First-principles hyperfine tensors for electrons and holes in GaAs and silicon

Understanding (and controlling) hyperfine interactions in semiconductor nanostructures is important for fundamental studies of material properties as well as for quantum information processing with electron, hole, and nuclear-spin states. Through a combination of first-principles density-functional theory (DFT) and k theory, we have calculated hyperfine tensors for electrons and holes in GaAs and crystalline silicon. Accounting for relativistic effects near the nuclear core, we find contact hyperfine interactions for electrons in GaAs that are consistent with Knight-shift measurements performed on GaAs quantum wells and are roughly consistent with prior estimates extrapolated from measurements on InSb. We find that a combination of DFT and k theory (DFT+k) is necessary to accurately determine the contact hyperfine interaction for electrons at a conduction-band minimum in silicon that is consistent with bulk Knight-shift measurements. For hole spins in GaAs, the overall magnitude of the hyperfine couplings we find from DFT is consistent with previous theory based on free-atom properties, and with heavy-hole Overhauser shifts measured in GaAs (and InGaAs) quantum dots. In addition, we theoretically predict that the heavy-hole hyperfine coupling to the As nuclear spins is stronger and almost purely Ising, while the (weaker) coupling to the Ga nuclear spins has significant non-Ising corrections. In the case of hole spins in silicon, we find (surprisingly) that the strength of the hyperfine interaction in the valence band is comparable to that in the conduction band and that the hyperfine tensors are highly anisotropic (Ising) in the heavy-hole subspace. These results suggest that the hyperfine coupling cannot be ruled out as a limiting mechanism for coherence (T₂^*) times recently measured for heavy holes in silicon quantum dots.