Near-band-gap photoinduced nuclear spin dynamics in semi-insulating GaAs: Hyperfine- and quadrupolar-driven relaxation

Abstract

Understanding and manipulating spin polarization and transport in the vicinity of semiconductor-hosted defects is a problem of present technological and fundamental importance. Here, we use high-field magnetic resonance to monitor the relaxation dynamics of spin-3/2 nuclei in semi-insulating GaAs. Our experiments benefit from the conditions created in the limit of low illumination intensities, where intermittent occupation of the defect site by photoexcited electrons leads to electric field gradient fluctuations and concomitant spin relaxation of the neighboring quadrupolar nuclei. We find indication of a heterogeneous distribution of polarization, governed by different classes of defects activated by either weak or strong laser excitation. Upon application of a train of light pulses of variable repetition rate and on/off ratio, we uncover an intriguing regime of mesoscale nuclear spin diffusion restricted by long-range, nonuniform electric field gradients. Given the slow time scale governing nuclear spin evolution, such optically induced polarization patterns could be exploited as a contrast mechanism to expose dark lattice defects or localized charges with nanoscale resolution.