Theory and algorithms for the excited states of large molecules and molecular aggregates

作     者：LIANG WanZhen WU Wei State 

作者机构：Key Laboratory of Physical Chemistry of Solid SurfacesCollaborative Innovation Center of Chemistry for Energy MaterialsFujian Provincial Key Laboratory of Theoretical and Computational Chemistryand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen University 

出 版 物：《Science China Chemistry》 (中国科学（化学英文版）)

年 卷 期：2013年第56卷第9期

页      面：1267-1270页

核心收录：

学科分类：07[理学] 070203[理学-原子与分子物理] 0702[理学-物理学] 

基　　金：the National Natrual Science Foundation of China (21290193) 

主　　题：molecular aggregates excited state effective model Hamiltonian time-dependent density functional theory (TDDFT) valence bond (VB) theory multiscale models 

摘      要：This project aims to attack the frontiers of electronic structure calculations on the excited states of large molecules and molecular aggregates by developing novel theoretical and computational methods. The methodology development is especially based on the time-dependent density functional theory (TDDFT) and valence bond (VB) theory, and is expected to be computationally effective and accurate as well. Research works on the following related subjects will be performed: (1) The analytical energy-derivative approaches for electronically excited state within TDDFT will be developed to reduce bypass the computational costs in the calculation of molecular excited-state properties. (2) The ab initio methods for electronically excited state based on VB theory and hybrid TDDFT-VB method will be developed to overcome the limitations of current TDDFT in simulating photophysics and photochemistry. (3) For larger aggregates, neither ab initio methods nor TDDFT is applicable. We intend to build the effective model Hamiltonian by developing novel theoretical and computational methods to calculate the involved microscopic physical parameters from the first-principles methods. The constructed effective Hamiltonian is then used to describe the excitonic states and excitonic dynamics of the natural or artificial photosynthesized systems, organic or inorganic photovoltaic cell. (4) The condensed phase environment is taken into account by combining the developed theories and algorithms based on TDDFT and VB with the polarizable continuum solvent models (PCM), molecular mechanism (MM), classical electrodynamics (ED) or molecular dynamics (MD) theory. (5) Highly efficient software packages will be designed and developed.