论文标题
使用Attosond脉冲列和软X射线拉曼光谱探测非绝热动力学
Probing Nonadiabatic Dynamics with Attosecond Pulse Trains and Soft X-ray Raman Spectroscopy
论文作者
论文摘要
线性非谐振X射线拉曼技术能够检测当光激发波数据包通过圆锥形交叉点时产生的超快电子相干。使用杂种飞秒或attsond探针脉冲来激发系统并刺激信号光子的发射，其中两个磁场都是混合脉冲方案的组成部分。在本文中，我们研究了高谐波生成过程提供的Attosend脉冲序列在此光谱技术的框架中以探针脉冲（而不是单个高斯脉冲）作为探针脉冲。我们探索探针脉冲的不同组合方案，以及脉冲序列参数对信号的影响。此外，我们还展示了拉曼选择规则和对称性考虑如何影响光谱信号，并讨论了振动对整体信号的重要性。我们使用两个不同的模型系统，代表不同对称性的分子和量子动力学模拟来研究光谱的差异。结果表明，这种脉冲列车非常适合捕获与电子相干相关的关键特征。
Linear off-resonant X-ray Raman techniques are capable of detecting the ultrafast electronic coherences generated when a photoexcited wave packet passes through a conical intersection. A hybrid femtosecond or attosecond probe pulse is employed to excite the system and stimulate the emission of the signal photon, where both fields are components of a hybrid pulse scheme. In this paper, we investigate how attosecond pulse trains, as provided by high-harmonic generation processes, perform as probe pulses in the framework of this spectroscopic technique, instead of single Gaussian pulses. We explore different combination schemes for the probe pulse, as well as the impact of parameters of the pulse trains on the signals. Furthermore, we show how Raman selection rules and symmetry consideration affect the spectroscopic signal, and we discuss the importance of vibrational contributions to the overall signal. We use two different model systems, representing molecules of different symmetry, and quantum dynamics simulations to study the difference in the spectra. The results suggest that such pulse trains are well suited to capture the key features associated with the electronic coherence.
