ArticleProceedings of the National Academy of Sciences of the United States of America2025
Solvation-induced local structure in liquids probed by high-harmonic spectroscopy.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2025. 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
High-harmonic generation (HHG) has been established as a powerful tool for studying structure and dynamics of quantum systems in gas and solid phases. To date, only a few studies have extended HHG spectroscopy to liquids, and much remains unresolved concerning the information that can be extracted from HHG spectra about the local liquid environment and the potential of HHG as a nonlinear probe of solvation dynamics. In this work, we investigate HHG in liquid binary solutions consisting of mixtures of aromatic benzene derivatives solvated in methanol. We observe evidence of a localized solvation structure that is imprinted on the harmonic spectra in the form of a strongly suppressed harmonic order, and an overall reduction of the total harmonic yield. We characterize this behavior as a function of laser parameters, concentration, and other halogenated benzene derivatives in methanol solution. Guided by theory, we interpret the results in terms of a localized solvation shell that is formed in specific solutions and acts like a local scattering barrier in the HHG process. This work demonstrates the potential of high-harmonic spectroscopy in liquids to extract detailed information about the structure and dynamics of solvation while expanding our understanding of the fundamental mechanism of HHG in systems with short-range order.
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