Response to “Comment on ‘Rethinking the evidence for a liquid–liquid transition in water: What decompression experiments reveal’” [J. Chem. Phys. 164, 024506 (2026)]

Ultrafast decompression experiments on deeply supercooled water have been interpreted as showing long-lived coexistence of high- and low-density liquids. We reassess this interpretation by separating the timescales of pressure release, structural relaxation, crystallization, and heat exchange. The experimental trajectories are adiabatic, and under these conditions, the two fitted wide-angle x-ray scattering components cannot represent equilibrium HDL and LDL persisting along a common thermodynamic path. We show instead that the spectra are consistent with a responsive liquid fraction evolving during decompression together with a structurally lagged, HDA-like fraction produced by heterogeneous heating. This framework also rationalizes the fluence dependence and clarifies the distinct information contained in the small-angle x-ray scattering response. The analysis identifies which observables can provide decisive evidence for a first-order liquid-liquid transition and constrain the location of its critical point.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2026-09-04
DOI
https://doi.org/10.1063/5.0352830
Primary Topic
Material Dynamics and Properties
Type
article
Field-Weighted Citation Impact
0.00

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article

Response to “Comment on ‘Rethinking the evidence for a liquid–liquid transition in water: What decompression experiments reveal’” [J. Chem. Phys. 164, 024506 (2026)]

Ingrid de Almeida Ribeiro, Valeria Molinero, Debdas Dhabal, Rajat Kumar
The Journal of Chemical Physics
Material Dynamics and Properties
article

Response to “Comment on ‘Rethinking the evidence for a liquid–liquid transition in water: What decompression experiments reveal’” [J. Chem. Phys. 164, 024506 (2026)]

Ingrid de Almeida Ribeiro, Valeria Molinero, Debdas Dhabal, Rajat Kumar
article en

Abstract

Ultrafast decompression experiments on deeply supercooled water have been interpreted as showing long-lived coexistence of high- and low-density liquids. We reassess this interpretation by separating the timescales of pressure release, structural relaxation, crystallization, and heat exchange. The experimental trajectories are adiabatic, and under these conditions, the two fitted wide-angle x-ray scattering components cannot represent equilibrium HDL and LDL persisting along a common thermodynamic path. We show instead that the spectra are consistent with a responsive liquid fraction evolving during decompression together with a structurally lagged, HDA-like fraction produced by heterogeneous heating. This framework also rationalizes the fluence dependence and clarifies the distinct information contained in the small-angle x-ray scattering response. The analysis identifies which observables can provide decisive evidence for a first-order liquid-liquid transition and constrain the location of its critical point.

The Journal of Chemical PhysicsVol. 165(9)
Indian Institute of Technology Guwahati (IN), University of Utah (US), Indian Institute of Information Technology Guwahati (IN)
U.S. Air Force, Multidisciplinary University Research Initiative, Air Force Office of Scientific Research
Clean water and sanitation
Openalex Percentile: Top 24%
Material Dynamics and Properties
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Response to “Comment on ‘Rethinking the evidence for a liquid–liquid transition in water: What decompression experiments reveal’” [J. Chem. Phys. 164, 024506 (2026)] — Ingrid de Almeida Ribeiro, Valeria Molinero, et al. · The Journal of Chemical Physics (2026) | TGRS Research Map | TGRS