Knowledge of the specific solvation structure and the molecular organization of a liquid or a liquid mixture in the vicinity of solid surfaces is crucial for understanding the physicochemical properties and functional roles of most surfaces. Interface-selective vibrational sum-frequency generation (VSFG) is used to obtain spectroscopic measurements of buried hydrophilic solid/liquid interfaces for a series of binary mixtures involving liquid methanol, acetonitrile, acetone and water. Here, we report the C-H and O-H stretch spectra and examine the role of Fermi coupling and the O-H stretching spectral lineshapes as reporters of competitive binding and interfacial intermolecular interactions. In addition, we use VSFG to experimentally investigate the interactions of water and charged surfactants at the mineral/liquid interface. The phase response of the third order susceptibility is observed to play a significant role in the spectral lineshapes sheding light into the hydrogen bonding network near the surface. We also examine intercalated solvent organization in the nanoconfinement region between a silica surface and carbon nanostructures.

Intermolecular interactions, partitioning, and preferential solvation at the mineral-liquid interface

ACS Fall 2021

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