Electron-nuclear spin dynamics of Ga$^{2+}$ paramagnetic centers probed by spin dependent recombination: A master equation approach

TL;DR

This paper develops a master equation model to describe electron-nuclear spin dynamics in gallium paramagnetic centers in GaAsN, explaining experimental observations and proposing a spectroscopy protocol for further investigation.

Contribution

It introduces a novel master equation approach to model spin interactions in gallium centers, elucidating relaxation mechanisms and spin filtering amplification.

Findings

Good agreement with experimental data

Hyperfine and relaxation mechanisms are key to spin filtering

Proposes a time-resolved spectroscopy protocol

Abstract

Similar to nitrogen-vacancy centers in diamond and impurity atoms in silicon, interstitial gallium deep paramagnetic centers in GaAsN have been proven to have useful characteristics for the development of spintronic devices. Among other interesting properties, under circularly polarized light, gallium centers in GaAsN act as spin filters that dynamically polarize free and bound electrons reaching record spin polarizations (100\%). Furthermore, the recent observation of the amplification of the spin filtering effect under a Faraday configuration magnetic field has suggested that the hyperfine interaction that couples bound electrons and nuclei permits the optical manipulation of its nuclear spin polarization. Even though the mechanisms behind the nuclear spin polarization in gallium centers are fairly well understood, the origin of nuclear spin relaxation and the formation of an Overhauser-like magnetic field remain elusive. In this work we develop a model based on the master equation approach to describe the evolution of electronic and nuclear spin polarizations of gallium centers interacting with free electrons and holes. Our results are in good agreement with existing experimental observations. In regard to the nuclear spin relaxation, the roles of nuclear dipolar and quadrupolar interactions are discussed. Our findings show that, besides the hyperfine interaction, the spin relaxation mechanisms are key to understand the amplification of the spin filtering effect and the appearance of the Overhauser-like magnetic field. Based on our model's results we propose an experimental protocol based on time resolved spectroscopy. It consists of a pump-probe photoluminescence scheme that would allow the detection and the tracing of the electron-nucleus flip-flops through time resolved PL measurements.