能量密度的分析与可视化。II. 来自线性响应含时密度泛函理论计算的见解。
Analysis and visualization of energy densities. II. Insights from linear-response time-dependent density functional theory calculations.
作者信息
Pei Zheng, Yang Junjie, Deng Jingheng, Mao Yuezhi, Wu Qin, Yang Zhibo, Wang Bin, Aikens Christine M, Liang Wanzhen, Shao Yihan
机构信息
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, P. R. China.
出版信息
Phys Chem Chem Phys. 2020 Dec 7;22(46):26852-26864. doi: 10.1039/d0cp04207b.
Abstract
Inspired by the analysis of Kohn-Sham energy densities by Nakai and coworkers, we extended the energy density analysis to linear-response time-dependent density functional theory (LR-TDDFT) calculations. Using ethylene-tetrafluoroethylene and oxyluciferin-water complexes as examples, distinctive distribution patterns were demonstrated for the excitation energy densities of local excitations (within a molecular fragment) and charge-transfer excitations (between molecular fragments). It also provided a simple way to compute the effective energy of both hot carriers (particle and hole) from charge-transfer excitations via an integration of the excitation energy density over the donor and acceptor grid points.
摘要
受中井及其同事对科恩-沙姆能量密度的分析启发，我们将能量密度分析扩展到线性响应含时密度泛函理论（LR-TDDFT）计算。以乙烯-四氟乙烯和氧化荧光素-水络合物为例，展示了局域激发（分子片段内）和电荷转移激发（分子片段间）的激发能量密度的独特分布模式。它还提供了一种简单的方法，通过在供体和受体网格点上对激发能量密度进行积分，来计算电荷转移激发产生的热载流子（粒子和空穴）的有效能量。
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