Coupling Real-Time Time-Dependent Density Functional Theory with Polarizable Force Field

被引：25

作者：

Donati, Greta ^{[1
]}

Wildman, Andrew ^{[1
]}

Caprasecca, Stefano ^{[2
]}

Lingerfelt, David B. ^{[1
]}

Lipparini, Filippo ^{[2
]}

Mennucci, Benedetta ^{[2
]}

Li, Xiaosong ^{[1
]}

机构：

[1] Univ Washington, Dept Chem, Seattle, WA 98195 USA

[2] Univ Pisa, Dipartimento Chim & Chim Ind, Via G Moruzzi 13, I-56124 Pisa, Italy

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2017年 / 8卷 / 21期

基金：

美国国家科学基金会;

关键词：

POLAR SOLVATION DYNAMICS; EXCITED-STATES; EXCITATION-ENERGIES; COUMARIN; 153; QUANTUM; MODEL; ABSORPTION; SPECTRA; DECOMPOSITION; SIMULATION;

D O I：

10.1021/acs.jpclett.7b02320

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Real-time time-dependent density functional theory (RT-TDDFT) is a powerful tool for obtaining spectroscopic observables and understanding complex, time-dependent properties. Currently, performing RT-TDDFT calculations on large, fully quantum mechanical systems is not computationally feasible. Previously, polarizable mixed quantum mechanical and molecular mechanical (QM/MMPol) models have been successful in providing accurate, yet efficient, approximations to a fully quantum mechanical system. Here we develop a coupling scheme between induced dipole based QM/MMPo1 and RT-TDDFT. Our approach is validated by comparing calculated spectra with both real-time and linear-response TDDFT calculations. The model developed within provides an accurate method for performing RT-TDDFT calculations on extended systems while accounting for mutual polarization between the quantum mechanical and molecular mechanical regions.

引用

页码：5283 / 5289

页数：7

共 87 条

[31] Can Quantized Vibrational Effects Be Obtained from Ehrenfest Mixed Quantum-Classical Dynamics? [J].