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

Abstract

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.

Authors:
 [1];  [1];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1250887
Alternate Identifier(s):
OSTI ID: 1397338
Report Number(s):
PNNL-SA-114712
Journal ID: ISSN 0039-6028; PII: S0039602816000042
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Surface Science
Additional Journal Information:
Journal Volume: 117; Journal Issue: C; Journal ID: ISSN 0039-6028
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; amorphous solid water; crystallization kinetics; surface nucleation; temperature-programmed desorption (TPD); reflection absorption infrared spectroscopy (RAIRS)

Citation Formats

Yuan, Chunqing, Smith, R. Scott, and Kay, Bruce D. Surface and bulk crystallization of amorphous solid water films: Confirmation of “top-down” crystallization. United States: N. p., 2016. Web. doi:10.1016/j.susc.2015.12.037.
Yuan, Chunqing, Smith, R. Scott, & Kay, Bruce D. Surface and bulk crystallization of amorphous solid water films: Confirmation of “top-down” crystallization. United States. https://doi.org/10.1016/j.susc.2015.12.037
Yuan, Chunqing, Smith, R. Scott, and Kay, Bruce D. Mon . "Surface and bulk crystallization of amorphous solid water films: Confirmation of “top-down” crystallization". United States. https://doi.org/10.1016/j.susc.2015.12.037. https://www.osti.gov/servlets/purl/1250887.
@article{osti_1250887,
title = {Surface and bulk crystallization of amorphous solid water films: Confirmation of “top-down” crystallization},
author = {Yuan, Chunqing and Smith, R. Scott and Kay, Bruce D.},
abstractNote = {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.},
doi = {10.1016/j.susc.2015.12.037},
journal = {Surface Science},
number = C,
volume = 117,
place = {United States},
year = {2016},
month = {1}
}

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