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Physical Review A

Multicolor-illuminated charge-state dynamics of the nitrogen-vacancy center in diamond

Peng Qian, Yunpeng Zhai, Jun Hu, Renfei Zheng, Bing Chen, Nanyang Xu

Published Sep 12, 2022• 12 citations
Publisher

Abstract

Charge-state conversion has been a very useful tool for improving the performance of nitrogen-vacancy (NV) centers in diamond in many application scenarios. Lasers of different colors are employed to manipulate the NV charge, ranging from blue to infrared. Here, we focus on the study of the charge-state dynamics under illumination of multicolors and their combination with infrared (IR) light, and the results are directly presented in terms of charge-state population. It is shown that each color of light serves some kind of superiority over others in charge-state conversion and a greatly improved conversion rate can be induced by the additional IR illumination. We report that the steady-state ${\mathrm{NV}}^{\ensuremath{-}}$ population is increased up to 82% by IR light, and it presents basically the same response trend to infrared power as that of fluorescence counts. We also report a fast-oscillating fluorescence time trace by modulating the IR power. We believe that our work offers some straightforward results that might be of interest to researchers and lead to a clearer understanding of the NV charge-state dynamics.

DOI
10.1103/physreva.106.033506

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Charge-state conversion has been a very useful tool for improving the performance of nitrogen-vacancy (NV) centers in diamond in many application scenarios. Lasers of different colors are employed to manipulate the NV charge, ranging from blue to infrared. Here, we focus on the study of the charge-state dynamics under illumination of multicolors and their combination with infrared (IR) light, and the results are directly presented in terms of charge-state population. It is shown that each color of light serves some kind of superiority over others in charge-state conversion and a greatly improved conversion rate can be induced by the additional IR illumination. We report that the steady-state NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath− population is increased up to 82% by IR light, and it presents basically the same response trend to infrared power as that of fluorescence counts. We also report a fast-oscillating fluorescence time trace by modulating the IR power. We believe that our work offers some straightforward results that might be of interest to researchers and lead to a clearer understanding of the NV charge-state dynamics.
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 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.
The vast research conducted on nitrogen-vacancy (NV) centers in diamond in recent years opened the door for a wide range of NV based applications. However, some properties of the NV center dynamics and energy levels remain unknown. In this work, we propose a charge-conversion pulsed sequence scheme for locating the NV center singlet manifold energy level, by multicolor excitation using a tunable laser. We present two approaches for readout, photoinduced current and NV0{\mathrm{NV}}^{0}NV0 population, and discuss their efficiency for different regimes in the relevant spectrum.
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.
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.
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.