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

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 () and Jake D. Koralek ()
Additional contact information
David J. Hoffman: SLAC National Accelerator Laboratory
Shane W. Devlin: University of California, Department of Chemistry
Douglas Garratt: SLAC National Accelerator Laboratory
Sasawat Jamnuch: Theiss Research
Jacob A. Spies: University of California, Department of Chemistry
Bailey R. Nebgen: University of California, Department of Chemistry
Daniel Schacher: University of Nevada, Nevada Extreme Conditions Laboratory
Alexandria Do: San Diego, Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California
Franky Bernal: University of California, Department of Chemistry
Erika J. Riffe: University of California, Department of Chemistry
Kristjan Kunnus: SLAC National Accelerator Laboratory
Christina Y. Hampton: SLAC National Accelerator Laboratory
Joseph Duris: SLAC National Accelerator Laboratory
David Cesar: SLAC National Accelerator Laboratory
Nicholas Sudar: SLAC National Accelerator Laboratory
Georgi L. Dakovski: SLAC National Accelerator Laboratory
Walter S. Drisdell: Lawrence Berkeley National Laboratory, Chemical Sciences Division
Keith V. Lawler: University of Nevada, Nevada Extreme Conditions Laboratory
Agostino Marinelli: SLAC National Accelerator Laboratory
Michael W. Zuerch: University of California, Department of Chemistry
Richard J. Saykally: University of California, Department of Chemistry
Craig P. Schwartz: University of Nevada, Nevada Extreme Conditions Laboratory
Tod A. Pascal: San Diego, Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California
Jake D. Koralek: SLAC National Accelerator Laboratory

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-65514-4

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