Global perspectives on the energy landscapes of liquids, supercooled liquids, and glassy systems: Geodesic pathways through the potential energy landscape

Abstract

How useful it is to think about the potential energy landscape of a complex many-body system depends in large measure on how direct the connection is to the system's dynamics. In this paper we show that, within what we call the potential energy landscape ensemble, it is possible to make direct connections between the geometry of the landscape and the long-time dynamical behaviors of systems such as supercooled liquids. We show, in particular, that the onset of slow dynamics in such systems is governed directly by the lengths of their geodesics - the shortest paths through their landscapes within the special ensemble. The more convoluted and labyrinthine these geodesics are, the slower that dynamics is. Geodesics in the landscape ensemble have sufficiently well-defined characteristics that is straightforward to search for them numerically, a point we illustrate by computing the geodesic lengths for an ordinary atomic liquid and a binary glass-forming atomic mixture. We find that the temperature dependence of the diffusion constants of these systems, including the precipitous drop as the glass-forming system approaches its mode-coupling transition, is predicted quantitatively by the growth of the geodesic path lengths.

arXiv comment50 pages, 9 figures

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Cited by in corpus (7)

• NVU dynamics. I. Geodesic motion on the constant-potential-energy hypersurface
• NVU dynamics. II. Comparing to four other dynamics
• Revisiting the Concept of Activation in Supercooled Liquids
• Manipulating the Glass Transition in Nanoscale
• NVU dynamics. III. Simulating molecules at constant potential energy
• The potential energy landscape and inherent dynamics of a hard-sphere fluid
• Viscous liquid dynamics modeled as random walks within overlapping hyperspheres