branch is hidden by the much stronger emission from 16 previous paper where the dynamics of a nonequilibrium the condensate and the upper branch. condensate was discussed at the mean-field level in terms of The physical process underlying our proposal is sketched a generalized nonequilibrium Gross-Pitaevskii equation. in Fig. 1. Elementary excitations are created on top of the This gives the following form for the dispersion of the condensate by injecting extra polaritons with a probe laser elementary excitations on top of a spatially homogeneous beam at a finite in-plane wave vector k tuned at a frequency nonequilibrium condensate: ␻. The response of the system is then observed via the co- herent light emission at an opposite wave vector k at an ␻ ͑ ͒ ␻ ⌫/ Ϯ ͱ͓␻ ͑ ͔͒2 ⌫2/ ͑ ͒ ␻ ␻ Ϯ k − c =−i 2 Bog k − 4, 1 energy 2 c − : the existence of a coherent coupling between ␻ ␻ ␻ the symmetrically located frequencies and 2 c − and which is plotted in Fig. 1 as a heavy solid line. In the low-k, wave vectors Ϯk stems from the fact that the elementary diffusive region of the spectrum the Ϯ signs correspond to, excitations of the condensate consist of a coherent superpo- ͑ ␻͒ ͑ ␻ ␻͒ 9,25 respectively, the phase and the density branches. In the sition of plane waves at k, and −k,2 c − . Equiva- high-k region where the standard equilibrium Bogoliubov lently, this same process can be interpreted in nonlinear op- dispersion is recovered, they instead correspond to the nor- tical terms as a stimulated parametric scattering where a pair mal and anomalous ghost branches. In what follows, specific of condensate polaritons is coherently scattered into one attention will be paid to the ghost branch which is a signature more probe polariton plus one FWM polariton of symmetric of coherent polariton-polariton interactions.9 wave vector and frequency. Within the standard language of

125311-2 PROBING THE EXCITATION SPECTRUM OF POLARITON… PHYSICAL REVIEW B 79, 125311 ͑2009͒ four-wave mixing, two of the three input beams are provided 2 2 µ µ by the condensate itself and only the third comes from the / ) )/ c c incident laser. ω 0 (a) ω 0 (b) − − ω ω ( −2 ( −2

A. Transmittivity 0 0.5 1 1.5 2 −2 −1.5 −1 −0.5 0 k ξ k ξ The same linearization procedure that was used in Ref. 16 to obtain the dispersion of the elementary excitations can be 15 0.8

straightforwardly used to determine the response of the sys- (c) 0 0.6 10 ͑ ͒ E ͑k ␻͒ 0 tem to a weak probe laser of amplitude pr , . The sim- 0.4 plest quantity to consider is the probe transmission. T/T 5 (d) ← /10 In the usual approximation that the effective reservoir re- FWM/T 0.2 ␥ 0 0 laxation rate R is much larger than all other frequency scales −4 −2 0 2 4 −4 −2 0 2 4 in the problem, the reservoir dynamics can be eliminated and (ω−ω )/µ (ω−ω )/µ c c the amplitude of the transmitted field has the following form: 6 6 0 0 ͱ 4 (e) 4 (f) ␥ ␧ ␻ ⌫/ (k)]/T T0 gnc + k + + i 2 ±

