Spectroscopic Signature of Stacking Disorder in Ice I

• Published in: The journal of physical chemistry letters 2014-07, Vol.5 (14), p.2469-2473
• Main Authors: Carr, Thomas H. G, Shephard, Jacob J, Salzmann, Christoph G
• Format: Article
• Language: English
• Subjects: Spectroscopy, Photochemistry, and Excited States
• ISSN: 1948-7185; 1948-7185
• DOI: 10.1021/jz500996p

There is a growing realization that the presence of stacking disorder in ice I strongly influences its physical and chemical properties. Using Raman spectroscopy, we gain new fundamental insights into the spectroscopic properties of ice. We show that stacking disorder can be detected and quantified by comparing the spectra of stacking disordered ice with spectra of the “ordinary” hexagonal ice Ih. The spectral signature of stacking disorder is thought to arise from a greater structural diversity on the local length scale, vibrational modes that appear due to the lower-symmetry environments, and a strengthening of the covalent bonds. Our findings are compared to results from diffraction and calorimetry, and we discuss the advantages and disadvantages of the three techniques with respect to detecting stacking disorder in ice I. Apart from characterizing stacking disordered ice in the research lab, our new method is perfectly suited for remote or telescopic applications aiming at the identification of stacking disordered ice in nature.