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arXiv:1806.09191 · Physical Review A

Charge-state dynamics during excitation and depletion of the nitrogen-vacancy center in diamond

Luke R. P. Hacquebard, Lilian Childress

Published Jun 13, 2018• 62 citations
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Abstract

The charge-state dynamics of the nitrogen-vacancy (NV) center in diamond play a key role in a wide range of applications, yet remain imperfectly understood. Using single picosecond pulses and pulse pairs, we quantitatively investigate the charge dynamics associated with excitation and fluorescence depletion of a single NV center. Our pulsed excitation approach permits significant modeling simplifications and allows us to extract relative rates of excitation, stimulated emission, ionization, and recombination under 531 and 766 nm illumination. By varying the duration between paired pulses, we can also investigate ionization and recombination out of metastable states. Our results are directly applicable to experiments employing stimulated emission-depletion imaging and can be used to predict optimal operating regimes where excitation and stimulated emission are maximized relative to charge-state-switching processes.

DOI
10.1103/physreva.97.063408

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The charge-state dynamics of the nitrogen-vacancy (NV) center in diamond play a key role in a wide range of applications, yet remain imperfectly understood. Using single picosecond pulses and pulse pairs, we quantitatively investigate the charge dynamics associated with excitation and fluorescence depletion of a single NV center. Our pulsed excitation approach permits significant modeling simplifications and allows us to extract relative rates of excitation, stimulated emission, ionization, and recombination under 531 and 766 nm illumination. By varying the duration between paired pulses, we can also investigate ionization and recombination out of metastable states. Our results are directly applicable to experiments employing stimulated emission-depletion imaging and can be used to predict optimal operating regimes where excitation and stimulated emission are maximized relative to charge-state-switching processes.
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 (NV) center in diamond has been widely used for quantum information processing, nanophotonics, and biological imaging. In this work, we experimentally studied the charge-state conversion and stimulated emission of the NV center with a near-infrared (NIR) pumping laser. The competition between these two processes resulted in a nonmonotonic dependence of the NV center’s fluorescence intensity on the NIR laser power. Fluorescence enhancement was observed with a weak NIR laser, while fluorescence depletion was observed with a high-power NIR laser. It led to the nonmonotonic change of the spatial resolution with stimulated emission depletion microscopy, which has been used for subdiffraction imaging of the NV center. Our work can help to further understand the optical mechanism and extend the applications of the NV center.
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 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.
Charged nitrogen-vacancy (NV) color centers in diamond are excellent luminescence sources for far-field fluorescence nanoscopy by stimulated emission depletion (STED). Here we show that these photostable color centers can be visualized by STED using simple continuous-wave or high repetition pulsed lasers (76 MHz) at wavelengths >700 nm for STED. Furthermore, we show that NV centers can be imaged in three dimensions (3D) inside the diamond crystal and present single-photon signatures of single color centers recorded in high density samples, demonstrating a new recording scheme for STED and related far-field nanoscopy approaches. Finally, we exemplify the potential of using nanodiamonds containing NV centers as luminescence tags in STED microscopy. Our results offer new experimental avenues in nanooptics, nanotechnology, and the life sciences.
The charge state stability of nitrogen-vacancy (NV) centers critically affects their application as quantum sensors and qubits. Understanding charge state conversion and equilibration is important not only for NV centers in diamond but also for defects and impurities in wide-bandgap materials in general. The mechanisms by which these centers change charge state upon optical or electronic excitation without the presence of mobile carriers remain unclear. Here, we elucidate this issue for the case of photoionization of NV center ensembles. Using pump-probe spectroscopy, we ionize negatively charged NV centers and monitor the recovery of NV^{-} on timescales of up to several seconds. We find that the recovery rate depends strongly on the concentration of surrounding nitrogen donors. Remarkably, the equilibration dynamics exhibit no discernible dependence on temperature, ruling out thermally activated processes. We develop a multiphonon-assisted electron-tunneling model, supported by density-functional calculations, that explains the measurements and identifies tunneling as the equilibration mechanism. Because tunneling rates depend exponentially on donor separation, the random distribution of nitrogen donors spreads recovery times from nanoseconds to hours or longer.