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arXiv:2011.08537 · Physical review. B./Physical review. B

Finding the nitrogen-vacancy singlet manifold energy level using charge-conversion pulse sequences

Idan Meirzada, Sigal A. Wolf, Nir Bar‐Gill

Published Oct 8, 2021• 3 citations
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Abstract

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 ${\mathrm{NV}}^{0}$ population, and discuss their efficiency for different regimes in the relevant spectrum.

DOI
10.1103/physrevb.104.155413

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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 ${\mathrm{NV}}^{\ensuremath{-}}$ 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.
Nitrogen-vacancy (NV) centers in diamond have been used in recent years for a wide range of applications, from nanoscale NMR to quantum computation. These applications depend strongly on the efficient readout of the NV center's spin state, which is currently limited. Here we suggest a method of reading the NV center's spin state, using the weak optical transition in the singlet manifold. We numerically calculate the number of photons collected from each spin state using this technique, and show that an order of magnitude enhancement in spin-readout signal-to-noise ratio is expected, making single-shot spin readout within reach. Thus, this method could lead to an order of magnitude enhancement in sensitivity for ubiquitous NV-based sensing applications, and remove a major obstacle from using NVs for quantum information processing.
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 exploited as reliable single-photon emitters, with applications in quantum technologies and metrology. Two charge states are known for NV centers: NV0 and NV–, with the latter being mostly studied due to its long electron spin coherence time. Therefore, control over the charge state of the NV centers is essential. However, the understanding of the dynamics between the different states still remains challenging. Here we show that electron excitation induces the conversion from NV– to NV0 through electron-induced carrier generation. We present for the first time ultrafast pump-probe cathodoluminescence spectroscopy, with electron pulses as pump, and laser pulses as probe, to prepare and read out the NV states. The experimental data is explained with a model considering carrier dynamics (0.8 ns), NV0 spontaneous emission (20 ns) and NV0NV– back transfer (500 ms). Our results provide new insights into the NV–NV0 conversion dynamics, and into the use of pump-probe cathodoluminescence as a nanoscale NV characterization tool.
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 singlet states of the negatively charged nitrogen-vacancy centers in diamond play a key role in its optical spin control and readout. In this work, the hitherto unknown ionization energy of the singlet is measured experimentally and found to be in the range 1.91--2.25 eV. This is obtained by analyzing photoluminescence measurements incorporating spin control and nitrogen-vacancy charge state differentiation, along with simulations based on the nitrogen-vacancy's master equation. This work establishes a protocol for a more accurate estimate of this ionization energy, which can possibly lead to improved readout methods.