论文标题
时间依赖的二阶绿色功能理论用于中性激发
Time dependent second order Green's function theory for neutral excitations
论文作者
论文摘要
我们开发了一个依赖时间的二阶绿色功能理论（GF2），以计算分子中的中性激发态。较小绿色功能的运动方程（GF）是在与自我能源的二阶近似值的绝热近似中得出的。在线性响应方案中，我们将依赖性的Kb方程重铸为贝尔氨基盐样方程（GF2-BSE），其内核近似于第二阶库仑自我能源。然后，我们将GF2-BSE应用于一组分子和原子，发现GF2-BSE优于与单身（CIS）和/或依赖时间的Hartree-fock（TDHF）的构型相互作用，尤其是在大多数情况下与CIS（CIS（d））相当的电荷传递激发，尤其是与CIS相比。
We develop a time dependent second order Green's function theory (GF2) for calculating neutral excited states in molecules. The equation of motion for the lesser Green's function (GF) is derived within the adiabatic approximation to the Kadanoff-Baym (KB) equation using the second order Born approximation for the self-energy. In the linear response regime, we recast the time dependent KB equation into a Bethe-Salpeter-like equation (GF2-BSE), with a kernel approximated by the second order Coulomb self-energy. We then apply our GF2-BSE to a set of molecules and atoms and find that GF2-BSE is superior to configuration interaction with singles (CIS) and/or time dependent Hartree-Fock (TDHF), particularly for charge transfer excitations, and is comparable to CIS with perturbative doubles (CIS(D)) in most cases.
