Uncovering Temperature-Dependent Exciton-Polariton Relaxation Mechanisms in Perovskites

التفاصيل البيبلوغرافية
العنوان: Uncovering Temperature-Dependent Exciton-Polariton Relaxation Mechanisms in Perovskites
المؤلفون: Laitz, Madeleine, Kaplan, Alexander E. K., Deschamps, Jude, Barotov, Ulugbek, Proppe, Andrew H., García-Benito, Inés, Osherov, Anna, Grancini, Giulia, deQuilettes, Dane W., Nelson, Keith, Bawendi, Moungi, Bulović, Vladimir
سنة النشر: 2022
المجموعة: Condensed Matter
مصطلحات موضوعية: Condensed Matter - Mesoscale and Nanoscale Physics, Condensed Matter - Quantum Gases
الوصف: 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 $k_{||}$ = 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 ($\hbar \Omega_{Rabi}$ = 260$\pm$5 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 $k_{||}$ = 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.
Comment: *Corresponding authors: danedeq@mit.edu, bulovic@mit.edu
نوع الوثيقة: Working Paper
DOI: 10.1038/s41467-023-37772-7
URL الوصول: http://arxiv.org/abs/2203.13816
رقم الأكسشن: edsarx.2203.13816
قاعدة البيانات: arXiv
الوصف
DOI:10.1038/s41467-023-37772-7