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arXiv 2602.14818cond-mat.mtrl-sci
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解析4H-SiC中硅空位中心的电子结构

Unraveling the electronic structure of silicon vacancy centers in 4H-SiC

Max-Planck Institut für Polymerforschung(马克斯·普朗克聚合物研究所);Department of Physics / Centre for Material Science and Nanotechnology, University of Oslo(奥斯陆大学物理系/材料科学与纳米技术中心);Department of Physics, Chemistry and Biology, Linköping University(林雪平大学物理、化学和生物学系);Takasaki Institute for Advanced Quantum Science, National Institutes for Quantum Science and Technology: QST(量子科学技术研究机构高崎高级量子科学研究所);Department of Materials Science, Tohoku University(东北大学材料科学系);Wigner Research Centre for Physics, Hungarian Academy of Sciences(匈牙利科学院维格纳物理研究中心);Department of Fundamental Research, Center for Physical Sciences and Technology (FTMC)(立陶宛维尔纽斯物理与技术中心基础研究部)
Ali Tayefeh Younesi, Minh Tuan Luu, Christopher Linderälv, Vytautas Žalandauskas, Marianne Etzelmüller Bathen, Nguyen Tien Son, Takeshi Ohshima, Gergő Thiering,… 展开作者

Ali Tayefeh Younesi, Minh Tuan Luu, Christopher Linderälv, Vytautas Žalandauskas, Marianne Etzelmüller Bathen, Nguyen Tien Son, Takeshi Ohshima, Gergő Thiering, Lukas Razinkovas, Ronald Ulbricht

AI总结:

本研究通过瞬态吸收光谱学首次观测到硅空位中心的 elusive V2' 四重态跃迁,并揭示其电子结构的完整能级分布。

摘要:

硅碳(SiC)中的点缺陷,特别是4H-SiC中带负电的硅空位(V_Si^-),因其有利的自旋-光学性质和与工业半导体制造工艺的兼容性,成为可扩展量子技术的领先候选者。对缺陷电子结构的全面了解对于解释自旋-光学动力学以及可靠设计和优化基于缺陷的量子设备至关重要。尽管已有广泛研究,我们对V_Si^-电子结构的认识仍然有限,因为关键激发态态的集合仍然无法通过传统稳态光谱学访问。在本研究中,利用瞬态吸收光谱学来探测V_Si^-的非平衡电子跃迁,并揭示此前未观测到的激发态。首次直接观测到 elusive V2' 四重态跃迁,并将其广谱特征归因于非绝热振动耦合。在自旋双态态集合中,即光学检测磁共振(ODMR)的核心但尚未被光谱学解析的部分,识别出多个光学跃迁。通过结合偏振解析光谱学、群论分析、量子嵌入计算和第一性原理光学线形度建模,阐明了相关能量范围内的完整电子能级结构。这些结果共同提供了V_Si^-电子结构的微观理解。我们的方法还建立了解析和理解宽禁带颜色中心复杂激发态集合的一般框架。

英文摘要:

Point defects in silicon carbide (SiC), particularly the negatively-charged silicon vacancy ($\mathrm{V_{Si}^{-}}$) in 4H-SiC, are leading candidates for scalable quantum technologies due to their favorable spin-optical properties and compatibility with industrial semiconductor fabrication processes. Comprehensive knowledge of a defect's electronic structure is essential for interpreting spin-optical dynamics and for the reliable design and optimization of defect-based quantum devices. Despite extensive study, our knowledge of the electronic structure of $\mathrm{V_{Si}^{-}}$\ is limited since key excited-state manifolds have remained inaccessible to conventional steady-state spectroscopy. In this study, transient absorption spectroscopy is utilized to probe non-equilibrium electronic transitions of $\mathrm{V_{Si}^{-}}$\ and to uncover previously unobserved excited states. The first direct observation of the elusive V2' quartet transition is presented, with its broad spectral signature attributed to nonadiabatic vibronic coupling. Within the spin-doublet manifold, which is central to optically detected magnetic resonance (ODMR) but has remained unresolved spectroscopically, multiple optical transitions are identified. The complete electronic level structure in the relevant energy range is elucidated by combining polarization-resolved spectroscopy, group-theoretical analysis, quantum embedding calculations and first-principles optical lineshape modeling. Collectively, these results provide a microscopic understanding of the $\mathrm{V_{Si}^{-}}$\ electronic structure. Our approach also establishes a general framework for resolving and understanding complex excited-state manifolds in wide-bandgap color centers.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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