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arXiv:1603.08066 · Physical review. B./Physical review. B

Charge state dynamics of the nitrogen vacancy center in diamond under 1064-nm laser excitation

Peng Ji, M. V. Gurudev Dutt

Published Jul 5, 2016• 56 citations
arXivHTMLPDF

Abstract

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 ${\mathrm{NV}}^{0}$ 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 ${\mathrm{NV}}^{0}$ 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.

DOI
10.1103/physrevb.94.024101

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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 NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath− under excitation with low power near-infrared (1064-nm) light, resulting in increased photoluminescence from the NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}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 NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}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.
The photophysics of the nitrogen-vacancy (NV) center in diamond has been extensively investigated. Especially the fast optical switch based on the NV centers' photoluminescence (PL) by the near-infrared laser (NIR) modulation has been demonstrated, but the photophysical processes behind it are still not fully understood. Here, the NIR modulation on the PL of an isolated single NV center in bulk diamond is probed and detected with precision at picosecond timescale. We thereby observe NIR optical excitation at the NV ground state as well as at the excited state. Meanwhile, a generalized model is constructed with additional energy levels that can be reached under NIR illumination. The transition rates from numerical simulations are demonstrated in good agreement with the experimental results. Our findings may provide insights into the understanding of the NV center's related photophysics and open intriguing prospects such as reversible optical switching, super-resolution microscopy, and so forth.
Nitrogen vacancy (NV) centers in diamond have been identified over the past few years as promising systems for a variety of applications, ranging from quantum information science to magnetic sensing. This relies on the unique optical and spin properties of the negatively charged NV. Many of these applications require shallow NV centers, i.e., NVs that are close (a few nm) to the diamond surface. In recent years there has been increasing interest in understanding the spin and charge dynamics of NV centers under various illumination conditions, specifically under infrared (IR) excitation, which has been demonstrated to have significant impact on the NV centers' emission and charge state. Nevertheless, a full understanding of all experimental data is still lacking, with further complications arising from potential differences between the photodynamics of bulk and shallow NVs. Here we suggest a generalized quantitative model for NV center spin- and charge-state dynamics under both green and IR excitation. We experimentally extract the relevant transition rates, providing a comprehensive model which reconciles all existing experimental results in the literature, except for highly nonlinear regimes. Moreover, we identify key differences between the photodynamics of bulk and shallow NVs, and use them to significantly enhance the initialization fidelity of shallow NVs to the useful negatively charged state.
The nitrogen–vacancy centre (NV) has drawn much attention for over a decade, yet detailed knowledge of the photophysics needs to be established. Under typical conditions, the NV can have two stable charge states, negative (NV − ) or neutral (NV 0 ), with photo-induced interconversion of these two states. Here, we present detailed studies of the ionization dynamics of single NV centres in bulk diamond at room temperature during illumination and its dependence on the excitation wavelength and power. We apply a recent method which allows us to directly measure the charge state of a single NV centre, and observe its temporal evolution. We find that the steady-state NV − population is always ⩽75% for 450–610 nm excitation wavelength. In combination with saturation measurements, we show that the optimal excitation wavelength is around 510–540 nm. Furthermore, the relative absorption cross-section of NV − is determined for 540–610 nm, revealing a double-peak structure. Finally, the energy of the NV − ground state of 2.6 eV below the conduction band is measured. These results reveal new insights into the charge state dynamics of the NV centre.
The nitrogen vacancy (NV) center in diamond is the most widely studied color center in diamond for its wide range of applications in both physics and biology. The negatively charged state ${\mathrm{NV}}^{\ensuremath{-}}$ is often favored for its better spin-optical properties, whereas the presence of the neutral charge state NV0{\mathrm{NV}}^{0}NV0 is often minimized or neglected by using a single optimized excitation wavelength. In many cases, the use of additional laser wavelengths has an important impact on the NV optical properties and can lead to a dramatically quenched fluorescence. Through measurements of the photophysics of the NV center we show in this work that this quenching mechanism is mediated by charge state interconversion providing additional channels for nonradiative decay. Our results show that this mechanism is also sensitive to the spin state of the ${\mathrm{NV}}^{\ensuremath{-}}$. A better understanding of this physical mechanism will help mitigate the spin and charge state depolarization effects that are detrimental for quantum technology applications.
Anti-Stokes optical cooling in diamond nitrogen-vacancy (NV) centers is investigated using photoluminescence (PL) spectroscopy, time-resolved measurements, and rate-equation modeling. Under excitation below the zero-phonon line, anti-Stokes emission from the negatively charged NV- state appears, but optical excitation also induces charge-state conversion between NV- and neutral NV0. Excitation-dependent PL dynamics reveal a reduction of the NV- population under strong excitation. A minimal rate-equation model constrained by nanosecond and millisecond PL measurements predicts that photoionization suppresses the NV--mediated cooling contribution and leads to self-limiting cooling behavior. The calculations further show that net cooling requires exceptionally high quantum efficiency and does not increase monotonically with excitation density. These results highlight photoinduced charge-state conversion as a key photophysical bottleneck for defect-based anti-Stokes optical cooling.
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.