Exciton Delocalization Suppresses Polariton Scattering

TL;DR

This study uses advanced microscopy to image exciton-polariton propagation across various materials, revealing how exciton delocalization suppresses scattering and enhances transport, crucial for energy and nonlinear optical applications.

Contribution

It establishes a scaling law linking exciton transfer integral to polariton scattering, showing materials with large exciton bandwidths are resistant to disorder effects.

Findings

Materials with large exciton bandwidths exhibit suppressed polariton scattering.

Exciton delocalization enhances polariton propagation and reduces disorder impact.

Linear optical properties alone cannot predict polariton transport behavior.

Abstract

Exciton-polaritons (EPs) are part-light part-matter quasiparticles that combine large exciton-mediated nonlinearities with long-range coherence, ideal for energy harvesting and nonlinear optics. Optimizing EPs for these applications is predicated on a still-elusive understanding of how disorder affects their propagation and dephasing times. Here, using cutting-edge femtosecond spatiotemporal microscopy, we directly image EP propagation at light-like speeds in systems ranging from two-dimensional semiconductors to amorphous molecular films with systematically varied exciton-phonon coupling, exciton delocalization, and static disorder. Despite possessing similar EP dispersions, we observe dramatically different transport velocities and scattering times across systems. We establish a robust scaling law linking EP scattering to exciton transfer integral, demonstrating that polaritons based on materials with large exciton bandwidths are immune to disorder even for highly excitonic EPs. This observation cannot be deduced from the systems' linear optical properties, including EP dispersion and linewidth disorder. Our work highlights the critical and often-overlooked role of the matter component in dictating polariton properties, and provides precise guidelines for simultaneously optimizing EP propagation and nonlinearities.