Isotopic dilution study of the water/vapor interface by phase-sensitivesum-frequency vibrational spectroscopy

• 摘要：

  (Figure Presented) Phase-sensitive sum-frequency vibrational spectroscopy (PS-SFVS) has been used to probe the isotopically diluted water/vapor interfaces in the spectral regions of OD (2200-2800 cm ^-1) and OH (3000-3800 cm ^-1) stretches. The experimentally measured Im X _S ⁽²⁾ spectra, where X _S ⁽²⁾ is the surface nonlinear susceptibility, permit direct characterization of resonances of the interfaces. The X _S ⁽²⁾ spectrum of the HDO/vapor interface that is intrinsically simpler to analyze can be deduced from the result of isotopic dilution. It exhibits in the bonded-OH region a broad band comprising two parts with opposite signs, in contrast to those deduced earlier from fitting of the |X _S ⁽²⁾| ² spectra and those calculated by MD simulation, but consistent with that obtained for the H ₂O/vapor interface.

• 作者：

  传山 田;元壤 沈

• 刊名：

  Journal of the American Chemical Society

• 在线出版时间：

  2009-3-4