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arXiv:2307.06433 · Materials for Quantum Technology

Probing NV and SiV charge state dynamics using high-voltage nanosecond pulse and photoluminescence spectral analysis

Artur Pambukhchyan, Sizhe Weng, Indu Aravind, Stephen B. Cronin, Susumu Takahashi

Published Sep 1, 2023• 4 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1088/2633-4356/acf750

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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.
ABSTRACT Defect and impurity centers in diamond can exist in multiple charge states. A notable example is a negatively and neutrally charged nitrogen‐vacancy center in diamond, whose optical and spin properties are very different. Recent DFT studies show that an energetically favorable charge state can be controlled by adjusting the chemical potential of the diamond sample, which often requires significant materials engineering. This study presents an alternative approach for the control of charge states with the use of nanosecond high‐voltage pulse discharges. We demonstrate the control of silicon‐vacancy (SiV) centers in diamond. Using time‐resolved photoluminescence (PL) spectroscopy measurement of the SiV centers with the application of nanosecond high‐voltage pulses, we show the emergence of the negatively charged SiV − state. We also employ the time‐resolved PL measurements and show that the population of the induced SiV − charge state decays exponentially, and the lifetime of the charge state is determined by 200–1100 ms. The observed long‐lived charge state is potentially useful for applications based on the SiV − center. This method also paved the way to access various charge states of defect and impurity centers in diamond and wide‐bandgap semiconductors.
Control over the charge states of color centers in solids is necessary to fully utilize them in quantum technologies. However, the microscopic charge dynamics of deep defects in wide-band-gap semiconductors are complex, and much remains unknown. We utilize a single-shot charge-state readout of an individual nitrogen-vacancy (NV) center to probe the charge dynamics of the surrounding defects in diamond. We show that the NV center charge state can be converted through the capture of holes produced by optical illumination of defects many micrometers away. With this method, we study the optical charge conversion of silicon-vacancy (SiV) centers and provide evidence that the dark state of the SiV center under optical illumination is SiV 2– . These measurements illustrate that charge carrier generation, transport, and capture are important considerations in the design and implementation of quantum devices with color centers and provide a novel way to probe and control charge dynamics in diamond.
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) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.
The charge state of a quantum point defect in a solid-state host strongly determines its optical and spin characteristics. Consequently, techniques for controlling the charge state are required to realize technologies for quantum networking and sensing. In this work, we demonstrate the use of deep-ultraviolet (DUV) radiation to dynamically neutralize nitrogen- (NV) and silicon-vacancy (SiV) centers. We first examine the neutralization of NV by correlating the NV – and NV 0 spectra, indicating > 99% polarization into NV 0 . We then examine the time dynamics of SiV – photoluminescence, observing an 80% reduction of intensity within a single 100 μs DUV pulse. Finally, we demonstrate that this DUV-induced bleaching is accompanied by a dramatic increase in the SiV 0 population that is robust to extended periods of near-infrared excitation. Our results indicate the potential of above-band gap excitation as a universal means of generating neutral charge states of quantum point defects on demand.
Silicon-vacancy defects have been identified as a promising optical transition for quantum communications, quantum control, and quantum information processing. In the work presented here, we demonstrate a voltage-controlled mechanism by which the photoluminescent (PL) emission from silicon-vacancy (Si-V) defects in diamond can be modulated. In particular, we can selectively produce emission from the negatively charged state of this defect (i.e., Si-V−), which exhibits narrow (Γ = 4 nm) emission at 738 nm at low laser power. This approach uses high voltage (2–5 kV) nanosecond pulses applied across top and bottom electrodes on a 0.5 mm thick diamond substrate. In the absence of high voltage pulses, we observe no emission at 738 nm. This feature increases monotonically with peak pulse voltage, pulse repetition rate (i.e., frequency), and incident laser intensity. We observe saturation of the PL intensity for pulse voltages above 3.2 kV and frequency above 100 Hz. Based on electrostatic simulations, we estimated the local electric field intensity near the tip of the Cu electrode to be 2.8 ×106 V/cm at these voltages. However, as a function of laser power, we observe a linear dependence of PL intensity without saturation. These saturating and non-saturating behaviors provide important insight into the voltage-induced charging mechanisms and kinetics associated with this process.