First-Principles Calculations of Internal Conversion Processes in Spin Defects
Phys. Rev. Lett. 137, 163603 – Published 14 October, 2026
DOI: https://doi.org/10.1103/y6z6-h16k
Abstract
Optically active spin defects are foundational for quantum technologies, yet common approximations underestimate their internal conversion (IC) rates by orders of magnitude. We propose a broad, predictive framework to compute IC rates that incorporates multiconfigurational effects via many-body wave functions in time-dependent density functional theory (TDDFT) and includes all-phonon-mode contributions via analytical nonadiabatic couplings. Our approach resolves discrepancies with experiment, achieving quantitative agreement for the center in diamond and identifying a previously overlooked nonradiative channel in the divacancy triplet lifetime in SiC.