Spin-polarized exciton quantum beating in hybrid organic–inorganic perovskites

Abstract

Hybrid organic–inorganic perovskites have emerged as a new class of semiconductors that exhibit excellent performance as active layers in photovoltaic solar cells. These compounds are also highly promising materials for the field of spintronics due to their large and tunable spin–orbit coupling, spin-dependent optical selection rules, and their predicted electrically tunable Rashba spin splitting. Here we demonstrate the optical orientation of excitons and optical detection of spin-polarized exciton quantum beating in polycrystalline films of the hybrid perovskite CH3NH3PbClxI3−x. Time-resolved Faraday rotation measurement in zero magnetic field reveals unexpectedly long spin lifetimes exceeding 1 ns at 4 K, despite the large spin–orbit couplings of the heavy lead and iodine atoms. The quantum beating of exciton states in transverse magnetic fields shows two distinct frequencies, corresponding to two g-factors of 2.63 and −0.33, which we assign to electrons and holes, respectively. These results provide a basic picture of the exciton states in hybrid perovskites, and suggest they hold potential for spintronic applications. Hybrid perovskites are known to have excellent optoelectronic properties, but the observation of exciton states with long spin lifetimes suggests that they may also have potential spintronics applications.