论文标题
钻石中氮 - 脱水中心的振动振动
Vibrationally resolved optical excitations of the nitrogen-vacancy center in diamond
论文作者
论文摘要
对固体中自旋缺陷的光学周期的全面描述需要了解具有不同自旋多样性的状态的电子和原子结构，包括从理论角度来看特别具有挑战性的单线状态。我们提出了一个基于自旋时间依赖性密度函数理论的一般框架，以确定自旋缺陷多体单线状态的激发状态势能表面。然后，我们预测了原型缺陷的单线搁架状态（钻石的氮 - 胶合中心）之间的振动分辨的吸收光谱。我们与实验非常吻合的结果提供了对测量光谱的解释，并揭示了特定声子在确定吸收过程中的关键作用以及非绝热相互作用的显着影响。从我们的计算中获得的见解可能有助于定义改善基于红外吸收的磁力测定法和光学泵送方案的策略。这里开发的理论框架是一般的，适用于其他各种旋转缺陷和材料。
A comprehensive description of the optical cycle of spin defects in solids requires the understanding of the electronic and atomistic structure of states with different spin multiplicity, including singlet states which are particularly challenging from a theoretical standpoint. We present a general framework, based on spin-flip time-dependent density function theory, to determine the excited state potential energy surfaces of the many-body singlet states of spin defects; we then predict the vibrationally resolved absorption spectrum between singlet shelving states of a prototypical defect, the nitrogen-vacancy center in diamond. Our results, which are in excellent agreement with experiments, provide an interpretation of the measured spectra and reveal the key role of specific phonons in determining absorption processes, and the notable influence of non-adiabatic interactions. The insights gained from our calculations may be useful in defining strategies to improve infrared-absorption-based magnetometry and optical pumping schemes. The theoretical framework developed here is general and applicable to a variety of other spin defects and materials.
