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arXiv:1204.4898 · Physical Review Letters

Optically Controlled Switching of the Charge State of a Single Nitrogen-Vacancy Center in Diamond at Cryogenic Temperatures

Petr Siyushev, Hugo Pinto, Márton Vörös, Ádám Gali, Fedor Jelezko, Jörg Wrachtrup

Published Apr 16, 2013• 250 citations
arXivHTMLPDF

Abstract

In this Letter, the photoinduced switching of the single nitrogen-vacancy (NV) center between two different charge states, negative (${\mathrm{NV}}^{\ensuremath{-}}$) and neutral (${\mathrm{NV}}^{0}$), is studied under resonant excitation at liquid helium temperature. We show that resonant conversion of ${\mathrm{NV}}^{0}$ to ${\mathrm{NV}}^{\ensuremath{-}}$ significantly improves spectral stability of the ${\mathrm{NV}}^{\ensuremath{-}}$ defect and allows high fidelity initialization of the spin qubit. Based on density functional theory calculations a novel mechanism involving an Auger ionization of ${\mathrm{NV}}^{\ensuremath{-}}$ and charge transfer of an electron from the valence band to ${\mathrm{NV}}^{0}$ is discussed. This study provides further insight into the charge dynamics of the NV center, which is relevant for quantum information processing based on an ${\mathrm{NV}}^{\ensuremath{-}}$ defect in diamond.

DOI
10.1103/physrevlett.110.167402

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In this Letter, the photoinduced switching of the single nitrogen-vacancy (NV) center between two different charge states, negative (NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath−) and neutral (NV0{\mathrm{NV}}^{0}NV0), is studied under resonant excitation at liquid helium temperature. We show that resonant conversion of NV0{\mathrm{NV}}^{0}NV0 to NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath− significantly improves spectral stability of the NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath− defect and allows high fidelity initialization of the spin qubit. Based on density functional theory calculations a novel mechanism involving an Auger ionization of NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath− and charge transfer of an electron from the valence band to NV0{\mathrm{NV}}^{0}NV0 is discussed. This study provides further insight into the charge dynamics of the NV center, which is relevant for quantum information processing based on an NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath− defect in diamond.
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.
We report a study of the 3E excited-state structure of single negatively charged nitrogen-vacancy (NV) defects in diamond, combining resonant excitation at cryogenic temperatures and optically detected magnetic resonance. A theoretical model is developed and shows excellent agreement with experimental observations. In addition, we show that the two orbital branches associated with the 3E excited state are averaged when operating at room temperature. This study leads to an improved physical understanding of the NV defect electronic structure, which is invaluable for the development of diamond-based quantum information processing.
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.
Charge state instabilities have been a bottleneck for the implementation of solid-state spin systems and pose a major challenge to the development of spin-based quantum technologies. Here we investigate the stabilization of negatively charged nitrogen-vacancy (NV−^-−) centers in phosphorus-doped diamond at liquid helium temperatures. Photoionization of phosphorous donors in conjunction with charge diffusion at the nanoscale enhances NV0^00 to NV−^-− conversion and stabilizes the NV−^-− charge state without the need for an additional repump laser. The phosphorus-assisted stabilization is explored and confirmed both with experiments and our theoretical model. Stable photoluminescence-excitation spectra are obtained for NV−^-− centers created during the growth. The fluorescence is continuously recorded under resonant excitation to real-time monitor the charge state and the ionization and recombination rates are extracted from time traces. We find a linear laser power dependence of the recombination rate as opposed to the conventional quadratic dependence, which is attributed to the photo-ionization of phosphorus atoms.
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 ${\text{NV}}^{\ensuremath{-}}$.
The photophysics and charge state dynamics of the nitrogen vacancy (NV) center in diamond has been extensively investigated, but is still not fully understood. In contrast to previous work, we find that NV0{\mathrm{NV}}^{0}NV0 converts to ${\mathrm{NV}}^{\ensuremath{-}}$ under excitation with low power near-infrared (1064-nm) light, resulting in increased photoluminescence from the ${\mathrm{NV}}^{\ensuremath{-}}$ state. We used a combination of spectral and time-resolved photoluminescence experiments and rate-equation modeling to conclude that NV0{\mathrm{NV}}^{0}NV0 converts to ${\mathrm{NV}}^{\ensuremath{-}}$ via absorption of 1064-nm photons from the valence band of diamond. We report fast quenching and recovery of the photoluminescence from both charge states of the NV center under low power 1064-nm laser excitation, which has not been previously observed. We also find, using optically detected magnetic resonance experiments, that the charge transfer process mediated by the 1064-nm laser is spin dependent.