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Two-dimensional infrared spectroscopy of isotope-diluted ice Ih


Perakis, F; Widmer, S; Hamm, P (2011). Two-dimensional infrared spectroscopy of isotope-diluted ice Ih. Journal of Chemical Physics, 134(20):204505.

Abstract

We present experimental 2D IR spectra of isotope diluted ice Ih (i.e., the OH stretch mode of HOD in D2O and the OD stretch mode of HOD in H2O) at T = 80 K. The main spectral features are the extremely broad 1-2 excited state transition, much broader than the corresponding 0-1 groundstate transition, as well as the presence of quantum beats. We do not observe any inhomogeneous broadening that might be expected due to proton disorder in ice Ih. Complementary, we perform simulations in the framework of the Lippincott-Schroeder model, which qualitatively reproduce the experimental observations. We conclude that the origin of the observed line shape features is the coupling of the OH-vibrational coordinate with crystal phonons and explain the beatings as a coherent oscillation of the O⋅⋅⋅O hydrogen bond degree of freedom.

Abstract

We present experimental 2D IR spectra of isotope diluted ice Ih (i.e., the OH stretch mode of HOD in D2O and the OD stretch mode of HOD in H2O) at T = 80 K. The main spectral features are the extremely broad 1-2 excited state transition, much broader than the corresponding 0-1 groundstate transition, as well as the presence of quantum beats. We do not observe any inhomogeneous broadening that might be expected due to proton disorder in ice Ih. Complementary, we perform simulations in the framework of the Lippincott-Schroeder model, which qualitatively reproduce the experimental observations. We conclude that the origin of the observed line shape features is the coupling of the OH-vibrational coordinate with crystal phonons and explain the beatings as a coherent oscillation of the O⋅⋅⋅O hydrogen bond degree of freedom.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:2011
Deposited On:09 Sep 2011 13:16
Last Modified:21 Nov 2017 15:28
Publisher:American Institute of Physics
ISSN:0021-9606
Funders:Swiss National Science Foundation (SNF) trough NCCR MUST
Additional Information:© 2011 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in J. Chem. Phys. 134, 204505 (2011) and may be found at http://jcp.aip.org/resource/1/jcpsa6/v134/i20/p204505_s1.
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1063/1.3592561
PubMed ID:21639454

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