͑ ␻͒ ͑ ␻͒ ͑ ͒ (k)]/T E k E k ω

, = , . 2 ± tr ͓␻ ␻ ͑ ͔͓͒␻ ␻ ͑ ͔͒ pr 2 − + k − − k ω 2 2 T[

0 FWM[ 0 0 0.5 1 1.5 2 0 0.5 1 1.5 2 The frequencies ␻Ϯ͑k͒ that appear in the resonant denomi- kξ kξ nators were defined in Eq. ͑1͒: the transmission is resonantly enhanced when the probe is on resonance with an elementary FIG. 2. ͑a͒ Transmittivity and ͑b͒ FWM spectra of a nonequi- excitation of the polariton condensate, either on the positive librium condensate excited with a probe laser at wave vector kϾ0 energy branch or on the negative energy ghost branch. A and frequency ␻. The full and dashed lines indicate the positive and ͉ / ͉2 complete density plot of the transmittivity T= Etr Epr in the negative Bogoliubov branches from Eq. ͑1͒. Cuts of the transmis- ͑␻,k͒ plane is shown in Fig. 2͑a͒. For the sake of simplicity, sion and FWM spectra at given k values are shown in panels ͑c͒ and the transmission T is normalized to the linear regime reso- ͑d͒; the corresponding k values are indicated by the vertical lines in ͑ ͒ ͑ ͒ nant transmittivity T0 of the unloaded cavity. panels a and b . The peak value of the transmittivity and the At large momenta k, the intensity of the ghost mode is FWM signal on, respectively, the normal and ghost Bogoliubov much weaker than the one of the upper, normal mode and branches are shown in ͑e͒ and ͑f͒ as solid and dashed lines. In ͑f͒ quickly tends to zero. Already for k␰=1, the ghost resonance the two quantities coincide. All spectra are normalized to the is extremely weak and almost invisible in the cut shown as a empty-cavity, linear regime transmittivity T0. System parameters: ⌫ ␥ dotted line in Fig. 2͑c͒. On the other hand, the normal reso- = =gnc. / nance tends to the unloaded cavity peak of height T T0 =1 and width ␥. For decreasing values of k, the intensities of the ͱ ␥ ⌫/ T0 gnc + i 2 two resonances get closer and eventually stick at the singular E ͑k,␻͒ =− FWM 2 ͓␻ − ␻ ͑k͔͓͒␻ − ␻ ͑k͔͒ point k␰=0.5 of the dispersion ͓Fig. 2͑e͔͒. + − ͒ ͑ ␻ ␻͒ ͑ ء ϫ In the low-k diffusive region where the two branches are Epr − k,2 c − . 3 degenerate Re͓␻Ϯ͔=0, the transmission intensity signifi- cantly exceeds the peak transmittivity T of the unloaded 0 The response function S =͉E /E ͉2 is plotted in the cavity ͓solid line in Fig. 2͑c͔͒: this gain feature is due to the FWM FWM pr upper-left panel of Fig. 2. Thanks to the symmetry under the condensate that is able to amplify the probe beam. A similar exchange ␻→−␻, the heights of the two peaks correspond- phenomenology was found and discussed in Ref. 15 for the ing to the normal and the ghost branches are equal. case of an optical parametric oscillator. This is a crucial advantage of the FWM technique as com- While the appearance of the ghost branch in the transmis- pared to the transmission spectroscopy discussed in Sec. sion spectra of Fig. 2 is a signature of the presence of the III A or the resonant Rayleigh scattering discussed in Ref. condensate, the transmittivity on the normal branch can ex- 18. Different from this latter scheme, FWM does not rely on ceed the linear regime value T even for pump intensities 0 the presence of a disorder potential and therefore is not af- well below the condensation threshold. Even if not sufficient fected by specklelike modulations of the detected signal. As to overcome losses, some gain is in fact present also in this it happened for the probe transmission, also the FWM signal case,17 as witnessed by the polariton linewidth decreasing results as strongly enhanced in the diffusive region and may below the unloaded cavity value ␥. eventually become stronger than the probe itself. On the other hand, it decreases quite quickly for larger values of k. B. FWM signal Note that both direct polariton-polariton collisions and nonlinear gain saturation effects contribute to the FWM sig- ⌫/ The same method can be used to obtain an expression for nal via, respectively, the terms gnc and i 2 in the numerator the amplitude of the four-wave mixing signal of Eq. ͑3͒: some FWM signal is therefore expected to appear

125311-3 MICHIEL WOUTERS AND IACOPO CARUSOTTO PHYSICAL REVIEW B 79, 125311 ͑2009͒ even for negligible polariton-polariton collisions but is in 6 6 this case peaked very close to the free polariton dispersion. 4 4 µ 2 µ 2 )/ )/

On the other hand, the presence of a FWM signal appears to c c

ω 0 ω 0 be conclusive evidence of the presence of a coherent conden- − −

ω −2 ω −2 sate: the same calculation below threshold would in fact give ( (a) ( (b) a vanishing coherent FWM amplitude in the weak probe −4 −4 −6 −6 limit. Gain saturation is in fact not active in this regime and 0 1 2 3 0 1 2 3 FWM processes involving the exciton reservoir only provide kξ kξ an incoherent background without any specific resonant fea- 2.5 10 ture. 2 8

C. Reflectivity 1.5 6 R R 1 4 As many microcavity samples are grown on an absorbing (d) substrate, transmission measurements are not always pos- 0.5 (c) 2 0 0 sible. While FWM expression ͑3͒ is the same in both reflec- −5 0 5 −5 0 5 tion and transmission geometries, the interference between ω/µ ω/µ direct reflections of light on the external mirror and the sec- 6 6 ondary emission from the cavity makes the following expres- sion of the reflection amplitude a bit more complicate than 4 4 (k)] (k)] transmission amplitude ͑2͒: ± ± ω ω

