Distinguishing between dynamical and static Rashba effects in hybrid perovskite nanocrystals using transient absorption spectroscopy

TL;DR

This study provides direct experimental evidence of the dynamical Rashba effect in hybrid perovskite nanocrystals using transient absorption spectroscopy, revealing ultrafast spin-split states and their dependence on photon helicity.

Contribution

First experimental observation of the dynamical Rashba effect in lead halide perovskite nanocrystals using transient absorption spectral imaging.

Findings

Observed a 240 meV initial splitting stabilizing to 60 meV over 500 ps

Demonstrated photon-helicity-dependent asymmetry in subband intensities

Proved the existence of Rashba spin-split edge states in lead halide perovskites

Abstract

The dynamical and static Rashba effects in hybrid methylammonium (MA) lead halide perovskites have recently been theoretically predicted. However, only the static effect was experimentally confirmed so far. Here we report on the dynamical Rashba effect observed using snapshot transient absorption spectral imaging with 400 nm pumping for a fully encapsulated film of 20-nm-sized 3D MAPbBr3 nanocrystals. The effect causes a 240 meV splitting of the lowest-energy absorption bleaching band, initially appearing over sub-ps timescale and progressively stabilizing to 60 meV during 500 ps. The integrated intensities of the split subbands demonstrate a photon-helicity-dependent asymmetry, thus proving the Rashba-type splitting and providing direct experimental evidence for the Rashba spin-split edge states in lead halide perovskite materials. The ultrafast dynamics is governed by the relaxation of two-photon-excited electrons in the Rashba spin-split system caused by a built-in electric field originating from dynamical charge separation in the entire MAPbBr3 nanocrystal.