Disorder Analysis in Infrared Spectroscopy of Acetylene Ice.

ABSTRACT

A new method to investigate disorder in ice films is proposed and applied to acetylene ice. It is based on a quantitative analysis of the infrared spectrum data, which includes the Brendel-Bormann model for the material's dielectric function; molecular vibration modes calculated by density functional theory (DFT); a monomer-dimer model for amorphous ice; and a peak-shape analysis through Levenberg-Marquardt nonlinear regression. Acetylene ice films with different degrees of disorder were investigated with the proposed method. The results provide an estimate of the degree of disorder in the films and indicate the possibility of existence of a second amorphous phase of acetylene ice grown at temperatures of about 15 K and then annealed. This phase would be similar to the high-density amorphous phase observed for water ice. The infrared data in this work is compared with those from the literature for acetylene gas, acetylene film, and acetylene aerosol. A qualitative analysis reveals differences in the degree of disorder in each system and points to a crystallinity limit for acetylene ice film; that is, the crystalline acetylene film has a higher degree of intrinsic disorder than the crystalline acetylene aerosol.