Uncovering Temperature-Dependent Exciton-Polariton Relaxation Mechanisms in Perovskites
arXiv:2203.13816 · doi:10.1038/s41467-023-37772-7
Abstract
State-of-the-art hybrid perovskites have demonstrated excellent functionality in photovoltaics and light-emitting applications, and have emerged as a promising candidate for exciton-polariton (polariton) optoelectronics. In the strong coupling regime, polariton formation and Bose-Einstein condensation (BEC) have been demonstrated at room-temperature in several perovskite formulations. Thermodynamically, low-threshold BEC requires efficient scattering to = 0, and many applications demand precise control of polariton interactions. Thus far, the primary mechanisms by which polaritons relax in perovskites remains unclear. In this work, we perform temperature-dependent measurements of polaritons in low-dimensional hybrid perovskites with high light-matter coupling strengths ( = 2605 meV). By embedding the perovskite active layer in a wedged cavity, we are able to tune the Hopfield coefficients and decouple the primary polariton relaxation mechanisms in this material for the first time. We observe the thermal activation of a bottleneck regime, and reveal that this effect can be overcome by harnessing intrinsic scattering mechanisms arising from the interplay between the different excitonic species, such as biexciton-assisted polariton relaxation pathways, and isoenergetic intracavity pumping. We demonstrate the dependence of the bottleneck suppression on cavity detuning, and are able to achieve efficient relaxation to = 0 even at cryogenic temperatures. This new understanding contributes to the design of ultra-low-threshold BEC and condensate control by engineering polariton dispersions resonant with efficient relaxation pathways, leveraging intrinsic material scattering mechanisms for next-generation polariton optoelectronics.
arXiv comment*Corresponding authors: [email protected], [email protected]
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- Circumventing the polariton bottleneck via dark excitons in 2D semiconductors
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