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Local order variations in confined hard-sphere fluids

Journal article
Authors Kim Nygård
Sten Sarman
Roland Kjellander
Published in Journal of Chemical Physics
Volume 139
Issue 16
Pages artikel nr 164701
ISSN 0021-9606
Publication year 2013
Published at Department of Chemistry and Molecular Biology
Pages artikel nr 164701
Language en
Links dx.doi.org/10.1063/1.4825176
https://gup.ub.gu.se/file/115809
Keywords liquid structure, inhomogeneous fluid, pair distribution, integral equation theory
Subject categories Surfaces and interfaces, Liquid physics, Mesoscopic physics, Physical Chemistry, Surface and colloid chemistry, Chemical physics, Statistical mechanics

Abstract

Pair distributions of fluids confined between two surfaces at close distance are of fundamental importance for a variety of physical, chemical, and biological phenomena, such as interactions between macromolecules in solution, surface forces, and diffusion in narrow pores. However, in contrast to bulk fluids, properties of inhomogeneous fluids are seldom studied at the pair-distribution level. Motivated by recent experimental advances in determining anisotropic structure factors of confined fluids, we analyze theoretically the underlying anisotropic pair distributions of the archetypical hard-sphere fluid confined between two parallel hard surfaces using first-principles statistical mechanics of inhomogeneous fluids. For this purpose, we introduce an experimentally accessible ensemble-averaged local density correlation function and study its behavior as a function of confining slit width. Upon increasing the distance between the confining surfaces, we observe an alternating sequence of strongly anisotropic versus more isotropic local order. The latter is due to packing frustration of the spherical particles. This observation highlights the importance of studying inhomogeneous fluids at the pair-distribution level.

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