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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 photo-excited 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, non-uniform 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.

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