Local Excitations of a Charged Nitrogen Vacancy in Diamond with Multireference Density Matrix Embedding Theory

28 February 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


We investigate the negatively charged nitrogen-vacancy center in diamond using periodic density matrix embedding theory (pDMET). To describe the strongly correlated excited states of this system, the complete active space self-consistent field (CASSCF) followed by n-electron valence state second-order perturbation theory (NEVPT2) was used as impurity solver. Since the NEVPT2-DMET energies show a linear dependence on the inverse of the size of the embedding subspace, we performed an extrapolation of the excitation energies to the non-embedding limit using linear regression. The extrapolated NEVPT2-DMET first triplet-triplet excitation energy is 2.31 eV and that for the optically inactive singlet-singlet transition is 1.02 eV, both in agreement with the experimentally observed vertical excitation energies of ~2.18 eV and ~1.26 eV, respectively. This is the first application of pDMET to a charged periodic system and the first investigation of the NV- defect using NEVPT2 for periodic supercell models.


Quantum Embedding
NV Defect in Diamond
Spin Qubit
Density Matrix Embedding Theory
Multireference Methods
Excited States
Electronic Structure
Strongly Correlated Systems
Localized Point Defects

Supplementary materials

Supporting Information
The finite cluster model, active space convergence, procedure to vary the size of embedding subspace, excitation energies using different numbers of embedding orbitals, extrapolation to the non-embedding limit, total energies and results with different basis sets.


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