Film Growth of Ice by Vapor Deposition at 128−185 K Studied by Fourier Transform Infrared Reflection−Absorption Spectroscopy: Evolution of the OH Stretch and the Dangling Bond with Film Thickness

The polycrystalline and noncrystalline ice films vapor-deposited at 128−185 K were investigated by grazing-angle Fourier transform Infrared Reflection−Absorption Spectroscopy (RAS). In particular, the polycrystalline ice phase was found above 155 K, whereas the noncrystalline phase was formed below 145 K. The nature of the polycrystalline and noncrystalline ice phases can be differentiated by comparing the respective RA spectra with spectral simulations based on the Fresnel reflection and Mie scattering methods. Furthermore, the OH stretching band (3800−2800 cm-1) exhibits complex behavior as a function of film thickness (from less than 10 nm to 1500 nm), which can be simulated and attributed primarily to the physics of absorption−reflection based on the Fresnel equations for reflection coefficients for parallel- and perpendicular-polarized light in a vacuum-dielectric film-metal system. The spectral evolution of the OH stretch with the film thickness is found to be similar for both polycrystalline and no...