Surface Charges at the CaF₂ /Water Interface Allow Very Fast Intermolecular Vibrational-Energy Transfer.

ABSTRACT: We investigate the dynamics of water in contact with solid calcium fluoride, where at low pH, localized charges can develop upon fluorite dissolution. We use 2D surface-specific vibrational spectroscopy to quantify the heterogeneity of the interfacial water (D₂ O) molecules and provide information about the sub-picosecond vibrational-energy-relaxation dynamics at the buried solid/liquid interface. We find that strongly H-bonded OD groups, with a vibrational frequency below 2500 cm^-1 , display very rapid spectral diffusion and vibrational relaxation; for weakly H-bonded OD groups, above 2500 cm^-1 , the dynamics slows down substantially. Atomistic simulations based on electronic-structure theory reveal the molecular origin of energy transport through the loca

SUBMITTER: Lesnicki D 

PROVIDER: S-EPMC7496624 | biostudies-literature | 2020 Jul

REPOSITORIES: biostudies-literature