Gao C-Z, Dinh P M, Reinhard P-G, Suraud E
Laboratoire de Physique Théorique, Université de Toulouse, CNRS, UPS, France.
Phys Chem Chem Phys. 2017 Aug 2;19(30):19784-19793. doi: 10.1039/c7cp00995j.
We study from a theoretical perspective the ionization of molecules and clusters induced by irradiation of a combined two-color laser field consisting of a train of attosecond XUV pulses in the presence of an IR field. We use time-dependent density-functional theory (TDDFT) in real time and real space as a theoretical tool. The calculated results are compared to experimental data when available. We also compare TDDFT with results obtained using a time-dependent Schrödinger equation (TDSE), which is well suited to simple systems while TDDFT allows dealing with more complex molecules and clusters. As a key observable, we study ionization versus delay time of the XUV pulses with respect to the IR background pulse. Experiments in simple atoms (He and Ar) show a regular modulation of this signal with half the IR period. This feature is recovered by TDDFT as well as by the TDSE (although total ionization differs by an order of magnitude). As more complex systems, we consider a C chain molecule and Na clusters. Here we encounter a different picture as the ionization signal develops a more involved pattern with several peaks per half IR period and as the TDSE produces a different pattern to TDDFT. Both effects could be related to the appearance of strong resonance modes in these more complex systems.
我们从理论角度研究了在红外场存在的情况下,由一系列阿秒极紫外(XUV)脉冲组成的双色激光场照射所诱导的分子和团簇的电离。我们使用实时实空间中的含时密度泛函理论(TDDFT)作为理论工具。如有可用的实验数据,将计算结果与之进行比较。我们还将TDDFT与使用含时薛定谔方程(TDSE)得到的结果进行比较,TDSE适用于简单系统,而TDDFT能够处理更复杂的分子和团簇。作为一个关键的可观测指标,我们研究了XUV脉冲相对于红外背景脉冲的电离与延迟时间的关系。在简单原子(He和Ar)中的实验表明,该信号以红外周期的一半进行规则调制。TDDFT以及TDSE都能重现这一特征(尽管总电离相差一个数量级)。作为更复杂的系统,我们考虑了一个C链分子和Na团簇。在这里,我们遇到了不同的情况,电离信号呈现出每半个红外周期有多个峰值的更复杂模式,并且TDSE产生的模式与TDDFT不同。这两种效应可能都与这些更复杂系统中强共振模式的出现有关。