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Communication: Disorder-suppressed vibrational relaxation in vapor-deposited high-density amorphous ice


Shalit, Andrey; Perakis, Fivos; Hamm, Peter (2014). Communication: Disorder-suppressed vibrational relaxation in vapor-deposited high-density amorphous ice. Journal of Chemical Physics, 140(15):151102.

Abstract

We apply two-dimensional infrared spectroscopy to differentiate between the two polyamorphous forms of glassy water – low-density (LDA) and high-density (HDA) amorphous ices, that were obtained by slow vapor deposition at 80 and 11 K respectively. Both the vibrational lifetime and the bandwidth of the 1–2 transition of the isolated OD stretch vibration of HDO in H2O exhibit characteristic differences when comparing hexagonal (Ih), LDA and HDA ices, which we attribute the different local structures – in particular the presence of interstitial waters in HDA ice – that cause different delocalization lengths of intermolecular phonon degrees of freedom. Moreover, temperature dependent measurements show that the vibrational lifetime closely follows the structural transition between HDA and LDA phases.

Abstract

We apply two-dimensional infrared spectroscopy to differentiate between the two polyamorphous forms of glassy water – low-density (LDA) and high-density (HDA) amorphous ices, that were obtained by slow vapor deposition at 80 and 11 K respectively. Both the vibrational lifetime and the bandwidth of the 1–2 transition of the isolated OD stretch vibration of HDO in H2O exhibit characteristic differences when comparing hexagonal (Ih), LDA and HDA ices, which we attribute the different local structures – in particular the presence of interstitial waters in HDA ice – that cause different delocalization lengths of intermolecular phonon degrees of freedom. Moreover, temperature dependent measurements show that the vibrational lifetime closely follows the structural transition between HDA and LDA phases.

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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:21 April 2014
Deposited On:09 Oct 2014 09:09
Last Modified:12 May 2016 12:52
Publisher:American Institute of Physics
ISSN:0021-9606
Funders:Swiss National Science Foundation (SNF) in a National Center of Competence and Research (NCCR) MUST, EU cofund IFP-MUST
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1063/1.4871476

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