Department of Chemistry, University of Wisconsin─Madison, Madison, Wisconsin 53706, United States.
Department of Physics, University of Wisconsin─Madison, Madison, Wisconsin 53706, United States.
J Phys Chem Lett. 2023 Jun 1;14(21):4908-4913. doi: 10.1021/acs.jpclett.3c00778. Epub 2023 May 18.
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 MoTe by theoretically demonstrating its multidimensional capabilities. Both parametric and non-parametric pathways are proposed to optimize the resolution of inhomogeneous broadening and -selective features.
由于具有实现原子光谱选择性的能力，因此人们非常有兴趣开发完全相干的多维 X 射线/极紫外（XUV）光谱技术。目前的提案基于使用多个 X 射线/XUV 激发脉冲顺序和相干地驱动核心激发，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，该方法创建了核心和光跃迁的纠缠，以形成形成定向和相干输出光束的 Floquet 态。通过在调谐光学频率穿过共振时测量输出光束的强度来获得多维光谱。这种方法通过理论上证明其多维能力扩展了以前的 MoTe 的光泵 XUV 探针光谱学。提出了参数和非参数途径来优化非均匀展宽和选择性特征的分辨率。
