Calculating Off-Site Excitations in Symmetric Donor-Acceptor Systems via Time-Dependent Density Functional Theory with Range-Separated Density Functionals.
Calculating Off-Site Excitations in Symmetric Donor-Acceptor Systems via Time-Dependent Density Functional Theory with Range-Separated Density Functionals.
复制标题
通过具有范围分离密度泛函的瞬态密度泛函理论计算对称供体-受体系统中的场外激励。
DOI：
--
复制
发表时间：
2012
影响因子：
5.5
通讯作者：
B. Dunietz
中科院分区：
文献类型：
--
作者：
Heidi Phillips;Eitan Geva;B. Dunietz
含时密度泛函理论与距离分离的混合泛函被用来计算场外激发，涉及空间分离的轨道之间的弱耦合系统的过渡。虽然这种离位激发涉及电荷转移，但对称系统中的轨道简并导致具有相等权重的离位激发的线性组合，因此净电荷转移特性为零。像其他类型的离位激发，这种“隐藏”的电荷转移激发是不准确地捕获传统的密度泛函。我们表明，最近推出的Baer-Neuhauser-Livshitz范围分离的混合功能准确地表征通过应用到乙烯二聚体模型系统和染料官能化的倍半硅氧烷等隐藏的场外激发能。
Time-dependent density functional theory with range-separated hybrid functionals is used to calculate off-site excitations involving transitions between spatially separated orbitals in weakly coupled systems. Although such off-site excitations involve charge transfer, orbital degeneracy in symmetrical systems results in linear combinations of off-site excitations with equal weights and therefore zero net charge-transfer character. Like other types of off-site excitations, such "hidden" charge-transfer excitations are not accurately captured by conventional density functionals. We show that the recently introduced Baer-Neuhauser-Livshitz range-separated hybrid functional accurately characterizes such hidden off-site excitation energies via applications to the ethene dimer model system and to dye-functionalized silsesquioxanes.
影响因子：
4.4
作者：
Henderson, Thomas M.;Janesko, Benjamin G.;Scuseria, Gustavo E.
通讯作者：
Scuseria, Gustavo E.