A combined time correlation function and instantaneous normal mode study of the sum frequency generation spectroscopy of the water/vapor interface

Theoretical approximations to the interface specific sum frequency generation (SFG) spectrum of O–H stretching at the water/vapor interface are constructed using time correlation function (TCF) and instantaneous normal mode (INM) methods. Both approaches lead to a (SSP polarization geometry) signal in excellent agreement with experimental measurements; the SFG spectrum of the entire water spectrum, both intermolecular and intramolecular, is reported. The observation that the INM spectrum is in agreement with the TCF result implies that motional narrowing effects play no role in the interfacial line shapes, in contrast to the O–H stretching dynamics in the bulk that leads to a narrowed line shape. This implies that (SSP) SFG spectroscopy is a probe of structure with dynamics not represented in the signal. The INM approach permits the elucidation of the molecular basis for the observed signal, and the motions responsible for the SFG line shape are well approximated as local O–H stretching modes. The complex...

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