Magneto-optical spectra of the split nickel-vacancy defect in diamond
Magneto-optical spectra of the split nickel-vacancy defect in diamond
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DOI：
10.1103/physrevresearch.3.043052
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发表时间：
2021-10-19
影响因子：
4.2
通讯作者：
Gali, Adam
中科院分区：
文献类型：
--
作者：
Thiering, Gergo;Gali, Adam
镍是高压高温金刚石中常见的杂质，可能会污染用于高功率电子或量子技术应用的化学气相沉积金刚石。镍的磁光指纹已经知道了几十年，然而，没有达成共识的微观起源镍相关的电子顺磁共振，光致发光，光学检测的磁共振光谱。金刚石中未知的镍相关缺陷结构使得难以控制它们或利用它们用于给定的应用。因此，镍被认为是钻石中的杂质，应避免或其浓度应最小化。从头算磁光光谱学发展的最新进展显着提高了其准确性和预测能力，可用于识别和深入表征钻石中的顺磁性色心。在这项研究中，我们扩展的准确性的从头算磁光光谱工具对自洽计算的二阶自旋轨道耦合的顺磁性色心在固体中。我们应用全套从头算磁光光谱工具来表征金刚石中最稳定的镍相关缺陷构型之一的分裂镍空位缺陷。其结果是，电子顺磁共振和光学中心的金刚石中的镍空位缺陷的各种电荷状态的积极确定。特别地，1.40-eV光学中心和NIRIM-2电子顺磁共振中心被确定为分裂的镍空位中心的单个负电荷状态。该缺陷具有S = 1/2自旋态和轨道二重态基态。我们发现，在低温下，基态自旋的相干时间约为0.1毫秒，可以通过A方案协议进行光学初始化和读出。由于缺陷具有反转对称性，因此光学信号对杂散电场不敏感，这对于创建不可区分的固态单光子源是有利的。我们预测，带负电荷的镍空位缺陷具有类似的光学性质，在金刚石中的众所周知的硅空位缺陷，但在电子自旋相干时间方面是上级。我们的研究解决了几十年来关于金刚石中镍相关光谱中心的争议，并将镍从杂质转变为量子技术应用中的资源。
Nickel is a common impurity in high-pressure high-temperature diamond and may contaminate chemical vapor deposited diamond used for high-power electronics or quantum technology applications. Magneto-optical fingerprints of nickel have been known since decades, however, no consensus has been reached about the microscopic origins of nickel-related electron paramagnetic resonance, photoluminescence, and optically detected magnetic resonance spectra. The unknown nickel-related defect structures in diamond make it difficult to control them or harness them for a given application. As a consequence, nickel is considered as an impurity in diamond that should be avoided or its concentration should be minimized Recent advances in the development of ab initio magneto-optical spectroscopy have significantly increased its accuracy and predictive power that can be employed for identification and in-depth characterization of paramagnetic color centers in diamond. In this study, we extend the accuracy of the ab initio magneto-optical spectroscopy tools towards self-consistent calculation of second-order spin-orbit coupling for paramagnetic color centers in solids. We apply the full arsenal of the ab initio magneto-optical spectroscopy tools to characterize the split nickel-vacancy defect in diamond which is one of the most stable nickel-related defect configurations. As a result, electron paramagnetic resonance and optical centers are positively identified in various charge states of the nickel-vacancy defect in diamond. In particular, the 1.40-eV optical center and the NIRIM-2 electron paramagnetic resonance center are identified as the single negative charge state of the split nickel-vacancy center. The defect possesses S = 1/2 spin state with an orbital doublet ground state. We find that the coherence time of the ground-state spin is about 0.1 ms at cryogenic temperatures which can be optically initialized and readout by a A-scheme protocol. Since the defect has inversion symmetry the optical signal is insensitive to the stray electric fields, which is an advantage for creating indistinguishable solid-state single-photon sources. We predict that the negatively charged nickel-vacancy defect has similar optical properties to those of the well-known silicon-vacancy defect in diamond but is superior in terms of electron spin coherence times. Our study resolves a few decades controversy about the nickel-related spectroscopy centers in diamond and turns nickel from an impurity to a resource in quantum technology applications.