论文标题
周期性方程式耦合群集实现，应用于碱性地球氧化物的$ f $中心
A periodic equation-of-motion coupled-cluster implementation applied to $F$-centers in alkaline earth oxides
论文作者
论文摘要
我们使用周期性边界条件和平面波基集提出了运动耦合群集单打和双打（EOM-CCSD）理论的实现。我们对EOM-CCSD理论的实施应用于使用定期超级细胞方法的碱性氧化物中的$ f $中心。探索了相对于轨道基集和系统尺寸的MGO，CAO和SRO晶体中中性色中心计算的电子激发能的收敛性。我们讨论了外推技术，该技术在完整的基集限制中近似激发能并减少有限尺寸误差。我们的发现表明，EOM-CCSD理论可以预测$ f $中心的光吸收能与实验非常吻合。此外，我们讨论了对应于从三重态到单线状态的衰减的计算出的发射能，这些发射能负责光致发光特性。我们的发现与文献中可用的实验和理论结果进行了比较。
We present an implementation of equation of motion coupled-cluster singles and doubles (EOM-CCSD) theory using periodic boundary conditions and a plane wave basis set. Our implementation of EOM-CCSD theory is applied to study $F$-centers in alkaline earth oxides employing a periodic supercell approach. The convergence of calculated electronic excitation energies for neutral color centers in MgO, CaO and SrO crystals with respect to orbital basis set and system size is explored. We discuss extrapolation techniques that approximate excitation energies in the complete basis set limit and reduce finite size errors. Our findings demonstrate that EOM-CCSD theory can predict optical absorption energies of $F$-centers in good agreement with experiment. Furthermore, we discuss calculated emission energies corresponding to the decay from triplet to singlet states, responsible for the photoluminescence properties. Our findings are compared to experimental and theoretical results available in literature.
