Various spectroscopic properties of Yb³⁺-doped Y₂SiO₅ crystal have been extensively investigated due to its promising application in quantum information processing. However, the local structure, electronic structure of Yb³⁺:Y₂SiO₅ crystal, and its optical and magnetic properties have not been comprehensively studied from a theoretical viewpoint. In this work, the geometric and electronic structures of Yb³⁺ that replaces two crystallographic Y³⁺ sites in the Y₂SiO₅ crystal are first obtained by the method of density functional theory (DFT). Then, the optical, electron paramagnetic resonance (EPR), and optically detected magnetic resonance (ODMR) spectra for ¹⁷¹Yb³⁺ (nuclear spin I = 1/2) at such two sites are simultaneously calculated in the framework of the complete diagonalization (of energy) matrix (CDM) based on the optimized local structure around ¹⁷¹Yb³⁺ ion by DFT. The various calculated spectroscopic properties by such combined theoretical approach are consistent with the experimental ones, which demonstrates that CDM is effective and particularly suitable for calculating hyperfine A-tensors under zero, low, and intermediate magnetic field. More importantly, based on the obtained accurate hyperfine structure of ¹⁷¹Yb³⁺ in Y₂SiO₅ crystal, the possible “clock transitions”, which can enhance the optical coherence time, can be assigned or predicted by the present approach. This study successfully explains the spectroscopic properties of ¹⁷¹Yb³⁺-doped Y₂SiO₅ and provides a feasible method to design and search for practical rare-earth-doped quantum information materials for the community.

中文翻译：

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171Yb3 +掺杂Y2SiO5晶体的电子结构和光学，EPR和ODMR光谱性质研究：组合理论方法。

由于Yb ³⁺掺杂的Y ₂ SiO ₅晶体在量子信息处理中的应用前景广阔，因此已对其进行了广泛的研究。但是，从理论的观点出发，尚未全面研究Yb ³⁺：Y ₂ SiO ₅晶体的局部结构，电子结构及其光学和磁性。在这项工作中，Yb ³⁺的几何和电子结构取代了Y ₂ SiO ₅中的两个晶体学Y ³⁺位点首先通过密度泛函理论（DFT）的方法获得晶体。然后，在完全对角化的框架下，同时计算这两个位置的¹⁷¹ Yb ³⁺（核自旋I = 1/2）的光学，电子顺磁共振（EPR）和光学检测的磁共振（ODMR）光谱（基于DFT在¹⁷¹ Yb ³⁺离子附近的优化局部结构的能量矩阵（CDM）。通过这种组合理论方法计算出的各种光谱性质与实验结果相一致，这表明CDM是有效的，特别适合于计算超细A-在零，低和中间磁场下的张量。更重要的是，基于在Y ₂ SiO ₅晶体中获得的¹⁷¹ Yb ^3+的精确超精细结构，可以通过本方法分配或预测可能会增加光学相干时间的“时钟跃迁”。这项研究成功地解释了¹⁷¹ Yb ³⁺掺杂的Y ₂ SiO ₅的光谱性质，并为社区设计和搜索实用的稀土掺杂量子信息材料提供了一种可行的方法。