Rapidly expanding spin-polarized exciton halo in a two-dimensional halide perovskite at room temperature.

Yumoto, Go; Sekiguchi, Fumiya; Hashimoto, Ruito; Nakamura, Tomoya; Wakamiya, Atsushi; Kanemitsu, Yoshihiko · Sci Adv · 2022

basic_science · Level V

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Abstract

Monitoring of the spatially resolved exciton spin dynamics in two-dimensional semiconductors has revealed the formation of a spatial pattern and long-range transport of the spin-polarized excitons, which holds promise for exciton-based spin-optoelectronic applications. However, the spatial evolution has been restricted to cryogenic temperatures because of the short exciton spin relaxation times at room temperature. Here, we report that two-dimensional halide perovskites can overcome this limitation owing to their relatively long exciton spin relaxation times and substantial exciton-exciton interactions. We demonstrate the emergence of a halo-like spatial profile in spin-polarized exciton population and its ultrafast expansion at room temperature by performing time-resolved Faraday rotation imaging of spin-polarized excitons in two-dimensional perovskite (C<sub>4</sub>H<sub>9</sub>NH<sub>3</sub>)<sub>2</sub>(CH<sub>3</sub>NH<sub>3</sub>)<sub>3</sub>Pb<sub>4</sub>I<sub>13</sub>. Exciton-exciton exchange interactions induce density-dependent nonlinear relaxation and ultrafast transport of exciton spins and give rise to a rapidly expanding halo-like spatial pattern. The density-dependent spatial control suggests the potential of using two-dimensional halide perovskites for spin-optoelectronic applications.