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Title: Thermal and Non-thermal Physiochemical Processes in Nanoscale Films of Amorphous Solid Water

Abstract

Amorphous solid water (ASW) is a metastable form of water created by vapor deposition onto a cold substrate (typically less than 130 K). Since this unusual form of water only exists on earth in laboratories with highly specialized equipment, it is fair to ask why there is any interest in studying this esoteric material. Much of the scientific interest involves using ASW as a model system to explore the physical and reactive properties of liquid water and aqueous solutions. Other researchers are interested in ASW because it is believed to be the predominate form of water in the extreme cold temperatures found in many astrophysical and planetary environments. In addition, ASW is a convenient model system for studying the stability of metastable systems (glasses) and the properties of highly porous materials. A fundamental understanding of such properties has applications in a diverse range of disciplines including cryobiology, food science, pharmaceuticals, astrophysics and nuclear waste storage among others.There exist several excellent reviews on the properties of ASW and supercooled liquid water and a new comprehensive review is beyond the scope of this Account. Instead, we focus on our research over the past 15 years using molecular beams and surface science techniquesmore » to probe the thermal and non thermal properties of nanoscale films of ASW. We use molecular beams to precisely control the deposition conditions (flux, incident, energy, incident angle) to create compositionally-tailored, nanoscale films of ASW at low temperatures. To study the transport properties (viscosity, diffusivity), the amorphous films can be heated above their glass transition temperatures, Tg, at which time they transform into deeply supercooled liquids prior to crystallization. The advantage of this approach is that at temperatures near Tg the viscosity is approximately 15 orders of magnitude larger than a normal liquid, and therefore the crystallization kinetics are dramatically slowed, increasing the time available for experiments. For example, near Tg, on a typical laboratory time scale (e.g. {approx}1000 s), a water molecule moves less than a molecular distance. For this reason, nanoscale films help to probe the behavior and reactions of supercooled liquid at these low temperatures. ASW films can be used for investigating the non-thermal reactions relevant to radiolysis. In this account we will present a survey of our research on the thermal and non thermal properties of ASW using this approach.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1034230
Report Number(s):
PNNL-SA-78512
Journal ID: ISSN 0001-4842; ACHRE4; 42300; 39898; KC0301020; TRN: US1200762
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Accounts of Chemical Research
Additional Journal Information:
Journal Volume: 45; Journal Issue: 1; Journal ID: ISSN 0001-4842
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; AQUEOUS SOLUTIONS; CRYSTALLIZATION; DEPOSITION; KINETICS; MOLECULAR BEAMS; POROUS MATERIALS; PROBES; RADIOACTIVE WASTES; RADIOLYSIS; STABILITY; SUBSTRATES; THERMODYNAMIC PROPERTIES; TRANSITION TEMPERATURE; VISCOSITY; Environmental Molecular Sciences Laboratory

Citation Formats

Smith, R Scott, Petrik, Nikolay G, Kimmel, Gregory A, and Kay, Bruce D. Thermal and Non-thermal Physiochemical Processes in Nanoscale Films of Amorphous Solid Water. United States: N. p., 2012. Web. doi:10.1021/ar200070w.
Smith, R Scott, Petrik, Nikolay G, Kimmel, Gregory A, & Kay, Bruce D. Thermal and Non-thermal Physiochemical Processes in Nanoscale Films of Amorphous Solid Water. United States. https://doi.org/10.1021/ar200070w
Smith, R Scott, Petrik, Nikolay G, Kimmel, Gregory A, and Kay, Bruce D. 2012. "Thermal and Non-thermal Physiochemical Processes in Nanoscale Films of Amorphous Solid Water". United States. https://doi.org/10.1021/ar200070w.
@article{osti_1034230,
title = {Thermal and Non-thermal Physiochemical Processes in Nanoscale Films of Amorphous Solid Water},
author = {Smith, R Scott and Petrik, Nikolay G and Kimmel, Gregory A and Kay, Bruce D},
abstractNote = {Amorphous solid water (ASW) is a metastable form of water created by vapor deposition onto a cold substrate (typically less than 130 K). Since this unusual form of water only exists on earth in laboratories with highly specialized equipment, it is fair to ask why there is any interest in studying this esoteric material. Much of the scientific interest involves using ASW as a model system to explore the physical and reactive properties of liquid water and aqueous solutions. Other researchers are interested in ASW because it is believed to be the predominate form of water in the extreme cold temperatures found in many astrophysical and planetary environments. In addition, ASW is a convenient model system for studying the stability of metastable systems (glasses) and the properties of highly porous materials. A fundamental understanding of such properties has applications in a diverse range of disciplines including cryobiology, food science, pharmaceuticals, astrophysics and nuclear waste storage among others.There exist several excellent reviews on the properties of ASW and supercooled liquid water and a new comprehensive review is beyond the scope of this Account. Instead, we focus on our research over the past 15 years using molecular beams and surface science techniques to probe the thermal and non thermal properties of nanoscale films of ASW. We use molecular beams to precisely control the deposition conditions (flux, incident, energy, incident angle) to create compositionally-tailored, nanoscale films of ASW at low temperatures. To study the transport properties (viscosity, diffusivity), the amorphous films can be heated above their glass transition temperatures, Tg, at which time they transform into deeply supercooled liquids prior to crystallization. The advantage of this approach is that at temperatures near Tg the viscosity is approximately 15 orders of magnitude larger than a normal liquid, and therefore the crystallization kinetics are dramatically slowed, increasing the time available for experiments. For example, near Tg, on a typical laboratory time scale (e.g. {approx}1000 s), a water molecule moves less than a molecular distance. For this reason, nanoscale films help to probe the behavior and reactions of supercooled liquid at these low temperatures. ASW films can be used for investigating the non-thermal reactions relevant to radiolysis. In this account we will present a survey of our research on the thermal and non thermal properties of ASW using this approach.},
doi = {10.1021/ar200070w},
url = {https://www.osti.gov/biblio/1034230}, journal = {Accounts of Chemical Research},
issn = {0001-4842},
number = 1,
volume = 45,
place = {United States},
year = {2012},
month = {1}
}