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Register a new userObservation of two thresholds leading to polariton condensation in 2D hybrid perovskites
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Two dimensional (2D) perovskites are promising materials for photonic applications, given their outstanding nonlinear optical properties, ease of fabrication and versatility. In particular, exploiting their high oscillator strength, the crystalline form of 2D perovskites can be used as excitonic medium in optical microcavities, allowing for the study of their optical properties in the strong light-matter coupling regime. While polariton condensation has been observed in different materials at room temperature, here we observe for the first time two distinct threshold processes in a 2D perovskite, a material that has never shown spontaneous phase transition up to now. In particular, we demonstrate lasing from the bi-exciton state which contributes to populate the lower polariton branch and, at higher excitation powers, eventually leads to the formation of a polariton condensate. The emission linewidth narrowing and a spatial coherence over 50 x 50 um2 area are the smoking gun, the formation of a quantum coherent state in 2D hybrid perovskite. Our results not only show the formation of a polariton condensate in 2D perovskites but they are also crucial for the understanding of the physical mechanisms that leads to coherent phase transition in perovskite-based polariton microcavities.
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Polaritonic devices exploit the coherent coupling between excitonic and photonic degrees of freedom to perform highly nonlinear operations with low input powers. Most of the current results exploit excitons in epitaxially grown quantum wells and require low temperature operation, while viable alternatives have yet to be found at room temperature. Here we show that large single-crystal flakes of two-dimensional layered perovskite are able to sustain strong polariton nonlinearities at room temperature with no need to be embedded in an optical cavity. In particular, exciton-exciton interaction energies are measured to be remarkably similar to the ones known for inorganic quantum wells at cryogenic temperatures, and more than one order of magnitude larger than alternative room temperature polariton devices reported so far. Thanks to their easy fabrication, large dipolar oscillator strengths and strong nonlinearities, these materials hold great promises to realize actual polariton devices at room temperature.
We demonstrate experimentally the condensation of exciton-polaritons through optical trapping. The non-resonant pump profile is shaped into a ring and projected to a high quality factor microcavity where it forms a 2D repulsive optical potential originating from the interactions of polaritons with the excitonic reservoir. Increasing the population of particles in the trap eventually leads to the emergence of a confined polariton condensate that is spatially decoupled from the decoherence inducing reservoir, before any build up of coherence on the excitation region. In a reference experiment, where the trapping mechanism is switched off by changing the excitation intensity profile, polariton condensation takes place for excitation densities more than two times higher and the resulting condensate is subject to a much stronger dephasing and depletion processes.
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)].
Microcavity polaritons are composite half-light half-matter quasi-particles, which have recently been demonstrated to exhibit rich physical properties, such as non-equilibrium Bose-Einstein condensation, parametric scattering and superfluidity. At the same time, polaritons have some important advantages over photons for information processing applications, since their excitonic component leads to weaker diffraction and stronger inter-particle interactions, implying, respectively, tighter localization and lower powers for nonlinear functionality. Here we present the first experimental observations of bright polariton solitons in a strongly coupled semiconductor microcavity. The polariton solitons are shown to be non-diffracting high density wavepackets, that are strongly localised in real space with a corresponding broad spectrum in momentum space. Unlike solitons known in other matter-wave systems such as Bose condensed ultracold atomic gases, they are non-equilibrium and rely on a balance between losses and external pumping. Microcavity polariton solitons are excited on picosecond timescales, and thus have significant benefits for ultrafast switching and transfer of information over their light only counterparts, semiconductor cavity lasers (VCSELs), which have only nanosecond response time.
Excitation localization involving dynamic nanoscale distortions is a central aspect of photocatalysis, quantum materials and molecular optoelectronics. Experimental characterization of such distortions requires techniques sensitive to the formation of point-defect-like local structural rearrangements in real time. Here, we visualize excitation-induced strain fields in a prototypical member of the lead halide perovskites via femtosecond resolution diffuse x-ray scattering measurements. This enables momentum-resolved phonon spectroscopy of the locally-distorted structure and reveals radially-expanding nanometer-scale elastic strain fields associated with the formation and relaxation of polarons in photoexcited perovskites. Quantitative estimates of the magnitude and the shape of this polaronic distortion are obtained, providing direct insights into the debated dynamic structural distortions in these materials. Optical pump-probe reflection spectroscopy corroborates these results and shows how these large polaronic distortions transiently modify the carrier effective mass, providing a unified picture of the coupled structural and electronic dynamics that underlie the unique optoelectronic functionality of the hybrid perovskites.
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