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Journal of Applied Physics

Photoexcitation and recombination processes of the neutral nitrogen-vacancy center in diamond from first principles

Gergő Thiering, Ádám Gali

Published Aug 27, 2024• 12 citations
Publisher

Abstract

Nitrogen-vacancy (NV) complex in diamond is one of the most prominent solid state defects as the negatively charged NV defect (NV−) is a leading contender for quantum technologies. In quantum information processing applications, NV− is photoexcited that often leads to photoionization to neutral NV defect, NV0, and re-ionization back to NV− should occur to control the S=1 spin of NV−. As a consequence, understanding the photophysics of NV0 is crucial for controlling NV−. Furthermore, recent studies have shown that the S=1/2 electron spin of NV0 can also be initialized and read out at certain conditions that turns single NV0 a potential quantum bit. Quantum optics protocols rest on detailed knowledge on the electronic structure of the given system, which is obviously missing for NV0 in diamond. In this study, we combine the group theory and density functional theory calculations toward exploring the nature of the ground and excited states of NV0. We show that the effective three-electron system of NV0 leads to high correlation effects that make this system very challenging for ab initio simulations.

DOI
10.1063/5.0221228

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Nitrogen-vacancy (NV) complex in diamond is one of the most prominent solid state defects as the negatively charged NV defect (NV−) is a leading contender for quantum technologies. In quantum information processing applications, NV− is photoexcited that often leads to photoionization to neutral NV defect, NV0, and re-ionization back to NV− should occur to control the S=1 spin of NV−. As a consequence, understanding the photophysics of NV0 is crucial for controlling NV−. Furthermore, recent studies have shown that the S=1/2 electron spin of NV0 can also be initialized and read out at certain conditions that turns single NV0 a potential quantum bit. Quantum optics protocols rest on detailed knowledge on the electronic structure of the given system, which is obviously missing for NV0 in diamond. In this study, we combine the group theory and density functional theory calculations toward exploring the nature of the ground and excited states of NV0. We show that the effective three-electron system of NV0 leads to high correlation effects that make this system very challenging for ab initio simulations.
The negatively charged nitrogen-vacancy defect (NV)−^-− in diamond has attracted much attention in recent years in qubit and biological applications. The negative charge is donated from nearby nitrogen donors that could limit or stem the successful application of (NV)−^-−. In this Letter, we unambiguously identify the \emph{neutral} nitrogen-vacancy defect (NV0^00) by \emph{ab initio} supercell calculations. Our analysis shows that i) the spin state can be \emph{selectively} occupied optically, ii) the electron spin state can be manipulated by time-varying magnetic field, and iii) the spin state may be read out optically. Based on this NV0^00 is a new hope for realizing qubit in diamond \emph{without} the need of nitrogen donors.
The negatively charged nitrogen-vacancy defect $({\text{NV}}^{\ensuremath{-}})$ in diamond has attracted much attention in recent years in qubit and biological applications. The negative charge is donated from nearby nitrogen donors that could limit or stem the successful application of ${\text{NV}}^{\ensuremath{-}}$. In this study, we identify the neutral nitrogen-vacancy defect (NV0)({\text{NV}}^{0})(NV0) by ab initio supercell calculations through the comparison of the measured and calculated hyperfine tensors of the 4A2{^{4}A}_{2}4A2​ excited state. Our analysis shows that (i) the spin state can be selectively occupied optically, (ii) the electron spin state can be manipulated by time-varying magnetic field, and (iii) the spin state may be read out optically. Based on this NV0{\text{NV}}^{0}NV0 is a hope for realizing qubit in diamond without the need of nitrogen donors. In addition, we propose that NV0{\text{NV}}^{0}NV0 may be more sensitive magnetometer than the ultrasensitive ${\text{NV}}^{\ensuremath{-}}$.
Abstract Nitrogen-vacancy (NV) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.
Nitrogen-vacancy center in diamond is a solid state defect qubit with favorable coherence time up to room temperature which could be harnessed in several quantum enhanced sensor and quantum communication applications, and has a potential in quantum simulation and computing. The quantum control largely depends on the intricate details about the electronic structure and states of the nitrogen-vacancy center, radiative and non-radiative rates between these states and the coupling of these states to external spins, electrical, magnetic and strain fields and temperature. In this review paper it is shown how first principles calculations contributed to understanding the properties of nitrogen-vacancy center, and will be briefly discussed the issues to be solved towards full \emph{ab initio} description of solid state defect qubits.
Abstract The nitrogen‐vacancy (NV) center in diamond is a solid‐state defect qubit with favorable coherence time up to room temperature, which could be harnessed in several quantum‐enhanced sensor and quantum communication applications, and has a potential in quantum simulation and computing. The quantum control largely depends on the intricate details about the electronic structure and states of the NV center, the radiative and nonradiative rates between these states, and the coupling of these states to external spins, electric, magnetic, and strain fields, and temperature. This review shows how first‐principles calculations contributed to understanding the properties of the NV center and briefly discusses the issues to be solved toward the full ab initio description of solid‐state defect qubits.
Optical initialization of the negatively charged nitrogen-vacancy (NV − ) center in diamond makes it one of the best candidates for realization of addressable spins in the solid state for quantum computing and other studies. However, its exact mechanism was not clear. We show that exact diagonalization of a many-electron Hamiltonian with parameters derived from ab initio GW calculations puts strong constraints on the mechanism. The energy surfaces of the low-energy many-body states and the relaxation processes of photoexcitation responsible for the optical initialization are calculated. Intersystem crossings are shown to be essential.