Core-excited states of SF6 probed with soft-x-ray femtosecond transient absorption of vibrational wave packets
Core-excited states of SF6 probed with soft-x-ray femtosecond transient absorption of vibrational wave packets
复制标题
DOI：
10.1103/physreva.108.012805
复制
发表时间：
2023-07-10
影响因子：
2.9
通讯作者：
Leone，Stephen R.
中科院分区：
文献类型：
--
作者：
Barreau，Lou;Ross，Andrew D.;Leone，Stephen R.
用脉冲受激拉曼散射和几个周期的红外脉冲产生了一个振动波包，并利用桌面软X射线在170-200 eV之间的瞬时吸收光谱同时映射到五个硫核激发态上。飞秒振动引起X射线吸收的实时能量漂移，其幅度强烈地依赖于核心激发态的性质。泵浦激光强度被用来控制叠加中的振动态的数目，从而获得S-F伸缩运动的各种扩展的核心激发能级。这使得能够确定对称伸缩模式的相对核能级势能梯度，与TDDFT计算很好地一致。本实验展示了一种表征核激发势能曲线的新方法。
A vibrational wavepacket inis created by impulsive stimulated Raman scattering with a few-cycle infrared pulse and mapped simultaneously onto five sulfur core-excited states using table-top soft x-ray transient absorption spectroscopy between 170 to 200 eV. The femtosecond vibrations induce real-time energy shifts of the x-ray absorption, whose amplitude depend strongly on the nature of the core-excited state. The pump laser intensity is used to control the number of vibrational states in the superposition, thereby accessing core-excited levels for various extensions of the S-F stretching motion. This enables the determination of the relative core-level potential energy gradients for the symmetric stretching mode, in good agreement with TDDFT calculations. This experiment demonstrates a new means of characterizing core-excited potential energy curves.