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arXiv:2609.00125

Temporal Signature of Bosonic Stimulation Induced by Dark Exciton in a Two-photon Pumped Polariton Condensate

Nadav Landau, Dmitry Panna, Sarit Feldman, Sebastian Brodbeck, Christian Schneider, Sven Höfling, Alex Hayat

cond-mat.quant-gasquant-phSubmitted Aug 31, 2026• Announced Sep 2, 2026
arXivHTMLPDF

Abstract

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.

Journal reference
Phys. Rev. Lett. 136, 256901 (2026)
DOI
10.1103/s7t5-l6xg

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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.
Two-photon absorption (TPA) allows accessing “dark” states of matter that are otherwise inaccessible to light, which serve as important building blocks for quantum information processing. In a semiconductor microcavity, TPA-driven condensation of strongly coupled light-matter exciton–polaritons can enable new solid-state quantum simulations of “dark” state-condensate interactions and was predicted to stimulate THz emission. Here, we report the first observation of two-photon-pumped polariton condensation, demonstrated by angle-resolved photoluminescence in a GaAs-based microcavity. TPA is evidenced in the quadratic emission dependence on pump power below and above the condensation threshold, and second-harmonic generation is ruled out by both this threshold behavior and by the emission peak energy showing no dependence on pump photon energy. Our results pave the way toward novel polariton-based sources and solid-state coherent control of collective quantum states with individual two-level systems.
Two-photon absorption (TPA) allows accessing dark states of matter otherwise inaccessible to light, which serve as important building blocks for quantum information processing. In a semiconductor microcavity, TPA driven condensation of strongly-coupled light-matter exciton-polaritons can enable new solid-state quantum simulations of dark state-condensate interactions, and was predicted to stimulate THz emission. Here, we report the first observation of two-photon pumped polariton condensation, demonstrated by angle-resolved photoluminescence in a GaAs-based microcavity. TPA is evidenced in the quadratic emission dependence on pump power below and above the condensation threshold, and second-harmonic generation is ruled out by both this threshold behaviour and by the emission peak energy showing no dependence on pump photon energy. Our results pave the way towards novel polariton-based sources and solid-state coherent control of collective quantum states with individual two-level systems.
Condensation of bosons causes spectacular phenomena such as superfluidity or superconductivity. Understanding the nature of the condensed particles is crucial for active control of such quantum phases. Fascinating possibilities emerge from condensates of light–matter-coupled excitations, such as exciton–polaritons, photons hybridized with hydrogen-like bound electron–hole pairs. So far, only the photon component has been resolved, while even the mere existence of excitons in the condensed regime has been challenged. Here we trace the matter component of polariton condensates by monitoring intra-excitonic terahertz transitions. We study how a reservoir of optically dark excitons forms and feeds the degenerate state. Unlike atomic gases, the atom-like transition in excitons is dramatically renormalized on macroscopic ground state population. Our results establish fundamental differences between polariton condensation and photon lasing and open possibilities for coherent control of condensates. Exciton–polaritons are bosonic quasi-particles resulting from strong coupling of excitons and photons but so far only their photon component had been resolved. Here, Menard et al. monitor the intra-excitonic transitions and study how a reservoir of optically dark excitons forms and feeds the degenerate state.
Bose-Einstein condensation (BEC) is a thermodynamic phase transition of an interacting Bose gas. Its key signatures are remarkable quantum effects like superfluidity and a phonon-like Bogoliubov excitation spectrum, which have been verified for atomic BECs. In the solid state, BEC of exciton-polaritons has been reported. Polaritons are strongly coupled light-matter quasiparticles in semiconductor microcavities and composite bosons. However, they are subject to dephasing and decay and need external pumping to reach a steady state. Accordingly the polariton BEC is a nonequilibrium process of a degenerate polariton gas in self-equilibrium, but out of equilibrium with the baths it is coupled to and therefore deviates from the thermodynamic phase transition seen in atomic BECs. Here we show that key signatures of BEC can even be observed without fulfilling the self-equilibrium condition in a highly photonic quantum degenerate nonequilibrium system.
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.
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