Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.408
Publication date: 16th December 2024
Non-equilibrium Bose-Einstein condensates of exciton-polaritons in metal halide perovskites present a versatile platform for fundamental and applied research. The transition to spontaneous coherence is widely believed to be driven by intricate many-body interactions between polaritons and the optically inaccessible reservoir of background excitons. To elucidate these interactions, we employ advanced optical spectroscopy techniques to probe the coherent dynamics of polaritons and identify the critical factors—ranging from material properties to multi-particle interactions—that determine the condensation threshold.
Focusing on two-dimensional Ruddlesden-Popper (RP) metal-halide semiconductors, we uncover key processes that hinder polariton condensation. Compared to the bare semiconductor, we find enhanced nonlinear exciton-exciton interactions in the microcavity environment. This is accompanied by ultrafast, parametric polariton scattering that prevents effective thermalization of sufficient population into the lowest-energy polariton state to enable condensation. Furthermore, we detect distinct spectral signatures of multi-particle correlations between polaritons and multiple excitonic transitions characteristic of RP perovskites.
Our findings suggest that the complex scattering landscape between the exciton reservoir and polaritons imposes significant limitations on polariton condensation in these materials. To address this, we propose strategies for reducing competing scattering pathways by systematically tuning the exciton fine structure via targeted organic cation substitutions. Finally, we discuss the broader implications of these results for highly polar materials, where lattice-mediated multi-particle correlations play a pivotal role in shaping many-body dynamics.
Funding from the National Science Foundation CAREER grant (CHE-2338663), start-up funds from Wake Forest University, and funding from the Center for Functional Materials at Wake Forest University.
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