Room-temperature defect-engineered spin functionalities in Ga(In)NAs alloys

Abstract: Semiconductor spintronics is one of the most interesting research fields that exploits both charge and spin properties for future photonics and electronic devices. Among many challenges of using spin in semiconductors, efficient generation of electron spin polarization at room temperature (RT) remains difficult. Recently, a new approach using defect-mediated spin filtering effect, employing -interstitial defects in Ga(In)NAs alloys, has been shown to turn the material into an efficient spin-polarized source capable of generating >40% conduction electron spin polarization at RT without an application of external fields. In order to fully explore the defectengineered spin functionalities, a better understanding and control of the spin filtering effects is required. This thesis work thus aims to advance our understanding, in terms of both physical and material insights, of the recently discovered spin filtering defects in Ga(In)NAs alloys. We have focused on the important issues of optimization and applications of the spin filtering effects.To improve spin filtering efficiency, important material and defect parameters must be addressed. Therefore, in Papers I–III formation of the  defects in Ga(In)NAs alloys has been examined under different growth and post-growth treatment conditions, as well as in different structures. We found that the  defects were the dominant and important nonradiative recombination centers in Ga(In)NAs epilayers and GaNAs/GaAs multiple quantum wells, independent of growth conditions and post-growth annealing. However, by varying growth and post-growth conditions, up to four configurations of the  defects, exhibiting different hyperfine  interaction (HFI) strengths between defect electron and nuclear (e-n) spins, have been found. This difference was attributed to different interstitial sites and/or complexes of  . Further studiesfocused on the effect of post-growth hydrogen (H) irradiation on the spin filtering effect. Beside the roles of H passivation of N resulting in bandgap reopening of the alloys, H treatment was shown to lead to complete quenching of the spin filtering effect, accompanied by strong suppression in the concentrations of the  defects. We concluded that the observed effect was due to the passivation of the  defects by H, most probably due to the formation of H- complexes.Optimizing spin filtering efficiency also requires detailed knowledge of spin interactions at the defect centers. This issue was addressed in Papers IV and V. From both experimental and theoretical studies, we were able to conclude that the HFI between e-n spins at the  defects led to e-n spin mixing, which degraded spin filtering efficiency at zero field.  Moreover, we have identified the microscopic origin of electron spin relaxation (T1) at the defect centers, that is, hyperfine-induced e-n spin cross-relaxation. Our finding thus provided a guideline to improve spin filtering efficiency by selectively incorporating the  defects with weak HFI by optimizing growth and post-growth treatment conditions, or by searching for new spin filtering defect centers containing zero nuclear spin.The implementation of the defect-engineered spin filtering effect has been addressed in Papers VI–VIII. First, we experimentally demonstrated for the first time at RT an efficient electron spin amplifier employing the  defects in Ga(In)NAs alloys, capable of amplifying a weak spin signal up to 27 times with a high cut-off frequency of 1 GHz. We further showed that the defectmediated spin amplification effect could turn the GaNAs alloy into an efficient RT optical spin detector. This enabled us to reliably conduct in-depth spin injection studies across a semiconductor heterointerface at RT. We found a strong reduction of electron spin polarization after optical spin injection from a GaAs layer into an adjacent GaNAs layer. This observation was attributed to severe spin loss across the heterointerface due to structural inversion asymmetry and probably also interfacial point defects.Finally, we went beyond the generation of strongly polarized electron spins. In Paper IX we focused on an interesting aspect of using strongly polarized electron spins to induce strong nuclear spin polarization at RT, relevant to solid-state quantum computation using a defect nuclear spin of long spin memory as a quantum bit (qubit). By combining the spin filtering effect and the HFI, we obtained a sizeable nuclear spin polarization of ~15% at RT that could be sensed by conduction electrons. This demonstrated the feasibility of controlling defect nuclear spins via conduction electrons even at RT, the first case ever being demonstrated in a semiconductor.