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Nano Letters

Ultrafast Conversion of Two Charge States of Nitrogen-Vacancy Centers in Diamond via Two-Photon Excitation

Zhicheng Su, Mengting Yang, Doudou Sun, Zheng-Yuan Xue, Yulong Wang, Y.H. Lu, Jiqiang Ning, Changcheng Zheng, Junpeng Lü, Shijie Xu, Zhenhua Ni

Published Oct 24, 2025• 1 citation
Publisher

Abstract

Ultrafast conversion dynamics between the NV 0 and NV – charge states in diamond is crucial for spin-state manipulation and readout. However, the underlying mechanism of the conversion, including the effective excitation wavelength, the time scales of the conversion, and the influencing factors, is still unclear. Here, we proposed a method to probe the ultrafast conversion of the two charge states via two-photon excitation with femtosecond laser pulses separated by 12.5 ns. We found that the highest conversion efficiency occurs at the excitation wavelength of around 532 nm, and the efficiency increases with temperature as well. The conversion time from NV 0 to NV – is obtained to be around 75 ps at 300 K. These findings advance the understanding of NV center charge-state dynamics and provide insights for high-speed spin readout in quantum information applications.

DOI
10.1021/acs.nanolett.5c05150

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Ultrafast conversion dynamics between the NV 0 and NV – charge states in diamond is crucial for spin-state manipulation and readout. However, the underlying mechanism of the conversion, including the effective excitation wavelength, the time scales of the conversion, and the influencing factors, is still unclear. Here, we proposed a method to probe the ultrafast conversion of the two charge states via two-photon excitation with femtosecond laser pulses separated by 12.5 ns. We found that the highest conversion efficiency occurs at the excitation wavelength of around 532 nm, and the efficiency increases with temperature as well. The conversion time from NV 0 to NV – is obtained to be around 75 ps at 300 K. These findings advance the understanding of NV center charge-state dynamics and provide insights for high-speed spin readout in quantum information applications.
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.
Abstract Nitrogen-vacancy (NV) centers in diamond are 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, an understanding of the dynamics between the different states still remains challenging. Here, conversion from NV– to NV0 due to electron-induced carrier generation is shown. Ultrafast pump–probe cathodoluminescence spectroscopy is presented for the first time, with electron pulses as pump and laser pulses as probe, to prepare and read out the NV states. The experimental data are explained with a model considering carrier dynamics (0.8 ns), NV0 spontaneous emission (20 ns), and NV0 → NV– back transfer (500 ms). The results provide new insights into the NV– → NV0 conversion dynamics and into the use of pump–probe cathodoluminescence as a nanoscale NV characterization tool.
The conversion between two nitrogen vacancy (NV) center charge states (NV0 and NV−) was experimentally studied with laser in the range from 378 to 492 nm. The wavelength and power dependent charge state conversion was proved to be single-photon process at short wavelength and two-photon process at long wavelength. Also, the presence of metastable state in NV− significantly affected the conversion process, which can be used to increase NV− population from 72.5% to 80.5% by applying a magnetic field under 532 nm excitation. The method can be used for improving the fidelity of charge state polarization and subsequently optimizing the quantum control with NV center and resolution in the magnetometric and biological sensoring.
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.
We demonstrate the use of two-photon excitation for observing the ground-state optically detected magnetic resonance (ODMR) of nitrogen-vacancy centers in diamonds at room temperature. An ultrafast femtosecond laser at 1040 nm was used for excitation, while fluorescence signal readout was achieved through a combination of a PMT and a lock-in amplifier. The imaging capability of two-photon excitation fluorescence (2PEF) was utilized to map the relative distribution of NV centers in a bulk diamond and micro-sized diamonds. For the first time, to the best of our knowledge, ODMR traces of the nitrogen-vacancy center are observed with two-photon excitation, providing a promising tool for fast 3D quantum sensing and imaging.
Abstract Nitrogen-vacancy (NV) and silicon-vacancy (SiV) color defects in diamond are promising systems for applications in quantum technology. The NV and SiV centers have multiple charge states, and their charge states have different electronic, optical and spin properties. For the NV centers, most investigations for quantum sensing applications are targeted on the negatively charged NV (NV−), and it is important for the NV centers to be in the NV− state. However, it is known that the NV centers are converted to the neutrally charged state (NV0) under laser excitation. An energetically favorable charge state for the NV and SiV centers depends on their local environments. It is essential to understand and control the charge state dynamics for their quantum applications. In this work, we discuss the charge state dynamics of NV and SiV centers under high-voltage nanosecond pulse discharges. The NV and SiV centers coexist in the diamond crystal. The high-voltage pulses enable manipulating the charge states efficiently. These voltage-induced changes in charge states are probed by their photoluminescence spectral analysis. The analysis result from the present experiment shows that the high-voltage nanosecond pulses cause shifts of the chemical potential and can convert the charge states of NV and SiV centers with the transition rates of ∼MHz. This result also indicates that the major population of the SiV centers in the sample is the doubly negatively charged state (SiV2−), which is often overlooked because of its non-fluorescent and non-magnetic nature. This demonstration paves a path for a method of rapid manipulation of the NV and SiV charge states in the future.