X-ray/Extreme Ultraviolet Floquet State Multidimensional Spectroscopy, an Analogue of Multiple Quantum Nuclear Magnetic Resonance,The Journal of Physical Chemistry Letters

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X-ray/Extreme Ultraviolet Floquet State Multidimensional Spectroscopy, an Analogue of Multiple Quantum Nuclear Magnetic Resonance
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2023-05-18 , DOI: 10.1021/acs.jpclett.3c00778
John C Wright ₁ , Daniel D Kohler ₁ , Uwe Bergmann ₂

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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 MoTe₂ by theoretically demonstrating its multidimensional capabilities. Both parametric and non-parametric pathways are proposed to optimize the resolution of inhomogeneous broadening and k-selective features.

中文翻译：

X 射线/极紫外 Floquet 态多维光谱学，多量子核磁共振的模拟

人们对开发完全相干的多维 X 射线/极紫外 (XUV) 光谱技术非常感兴趣，因为它们能够实现原子光谱选择性。目前的建议依赖于使用具有多个 X 射线/XUV 激发脉冲的顺序和相干驱动的核心激发，并使用时域傅立叶变换方法测量输出。在本文中，我们提出了一种替代方法，该方法创建核心和光学跃迁的纠缠以形成 Floquet 状态，从而创建定向和相干的输出光束。多维光谱是通过测量输出光束的强度同时调谐跨共振的光频率获得的。这种方法扩展了之前的光泵——MoTe _{2的 XUV 探针光谱}通过从理论上证明其多维能力。提出了参数化和非参数化路径来优化非均匀加宽和k选择性特征的分辨率。

更新日期：2023-05-18

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