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Femtosecond Soft-X-ray Absorption Spectroscopy of Liquids with a Water-Window High-Harmonic Source

Smith, Adam D.
Zinchenko, Kristina
Nunes, Fernanda B.
Rossi, Emanuele
Svoboda, Vít
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Published in Journal of Physical Chemistry Letters. 2020, vol. 11, no. 6, p. 1981-1988
Abstract 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 femtosliced 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 tabletop source covering the entire water-window range (284-538 eV). Our work represents the first extension of tabletop 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 and 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 elemental, orbital, and site sensitivity.
Keywords Soft X rayTransient absorptionLiquidsWater windowHigh harmonics generationEthanolMethanol
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Research group Groupe Wolf
Projects FNS: NCCR MUST (20021_172946)
ERC Consolidator Grant (772797-ATTOLIQ)
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SMITH, Adam D. et al. Femtosecond Soft-X-ray Absorption Spectroscopy of Liquids with a Water-Window High-Harmonic Source. In: Journal of Physical Chemistry Letters, 2020, vol. 11, n° 6, p. 1981-1988. doi: 10.1021/acs.jpclett.9b03559 https://archive-ouverte.unige.ch/unige:132260

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Deposited on : 2020-03-13

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