Surface-specific vibrational spectroscopic responses at isotope diluted ice and amorphous ice are investigated by molecular dynamics (MD) simulations combined with quantum mechanics/molecular mechanics calculations. The intense response specific to the ordinary crystal ice surface is predicted to be significantly suppressed in the isotopically diluted and amorphous ices, demonstrating the vibrational delocalization at the ordinary ice surface. The collective vibration at the ice surface is also analyzed with varying temperature by the MD simulation.
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The present system of isotope dilution contains a H2O molecule rather than HOD to facilitate the sampling of OH vibrational spectra. The intramolecular coupling in H2O has a marginal effect compared to the intermolecular coupling and charge transfer effects.
29.
One may notice in the calculated spectra of Fig. 2 some wiggling behaviors due to a limited amount of sampling. We can nevertheless define the peak amplitude for the dangling signal at 3700
$\protect \mathrm{cm}^{-1}$
by properly separating the wiggling noise. By considering the decomposition analysis by depth (see Fig. 3 (Case 1) in Ref. 12), we found that the dangling peak comes from the topmost bilayer while the wiggling noise originates from the deeper region.© 2014 AIP Publishing LLC.
2014
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