X-ray/Extreme Ultraviolet Floquet State Multidimensional Spectroscopy, an Analogue of Multiple Quantum Nuclear Magnetic Resonance
X-ray/Extreme Ultraviolet Floquet State Multidimensional Spectroscopy, an Analogue of Multiple Quantum Nuclear Magnetic Resonance
复制标题
X射线/极紫外Floquet态多维光谱，多量子核磁共振的模拟
DOI：
10.1021/acs.jpclett.3c00778
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Bergmann, Uwe
中科院分区：
文献类型：
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作者：
Wright, John C.;Kohler, Daniel D.;Bergmann, Uwe
由于具有实现原子光谱选择性的能力，人们对开发全相干多维x射线/极紫外（XUV）光谱技术非常感兴趣。目前的建议是使用顺序和相干驱动的磁芯激励与多个x射线/XUV激励脉冲，并使用时域傅里叶变换方法测量输出。在本文中，我们提出了一种替代方法，该方法可以产生核心和光跃迁的纠缠，从而形成Floquet状态，从而产生定向和相干输出光束。多维光谱是通过测量输出光束的强度，同时调整跨共振的光学频率来获得的。该方法扩展了先前mote2的光泵浦- xuv探针光谱，从理论上证明了它的多维能力。提出了参数化和非参数化两种途径来优化非均匀展宽和k-选择性特征的分辨率。
There is great interest in developing fully coherent multidimensional X-ray/extreme ultraviolet (XUV) spectroscopic techniques because of their capability for achieving atomic spectral selectivity. Current proposals rest on using sequentially and coherently driven core excitations with multiple X-ray/XUV excitation pulses and measuring the output using time domain Fourier transform methods. In this paper, we propose an alternative method that creates an entanglement of core and optical transitions to form a Floquet state that creates directional and coherent output beams. Multidimensional spectra are obtained by measuring the intensity of output beams while tuning the optical frequencies across resonances. This approach expands on previous optical pump–XUV probe spectroscopy of MoTe2by theoretically demonstrating its multidimensional capabilities. Both parametric and non-parametric pathways are proposed to optimize the resolution of inhomogeneous broadening andk-selective features.