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

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. 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 lasermore » 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] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Physical Sciences Division, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, USA
Publication Date:
OSTI Identifier:
1327144
Report Number(s):
PNNL-SA-115728
Journal ID: ISSN 0021-9606; 49144; KC0301050
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 144; Journal Issue: 16
Publisher:
American Institute of Physics (AIP)
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
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