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Related Experiment Videos

Transport in amorphous solid water films: implications for self-diffusivity.

Sean M McClure1, Evan T Barlow, Minta C Akin

  • 1Institute for Theoretical Chemistry and Texas Materials Institute, Department of Chemical Engineering, University of Texas at Austin, Texas 78712-0321, USA.

The Journal of Physical Chemistry. B
|September 8, 2006
PubMed
Summary
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Investigating water transport in nanoscale films reveals that interlayer mixing occurs via vapor-phase transport through cracks, not bulk diffusion. Amorphous solid water (ASW) self-diffusivity is lower than expected for a fragile liquid before crystallization.

Area of Science:

  • Materials Science
  • Physical Chemistry
  • Surface Science

Background:

  • Understanding transport mechanisms in nanoscale films is crucial for materials development.
  • Amorphous solid water (ASW) plays a role in various scientific fields, including astrophysics and atmospheric science.
  • Nanoscale films with organic spacer layers present unique challenges for studying diffusion and phase transitions.

Purpose of the Study:

  • To investigate water self-transport mechanisms in structured nanoscale films consisting of amorphous solid water (ASW) and organic spacer layers.
  • To determine the effectiveness of organic spacer layers as diffusion barriers.
  • To elucidate the role of vapor-phase transport versus bulk diffusion in interlayer mixing during ASW crystallization.

Main Methods:

Related Experiment Videos

  • Thermal desorption spectroscopy (TDS) was used to examine transport mechanisms in labeled ASW (H(2)(18)O, H(2)(16)O) and organic spacer layers (CCl(4), CHCl(3)).
  • Isothermal desorption measurements were combined with gas uptake measurements (CClF(2)H) to study ASW self-transport and morphology changes.
  • CCl(4) desorption was used to investigate vapor-phase transport influenced by ASW film thickness and heating schedules.

    • Main Results:

    • Interlayer mixing observed near 150-160 K is inconsistent with bulk diffusion, suggesting vapor-phase transport through cracks.
    • Organic spacer layers showed limited effectiveness as bulk diffusion barriers.
    • ASW self-diffusivity prior to crystallization is significantly lower than predicted for a fragile liquid.

    Conclusions:

    • Intermixing in ASW/organic films occurs via vapor-phase transport through cracks formed during crystallization, not bulk diffusion.
    • The self-diffusivity of ASW below 160 K is substantially lower than expected for a fragile liquid.
    • Water likely undergoes a glass transition or a fragile-to-strong transition at temperatures above 160 K.