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Issue 18, 2012
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Two-dimensional infrared spectroscopy of neat ice Ih

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Abstract

The OH stretch line shape of ice Ih exhibits distinct peaks, the assignment of which remains controversial. We address this longstanding question using two dimensional infrared (2D IR) spectroscopy of the OH stretch of H2O and the OD stretch of D2O of ice Ih at T = 80 K. The isotropic response is dominated by a 2D line shape component which does not depend on the pump pulse frequency. The decay time of the component that does depend on the pump frequency is calculated using singular value decomposition (bi-exponential decay H2O: 30 fs, 490 fs; D2O: 40 fs, 690 fs). The anisotropic contribution exhibits on-diagonal peaks, which decay on a very fast timescale (H2O: 85 fs; D2O: 65 fs), with no corresponding anisotropic cross-peaks. Both isotropic and anisotropic results indicate that randomization of excited dipoles occurs with a very rapid rate, just like in neat liquid water. We conclude that the underlying mechanism relates to the complex interplay between exciton migration and exciton–phonon coupling.

Graphical abstract: Two-dimensional infrared spectroscopy of neat ice Ih

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Publication details

The article was received on 23 Nov 2011, accepted on 16 Dec 2011 and first published on 19 Dec 2011


Article type: Paper
DOI: 10.1039/C2CP23710E
Citation: Phys. Chem. Chem. Phys., 2012,14, 6250-6256
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    Two-dimensional infrared spectroscopy of neat ice Ih

    F. Perakis and P. Hamm, Phys. Chem. Chem. Phys., 2012, 14, 6250
    DOI: 10.1039/C2CP23710E

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