Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites

Abstract

In two-dimensional hybrid organic-inorganic metal-halide perovskites, the intrinsic optical lineshape reflects multiple excitons with distinct binding energies, each dressed differently by the hybrid lattice. Given this complexity, a fundamentally far-reaching issue is how Coulomb-mediated many-body interactions --- elastic scattering such as excitation-induced dephasing, inelastic exciton bimolecular scattering, and multi-exciton binding --- depend upon the specific exciton-lattice coupling. We report the intrinsic and density-dependent exciton pure dephasing rates and their dependence on temperature by means of a coherent nonlinear spectroscopy. We find exceptionally strong screening effects on multi-exciton scattering relative to other two-dimensional single-atomic-layer semiconductors. Importantly, the exciton-density dependence of the dephasing rates is markedly different for distinct excitons. These findings establish the consequences of particular lattice dressing on exciton many-body quantum dynamics, which critically define fundamental optical properties that underpin photonics and quantum optoelectronics in relevant exciton density regimes.