We observe for the first time two-photon excited condensation of exciton-polaritons. The angle-resolved photoluminescence (PL) from the Lower Polariton (LP) ground state in our planar GaAs-based microcavity structure exhibits a clear intensity threshold as a function of increased two-photon excitation power, coinciding with an interaction-induced blueshift and a narrowing of spectral linewidth, characteristic of the transition from a thermal distribution of lower polaritons to polariton condensation. Two-Photon Absorption (TPA) is evidenced in the quadratic dependence of the input-output curves below and above the threshold region. Second Harmonic Generation (SHG) is ruled out by both this threshold behavior and by scanning the pump photon energy and observing a lack of dependence of the LP emission peak energy. Our results pave the way towards realization of a polariton-based stimulated THz radiation source, stemming from the dipole-allowed transition from the Quantum Well (QW) 2p dark exciton state to the 1s-exciton-based LP ground state, as theoretically predicted in [A. V. Kavokin et al., Phys. Rev. Lett. 108, 197401 (2012)].
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