Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses
Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses
复制标题
DOI：
10.1088/0031-8949/t169/1/014002
复制
发表时间：
2016-03-14
期刊：
影响因子：
2.9
通讯作者：
Mukamel, Shaul
中科院分区：
文献类型：
--
作者：
Bennett, Kochise;Zhang, Yu;Mukamel, Shaul
新型X射线自由电子激光(XFEL)和高次谐波(HHG)光源能够产生短而强的脉冲，使X射线非线性光谱分析成为可能。多维光谱技术长期以来一直用于核磁共振、红外和光学领域，通过具有可变延迟的短脉冲序列来探测分子的电子结构和核动力学，因此可以扩展到阿秒X射线领域。这为探测核-电子结构和耦合，实时跟踪脉冲产生的价电子波包和电子相干，以及监测锥形交叉点附近的非绝热电子-核动力学等超快过程提供了可能性。我们综述了各种可能的多维x射线光谱技术，并展示了它们可以提供的关于分子的新信息。
New x-ray free electron laser (XFEL) and high harmonic generation (HHG) light sources are capable of generating short and intense pulses that make x-ray nonlinear spectroscopy possible. Multidimensional spectroscopic techniques, which have long been used in the nuclear magnetic resonance, infrared, and optical regimes to probe the electronic structure and nuclear dynamics of molecules by sequences of short pulses with variable delays, can thus be extended to the attosecond x-ray regime. This opens up the possibility of probing core-electronic structure and couplings, the real-time tracking of impulsively created valence-electronic wavepackets and electronic coherences, and monitoring ultrafast processes such as nonadiabatic electron-nuclear dynamics near conical-intersection crossings. We survey various possible types of multidimensional x-ray spectroscopy techniques and demonstrate the novel information they can provide about molecules.