Using ground state and excited state density functional theory to decipher 3d dopant defects in GaN

Abstract

Using ground state density functional theory (DFT) and implementing an occupation-constrained DFT (occ-DFT) for self-consistent excited state calculations, we decipher the electronic structure of the Mn dopant and other 3d defects in GaN across the band gap. Our analysis, validated with broad agreement with defect levels (ground state calculations) and photoluminescence data (excited state calculations), mandates broad reinterpretation of 3d defect data in GaN. The MnGa defect spans stable charge states from (1-) in n-type GaN through (2+) in p-type GaN. The Mn(2+) is predicted to be a d2 ground state spin triplet defect with a singlet excited state, isoelectronic with the defect associated with the 1.19 eV photoluminescence in n-type GaN. The combined analysis of defect levels and excited states invites reassessment of all d2-capable dopants in GaN. We demonstrate that the 1.19 eV defect, a candidate defect for optically controlled quantum applications, cannot be the Cr(1+) assumed in literature and instead must be the V(0). The combined ground-state/excited-state DFT analysis is shown to be able to chemically fingerprint defects.