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An ab Initio Linear Response Method for Computing Magnetic Circular Dichroism Spectra with Nonperturbative Treatment of Magnetic Field
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2019-04-01 00:00:00 , DOI: 10.1021/acs.jctc.9b00095 Shichao Sun 1 , David Williams-Young 1 , Xiaosong Li 1
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2019-04-01 00:00:00 , DOI: 10.1021/acs.jctc.9b00095 Shichao Sun 1 , David Williams-Young 1 , Xiaosong Li 1
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Magnetic circular dichroism (MCD) experiments provide a sensitive tool for exploring geometric, magnetic, and electronic properties of chemical complexes and condensed matter systems. They are also challenging to simulate because of the need to simultaneously treat the perturbations of a finite magnetic field as well as an optical field. In this work, we introduce an ab initio approach that treats the external magnetic field nonperturbatively with London orbitals for simulating the MCD spectra of closed-shell systems. Effects of a magnetic field are included variationally in the spin-free nonrelativistic Hamiltonian, followed by a linear response formalism to directly calculate the difference in absorption between the left and right circularly polarized light. In addition to the presentation of underlying mathematical formalism and implementation, the method developed in this paper has been applied to simulations of MCD spectra of the sodium anion, 2,2,6,6-tetramethylcyclohexanone, and 3-methyl-2-hexanone. Results are discussed and compared to experiments.
中文翻译：
从头算线性响应计算磁场的非扰动处理圆圆二色性光谱
磁性圆二色性（MCD）实验提供了一种灵敏的工具，可用于探索化学络合物和凝聚态系统的几何，磁性和电子性质。由于需要同时处理有限磁场和光场的扰动，因此它们的仿真也颇具挑战性。在这项工作中，我们引入了从头算的方法，该方法从伦敦轨道无扰动地处理外部磁场，以模拟闭壳系统的MCD谱。无自旋的非相对论哈密顿量包含磁场的影响，然后通过线性响应形式来直接计算左右圆偏振光的吸收差异。除了介绍基本的数学形式主义和实现方法外，本文开发的方法已应用于模拟钠阴离子，2,2,6,6-四甲基环己酮和3-甲基-2-己酮的MCD光谱。对结果进行了讨论并与实验进行了比较。
更新日期：2019-04-01
中文翻译：
从头算线性响应计算磁场的非扰动处理圆圆二色性光谱
磁性圆二色性（MCD）实验提供了一种灵敏的工具，可用于探索化学络合物和凝聚态系统的几何，磁性和电子性质。由于需要同时处理有限磁场和光场的扰动，因此它们的仿真也颇具挑战性。在这项工作中，我们引入了从头算的方法，该方法从伦敦轨道无扰动地处理外部磁场，以模拟闭壳系统的MCD谱。无自旋的非相对论哈密顿量包含磁场的影响，然后通过线性响应形式来直接计算左右圆偏振光的吸收差异。除了介绍基本的数学形式主义和实现方法外，本文开发的方法已应用于模拟钠阴离子，2,2,6,6-四甲基环己酮和3-甲基-2-己酮的MCD光谱。对结果进行了讨论并与实验进行了比较。
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