Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 12, Issue 15, Pages 3827-3836Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c00257
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Funding
- Grant ANR DYNAWIN [ANR-14-CE35-0011-01]
- GENCI-France Grant [072484]
- Cluster of Excellence RESOLV - Deutsche Forschungsgemeinschaft (DFG) [EXC2033]
- Research Training Group Confinement-controlled Chemistry - Deutsche Forschungsgemeinschaft (DFG) [GRK2376/331085229]
- ERC [695437]
- European Research Council (ERC) [695437] Funding Source: European Research Council (ERC)
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The hydrophobicity/hydrophilicity of aqueous interfaces is influenced by a delicate balance between water-water and water-surface interactions. Through DFT-MD, SFG, and THz-IR absorption spectroscopies, it has been shown that water at interfaces forms a two-dimensional hydrogen-bonded network, revealing the competition between water-surface and water-water interactions. Combining SFG and THz-IR spectroscopies provides a powerful tool for characterizing molecular hydrophobicity at aqueous interfaces.
Hydrophobicity/hydrophilicity of aqueous interfaces at the molecular level results from a subtle balance in the water-water and water-surface interactions. This is characterized here via density functional theory-molecular dynamics (DFT-MD) coupled with vibrational sum frequency generation (SFG) and THz-IR absorption spectroscopies. We show that water at the interface with a series of weakly interacting materials is organized into a two-dimensional hydrogen-bonded network (2D-HB-network), which is also found above some macroscopically hydrophilic silica and alumina surfaces. These results are rationalized through a descriptor that measures the number of vertical and horizontal hydrogen bonds formed by interfacial water, quantifying the competition between water-surface and water-water interactions. The 2D-HB-network is directly revealed by THz-IR absorption spectroscopy, while the competition of water-water and water-surface interactions is quantified from SFG markers. The combination of SFG and THz-IR spectroscopies is thus found to be a compelling tool to characterize the finest details of molecular hydrophobicity at aqueous interfaces.
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