ArticleNature communications2026
Multipolar electric and magnetic contributions to sum-frequency generation spectra reveal biaxial interfacial water structure.
Article in Nature communications, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Liquid interfaces play central roles in biological and physicochemical processes. Sum-frequency-generation (SFG) spectroscopy is intrinsically interface-specific, but the insight gained from SFG spectra into molecular interfacial structure has been limited since spectral analysis is usually done within the electric-dipole approximation, neglecting higher-order multipole contributions. Here we introduce a general framework that includes electric and magnetic multipoles for calculating SFG spectra from molecular simulations, achieving quantitative agreement between predicted and experimental SFG spectra of the air-water interface. We show that the electric-dipole approximation breaks completely down in the water bending region and remains only qualitatively valid in the OH-stretch region. When accounting for multipole contributions, the analysis of the SFG bending band reveals pronounced biaxial water ordering in a triple-layer structure with a width of only about 0.8 nanometers. By resolving a fundamental limitation of the interpretation of SFG spectroscopy, our framework allows for the detailed extraction of interfacial molecular ordering from SFG spectra.
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