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physica status solidi (a)

X‐Rays in Diamond Photonics: A New Way to Control Charge States of Color Centers

Eduard S. Sektarov, Vadim Sedov, Victor Ralchenko, Kirill N. Boldyrev

Published Sep 21, 2022• 5 citations
Publisher

Abstract

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.

DOI
10.1002/pssa.202200283

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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.
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.
Atomic‐scale impurity spins, also called color centers, in an otherwise spin‐free diamond host lattice have proven to be versatile tools for applications in solid‐state‐based quantum technologies ranging from quantum information processing (QIP) to quantum‐enhanced sensing and metrology. Due to its wide band gap, diamond can host hundreds of different color centers. However, their suitability for QIP or sensing applications has only been tested for a handful of these, with the nitrogen vacancy (NV) strongly dominating this field of research. Due to its limited optical properties, the success of the NV for QIP applications however strongly depends on the development of efficient photonic interfaces. In the past years the negatively charged silicon vacancy (SiV−) center received significant attention due to its highly favourable spectral properties such as narrow zero phonon line transitions and weak phonon sidebands. Here, the recent work investigating the SiV center's orbital and electron spin coherence properties is reviewed as well as techniques to coherently control its quantum state using microwave as well as optical fields. Also, potential future experimental directions to improve the SiV's coherence time scale and to develop it into a valuable tool for QIP applications are outlined.
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) color center in diamond has recently emerged as a promising qubit for quantum photonics. However, the electrical control and excitation of the SiV centers are challenging due to the low density of free carriers in doped diamond. Here, we realize electrical excitation of SiV centers in a single-crystal diamond membrane, which is promising for scalable photonic architectures. We further demonstrate electrical switching of the charge states of the SiV centers by applying a forward bias voltage to the fabricated diamond-membrane devices and identify the position of the SiV−/SiV0 charge transition level. Our findings provide a perspective toward electrical triggering of color centers in diamond and accelerate the development of scalable quantum nanophotonic technologies.
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.
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.