R[ 2 R[ 2 ␥ gn + ␧ + ␻ + i⌫/2 (e) (f) E ͑k,␻͒ = ͩ1−i ph c k ͪE ͑k,␻͒. r ͓␻ ␻ ͑ ͔͓͒␻ ␻ ͑ ͔͒ pr 2 − + k − − k 0 0 0 1 2 3 0 1 2 3 ͑4͒ kξ kξ ␥ Note that the linewidth ph that appears in the numerator of FIG. 3. Panels ͑a͒ and ͑b͒: ͑k,␻͒ plot of the reflectivity for ͑a͒ ͑ ͒ Eq. 4 is the linewidth of the cavity- mode in the ␥=⌫=gnc and ͑b͒ ⌫=0.4␥=gnc. ͑c͒ and ͑d͒ show reflection spectra absence of any excitonic resonance. This quantity is to be at fixed values of k as indicated by the vertical lines in panels ͑a͒ distinguished from the linewidth ␥ of the polariton branch and ͑b͒. The peak values of the reflectivity on the normal and ghost that appeared in the previous formulas. In terms of the Bogoliubov branches are, respectively, shown in ͑e͒ and ͑f͒ as solid LP ␥ ␥ ␥ Hopfield coefficients Uph,x that quantify the cavity-photonic and dashed lines. Parameters: = ph= x. and the excitonic contents of the lower polariton branch, the ␥ ␥ polariton , exciton, and cavity-photon x,ph linewidths are closer to the threshold. As a consequence of the narrower related by24 resonance line, the reflected beam is now more intense than the incident one on both the normal and the ghost branches. ␥ = ␥ ͉ULP͉2 + ␥ ͉ULP͉2. ͑5͒ x x ph c The amplification in the low-k diffusive region is also stron- ӷ As it involves subtle interference effects, the reflection ger than in the case P Pth considered before. spectrum turns out to be sensitive to the ratio of the linewidth ␥/⌫Ն of excitations in the empty and pumped cavity 1, as IV. PROBING THE ELEMENTARY EXCITATION well as to the ratio between the cavity-photon and the polar- ␥ /␥ SPECTRUM IN FINITE-SIZE AND/OR iton linewidths ph . Here we focus our attention on the ␥ ␥ ␥ DISORDERED CONDENSATES experimentally most relevant case where ph= x = . Ex- amples of spectra are shown in Fig. 3 for different values of Even in the absence of trapping potentials, the spatial ex- the pumping intensity. Panels ͑a͒ and ͑c͒ refer to a case well tension of polariton condensates is generally limited by the above threshold for which ⌫/␥Ӎ1, while panels ͑b͒ and ͑d͒ size of the laser spot that is used to pump the microcavity.22 are made for a lower ͑but still above threshold͒ value of the Typically, state-of-the-art polariton condensates have a typi- pump intensity at which ⌫/␥=0.4. cal size on the order of tens of microns and may show a In panel ͑a͒, a minimum in the reflectivity is visible on considerable inhomogeneous broadening of their spectral resonance with the positive Bogoliubov branch, while the features as a consequence of the inhomogeneous density pro- reflected intensity on resonance with the negative branch ex- file. Although this effect can be reduced by choosing top-hat ceeds the incident intensity. As for the transmission and the pump beams, the interpretation of FWM experiments is the FWM signal, the amplification effect is the strongest in the clearest if one focuses the probe spot onto a small region at diffusive region at low k ͓panel ͑c͔͒. At high values of k, the the center of the condensate where the density is almost flat dip corresponding to the normal branch remains fully visible, and one spatially selects the emission from the same central while the peak corresponding to the ghost branch disappears. region. This once again confirms that the FWM mixing scheme is The result of numerical calculations based on the full po- the most suited tool for the detection of the ghost branch. lariton Gross-Pitaevskii equation16 is summarized in Fig. 4. The same quantities are plotted in panels ͑b͒, ͑d͒, and ͑f͒ The case of a probe beam of diameter 1 ␮m much smaller for a smaller value of ⌫/␥=0.4, i.e., for a pump intensity than the full condensate size and tuned at a frequency

