Loughborough University
Leicestershire, UK
LE11 3TU
+44 (0)1509 263171
Loughborough University

Loughborough University Institutional Repository

Please use this identifier to cite or link to this item: https://dspace.lboro.ac.uk/2134/26049

Title: The van Hove distribution function for Brownian hard spheres: Dynamical test particle theory and computer simulations for bulk dynamics.
Authors: Hopkins, Paul
Fortini, Andrea
Archer, Andrew J.
Schmidt, Matthias
Issue Date: 2010
Publisher: © the Authors. Published by AIP
Citation: HOPKINS, P. ...et al., 2010. The van Hove distribution function for Brownian hard spheres: Dynamical test particle theory and computer simulations for bulk dynamics. Journal of Chemical Physics , 133: 224505.
Abstract: We describe a test particle approach based on dynamical density functional theory (DDFT) for studying the correlated time evolution of the particles that constitute a fluid. Our theory provides a means of calculating the van Hove distribution function by treating its self and distinct parts as the two components of a binary fluid mixture, with the “self ” component having only one particle, the “distinct” component consisting of all the other particles, and using DDFT to calculate the time evolution of the density profiles for the two components.We apply this approach to a bulk fluid of Brownian hard spheres and compare to results for the van Hove function and the intermediate scattering function from Brownian dynamics computer simulations. We find good agreement at low and intermediate densities using the very simple Ramakrishnan–Yussouff [Phys. Rev. B 19, 2775 (1979)] approximation for the excess free energy functional. Since the DDFT is based on the equilibrium Helmholtz free energy functional, we can probe a free energy landscape that underlies the dynamics. Within the mean-field approximation we find that as the particle density increases, this landscape develops a minimum, while an exact treatment of a model confined situation shows that for an ergodic fluid this landscape should be monotonic. We discuss possible implications for slow, glassy, and arrested dynamics at high densities.
Description: 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 HOPKINS, P. ...et al., 2010. The van Hove distribution function for Brownian hard spheres: Dynamical test particle theory and computer simulations for bulk dynamics. Journal of Chemical Physics , 133: 224505. and may be found at http://dx.doi.org/10.1063/1.3511719
Sponsor: P.H. thanks the EPSRC for funding under Grant EP/E065619/1 and A.J.A. gratefully acknowledges financial support from RCUK M.S. and A.F. thank the DFG for support via SFB840/A3.
Version: Published
DOI: 10.1063/1.3511719
URI: https://dspace.lboro.ac.uk/2134/26049
Publisher Link: http://dx.doi.org/10.1063/1.3511719
ISSN: 0021-9606
Appears in Collections:Published Articles (Maths)

Files associated with this item:

File Description SizeFormat
Archer_1.3511719.pdfPublished version1.3 MBAdobe PDFView/Open

 

SFX Query

Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.