Femtosecond X-ray absorption spectroscopy (XAS) is a powerful method to investigate the dynamical behavior of a system after photoabsorption in real time. So far, the application of this technique has remained limited to large-scale facilities, such as femto-sliced synchrotrons and free-electron lasers (FEL). In this work, we demonstrate femtosecond time-resolved soft-X-ray absorption spectroscopy of liquid samples by combining a sub-micrometer-thin flat liquid jet with a high-harmonic table-top source covering the entire water-window range (284 - 538 eV). Our work represents the first extension of table-top XAS to the oxygen edge of a chemical sample in the liquid phase. In the time domain, our measurements resolve the gradual appearance of absorption features below the carbon K-edge of ethanol and methanol during strong-field ionization, which trace the valence-shell ionization dynamics of the liquid alcohols with a temporal resolution of 30 fs. This technique opens unique opportunities to study molecular dynamics of chemical systems in the liquid phase with element, orbital and site sensitivity.
Femtosecond X-ray absorption spectroscopy (XAS) is a powerful method to investigate the dynamical behavior of a system after photoabsorption in real time. So fpan class="Chemical">ar, the application of this technique has remained limited to large-scale facilities, such as femto-sliced synchrotrons and free-electron lasers (FEL). In this work, we demonstrate femtosecond time-resolved soft-X-ray absorption spectroscopy of liquid samples by combining a sub-micrometer-thin flat liquid jet with a high-harmonic table-top source covering the entire water-window range (284 - 538 eV). Our work represents the first extension of table-top XAS to the oxygen edge of a chemical sample in the liquid phase. In the time domain, our measurements resolve the gradual appearance of absorption features below the carbon K-edge of ethanol and methanol during strong-field ionization, which trace the valence-shell ionization dynamics of the liquid alcohols with a temporal resolution of 30 fs. This technique opens unique opportunities to study molecular dynamics of chemical systems in the liquid phase with element, orbital and site sensitivity.
Authors: Yohei Uemura; Ahmed S M Ismail; Sang Han Park; Soonnam Kwon; Minseok Kim; Hebatalla Elnaggar; Federica Frati; Hiroki Wadati; Yasuyuki Hirata; Yujun Zhang; Kohei Yamagami; Susumu Yamamoto; Iwao Matsuda; Ufuk Halisdemir; Gertjan Koster; Christopher Milne; Markus Ammann; Bert M Weckhuysen; Frank M F de Groot Journal: J Phys Chem Lett Date: 2022-05-05 Impact factor: 6.888