Anomalously large isotope effect in the glass transition of water

Gainaru, Catalin; Agapov, Alexander L.; Fuentes-Landete, Violeta; Amann-Winkel, Katrin; Nelson, Helge; Köster, Karsten W.; Kolesnikov, Alexander I.; Novikov, Vladimir N.; Richert, Ranko; Böhmer, Roland; Loerting, Thomas; Sokolov, Alexei P.

doi:10.1073/pnas.1411620111

Title: Anomalously large isotope effect in the glass transition of water

Journal Article · Mon Nov 24 00:00:00 EST 2014 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1411620111· OSTI ID:1286807

Gainaru, Catalin ^[1]; Agapov, Alexander L. ^[2]; Fuentes-Landete, Violeta ^[3]; Amann-Winkel, Katrin ^[3]; Nelson, Helge ^[1]; Köster, Karsten W. ^[1]; Kolesnikov, Alexander I. ^[4]; Novikov, Vladimir N. ^[2]; Richert, Ranko ^[5]; Böhmer, Roland ^[1]; Loerting, Thomas ^[3]; Sokolov, Alexei P. ^[2]

Dortmund Univ. of Technology (Germany). Dept. of Physics
Univ. of Tennessee, Knoxville, TN (United States). Joint Inst. for Neutron Sciences, Dept. of Chemistry; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Science Division
Univ. of Innsbruck, Innsbruck (Austria). Inst. of Physical Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
Arizona State Univ., Tempe, AZ (United States). Dept. of Chemistry and Biochemistry

Here we present the discovery of an unusually large isotope effect in the structural relaxation and the glass transition temperature T_g of water. Dielectric relaxation spectroscopy of low-density as well as of vapor deposited amorphous water reveal T_g differences of 10±2K between H₂O and D₂O, sharply contrasting with other hydrogen bonded liquids for which H/D exchange increases T_g by typically less than 1K. We show that the large isotope effect and the unusual variation of relaxation times in water at low temperatures can be explained in terms of quantum effects. Thus, our findings shed new light on water's peculiar low-temperature dynamics and the possible role of quantum effects in its structural relaxation, and possibly in dynamics of other low molecular weight liquids.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725; CHE-1213444; CHE-1026124; BO1301

OSTI ID:: 1286807

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Vol. 111, Issue 49; ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 52 works

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Diffusive dynamics during the high-to-low density transition in amorphous ice Perakis, Fivos; Amann-Winkel, Katrin; Lehmkühler, Felix Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2017-08683	text	January 2017
Thermodynamic and kinetic isotope effects on the order–disorder transition of ice XIV to ice XII Fuentes-Landete, Violeta; Köster, Karsten W.; Böhmer, Roland Physical Chemistry Chemical Physics, Vol. 20, Issue 33 https://doi.org/10.1039/c8cp03786h	journal	January 2018
Structural differences between unannealed and expanded high-density amorphous ice based on isotope substitution neutron diffraction Amann-Winkel, Katrin; Bowron, Daniel T.; Loerting, Thomas Molecular Physics, Vol. 117, Issue 22 https://doi.org/10.1080/00268976.2019.1649487	journal	August 2019
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Origin of the emergent fragile-to-strong transition in supercooled water Shi, Rui; Russo, John; Tanaka, Hajime Proceedings of the National Academy of Sciences, Vol. 115, Issue 38 https://doi.org/10.1073/pnas.1807821115	journal	September 2018
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Water: A Tale of Two Liquids Gallo, Paola; Amann-Winkel, Katrin; Angell, Charles Austen Chemical Reviews, Vol. 116, Issue 13 https://doi.org/10.1021/acs.chemrev.5b00750	journal	April 2016

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Title: Anomalously large isotope effect in the glass transition of water

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