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Gaussian approximation to single particle correlations at and below the picosecond scale for Lennard-Jones and nanoparticle fluids

REVIEW ARTICLE

Ramses van Zon1,3, S S Ashwin2,3 and E G D Cohen3

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INVITED ARTICLE

Recommended by J R Dorfman

To describe short time (picosecond) and small scale (nanometre) transport in fluids, a Green's function approach was recently developed. This approach relies on an expansion of the distribution of single particle displacements around a Gaussian function, yielding an infinite series of correction terms. Applying a recent theorem (van Zon and Cohen 2006 J. Stat. Phys. 123 1–37) shows that for sufficiently small times the terms in this series become successively smaller, so that truncating the series near or at the Gaussian level might provide a good approximation. In this paper, we derive a theoretical estimate for the time scale at which truncating the series at or near the Gaussian level could be supposed to be accurate for equilibrium nanoscale systems. In order to numerically estimate this time scale, the coefficients for the first few terms in the series are determined in computer simulations for a Lennard-Jones (LJ) fluid, an isotopic LJ mixture and a suspension of a LJ-based model of nanoparticles in a LJ fluid. The results suggest that for LJ fluids an expansion around a Gaussian is accurate at time scales up to a picosecond, while for nanoparticles in suspension (a nanofluid), the characteristic time scale up to which the Gaussian is accurate becomes of the order of 5–10 ps.


PACS

61.20.Ja Computer simulation of liquid structure

61.25.-f Studies of specific liquid structures

82.70.Kj Emulsions and suspensions

MSC

76T20 Suspensions

68U20 Simulation (See also 65Cxx)

82C70 Transport processes

60G15 Gaussian processes

82D15 Liquids

Subjects

Soft matter, liquids and polymers

Chemical physics and physical chemistry

Dates

Issue 5 (May 2008)

Received 31 January 2007

Published 4 April 2008



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