eprintid: 123680
rev_number: 43
eprint_status: archive
userid: 608
dir: disk0/00/12/36/80
datestamp: 2010-10-23 16:52:02
lastmod: 2021-11-01 02:03:38
status_changed: 2015-12-15 11:39:15
type: article
metadata_visibility: show
item_issues_count: 0
creators_name: Ford, IJ
creators_name: Harris, SA
title: Molecular cluster decay viewed as escape from a potential of mean force
ispublished: pub
divisions: UCL
divisions: B04
divisions: C06
divisions: F60
keywords: Monte-Carlo-simulation, homogeneous nucleation rate, vapor-liquid nucleation, physical clusters, equilibrium, definition, transition, gases, water
note: © 2004 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. The following article appeared in Ford, IJ; Harris, SA; (2004) Molecular cluster decay viewed as escape from a potential of mean force. Journal of Chemical Physics , 120 (9) 4428 - 4440. and may be found at http://dx.doi.org/10.1063/1.1644533.
abstract: We show that evaporation from a quasistable molecular cluster may be treated as a kinetic problem involving the stochastically driven escape of a molecule from a potential of mean force. We derive expressions for the decay rate, and a relationship between the depth of the potential and the change in system free energy upon loss of a molecule from the cluster. This establishes a connection between kinetic and thermodynamic treatments of evaporation, but also reveals differences in the prefactor in the rate expression. We perform constant energy molecular dynamics simulations of cluster dynamics to calculate potentials of mean force, friction coefficients and effective temperatures for use in the kinetic analysis, and to compare the results with the directly observed escape rates. We also use the simulations to estimate the escape rates by a probabilistic analysis. It is much more efficient to calculate the decay rate by the methods we have developed than it is to monitor escape directly, making these approaches potentially useful for the assessment of molecular cluster stability. (C) 2004 American Institute of Physics.
date: 2004-03-01
publisher: AMER INST PHYSICS
official_url: http://dx.doi.org/10.1063/1.1644533
vfaculties: VMPS
oa_status: green
full_text_type: other
language: eng
primo: open
primo_central: open_green
article_type_text: Article
verified: verified_manual
elements_source: Web of Science
elements_id: 48915
doi: 10.1063/1.1644533
language_elements: EN
lyricists_name: Ford, Ian
lyricists_id: IJFOR04
full_text_status: public
publication: Journal of Chemical Physics
volume: 120
number: 9
pagerange: 4428 - 4440
issn: 0021-9606
citation:        Ford, IJ;    Harris, SA;      (2004)    Molecular cluster decay viewed as escape from a potential of mean force.                   Journal of Chemical Physics , 120  (9)   4428 - 4440.    10.1063/1.1644533 <https://doi.org/10.1063/1.1644533>.       Green open access   
 
document_url: https://discovery.ucl.ac.uk/id/eprint/123680/7/Ford_escapepaper2.pdf