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Optica

Two-photon pumped exciton-polariton condensation

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

Published Oct 17, 2022• 7 citations
Publisher

Abstract

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.

DOI
10.1364/optica.471345

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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.
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.
A phase transition from a classical thermal mixed state to a quantum-mechanical pure state of exciton polaritons is observed in a GaAs multiple quantum-well microcavity from the decrease of the second-order coherence function. Supporting evidence is obtained from the observation of a nonlinear threshold behavior in the pump-intensity dependence of the emission, a polariton-like dispersion relation above threshold, and a decrease of the relaxation time into the lower polariton state. The condensation of microcavity exciton polaritons is confirmed.
Bose-Einstein condensate of exciton polaritons in a semiconductor microcavity is a macroscopically populated coherent quantum state subject to concurrent pumping and decay. Debates about the fundamental nature of the condensed phase in this open quantum system still persist. Here, we gain a new insight into the spontaneous condensation process by imaging long-lifetime exciton polaritons in a high-quality inorganic microcavity in the single-shot optical excitation regime, without averaging over multiple condensate realisations. In this highly non-stationary regime, a condensate is strongly influenced by the `hot' incoherent reservoir, and reservoir depletion is critical for the transition to the ground energy and momentum state. Condensates formed by more photonic exciton polaritons exhibit dramatic reservoir-induced density filamentation and shot-to-shot fluctuations. In contrast, condensates of more excitonic quasiparticles display smooth density and are second-order coherent. Our observations show that the single-shot measurements offer a unique opportunity to study formation of macroscopic phase coherence during a quantum phase transition in a solid state system.
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.
Polaritons are quasi-particles that originate from the coupling of light with matter and that demonstrate quantum phenomena at the many-particle mesoscopic level, such as Bose-Einstein condensation and superfluidity. A highly sought and long-time missing feature of polaritons is a genuine quantum manifestation of their dynamics at the single-particle level. Although they are conceptually perceived as entangled states and theoretical proposals abound for an explicit manifestation of their single-particle properties, so far their behavior has remained fully accounted for by classical and mean-field theories. We report the first experimental demonstration of a genuinely quantum state of the microcavity polariton field, by swapping a photon for a polariton in a two-photon entangled state generated by parametric downconversion. When bringing this single-polariton quantum state in contact with a polariton condensate, we observe a disentangling with the external photon. This manifestation of a polariton quantum state involving a single quantum unlocks new possibilities for quantum information processing with interacting bosons.