Excited-State Dynamics and Optically Detected Magnetic Resonance of Solid-State Spin Defects from First Principles
arxiv(2024)
摘要
Optically detected magnetic resonance (ODMR) is an efficient and reliable
method that enables initialization and readout of spin states through
spin-photon interface. In general, high quantum efficiency and large
spin-dependent photoluminescence (PL) contrast are desirable for reliable
quantum information readout. However, reliable prediction of the ODMR contrast
from first-principles requires accurate description of complex spin
polarization mechanisms of spin defects. These mechanisms often include
multiple radiative and nonradiative processes in particular intersystem
crossing (ISC) among multiple excited electronic states. In this work we
present our implementation of the first-principles ODMR contrast, by solving
kinetic master equation with calculated rates from ab initio electronic
structure methods then benchmark the implementation on the case of the
negatively-charged nitrogen vacancy (NV) center in diamond. We show the
importance of correct description of multi-reference electronic states for
accurate prediction of excitation energy, spin-orbit coupling, and the rate of
ISC. Moreover, we underscore the importance of pseudo Jahn-Teller effect for
the spin-orbit coupling, and the dynamical Jahn-Teller effect for
electron-phonon coupling, key factors determining ISC rates and ODMR contrast.
We show good agreement between our first-principles calculations and the
experimental ODMR contrast under magnetic field. We then demonstrate reliable
predictions of magnetic field direction, pump power, and microwave frequency
dependency, as important parameters for ODMR experiments. Our work clarifies
the important excited-state relaxation mechanisms determining ODMR contrast and
provides a predictive computational platform for spin polarization and optical
readout of solid-state quantum defects from first principles.
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