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

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4947304· OSTI ID:1327144

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.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Organization:
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)
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1327144
Alternate ID(s):
OSTI ID: 1249957
Report Number(s):
PNNL-SA-115728; JCPSA6; 49144; KC0301050
Journal Information:
Journal of Chemical Physics, Vol. 144, Issue 16; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science

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Cited By (3)

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Homogeneous ice nucleation rates and crystallization kinetics in transiently-heated, supercooled water films from 188 K to 230 K journal May 2019
Growth rate of crystalline ice and the diffusivity of supercooled water from 126 to 262 K journal December 2016