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Updated: Jul 24, 2025

Direct Imaging of Laser-driven Ultrafast Molecular Rotation
Published on: February 4, 2017
Ultrafast imaging of polariton propagation and interactions
Ding Xu1, Arkajit Mandal1, James M Baxter1
1Department of Chemistry, Columbia University, New York, NY, 10027, US.
Abstract:
Semiconductor 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.
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