DOI: 10.1063/1.4993790. Relaxation dynamics and transformation kinetics of deeply supercooled water: Temperature, pressure, doping, and proton/deuteron isotope effects

Relaxation dynamics and transformation kinetics of deeply supercooled water: Temperature, pressure, doping, and proton/deuteron isotope effects

10.1063/1.4993790

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

Above its glass transition, the equilibrated high-density amorphous ice (HDA) transforms to the low-density pendant (LDA). The temperature dependence of the transformation is monitored at ambient pressure using dielectric spectroscopy and at elevated pressures using dilatometry. It is found that near the glass transition temperature of deuterated samples, the transformation kinetics is 300 times slower than the structural relaxation, while for protonated samples, the time scale separation is at least 30 000 and insensitive to doping. The kinetics of the HDA to LDA transformation lacks a proton/deuteron isotope effect, revealing that this process is dominated by the restructuring of the oxygen network. The x-ray diffraction experiments performed on samples at intermediate transition stages reflect a linear combination of the LDA and HDA patterns implying a macroscopic phase separation, instead of a local intermixing of the two amorphous states.

Bibliography

Lemke, S., Handle, P. H., Plaga, L. J., Stern, J. N., Seidl, M., Fuentes-Landete, V., Amann-Winkel, K., KÃ¶ster, K. W., Gainaru, C., Loerting, T., & BÃ¶hmer, R. (2017). Relaxation dynamics and transformation kinetics of deeply supercooled water: Temperature, pressure, doping, and proton/deuteron isotope effects. The Journal of Chemical Physics, 147(3).

Authors 11

Sonja Lemke (first)
Philip H. Handle (additional)
Lucie J. Plaga (additional)
Josef N. Stern (additional)
Markus Seidl (additional)
Violeta Fuentes-Landete (additional)
Katrin Amann-Winkel (additional)
Karsten W. Köster (additional)
Catalin Gainaru (additional)
Thomas Loerting (additional)
Roland Böhmer (additional)

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Dates

Type	When
Created	8 years, 1 month ago (July 20, 2017, 9:44 a.m.)
Deposited	2 years, 1 month ago (July 15, 2023, 9:22 p.m.)
Indexed	3 weeks, 4 days ago (July 30, 2025, 7:10 a.m.)
Issued	8 years, 1 month ago (July 20, 2017)
Published	8 years, 1 month ago (July 20, 2017)
Published Online	8 years, 1 month ago (July 20, 2017)
Published Print	8 years, 1 month ago (July 21, 2017)

Funders 2

Deutsche Forschungsgemeinschaft 10.13039/501100001659
Region: Europe
gov (National government)
Labels3
1. German Research Association
2. German Research Foundation
3. DFG
Awards1
1. BO1301/12-1
Austrian Science Fund 10.13039/501100002428
Region: Europe
gov (National government)
Labels8
1. Fonds zur Förderung der Wissenschaftlichen Forschung
2. FWF Der Wissenschaftsfonds
3. FWF Austrian Science Fund
4. Der Wissenschaftsfonds FWF
5. Österreichischer Wissenschaftsfonds
6. FWF
7. FFWF
8. FWF EN
Awards1
1. I1392

BibTeX

@article{Lemke_2017, title={Relaxation dynamics and transformation kinetics of deeply supercooled water: Temperature, pressure, doping, and proton/deuteron isotope effects}, volume={147}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.4993790}, DOI={10.1063/1.4993790}, number={3}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Lemke, Sonja and Handle, Philip H. and Plaga, Lucie J. and Stern, Josef N. and Seidl, Markus and Fuentes-Landete, Violeta and Amann-Winkel, Katrin and Köster, Karsten W. and Gainaru, Catalin and Loerting, Thomas and Böhmer, Roland}, year={2017}, month=jul }

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