频率依赖的二次响应特性和来自相对论运动方程合集群理论的两光子吸收
Xiang Yuan1,2, Loïc Halbert1, Lucas Visscher2
1Physique des Lasers Atomes et Molecules, Universite de Lille, F-59000 Lille, France.
Journal of chemical theory and computation
|December 11, 2023
概括
这项研究引入了一种新的计算方法,用于使用相对论运动方程合集群理论来预测分子性质. 多功能方法准确计算各种原子和分子的电子和磁光学特性.
科学领域:
- 计算化学计算化学
- 量子化学 是一个量子化学.
- 理论化学 理论化学
背景情况:
- 准确预测分子性质对于理解化学现象至关重要.
- 相对论效应和电子相关性显著影响分子性质,特别是重元素.
- 现有的计算方法在处理这些复杂效应方面可能存在局限性.
研究的目的:
- 实施和验证基于相对论运动方程合集群 (EOM-CC) 方法的二次响应理论.
- 评估该方法在计算静态和动态电子和磁光学属性的能力.
- 为密度函数理论 (DFT) 等近似模型提供一个基准.
主要方法:
- 在相对论运动方程合集群 (EOM-CC) 框架内实施二次响应理论.
- 对化 (HX) 的静态和频率依赖的超极化度的计算.
- 对贵重气体 (Xe,Rn) 的维德特常数和Ga+和In+的两光子吸收截面的评估.
主要成果:
- 开发的EOM-CC方法准确计算电子和磁光学特性,包括超极化性和维德特常数.
- 发现相对论和电子相关性效应对于研究的磁光学性质很重要.
- 与达尔顿代码的CC实现进行比较时,差异通常小于5%.
结论:
- 实施的相对论EOM-CC方法对一系列分子性质具有多功能性和准确性.
- 该研究强调了相对论和电子相关性效应在准确的属性预测中的重要性.
- 该方法作为化学中的其他计算模型的有价值的基准.
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