Duality of liquids

Liquids flow, making them remarkably distinct from solids and close to gases. At the same time, interactions in liquids are strong as in solids. The combination of these two properties is believed to be the ultimate obstacle to constructing a general theory of liquids. Here, we adopt a new approach to liquids: instead of focusing on the problem of strong interactions, we zero in on the relative contributions of vibrational and diffusional motion in liquids. We subsequently show that from the point of view of thermodynamics, liquid energy and specific heat are given, to a very good approximation, by their vibrational contributions as in solids, for relaxation times spanning 15 orders of magnitude. We therefore find that liquids show an interesting {\it duality} not hitherto known: they are close to solids from the thermodynamical point of view and to gases from the point of view of flow. We discuss the experimental implications of this approach.Comment: In Scientific Reports 201

Evidence for structural crossover in the supercritical state

The state of matter above the critical point is terra incognita, and is loosely discussed as a physically homogeneous flowing state where no differences can be made between a liquid and a gas and where properties undergo no marked or distinct changes with pressure and temperature. In particular, the structure of supercritical state is currently viewed to be the same everywhere on the phase diagram, and to change only gradually and in a featureless way while moving along any temperature and pressure path above the critical point. Here, we demonstrate that this is not the case, but that there is a well-defined structural crossover instead. Evidenced by the qualitative changes of distribution functions of interatomic distances and angles, the crossover demarcates liquid-like and gas-like configurations and the presence of medium-range structural correlations. Importantly, the discovered structural crossover is closely related to both dynamic and thermodynamic crossovers operating in the supercritical state, providing new unexpected fundamental interlinks between the supercritical structure, dynamics and thermodynamics.Comment: 5 pages, 4 figure

Solid-state diffusion in amorphous zirconolite

his research utilised Queen Mary's MidPlus computational facilities, supported by QMUL Research-IT and funded by EPSRC grant EP/K000128/1. We are grateful to E. Maddrell for discussions and to CSC for support