Optical spin orientation of localized electrons and holes interacting with nuclei in an FA_0.9Cs_0.1PbI_2.8Br_0.2 perovskite crystal

Optical orientation of carrier spins by circularly polarized light is the basic concept and tool of spin physics in semiconductors. We study the optical orientation of electrons and holes in a crystal of the FA_0.9Cs_0.1PbI_2.8Br_0.2 lead halide perovskite by means of polarized photoluminescence, time-resolved differential reflectivity, and time-resolved Kerr rotation. At the cryogenic temperature of 1.6 K the optical orientation degree measured for continuous-wave excitaton reaches 6 localized electrons and 2% for localized holes. Their contributions are distinguished from each other and from exciton optical orientation through the pronounced Hanle effect in transverse magnetic fields and the polarization recovery effect in longitudinal magnetic fields. The optical orientation degree is highly stable against detuning of the laser photon energy from the band gap by up to 0.25 eV, showing then a gradual decrease for detunings up to 0.9 eV. This evidences the inefficiency of spin relaxation mechanisms for free carriers during their energy relaxation. Spin relaxation for localized electrons and holes is provided by the hyperfine interaction with the nuclear spins. Dynamic polarization of nuclear spins is demonstrated by the Overhauser field reaching 4 mT acting on the electrons and -76 mT acting on the holes. This confirms the specifics of lead halide perovskite semiconductors, where the hole hyperfine interaction with the nuclei considerably exceeds that of the electron.