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Title: A nanosecond pulsed laser heating system for studying liquid and supercooled liquid films in ultrahigh vacuum

Abstract

A pulsed laser heating system has been developed that enables investigations of the dynamics and kinetics of nanoscale liquid films and liquid/solid interfaces on the nanosecond timescale in ultrahigh vacuum (UHV). Details of the design, implementation and characterization of a nanosecond pulsed laser system for transiently heating nanoscale films are described herein. Nanosecond pulses from a Nd:YAG laser are used to rapidly heat thin films of adsorbed water or other volatile materials on a clean, well-characterized Pt(111) crystal in UHV. Heating rates of ~1010 K/s for temperature increases of ~100 – 200 K are obtained. Subsequent rapid cooling (~5 × 109 K/s) quenches the film, permitting in-situ, post-mortem analysis using a variety of surface science techniques. Lateral variations in the laser pulse energy are ~ ± 3% leading to a temperature uncertainty of ~ ± 5 K for a temperature jump of 200 K. Initial experiments with the apparatus demonstrate that crystalline ice films initially held at 90 K can be rapidly transformed into liquid water films with T > 273 K. No discernable recrystallization occurs during the rapid cooling back to cryogenic temperatures. In contrast, amorphous solid water films heated below the melting point rapidly crystallize. The nanosecond pulsedmore » laser heating system can prepare nanoscale liquid and supercooled liquid films that persist for nanoseconds per heat pulse in an UHV environment, enabling experimental studies of a wide range of phenomena in liquids and at liquid/solid interfaces.« less

Authors:
 [1];  [1];  [2]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [1]
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  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical Sciences Division
  2. Physical Sciences Division, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, USA
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1327144
Alternate Identifier(s):
OSTI ID: 1249957
Report Number(s):
PNNL-SA-115728
Journal ID: ISSN 0021-9606; JCPSA6; 49144; KC0301050
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 144; Journal Issue: 16; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
47 OTHER INSTRUMENTATION; nanosecond pulsed laser heating; nanoscale liquid and liquid/solid interface far from equilibrium; chemical dynamics and kinetics; fast heating and cooling; Environmental Molecular Sciences Laboratory

Citation Formats

Xu, Yuntao, Dibble, Collin J., Petrik, Nikolay G., Smith, R. Scott, Joly, Alan G., Tonkyn, Russell G., Kay, Bruce D., and Kimmel, Greg A. A nanosecond pulsed laser heating system for studying liquid and supercooled liquid films in ultrahigh vacuum. United States: N. p., 2016. Web. doi:10.1063/1.4947304.
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Xu, Yuntao, Dibble, Collin J., Petrik, Nikolay G., Smith, R. Scott, Joly, Alan G., Tonkyn, Russell G., Kay, Bruce D., & Kimmel, Greg A. A nanosecond pulsed laser heating system for studying liquid and supercooled liquid films in ultrahigh vacuum. United States. https://doi.org/10.1063/1.4947304
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Xu, Yuntao, Dibble, Collin J., Petrik, Nikolay G., Smith, R. Scott, Joly, Alan G., Tonkyn, Russell G., Kay, Bruce D., and Kimmel, Greg A. Tue . "A nanosecond pulsed laser heating system for studying liquid and supercooled liquid films in ultrahigh vacuum". United States. https://doi.org/10.1063/1.4947304. https://www.osti.gov/servlets/purl/1327144.
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@article{osti_1327144,
title = {A nanosecond pulsed laser heating system for studying liquid and supercooled liquid films in ultrahigh vacuum},
author = {Xu, Yuntao and Dibble, Collin J. and Petrik, Nikolay G. and Smith, R. Scott and Joly, Alan G. and Tonkyn, Russell G. and Kay, Bruce D. and Kimmel, Greg A.},
abstractNote = {A pulsed laser heating system has been developed that enables investigations of the dynamics and kinetics of nanoscale liquid films and liquid/solid interfaces on the nanosecond timescale in ultrahigh vacuum (UHV). Details of the design, implementation and characterization of a nanosecond pulsed laser system for transiently heating nanoscale films are described herein. Nanosecond pulses from a Nd:YAG laser are used to rapidly heat thin films of adsorbed water or other volatile materials on a clean, well-characterized Pt(111) crystal in UHV. Heating rates of ~1010 K/s for temperature increases of ~100 – 200 K are obtained. Subsequent rapid cooling (~5 × 109 K/s) quenches the film, permitting in-situ, post-mortem analysis using a variety of surface science techniques. Lateral variations in the laser pulse energy are ~ ± 3% leading to a temperature uncertainty of ~ ± 5 K for a temperature jump of 200 K. Initial experiments with the apparatus demonstrate that crystalline ice films initially held at 90 K can be rapidly transformed into liquid water films with T > 273 K. No discernable recrystallization occurs during the rapid cooling back to cryogenic temperatures. In contrast, amorphous solid water films heated below the melting point rapidly crystallize. The nanosecond pulsed laser heating system can prepare nanoscale liquid and supercooled liquid films that persist for nanoseconds per heat pulse in an UHV environment, enabling experimental studies of a wide range of phenomena in liquids and at liquid/solid interfaces.},
doi = {10.1063/1.4947304},
journal = {Journal of Chemical Physics},
number = 16,
volume = 144,
place = {United States},
year = {Tue Apr 26 00:00:00 EDT 2016},
month = {Tue Apr 26 00:00:00 EDT 2016}
}
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https://doi.org/10.1063/1.4947304
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