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Unveiling a common phase transition pathway of high-density amorphous ices through time-resolved x-ray scattering
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Number of Authors: 152024 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 160, no 24, article id 244503Article in journal (Refereed) Published
Abstract [en]

Here, we investigate the hypothesis that despite the existence of at least two high-density amorphous ices, only one high-density liquid state exists in water. We prepared a very-high-density amorphous ice (VHDA) sample and rapidly increased its temperature to around 205 ± 10 K using laser-induced isochoric heating. This temperature falls within the so-called “no-man’s land” well above the glass-liquid transition, wherein the IR laser pulse creates a metastable liquid state. Subsequently, this high-density liquid (HDL) state of water decompresses over time, and we examined the time-dependent structural changes using short x-ray pulses from a free electron laser. We observed a liquid–liquid transition to low-density liquid water (LDL) over time scales ranging from 20 ns to 3 μs, consistent with previous experimental results using expanded high-density amorphous ice (eHDA) as the initial state. In addition, the resulting LDL derived both from VHDA and eHDA displays similar density and degree of inhomogeneity. Our observation supports the idea that regardless of the initial annealing states of the high-density amorphous ices, the same HDL and final LDL states are reached at temperatures around 205 K.

Place, publisher, year, edition, pages
2024. Vol. 160, no 24, article id 244503
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Atom and Molecular Physics and Optics
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URN: urn:nbn:se:su:diva-238609DOI: 10.1063/5.0216904ISI: 001284555500002PubMedID: 38916268Scopus ID: 2-s2.0-85197006209OAI: oai:DiVA.org:su-238609DiVA, id: diva2:1933100
Available from: 2025-01-30 Created: 2025-01-30 Last updated: 2025-01-30Bibliographically approved

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Eklund, TobiasSpäh, AlexanderPathak, HarshadPerakis, FivosNilsson, AndersAmann-Winkel, Katrin

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