All-electron density functional calculations for electron and nuclear spin interactions in molecules and solids

Abstract

The interaction between electronic and nuclear spins in the presence of external magnetic fields can be described by a spin Hamiltonian, with parameters obtained from first principles, electronic structure calculations. We describe an approach to compute these parameters, applicable to both molecules and solids, which is based on Density Functional Theory (DFT) and real-space, all-electron calculations using finite elements (FE). We report results for hyperfine tensors, zero field splitting tensors (spin-spin component) and nuclear quadrupole tensors of a series of molecules and of the nitrogen-vacancy center in diamond. We compare our results with those of calculations using Gaussian orbitals and plane-wave basis sets, and we discuss their numerical accuracy. We show that calculations based on FE can be systematically converged with respect to the basis set, thus allowing one to establish reference values for the spin Hamiltonian parameters, at a given level of DFT.

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Cited by in corpus (8)

• First-principles hyperfine tensors for electrons and holes in GaAs and silicon
• First-principles Studies of Strongly Correlated States in Defect Spin Qubits in Diamond
• Fast and robust all-electron density functional theory calculations in solids using orthogonalized enriched finite elements
• Decoherence of Nuclear Spins in the Proximity of Nitrogen Vacancy Centers in Diamond
• High temperature spectroscopy of nitrogen vacancy centers in diamond
• Ionic forces and stress tensor in all-electron DFT calculations using enriched finite element basis
• Generalized scaling of spin qubit coherence in over 12,000 host materials
• Finite-element methods for noncollinear magnetism and spin-orbit coupling in real-space pseudopotential density functional theory