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arXiv:2403.10941 · Advanced Science

Photo‐Induced Charge State Dynamics of the Neutral and Negatively Charged Silicon Vacancy Centers in Room‐Temperature Diamond

G. Garcia‐Arellano, Gabriel I. López‐Morales, Neil B. Manson, Johannes Flick, A. A. Wood, Carlos A. Meriles

Published Mar 12, 2024• 12 citations
arXivHTMLPDF

Abstract

Abstract The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi‐color confocal microscopy and density functional theory are used to examine photo‐induced SiV recombination — from neutral, to single‐, to double‐negatively charged — over a broad spectral window in chemical‐vapor‐deposition (CVD) diamond under ambient conditions. For the SiV0 to SiV‐ transition, a linear growth of the photo‐recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV‒, on the other hand, yields only fractional recombination into SiV2‒, a finding that is interpreted in terms of a photo‐activated electron tunneling process from proximal nitrogen atoms.

DOI
10.1002/advs.202308814

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Abstract The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi‐color confocal microscopy and density functional theory are used to examine photo‐induced SiV recombination — from neutral, to single‐, to double‐negatively charged — over a broad spectral window in chemical‐vapor‐deposition (CVD) diamond under ambient conditions. For the SiV0 to SiV‐ transition, a linear growth of the photo‐recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV‒, on the other hand, yields only fractional recombination into SiV2‒, a finding that is interpreted in terms of a photo‐activated electron tunneling process from proximal nitrogen atoms.
The silicon vacancy (SiV) center in diamond is typically found in three stable charge states, SiV 0, SiV –, and SiV 2–, but studying the processes leading to their formation is challenging, especially at room temperature, due to their starkly different photoluminescence rates. Here, we use confocal fluorescence microscopy to activate and probe charge interconversion between all three charge states under ambient conditions. In particular, we witness the formation of SiV 0 via the two-step capture of diffusing, photogenerated holes, a process we expose both through direct SiV 0 fluorescence measurements at low temperatures and confocal microscopy observations in the presence of externally applied electric fields. In addition, we show that continuous red illumination induces the converse process, first transforming SiV 0 into SiV – and then into SiV 2– . Our results shed light on the charge dynamics of SiV and promise opportunities for nanoscale sensing and quantum information processing.
Point defects in wide-band-gap semiconductors are emerging as versatile resources for nanoscale sensing and quantum information science, but our understanding of the photoionization dynamics is presently incomplete. Here, we use two-color confocal microscopy to investigate the dynamics of charge in type 1b diamond hosting nitrogen-vacancy (NV) and silicon-vacancy (SiV) centers. By examining the nonlocal fluorescence patterns emerging from local laser excitation, we show that, in the simultaneous presence of photogenerated electrons and holes, SiV (NV) centers selectively transform into the negative (neutral) charge state. Unlike NVs, 532 nm illumination ionizes SiV^{-} via a single-photon process, thus hinting at a comparatively shallower ground state. In particular, slower ionization rates at longer wavelengths suggest the latter lies approximately ∼1.9 eV below the conduction band minimum. Building on the above observations, we demonstrate on-demand SiV and NV charge initialization over large areas via green laser illumination of variable intensity.
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.
The nitrogen–vacancy centre (NV) has drawn much attention for over a decade, yet detailed knowledge of the photophysics needs to be established. Under typical conditions, the NV can have two stable charge states, negative (NV − ) or neutral (NV 0 ), with photo-induced interconversion of these two states. Here, we present detailed studies of the ionization dynamics of single NV centres in bulk diamond at room temperature during illumination and its dependence on the excitation wavelength and power. We apply a recent method which allows us to directly measure the charge state of a single NV centre, and observe its temporal evolution. We find that the steady-state NV − population is always ⩽75% for 450–610 nm excitation wavelength. In combination with saturation measurements, we show that the optimal excitation wavelength is around 510–540 nm. Furthermore, the relative absorption cross-section of NV − is determined for 540–610 nm, revealing a double-peak structure. Finally, the energy of the NV − ground state of 2.6 eV below the conduction band is measured. These results reveal new insights into the charge state dynamics of the NV centre.
This work is focused on the investigation of the X‐ray's interaction with the color centers in diamond. X‐rays have the high penetrating power of radiation, which allows performing unhindered modifications deeply in the bulk of diamond crystals. Herein, it is shown that X‐rays irradiation of diamond can change the charge states of its defects, including silicon‐vacancy (SiV) and nitrogen‐vacancy (NV) color centers. By studying low‐temperature absorption spectra, it is shown that negatively charged SiV− and NV− centers partially transform into neutrally charged SiV0 and NV0 centers, accordingly. In addition, new absorption lines are registered, which may belong to other charge states of color centers. The results open a new way for the study of charge states for defects in various crystals (not limited to diamond), as well as allow the control over the charge state of color centers for diamond‐based quantum optics.
Diamond nanoparticles with optically active color centers can be used in nanoscale devices for quantum networking and sensing. A particular interest is focused on nanodiamonds (NDs) containing a small ensemble of negatively charged silicon‐vacancy (SiV) centers. Such NDs can be integrated with on‐chip optical structures. Here, chemical vapor deposition (CVD) is used to synthesize diamond particles of less than 100 nm in size containing 10–20 centers per ND. Two types of NDs grown on a Si substrate are studied, seeded with detonation NDs and without any seeding. The SiV luminescence under off‐resonant and resonant laser excitation at the temperature of 15 K is investigated. The emission lines of SiVs of individual NDs are well resolved and found to be spread in the range of 730–750 nm. The typical SiV linewidth is within 1–2 GHz for spontaneous NDs, which is only a factor of 2.5–5 broader than the lifetime limited linewidth of the SiV at 15 K. The emission of a single SiV is highly stable for both types of samples. This work is a critical step toward the synthesis of SiVs suitable for the realization of integrated quantum photonic devices.