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research article

Dynamical heterogeneity in supercooled water and its spectroscopic fingerprints

Malosso, Cesare  
•
Donkor, Edward Danquah
•
Baroni, Stefano
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October 10, 2025
The Journal of Chemical Physics

A growing body of theoretical and experimental evidence strongly supports the existence of a second liquid–liquid critical point (LLCP) in deeply supercooled water leading to the co-existence of two phases: a high- and low-density liquid (HDL and LDL). While the thermodynamics associated with this putative LLCP has been well characterized through numerical simulations, the dynamical properties of these two phases close to the critical point remain much less understood. In this work, we investigate their dynamical and spectroscopic features using machine-learning interatomic potentials. Dynamical analyses using the van Hove correlation function reveal that LDL exhibits very sluggish and heterogeneous molecular mobility, in contrast to the faster and more homogeneous dynamics of HDL. Infrared absorption (IR) spectra further show clear vibrational distinctions between LDL and HDL, in particular in the far IR region between 400 and 1000 cm−1. Together, these findings provide new dynamical fingerprints that clarify the microscopic behavior of supercooled water and offer valuable guidance for experimental efforts aimed at detecting the long-sought liquid–liquid transition.

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Type
research article
DOI
10.1063/5.0288343
Author(s)
Malosso, Cesare  

École Polytechnique Fédérale de Lausanne

Donkor, Edward Danquah

Polytechnic University of Turin

Baroni, Stefano

Scuola Internazionale Superiore di Studi Avanzati

Hassanali, Ali

The Abdus Salam International Centre for Theoretical Physics (ICTP)

Date Issued

2025-10-10

Publisher

AIP Publishing

Published in
The Journal of Chemical Physics
Volume

163

Issue

14

Article Number

144508

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
FunderFunding(s)Grant NumberGrant URL

European Commission

101093374

Ministero dell’Università e della Ricerca

2022W2BPCK

NextGenerationEU

CN00000013

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Available on Infoscience
October 14, 2025
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/254889
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