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ACS Photonics

Charge State Manipulation of NV Centers in Diamond under Phonon-Assisted Anti-Stokes Excitation of NV0

Yuanfei Gao, Jia‐Min Lai, Yujia Sun, Xue‐Lu Liu, Chaonan Lin, Ping‐Heng Tan, Chongxin Shan, Jun Zhang

Published Apr 26, 2022• 21 citations
Publisher

Abstract

The manipulation of the charge states of nitrogen-vacancy (NV) centers in diamond is a prerequisite for next-generation quantum sensing, communication, and computing. Here, we use phonon-assisted anti-Stokes excitation to realize the reversible conversion between the NV 0 and NV – states. In this case, we observe two decay processes of NV – centers with lifetimes as long as tens of seconds. By studying the kinetics of spectral structure evolution of NV – states, we find that the spectral structure of the NV – center is modulated by the charge state transition process under anti-Stokes excitation. We propose that the main reason is the local electric field generated by the ionization of the NV –, which changes the radiation environment of the color centers. Our results might provide an alternative method to control the charge states of nitrogen-vacancy centers.

DOI
10.1021/acsphotonics.1c01928

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•Jun 17, 2019•0 citations
The manipulation of the charge states of nitrogen-vacancy (NV) centers in diamond is a prerequisite for next-generation quantum sensing, communication, and computing. Here, we use phonon-assisted anti-Stokes excitation to realize the reversible conversion between the NV 0 and NV – states. In this case, we observe two decay processes of NV – centers with lifetimes as long as tens of seconds. By studying the kinetics of spectral structure evolution of NV – states, we find that the spectral structure of the NV – center is modulated by the charge state transition process under anti-Stokes excitation. We propose that the main reason is the local electric field generated by the ionization of the NV –, which changes the radiation environment of the color centers. Our results might provide an alternative method to control the charge states of nitrogen-vacancy centers.
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.
The nitrogen-vacancy (NV) centre in diamond is a leading platform for room-temperature quantum sensing. Improvements in sensitivity require precise control of the NV charge state. Transitions from the neutral NV0^00 charge state to the negative NV−^-− charge state can occur during excitation with photon energies below the ZPL transition of NV0^00. These sub-resonant charge transitions limit modern initialisation protocols and have not been studied in full detail. In this paper we show that sub-resonant charge cycling arises from phonon-assisted anti-Stokes excitation. We further uncover the phonon states which contribute most strongly to the anti-Stokes transition via the development of novel quantitative models. The models indicate that low energy acoustic phonons strongly contribute to the transition close to the ZPL. At longer wavelengths a 43\,meV mode additionally impacts the charge cycling dynamics.
Anti-Stokes optical cooling in diamond nitrogen-vacancy (NV) centers is experimentally and numerically investigated. Photoluminescence-excitation spectroscopy reveals pronounced phonon-assisted anti-Stokes emission under excitation below the zero-phonon line (ZPL). However, the below-ZPL excitation drives photoinduced charge-state conversion between negatively-charged NV- and neutral NV0, thereby suppressing the NV- mediated cooling channel. Time-resolved photoluminescence (PL) measurements reveal an increase in the effective PL lifetime with excitation density, reflecting an increasing NV0 contribution. By fitting nanosecond and millisecond PL dynamics with a minimal rate-equation model, we extract effective optical pumping and charge-conversion rates, which enables us to quantitatively simulate the cooling performance. The simulations predict a self-limiting behavior of anti-Stokes cooling and clarify the excitation conditions under which net cooling can be sustained within this effective model. The estimated cooling power per NV center is comparable, on a microscopic basis, to values discussed for semiconductor quantum dots and rare-earth optical coolers. These results identify charge-state conversion as a key bottleneck for defect-based optical refrigeration.
The nitrogen-vacancy (NV) center in nanodiamonds has emerged as an excellent platform in quantum technologies due to its applications in spin manipulation and nanoscale sensing. However, their use is limited by the unavoidable charge-state conversion under optical pumping. In this study, we investigate the control of charge-state conversion in NV centers using an engineered photonic environment and thus change the available local density of optical states (LDOS). The spectral- and pump-dependent decay rate measurements are performed to study the redistribution of emission rates due to the change in LDOS and their effect on charge-state conversion. We have achieved an 8% enhancement of emission rate at the zero phonon line which is accompanied with a 10% suppression in the phonon sideband emission rate in the low-pump-power regime. In the high-pump-power regime, the charge-state conversion becomes inevitable and leads to the deterioration of LDOS-induced modification in the NV center emission lifetimes. The results are useful for efficient NV center spin readout and charge-state depletion microscopy utilizing reversible charge-state conversion.
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.
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.