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Title: Surface and bulk crystallization of amorphous solid water films: Confirmation of “top-down” crystallization

Journal Article · · Surface Science
 [1];  [1];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
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Here, the crystallization kinetics of nanoscale amorphous solid water (ASW) films are investigated using temperature-programmed desorption (TPD) and reflection absorption infrared spectroscopy (RAIRS). TPD measurements are used to probe surface crystallization and RAIRS measurements are used to probe bulk crystallization. Isothermal TPD results show that surface crystallization is independent of the film thickness (from 100 to 1000 ML). Conversely, the RAIRS measurements show that the bulk crystallization time increases linearly with increasing film thickness. These results suggest that nucleation and crystallization begin at the ASW/vacuum interface and then the crystallization growth front propagates linearly into the bulk. This mechanism was confirmed by selective placement of an isotopic layer (5% D2O in H2O) at various positions in an ASW (H2O) film. In this case, the closer the isotopic layer was to the vacuum interface, the earlier the isotopic layer crystallized. These experiments provide direct evidence to confirm that ASW crystallization in vacuum proceeds by a “top-down” crystallization mechanism.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1250887
Alternate ID(s):
OSTI ID: 1397338
Report Number(s):
PNNL-SA-114712; PII: S0039602816000042
Journal Information:
Surface Science, Vol. 117, Issue C; ISSN 0039-6028
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

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Cited By (6)

Homogeneous ice nucleation rates and crystallization kinetics in transiently-heated, supercooled water films from 188 K to 230 K journal May 2019
Thickness dependent homogeneous crystallization of ultrathin amorphous solid water films journal January 2020
Crystallization growth rates and front propagation in amorphous solid water films journal June 2019
Communication: Proton exchange in low temperature co-mixed amorphous H 2 O and D 2 O films: The effect of the underlying Pt(111) and graphene substrates journal August 2018
Perspective: Surface freezing in water: A nexus of experiments and simulations journal August 2017
Perspective: Surface Freezing in Water: A Nexus of Experiments and Simulations text January 2017

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
amorphous solid water
crystallization kinetics
surface nucleation
temperature-programmed desorption (TPD)
reflection absorption infrared spectroscopy (RAIRS)