Time-dependent spatial modulation of a quantum condensate plays a key role in the investigation of the dynamics of collective coherent systems. Cold-atom condensates were already manipulated into forming solitons, vortices and optical lattices via the dynamic Stark effect. In the solid-state framework, semiconductor microcavity exciton-polaritons present an excellent platform for observing nonequilibrium condensate dynamics. Furthermore, the dynamic manipulation of exciton-polariton condensates offers numerous potential implementations in all-optical logic devices. We report the first observation of the energy modulation of an exciton-polariton condensate via the dynamic Stark effect. A Stark pulse is employed to induce a transient, coherence-preserving blueshift in the energy of the condensate of femtosecond-scale duration. A novel approach is presented for discerning the Stark effect in a condensate from the uncondensed case according to distinctive features in differential reflectance spectra, including spectro-temporal oscillations enabling to detect the buildup of coherence. The ultrafast and non-invasive modulation of the exciton-polariton condensate demonstrated here opens new research avenues of nonequilibrium physics of solid-state condensates as well as opportunities for polariton-based elements in both classical and quantum information technologies.
Time-dependent spatial modulation of a quantum condensate plays a key role in the investigation of the dynamics of collective coherent systems. Cold-atom condensates were already manipulated into forming solitons, vortices and optical lattices via the dynamic Stark effect. In the solid-state framework, semiconductor microcavity exciton-polaritons present an excellent platform for observing nonequilibrium condensate dynamics. Furthermore, the dynamic manipulation of exciton-polariton condensates offers numerous potential implementations in all-optical logic devices. We report the first observation of the energy modulation of an exciton-polariton condensate via the dynamic Stark effect. A Stark pulse is employed to induce a transient, coherence-preserving blueshift in the energy of the condensate of femtosecond-scale duration. A novel approach is presented for discerning the Stark effect in a condensate from the uncondensed case according to distinctive features in differential reflectance spectra, including spectro-temporal oscillations enabling to detect the buildup of coherence. The ultrafast and non-invasive modulation of the exciton-polariton condensate demonstrated here opens new research avenues of nonequilibrium physics of solid-state condensates as well as opportunities for polariton-based elements in both classical and quantum information technologies.
Summary form only given. Bosons can populate quantum states macroscopically, forming various kinds of thermal-equilibrium, and quasi-equilibrium condensates, which exhibit a wide range of collective phenomena including superfluidity and macroscopic coherence in matter. Interferometry has been employed to demonstrate long-range off-diagonal order in cold-atom systems, and, recently, in the rapidly developing field of exciton-polariton condensates. However, all such interferometric measurements have been performed on steady-state condensates, unable to access the temporal off-diagonal order and non-equilibrium dynamics. Moreover, in solid-state systems, interference between two separate condensates has not been observed before. Here we use optical injection to resonantly generate two dynamic exciton-polariton condensates with distinct momenta and at different times. We characterize the interference between condensates, demonstrating their long-range temporal order. We show that the build-up of the temporal long-range order strongly depends on the strength of polariton interactions, as well as the temperature and particle density. Moreover, polariton interactions yield a blue shift of the dynamic condensate energy, acting as an extremely large optical nonlinearity. These results provide direct evidence of temporal long-range order in dynamic condensates as well as demonstrate a new approach for probing the ultrafast coherent dynamics of exciton-polaritons, opening new directions in the fundamental study of coherence in matter as well as in practical applications such as quantum information processing and ultrafast logic.
Development of spontaneous coherence is one of the hallmarks of bosonic condensation in a variety of physical systems, such as cold atoms, confined photons, and hybrid light-matter quasiparticles like exciton polaritons in semiconductors. While spatial coherence is well understood once a steady-state condensate has been established, its temporal evolution as the condensate forms is largely unexplored. Here, we explore the dynamical formation of a non-equilibrium, driven-dissipative exciton-polariton condensate through both time-resolved experiments and numerical modeling. Our study reveals that the spatial coherence is established through two distinct stages. The early-time stage is interaction-driven and features transient oscillations in spatial coherence. This stage is followed by a steady-state regime characterized by a spatially-uniform high degree of coherence that extends over the entire size of the system and persists over time. These stages of spatial coherence development occur in both free flowing and confined exciton-polariton systems that undergo a quench - rapid growth of the condensate starting from two different initial settings. Our study offers a deep insight into the process by which long-range spatial coherence is established in a non-equilibrium bosonic condensate.
