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Time-resolved x-ray absorption spectroscopy with a water window high-harmonic source

机译:具有水窗高谐波源的时间分辨X射线吸收光谱

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摘要

Time-resolved x-ray absorption spectroscopy (TR-XAS) has so far practically been limited to large-scale facilities, to subpicosecond temporal resolution, and to the condensed phase. We report the realization of TR-XAS with a temporal resolution in the low femtosecond range by developing a tabletop high-harmonic source reaching up to 350 electron volts, thus partially covering the spectral region of 280 to 530 electron volts, where water is transmissive. We used this source to follow previously unexamined light-induced chemical reactions in the lowest electronic states of isolated CF4+ and SF6+ molecules in the gas phase. By probing element-specific core-to-valence transitions at the carbon K-edge or the sulfur L-edges, we characterized their reaction paths and observed the effect of symmetry breaking through the splitting of absorption bands and Rydberg-valence mixing induced by the geometry changes.
机译:到目前为止,时间分辨X射线吸收光谱法(TR-XAS)实际上仅限于大型设备,亚皮秒时间分辨率和浓缩阶段。我们报告了通过开发高达350电子伏特的台式高谐波源,从而实现了在低飞秒范围内具有时间分辨率的TR-XAS的实现,从而可以部分覆盖280至530电子伏特的光谱区域,其中水可以透过。我们使用这种来源跟踪气相中分离出的CF4 +和SF6 +分子处于最低电子态的先前未经检查的光诱导化学反应。通过探测碳K边缘或硫L边缘的元素特定的核价转变,我们表征了它们的反应路径,并观察到对称性打破了吸收带的分裂和由Rydberg价混合引起的对称作用。几何形状的变化。

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  • 来源
    《Science》 |2017年第6322期|264-267|共4页
  • 作者单位

    ETH, Lab Phys Chem, CH-8092 Zurich, Switzerland;

    Univ Geneva, GAP Biophoton, CH-1205 Geneva, Switzerland;

    ETH, Lab Phys Chem, CH-8092 Zurich, Switzerland|Univ Geneva, GAP Biophoton, CH-1205 Geneva, Switzerland;

    Univ Geneva, GAP Biophoton, CH-1205 Geneva, Switzerland|Univ Sheffield, Dept Chem, Sheffield S3 7HF, S Yorkshire, England;

    ETH, Lab Phys Chem, CH-8092 Zurich, Switzerland;

    ETH, Lab Phys Chem, CH-8092 Zurich, Switzerland;

    ETH, Lab Phys Chem, CH-8092 Zurich, Switzerland;

    ETH, Lab Phys Chem, CH-8092 Zurich, Switzerland;

    ETH, Lab Phys Chem, CH-8092 Zurich, Switzerland;

    Univ Geneva, GAP Biophoton, CH-1205 Geneva, Switzerland;

    ETH, Lab Phys Chem, CH-8092 Zurich, Switzerland;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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