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<p>The microscopic structure of water’s surface is crucial to many natural and industrial processes, but studying its hydrogen bond (H-bond) network directly remains challenging due to the required interfacial sensitivity of experimental techniques. By leveraging advances in flat liquid sheet microjets and terawatt-scale attosecond soft X-ray pulses from the LCLS X-ray free electron laser, we employed soft X-ray second harmonic generation (SXSHG) spectroscopy to examine the liquid water/vapor interface. SXSHG combines the elemental selectivity of X-ray spectroscopies with the surface selectivity of SHG and gives access to the electronic structure of interfacial species. Here, we show the SXSHG spectrum differs from bulk water’s X-ray absorption, with its peak shifted several eV, indicating a vastly different electronic environment at the interface as compared to the bulk. First-principles electronic structure calculations show the signal is highly sensitive to H-bond interactions, such as water molecules accepting a single H-bond, which are surface abundant.</p>

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Surface structure of water from soft X-ray second harmonic generation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月26日

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  • David J. Hoffman,
  • Shane W. Devlin,
  • Douglas Garratt,
  • Sasawat Jamnuch,
  • Jacob A. Spies,
  • Bailey R. Nebgen,
  • Daniel Schacher,
  • Alexandria Do,
  • Franky Bernal,
  • Erika J. Riffe,
  • Kristjan Kunnus,
  • Christina Y. Hampton,
  • Joseph Duris,
  • David Cesar,
  • Nicholas Sudar,
  • Georgi L. Dakovski,
  • Walter S. Drisdell,
  • Keith V. Lawler,
  • Agostino Marinelli,
  • Michael W. Zuerch,
  • Richard J. Saykally,
  • Craig P. Schwartz,
  • Tod A. Pascal,
  • Jake D. Koralek

摘要

The microscopic structure of water’s surface is crucial to many natural and industrial processes, but studying its hydrogen bond (H-bond) network directly remains challenging due to the required interfacial sensitivity of experimental techniques. By leveraging advances in flat liquid sheet microjets and terawatt-scale attosecond soft X-ray pulses from the LCLS X-ray free electron laser, we employed soft X-ray second harmonic generation (SXSHG) spectroscopy to examine the liquid water/vapor interface. SXSHG combines the elemental selectivity of X-ray spectroscopies with the surface selectivity of SHG and gives access to the electronic structure of interfacial species. Here, we show the SXSHG spectrum differs from bulk water’s X-ray absorption, with its peak shifted several eV, indicating a vastly different electronic environment at the interface as compared to the bulk. First-principles electronic structure calculations show the signal is highly sensitive to H-bond interactions, such as water molecules accepting a single H-bond, which are surface abundant.