Bose-Einstein condensates of exciton-polaritons in inorganic semiconductor microcavities are known to possess strong interparticle interactions attributed to their excitonic component. The interactions play a crucial role in the nonlinear dynamics of such systems and can be witnessed as the high energy shift of polariton states. However, the localised nature of Frenkel excitons in strongly coupled organic microcavities precludes interparticle Coulomb exchange-interactions that affect nonlinear dynamics and change mechanisms of polariton energy shifts accordingly. We have scrutinized the origins of energy shifts in connection with nonlinear dynamics in Frenkel exciton-polariton condensates and examined the possible contributions: intracavity optical Kerr-effect, gain-induced frequency pulling, polariton interactions and effects related to saturation of optical transitions for "dark"- and "bright" molecules [1]. Unlike the conventional strongly coupled semiconductor microcavities, we have shown that nonlinear interactions within the condensate do not rely on polariton interactions but instead originated from Pauli-blocking principle forbidding double excitation of the same molecular states. We have developed a theoretical model explaining the omnipresent energy shift of the condensate wavefunction together with its spectral and polarization features at the BEC transition in a consistent way. The crucial role of intermolecular energy transfer and “dark” exciton reservoir has been demonstrated for the first time. We believe the principles explored in this work are relevant to other systems exhibiting strong coupling of Frenkel excitons with a cavity mode, regardless of a cavity type, whether one dealing with Fabry-Perot cavities or plasmonic nanocavities etc and; therefore, provide general insight on nonlinear phenomena in composite light-matter condensates. [1] T. Yagafarov, D. Sannikov, A. Zasedatelev, K. Georgiou, A. Baranikov, O. Kyriienko, I. Shelykh, L. Gai, Z. Shen, D. G. Lidzey, P. Lagoudakis, Mechanisms of blueshifts in organic polariton condensates, Commun Phys 3, 18 (2020). https://doi.org/10.1038/s42005-019-0278-6
Irradiation of a medium with non-resonant light leads to a shift of the energy levels in the system. This optical, or dynamical Stark effect has been studied for many years in atomic gases. It is only recently, however, that it could be detected for excitonic transitions in solids. This development has stirred considerable interest, because the optical Stark effect has inherent features which makes it well suited for applications such as in ultrafast all-optical data processing. Since the pump light beam falls in a transparency region of the medium, it experiences little loss, in contrast to optical non-linearities based on a saturation mechanism. Also, because virtual transitions are involved, the light-induced shift of exciton levels follows closely the pump pulse duration, making it possible to design ultrafast all-optical logic gates with subpicosecond switch-on and -off times.
Strongly-coupled light-matter exciton-polaritons constitute an on-chip solid-state platform where the macroscopic quantum phenomenon of condensation is not only achievable at elevated temperatures, but can also be optically controlled, including through their interaction with inaccessible "dark" states. A recent study has shown that polariton condensation can be established under nonlinear two-photon pumping, paving the way towards dark state-condensate coherent control and highly-efficient terahertz (THz) lasing. In this letter, we show for the first time a temporal signature of dark exciton induced bosonic stimulation by investigating one- and two-photon pumped condensation with time-resolved photoluminescence spectroscopy. Our results show a clear difference in the detuning dependence of the buildup and relaxation rates of the condensate-induced blueshifts under one- and two-photon pumping. This difference is associated with the stronger exciton-fraction dependence expected for one-photon pumped condensation, where polariton-polariton stimulation dominates, compared with two-photon pumped condensation, where a 2p-exciton-to-lower-polariton THz transition can provide another stimulation channel, together with various spin-flip, electron-hole exchange and phonon-based mechanisms. These observations indicate the presence of a new dark state originated stimulation channel that could facilitate highly-efficient THz lasing in semiconductor microcavities.