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    First-Principles Calculations of Internal Conversion Processes in Spin Defects

    Stefano Paolo Villani1,*, Yu Jin1,2, and Giulia Galli1,3,4,†

    • *Contact author: svillani@uchicago.edu
    • †Contact author: gagalli@uchicago.edu

    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 NV− center in diamond and identifying a previously overlooked nonradiative channel in the divacancy triplet lifetime in SiC.

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