Giant Rashba Splitting in CH3NH3PbBr3 Organic-Inorganic Perovskite

TL;DR

This study uses angle-resolved photoelectron spectroscopy to reveal a giant Rashba spin splitting in the valence band of CH3NH3PbBr3 perovskite, highlighting strong spin-orbit coupling effects relevant for optoelectronic applications.

Contribution

First direct measurement of the valence band dispersion and Rashba splitting in CH3NH3PbBr3 perovskite using ARPES, demonstrating significant spin-orbit coupling effects.

Findings

Giant Rashba spin splitting observed in the valence band.

Strong spin-orbit coupling confirmed in both low-temperature and room-temperature phases.

Surface electronic structure consistent with bulk properties.

Abstract

As they combine decent mobilities with extremely long carrier lifetimes, organic-inorganic perovskites have opened a whole new field in opto\-electronics. Measurements of their underlying electronic structure, however, are still lacking. Using angle-resolved photoelectron spectroscopy, we measure the valence band dispersion of single-crystal CH$_3$NH$_3$PbBr$_3$. The dispersion of the highest energy band is extracted applying a modified leading edge method, which accounts for the particular density of states of organic-inorganic perovskites. The surface Brillouin zone is consistent with bulk-terminated surfaces both in the low-temperature orthorhombic and the high-temperature cubic phase. In the low-temperature phase, we find a ring-shaped valence band maximum with a radius of 0.043 {\AA}$^{-1}$, centered around a 0.16 eV deep local minimum in the dispersion of the valence band at the high-symmetry point. Intense circular dichroism is observed. This dispersion is the result of strong spin-orbit coupling. Spin-orbit coupling is also present in the room-temperature phase. The coupling strength is one of the largest reported so far.