125311-4 PROBING THE EXCITATION SPECTRUM OF POLARITON… PHYSICAL REVIEW B 79, 125311 ͑2009͒

FIG. 4. ͑Color online͒ Numerical results for the ͑k,␻͒ emission pattern from a probed polariton condensate in a transmission geom- etry. The condensate frequency is ␻c =0.83 meV and probe laser hasa1 ␮m diameter. The central wave vector and the frequency of FIG. 5. ͑Color online͒ Emission pattern for the same configura- −1 the probe are kp =0.6 ␮m and ␻p =0.3 meV ͑left panel͒ and kp tion as in the right-hand panel of Fig. 4 but in the presence of a −1 =1.5 ␮m and ␻p =−0.2 meV ͑right panel͒. The full and dashed disorder potential acting on the polaritons. The height of the disor- lines show the analytical prediction, the excitation spectrum, and der potential is in the 1 meV range. Inset: density profile of the the linear regime polariton dispersion. The central surface plot disordered condensate. shows the real-space polariton density profile corresponding to the right-hand panel. In all panels, the condensate is excited with a ␮ the condensate is hardly obtained in this configuration, the top-hat laser with a 30 m diameter and only the emission origi- very presence of a FWM signal is still a direct proof of the nating from a central region with a 20 ␮m diameter is recorded in presence of a coherent condensate. the left and right panels. The finite frequency spread of the emission The situation is a bit more complex in the presence of lines originates from the finite time window of about 12 ps from which the spectrum was extracted. disorder. As any experimental sample is inevitably far from being perfectly homogeneous, it is important to briefly sum- ␻ marize the main features that we observe in our numerical slightly below the condensate frequency c is considered. simulations when a disorder potential acting on polaritons is The case of a quite high probe wave vector kp =1.5 ␮m−1 tuned close to resonance with the ghost branch is included. A complete study is postponed to further work. shown in the right panel of Fig. 4. As the k distribution is The case of a weak disorder is illustrated in Fig. 5: the narrow as compared to the central wave vector k , the re- strength of the disorder potential is chosen to be strong p ͑ sponse closely resembles the one of the spatially homoge- enough to substantially modulate the polariton density see ͒ neous case discussed in Sec. III. A single FWM response inset but weak enough not to split the condensate into sev- eral frequency components.27 In this case, the FWM signal peak appears around kp and with a k-space linewidth nar- rower than the one of the incident probe: only those wave remains clearly visible: the wave vector distribution is vector components that are on resonance with the ghost strongly broadened by the disorder, but the main features that branch effectively contribute to the FWM signal. were observed in the right panel of Fig. 4 are still apparent. A remarkable feature of the ghost branch is visible in the The situation is dramatically different whenever multiple real-space density profile of the probed condensate shown in condensates are present with a substantial spatial overlap. In the central panel of Fig. 4: as the group velocity of the ghost this case, the main effect of the probe beam is to redistribute branch is opposite to the wave vector k, the perturbation due the intensity among the different condensate frequencies and ͑ Ͼ no clear FWM signal is easily identified among the many to the probe laser with a central wave vector kp 0 pointing to the right͒ propagates through the condensate in the left- spectral lines forming the emission spectrum. wards direction and concentrates on the left-hand side of the probe spot. The case of a probe laser with a smaller wave vector and V. CONCLUSIONS a frequency closer to but still below the condensate fre- quency is shown in the left panel. This choice dramatically We have proposed and analyzed a four-wave mixing spec- modifies the qualitative shape of the response. In particular, troscopy scheme to probe the excitation spectrum of a non- note how the maximum of the response at the probe fre- equilibrium polariton condensate. Clear evidence of the quency lies between the two excitation branches of the ho- negative frequency ghost branch is predicted to appear in the mogeneous system, a spectral region where collective modes FWM spectra. The presence of this feature depends crucially are strongly affected by the finite size of the system and on the coherent nature of the condensate and can therefore be possibly by the nontrivial spectral shape of the conden- used as an additional probe of the condensate coherence. sate.22,26 Although information on the excitation modes of Mapping out the FWM resonance as a function of frequency

125311-5 MICHIEL WOUTERS AND IACOPO CARUSOTTO PHYSICAL REVIEW B 79, 125311 ͑2009͒ and wave vector gives precise access to the elementary ex- ACKNOWLEDGMENTS citation spectrum. We have numerically demonstrated that a We wish to thank V. Savona, D. Sarchi, M. Richard, K. spatially localized probe can be used to overcome inhomo- Lagoudakis, A. Baas, and B. Pietka for continuous stimulat- geneous broadening effects by restricting the measurement to ing discussions on polariton condensates. I.C. acknowledges the central region of the condensate where the density is financial support from the Italian MIUR, the EuroQUAM- almost flat. FerMix program, and the French IFRAF.

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