Liquid-liquid phase separation in supercooled water from ultrafast heating of low-density amorphous ice

Amann-Winkel, Katrin; Kim, Kyung Hwan; Giovambattista, Nicolas; Ladd-Parada, Marjorie; Späh, Alexander; Perakis, Fivos; Pathak, Harshad; Yang, Cheolhee; Eklund, Tobias; Lane, Thomas J.; You, Seonju; Jeong, Sangmin; Lee, Jae Hyuk; Eom, Intae; Kim, Minseok; Park, Jaeku; Chun, Sae Hwan; Poole, Peter H.; Nilsson, Anders

doi:10.1038/s41467-023-36091-1

Liquid-liquid phase separation in supercooled water from ultrafast heating of low-density amorphous ice

Journal Article · Fri Jan 27 00:00:00 EST 2023 · Nature Communications

DOI:https://doi.org/10.1038/s41467-023-36091-1· OSTI ID:2005034

^[1]; Kim, Kyung Hwan ^[2]; ^[3]; ^[4]; Späh, Alexander ^[5]; ^[5]; Pathak, Harshad ^[5]; Yang, Cheolhee ^[2]; Eklund, Tobias ^[5]; ^[6]; ^[2]; Jeong, Sangmin ^[2]; ^[7]; ^[7]; Kim, Minseok ^[7]; ^[7]; ^[7]; ^[8]; ^[5]

Stockholm Univ. (Sweden); Max Planck Institute for Polymer Research, Mainz (Germany); Johannes Gutenberg Univ., Mainz (Germany); SLAC
Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
City Univ. of New York (CUNY), Brooklyn, NY (United States). Brooklyn College
KTH Royal Inst. of Technology, Stockholm (Sweden); Stockholm Univ. (Sweden)
Stockholm Univ. (Sweden)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Pohang Accelerator Lab. (PAL) (Korea, Republic of)
St. Francis Xavier Univ., Antigonish, NS (Canada)

Recent experiments continue to find evidence for a liquid-liquid phase transition (LLPT) in supercooled water, which would unify our understanding of the anomalous properties of liquid water and amorphous ice. These experiments are challenging because the proposed LLPT occurs under extreme metastable conditions where the liquid freezes to a crystal on a very short time scale. Here, we analyze models for the LLPT to show that coexistence of distinct high-density and low-density liquid phases may be observed by subjecting low-density amorphous (LDA) ice to ultrafast heating. We then describe experiments in which we heat LDA ice to near the predicted critical point of the LLPT by an ultrafast infrared laser pulse, following which we measure the structure factor using femtosecond x-ray laser pulses. Consistent with our predictions, we observe a LLPT occurring on a time scale <100 ns and widely separated from ice formation, which begins at times >1 μs.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Research Foundation of Korea (NRF); National Science Foundation (NSF); Natural Sciences and Engineering Research Council of Canada (NSERC); Ragnar Söderbergs Stiftelse; Swedish National Research Council; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2005034

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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