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Multiple reentrant glass transitions in confined hard-sphere glasses

S. Mandal,S. Lang,M. Gross,M. Oettel,D. Raabe,T. Franosch,F. Varnik

Published 2014 in Nature Communications

ABSTRACT

Glass-forming liquids exhibit a rich phenomenology upon confinement. This is often related to the effects arising from wall–fluid interactions. Here we focus on the interesting limit where the separation of the confining walls becomes of the order of a few particle diameters. For a moderately polydisperse, densely packed hard-sphere fluid confined between two smooth hard walls, we show via event-driven molecular dynamics simulations the emergence of a multiple reentrant glass transition scenario upon a variation of the wall separation. Using thermodynamic relations, this reentrant phenomenon is shown to persist also under constant chemical potential. This allows straightforward experimental investigation and opens the way to a variety of applications in micro- and nanotechnology, where channel dimensions are comparable to the size of the contained particles. The results are in line with theoretical predictions obtained by a combination of density functional theory and the mode-coupling theory of the glass transition. Wall–fluid interactions are known to have a large influence on the physics of confined glasses. Here, the authors observe a multiple re-entrant glass transition for a polydisperse hard-sphere system confined between two surfaces, when the wall separation distance is of the order of a few particle diameters.

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