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Nature Research, Nature Communications, 1(14), 2023

DOI: 10.1038/s41467-023-39550-x

Physical Chemistry of Semiconductor Materials and Interfaces XXI, 2022

DOI: 10.1117/12.2635895

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Ultrafast imaging of polariton propagation and interactions

This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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Data provided by SHERPA/RoMEO

Abstract

AbstractSemiconductor excitations can hybridize with cavity photons to form exciton-polaritons (EPs) with remarkable properties, including light-like energy flow combined with matter-like interactions. To fully harness these properties, EPs must retain ballistic, coherent transport despite matter-mediated interactions with lattice phonons. Here we develop a nonlinear momentum-resolved optical approach that directly images EPs in real space on femtosecond scales in a range of polaritonic architectures. We focus our analysis on EP propagation in layered halide perovskite microcavities. We reveal that EP–phonon interactions lead to a large renormalization of EP velocities at high excitonic fractions at room temperature. Despite these strong EP–phonon interactions, ballistic transport is maintained for up to half-exciton EPs, in agreement with quantum simulations of dynamic disorder shielding through light-matter hybridization. Above 50% excitonic character, rapid decoherence leads to diffusive transport. Our work provides a general framework to precisely balance EP coherence, velocity, and nonlinear interactions.