Coherent Spin Dynamics of Electrons in Two-Dimensional (PEA)$_2$PbI$_4$ Perovskites

TL;DR

This study investigates the coherent spin dynamics of electrons in two-dimensional (PEA)$_2$PbI$_4$ perovskites using pump-probe Kerr rotation, revealing long spin relaxation times and anisotropic g-factors, which advance understanding of spin properties in 2D perovskites.

Contribution

It provides new experimental insights into electron spin coherence, relaxation times, and g-factor anisotropy in 2D perovskites, a previously less explored area.

Findings

Larmor spin precession with a 190 ps dephasing time identified.

Longitudinal spin relaxation time of 25 microseconds measured.

Significant anisotropy in electron g-factor observed.

Abstract

The versatile potential of lead halide perovskites and two-dimensional materials is merged in the Ruddlesen-Popper perovskites having outstanding optical properties. Here, the coherent spin dynamics in Ruddlesen-Popper (PEA)$_2$PbI$_4$ perovskites are investigated by picosecond pump-probe Kerr rotation in an external magnetic field. The Larmor spin precession of resident electrons with a spin dephasing time of 190~ps is identified. The longitudinal spin relaxation time in weak magnetic fields measured by the spin inertia method is as long as 25~$\mu$s. A significant anisotropy of the electron $g$-factor with the in-plane value of $+2.45$ and out-of-plane value of $+2.05$ is found. The exciton out-of-plane $g$-factor is measured to be of $+1.6$ by magneto-reflectivity. This work contributes to the understanding of the spin-dependent properties of two-dimensional perovskites and their spin dynamics.