Time-dependent broken-symmetry density functional theory simulation of the optical response of entangled paramagnetic defects: Color centers in lithium fluoride

Article

关键词: GENERALIZED GRADIENT APPROXIMATION;    HARTREE-FOCK;    F-CENTER;    EXCITATION-ENERGIES;    CIRCULAR-DICHROISM;    SPIN QUBITS;    EXCHANGE;    RANGE;    STATES;    THERMOCHEMISTRY;   

DOI  :  10.1103/PhysRevB.97.085138

来源: SCIE

【 摘 要 】

Parameter-free atomistic simulations of entangled solid-state paramagnetic defects may aid in the rational design of devices for quantum information science. This work applies time-dependent density functional theory (TDDFT) embedded-cluster simulations to a prototype entangled-defect system, namely two adjacent singlet-coupled F color centers in lithium fluoride. TDDFT calculations accurately reproduce the experimental visible absorption of both isolated and coupled F centers. The most accurate results are obtained by combining spin symmetry breaking to simulate strong correlation, a large fraction of exact (Hartree-Fock-like) exchange to minimize the defect electrons' self-interaction error, and a standard semilocal approximation for dynamical correlations between the defect electrons and the surrounding ionic lattice. These results motivate application of two-reference correlated ab initio approximations to the M-center, and application of TDDFT in parameter-free simulations of more complex entangled paramagnetic defect architectures.

【 授权许可】

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