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XUV pump–XUV probe transient absorption spectroscopy at FELs
Faraday Discussions ( IF 3.3 ) Pub Date : 2020-11-7 , DOI: 10.1039/d0fd00107d Thomas Ding 1, 2, 3 , Marc Rebholz 1, 2, 3 , Lennart Aufleger 1, 2, 3 , Maximilian Hartmann 1, 2, 3 , Veit Stooß 1, 2, 3 , Alexander Magunia 1, 2, 3 , Paul Birk 1, 2, 3 , Gergana Dimitrova Borisova 1, 2, 3 , Carina da Costa Castanheira 1, 2, 3 , Patrick Rupprecht 1, 2, 3 , Yonghao Mi 1, 2, 3 , Thomas Gaumnitz 4, 5, 6, 7 , Zhi-Heng Loh 8, 9, 10, 11, 12 , Sebastian Roling 3, 13, 14 , Marco Butz 3, 14, 15 , Helmut Zacharias 3, 14, 15 , Stefan Düsterer 3, 16, 17 , Rolf Treusch 3, 16, 17 , Christian Ott 1, 2, 3 , Thomas Pfeifer 1, 2, 3
Faraday Discussions ( IF 3.3 ) Pub Date : 2020-11-7 , DOI: 10.1039/d0fd00107d Thomas Ding 1, 2, 3 , Marc Rebholz 1, 2, 3 , Lennart Aufleger 1, 2, 3 , Maximilian Hartmann 1, 2, 3 , Veit Stooß 1, 2, 3 , Alexander Magunia 1, 2, 3 , Paul Birk 1, 2, 3 , Gergana Dimitrova Borisova 1, 2, 3 , Carina da Costa Castanheira 1, 2, 3 , Patrick Rupprecht 1, 2, 3 , Yonghao Mi 1, 2, 3 , Thomas Gaumnitz 4, 5, 6, 7 , Zhi-Heng Loh 8, 9, 10, 11, 12 , Sebastian Roling 3, 13, 14 , Marco Butz 3, 14, 15 , Helmut Zacharias 3, 14, 15 , Stefan Düsterer 3, 16, 17 , Rolf Treusch 3, 16, 17 , Christian Ott 1, 2, 3 , Thomas Pfeifer 1, 2, 3
Affiliation
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The emergence of ultra-intense extreme-ultraviolet (XUV) and X-ray free-electron lasers (FELs) has opened the door for the experimental realization of non-linear XUV and X-ray spectroscopy techniques. Here we demonstrate an experimental setup for an all-XUV transient absorption spectroscopy method for gas-phase targets at the FEL. The setup combines a high spectral resolving power of E/ΔE ≈ 1500 with sub-femtosecond interferometric resolution, and covers a broad XUV photon-energy range between approximately 20 and 110 eV. We demonstrate the feasibility of this setup firstly on a neon target. Here, we intensity- and time-resolve key aspects of non-linear XUV-FEL light–matter interactions, namely the non-resonant ionization dynamics and resonant coupling dynamics of bound states, including XUV-induced Stark shifts of energy levels. Secondly, we show that this setup is capable of tracking the XUV-initiated dissociation dynamics of small molecular targets (oxygen and diiodomethane) with site-specific resolution, by measuring the XUV transient absorption spectrum. In general, benefitting from a single-shot detection capability, we show that the setup and method provides single-shot phase-locked XUV pulse pairs. This lays the foundation to perform, in the future, experiments as a function of the XUV interferometric time delay and the relative phase, which enables advanced coherent non-linear spectroscopy schemes in the XUV and X-ray spectral range.
中文翻译：
XEL泵上的XUV泵–XUV探针瞬态吸收光谱
超强极紫外（XUV）和X射线自由电子激光器（FEL）的出现为非线性XUV和X射线光谱技术的实验实现打开了大门。在这里，我们展示了一种用于全XUV瞬态吸收光谱法的实验装置，该方法用于在FEL处气相目标。该设置结合了E / ΔE的高光谱分辨能力≈1500，具有亚飞秒级的干涉测量分辨率，并覆盖了大约20到110 eV之间的宽XUV光子能量范围。我们首先在霓虹灯目标上演示了此设置的可行性。在这里，我们强度和时间分辨了非线性XUV-FEL光-物质相互作用的关键方面，即键合态的非共振电离动力学和共振耦合动力学，包括XUV引起的能级Stark位移。其次，我们表明该设置能够通过测量XUV瞬态吸收光谱来跟踪具有特定位点分辨率的小分子目标（氧气和二碘甲烷）的XUV引发的离解动力学。通常，得益于单次检测功能，我们表明该设置和方法提供了单次锁相XUV脉冲对。
更新日期：2020-11-07
中文翻译：
XEL泵上的XUV泵–XUV探针瞬态吸收光谱
超强极紫外（XUV）和X射线自由电子激光器（FEL）的出现为非线性XUV和X射线光谱技术的实验实现打开了大门。在这里，我们展示了一种用于全XUV瞬态吸收光谱法的实验装置，该方法用于在FEL处气相目标。该设置结合了E / ΔE的高光谱分辨能力≈1500，具有亚飞秒级的干涉测量分辨率，并覆盖了大约20到110 eV之间的宽XUV光子能量范围。我们首先在霓虹灯目标上演示了此设置的可行性。在这里，我们强度和时间分辨了非线性XUV-FEL光-物质相互作用的关键方面，即键合态的非共振电离动力学和共振耦合动力学，包括XUV引起的能级Stark位移。其次，我们表明该设置能够通过测量XUV瞬态吸收光谱来跟踪具有特定位点分辨率的小分子目标（氧气和二碘甲烷）的XUV引发的离解动力学。通常，得益于单次检测功能，我们表明该设置和方法提供了单次锁相XUV脉冲对。
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