论文标题
部分可观测时空混沌系统的无模型预测
Intersystem Crossing and Exciton-Defect Coupling of Spin Defects in Hexagonal Boron Nitride
论文作者
论文摘要
尽管将二维（2D）系统识别为单个光子发射器或自旋量子的新兴和可扩展的宿主材料，但这些量子缺陷的不受控制和未定的化学性质是进一步发展的障碍。利用外部缺陷的设计可以避免这些持续的问题并提供最终的解决方案。在这里，我们建立了一个完整的理论框架，以准确，系统地设计宽带2D系统中的量子缺陷。通过这种方法，对于旋转量子目标发现，同样考虑了必需的静态和动力学特性。特别是，多体相互作用（例如缺陷）耦合对于描述Ultrathin 2D系统中缺陷的激发状态特性至关重要。同时，非放射性过程（例如声子辅助衰减和间间交叉率）需要仔细评估，这与辐射过程竞争。从基于第一原理计算的缺陷进行彻底筛选，我们确定了有希望的单个光子发射器，例如siVV和旋转量子，例如己二硼硼中的TIVV和MOVV。这项工作为2D材料中的缺陷设计提供了完整的第一原理理论框架。
Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single photon emitters or spin qubits, uncontrolled and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect-exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which compete together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single photon emitters such as SiVV and spin qubits such as TiVV and MoVV in hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.
