A multiconfigurational study of the negatively charged nitrogen-vacancy center in diamond

Abstract

Deep defects in wide band gap semiconductors have emerged as leading qubit candidates for realizing quantum sensing and information applications. Due to the spatial localization of the defect states, these deep defects can be considered as artificial atoms/molecules in a solid state matrix. Here we show that unlike single-particle treatments, the multiconfigurational quantum chemistry methods, traditionally reserved for atoms/molecules, accurately describe the many-body characteristics of the electronic states of these defect centers and correctly predict properties that single-particle treatments fail to obtain. We choose the negatively charged nitrogen-vacancy (NV${}^{-}$) center in diamond as the prototype defect to study with these techniques due to its importance for quantum information applications and because its properties are well-known, which makes it an ideal benchmark system. By properly accounting for electron correlations and including spin-orbit coupling and dipolar spin-spin coupling in the quantum chemistry calculations, for the NV${}^{-}$ center in diamond clusters, we are able to: (i) show the correct splitting of the ground (first-excited) triplet state into two levels (four levels), (ii) calculate zero-field splitting values of the ground and excited triplet states, in good agreement with experiment, and (iii) calculate the energy differences between ground and exited spin-triplet and spin-singlet states, as well as their ordering, which are also found to be in good agreement with recent experimental data. The numerical procedure we have developed is general and it can screen other color centers whose properties are not well known but promising for applications.

arXiv comment14 pages and 5 figures

References in corpus (33)

• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Experimental loophole-free violation of a Bell inequality using entangled electron spins separated by 1.3 km
• Solid-state electronic spin coherence time approaching one second
• High-fidelity projective readout of a solid-state spin quantum register
• Coherent control of single spins in silicon carbide at room temperature
• The nitrogen-vacancy center in diamond re-visited
• Quantum error correction in a solid-state hybrid spin register
• Deterministic delivery of remote entanglement on a quantum network
• Properties of nitrogen-vacancy centers in diamond: group theoretic approach
• Universal control and error correction in multi-qubit spin registers in diamond
• Temperature and magnetic field dependent longitudinal spin relaxation in nitrogen-vacancy ensembles in diamond
• Ab initio supercell calculations on nitrogen-vacancy center in diamond: its electronic structure and hyperfine tensors
• High-fidelity spin and optical control of single silicon vacancy centres in silicon carbide
• Measurement and Control of Single Nitrogen-Vacancy Center Spins above 600 K
• Sensing remote nuclear spins
• Observation of the dynamic Jahn-Teller effect in the excited states of nitrogen-vacancy centers in diamond
• Low temperature studies of the excited-state structure of Nitrogen-Vacancy color centers in diamond
• Observation of an environmentally insensitive solid state spin defect in diamond
• The negatively charged nitrogen-vacancy centre in diamond: the electronic solution
• Optical properties of the nitrogen-vacancy singlet levels in diamond
• Coherent control of the silicon-vacancy spin in diamond
• New infrared emission of the NV centre in diamond: Zeeman and uniaxial stress studies
• Phonon-Induced Population Dynamics and Intersystem Crossing in Nitrogen-Vacancy Centers
• An \emph{ab initio} study on split silicon-vacancy defect in diamond: electronic structure and related properties
• Optical addressing of an individual erbium ion in silicon
• Quantum simulations of materials on near-term quantum computers
• All-optical control of a solid-state spin using coherent dark states
• \emph{Ab initio} calculation of spin-orbit coupling for NV center in diamond exhibiting dynamic Jahn-Teller effect
• Silicon vacancy center in 4H-SiC: Electronic structure and spin-photon interfaces
• The Delicate Balance of Static and Dynamic Electron Correlation
• The Infrared Absorption Band and Vibronic Structure of the Nitrogen-Vacancy Center in Diamond
• Solid-state electron spin lifetime limited by phononic vacuum modes
• Sensing individual nuclear spins with a single rare-earth electron spin

Cited by in corpus (13)

• Green's function formulation of quantum defect embedding theory
• Quantum embedding methods for correlated excited states of point defects: Case studies and challenges
• Electronic excitations of the charged nitrogen-vacancy center in diamond obtained using time-independent variational density functional calculations
• First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation
• Quantum Vibronic Effects on the Excitation Energies of the Nitrogen-Vacancy Center in Diamond
• Calculation of the energies of the multideterminant states of the nitrogen vacancy center in diamond with quantum Monte Carlo
• High temperature spectroscopy of nitrogen vacancy centers in diamond
• Computational Insights into Electronic Excitations, Spin-Orbit Coupling Effects, and Spin Decoherence in Cr(IV)-based Molecular Qubits
• Quantum Computation of Electronic Structure with Projector Augmented-Wave Method and Plane Wave Basis Set
• Optimum surface-passivation schemes for near-surface spin defects in silicon carbide
• Scalable surface ion trap design for magnetic quantum sensing and gradiometry
• Simulating one hundred entangled atoms using projected-interacting full configuration interaction wavefunctions corrected by projected density functionals
• Elucidating the Inter-system Crossing of the Nitrogen-Vacancy Center up to Megabar Pressures