Simulation of Near-Edge X-ray Absorption Fine Structure with Time-Dependent Equation-of-Motion Coupled-Cluster Theory.
Simulation of Near-Edge X-ray Absorption Fine Structure with Time-Dependent Equation-of-Motion Coupled-Cluster Theory.
复制标题
利用瞬态运动方程耦合团簇理论模拟近边缘 X 射线吸收精细结构。
DOI：
10.1021/acs.jpclett.7b01206
复制
发表时间：
2017
期刊：
影响因子：
--
通讯作者：
A. DePrince
中科院分区：
文献类型：
--
作者：
Daniel R. Nascimento;A. DePrince
采用显式含时(TD)方法对分子体系中的运动方程(EOM)单激发和双激发(CCSD)耦合团簇理论进行了数值模拟。TD-EOM-CCSD吸收线形函数由CCSD偶极子自相关函数的傅里叶变换给出。我们用它的Padé近似来表示这种变换，它在比傅立叶形式所要求的更短的模拟时间内提供了收敛的频谱。这一结果为宽带吸收光谱的黑盒模拟提供了一个强有力的框架。从吸收线形函数的实部得到了碳、氮和氧在几个小分子中的K边X射线吸收谱，并与实验进行了比较。计算值与实验值吻合较好，预测峰位置的平均无符号误差仅为1.2 eV。我们还探索了这些分子中质子化的光谱特征。
An explicitly time-dependent (TD) approach to equation-of-motion (EOM) coupled-cluster theory with single and double excitations (CCSD) is implemented for simulating near-edge X-ray absorption fine structure in molecular systems. The TD-EOM-CCSD absorption line shape function is given by the Fourier transform of the CCSD dipole autocorrelation function. We represent this transform by its Padé approximant, which provides converged spectra in much shorter simulation times than are required by the Fourier form. The result is a powerful framework for the blackbox simulation of broadband absorption spectra. K-edge X-ray absorption spectra for carbon, nitrogen, and oxygen in several small molecules are obtained from the real part of the absorption line shape function and are compared with experiment. The computed and experimentally obtained spectra are in good agreement; the mean unsigned error in the predicted peak positions is only 1.2 eV. We also explore the spectral signatures of protonation in these molecules.
大型系统 X 射线吸收光谱的快速瞬态密度泛函理论计算。
影响因子：
5.5
作者：
Besley NA
通讯作者：
Besley NA
影响因子：
5.5
作者：
Parrish RM;Burns LA;Smith DGA;Simmonett AC;DePrince AE 3rd;Hohenstein EG;Bozkaya U;Sokolov AY;Di Remigio R;Richard RM;Gonthier JF;James AM;McAlexander HR;Kumar A;Saitow M;Wang X;Pritchard BP;Verma P;Schaefer HF 3rd;Patkowski K;King RA;Valeev EF;Evangelista FA;Turney JM;Crawford TD;Sherrill CD
通讯作者：
Sherrill CD