INSTITUTE OF PHYSICS PUBLISHING JOURNAL OF PHYSICS: CONDENSED MATTER
J. Phys.: Condens. Matter 14 (2002) 5699–5709 PII: S0953-8984(02)30298-4
Properties of a confined molecular glass-forming liquid
Victor Teboul
1
and Christiane Alba Simionesco
Laboratoire de Chimie Physique, UMR 8000, Universit´ e de Paris Sud, Bat. 349,
91405 Orsay cedex, France
Received 31 October 2001, in final form 20 March 2002
Published 30 May 2002
Online at stacks.iop.org/JPhysCM/14/5699
Abstract
We use molecular dynamics (MD) simulations to investigate the modification of
the dynamic and static properties of liquid toluene when confined in cylindrical
mesopores a few molecular diameters across. Due to the strong influence of the
substrate on the dynamics of the confined liquid, we choose a procedure where
no additional thermal interactions between the wall and the liquid are taken
into account. We observe the characteristic oscillations of molecular density
profiles (layering) when temperature and pore size are changed. Mean square
displacements and intermediate incoherent scattering functions of the centre of
mass of the molecules are calculated as functions of different distances from
the wall along the principal axis of the pore z and along the perpendicular x -
and y -directions. At 200 K the relaxations of the two correlation functions slow
down by one order of magnitude as compared to the bulk, with a slightly more
pronounced slowing down in the x -direction. This slowing down increases
strongly when the wall is approached. However, we do not observe any layer-
specific dependence of the dynamics, but instead a continuous change. When
the molecules are arrested near the wall in the time window (1 ns) of the
simulations, we find hopping processes.
1. Introduction
When a liquid is confined into a pore a few molecular diameters across, its properties are deeply
modified. The cooperative length postulated by most glass transition theories [1] in order to
explain the formidable increase of the viscosity near the glass transition will not be able to
extend to distances greater than the pore diameter. This effect may then lead to a different
dynamical regime, and then to indirect information on this length scale. Unfortunately, reality is
more complex and the limited length scale is not the only mechanism to take into account when
a supercooled liquid is introduced into a pore: the dimensionality can be changed from three to
one dimension (for a tube), finite-size effects appear, interactions with the surface may lead to
1
Permanent address: Laboratoire de Physique des Mat´ eriaux et Applications, UMR 6136, Universit´ e d’Angers,
2 Boulevard Lavoisier, 49045 Angers cedex, France.
0953-8984/02/235699+11$30.00 © 2002 IOP Publishing Ltd Printed in the UK 5699