Diffusive dynamics during the high-to-low density transition in amorphous ice

Perakis, Fivos; Amann-Winkel, Katrin; Lehmkuhler, Felix; Sprung, Michael; Mariedahl, Daniel; Sellberg, Jonas A.; Pathak, Harshad; Spah, Alexander; Cavalca, Filippo; Schlesinger, Daniel; Ricci, Alessandro; Jain, Avni; Massani, Bernhard; Aubree, Flora; Benmore, Chris J.; Loerting, Thomas; Grubel, Gerhard; Pettersson, Lars G. M.; Nilsson, Anders

doi:10.1073/pnas.1705303114

Title: Diffusive dynamics during the high-to-low density transition in amorphous ice

Journal Article · 26 June 2017 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.1705303114 · OSTI ID:1390292

Perakis, Fivos ^[1]; Amann-Winkel, Katrin ^[2]; Lehmkuhler, Felix ^[3]; Sprung, Michael ^[4]; Mariedahl, Daniel ^[2]; Sellberg, Jonas A. ^[5]; Pathak, Harshad ^[2]; Spah, Alexander ^[2]; Cavalca, Filippo ^[1]; Schlesinger, Daniel ^[2]; Ricci, Alessandro ^[2]; Jain, Avni ^[4]; Massani, Bernhard ^[6]; Aubree, Flora ^[6]; Benmore, Chris J. ^[7];

^[6]; Grubel, Gerhard ^[3]; Pettersson, Lars G. M. ^[2]; Nilsson, Anders ^[2]

Stockholm Univ., Stockholm (Sweden); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stockholm Univ., Stockholm (Sweden)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
KTH Royal Institute of Technology, Stockholm (Sweden)
Univ. of Innsbruck, Innsbruck (Austria)
Argonne National Lab. (ANL), Argonne, IL (United States)

Water exists in high- and low-density amorphous ice forms (HDA and LDA), which could correspond to the glassy states of high- (HDL) and low-density liquid (LDL) in the metastable part of the phase diagram. However, the nature of both the glass transition and the high-to-low-density transition are debated and new experimental evidence is needed. Here we combine wide-angle X-ray scattering (WAXS) with X-ray photon-correlation spectroscopy (XPCS) in the small-angle X-ray scattering (SAXS) geometry to probe both the structural and dynamical properties during the high-to-low-density transition in amorphous ice at 1 bar. By analyzing the structure factor and the radial distribution function, the coexistence of two structurally distinct domains is observed at T = 125 K. XPCS probes the dynamics in momentum space, which in the SAXS geometry reflects structural relaxation on the nanometer length scale. The dynamics of HDA are characterized by a slow component with a large time constant, arising from viscoelastic relaxation and stress release from nanometer-sized heterogeneities. Above 110 K a faster, strongly temperature-dependent component appears, with momentum transfer dependence pointing toward nanoscale diffusion. This dynamical component slows down after transition into the low-density form at 130 K, but remains diffusive. In conclusion, the diffusive character of both the high- and low-density forms is discussed among different interpretations and the results are most consistent with the hypothesis of a liquid–liquid transition in the ultraviscous regime.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-76SF00515; 667205; 2013-3737-VR; P2ZHP2 148666; I1392; EXC1074; AC02-06CH11357

OSTI ID:: 1390292

Alternate ID(s):: OSTI ID: 1393142

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Vol. 114, Issue 31; ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 131 works

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71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
liquid–liquid transition
glass transition
amorphous ice
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supercooled water