论文标题
时间依赖性耦合簇理论用于超快瞬态吸收光谱
Time-dependent coupled cluster theory for ultrafast transient absorption spectroscopy
论文作者
论文摘要
我们提出了一个自旋适应的时间依赖性耦合簇单打，并为分子响应对一系列超短激光脉冲的分子响应。该实现用于计算对价激发泵脉冲的电子响应，以及随后的核心激发探针脉冲。我们评估用于解决动态耦合群集方程的集成程序的准确性，以便在计算成本和准确性之间找到妥协。计算氟化锂的瞬时吸收光谱，以相对于泵脉冲的各种探针脉冲延迟。我们观察到，瞬态探针吸收会随泵探针延迟振荡，这归因于状态在泵引起的叠加中的干扰。
We present a spin-adapted time-dependent coupled cluster singles and doubles model for the molecular response to a sequence of ultrashort laser pulses. The implementation is used to calculate the electronic response to a valence-exciting pump pulse, and a subsequent core-exciting probe pulse. We assess the accuracy of the integration procedures used in solving the dynamic coupled cluster equations, in order to find a compromise between computational cost and accuracy. The transient absorption spectrum of lithium fluoride is calculated for various delays of the probe pulse with respect to the pump pulse. We observe that the transient probe absorption oscillates with the pump-probe delay, an effect that is attributed to the interference of states in the pump-induced superposition.
