Transitions between metastable states in silica clusters

TL;DR

This paper investigates the energy landscape of silica clusters to understand transition processes between metastable states, which are crucial for explaining low-temperature anomalies in disordered solids.

Contribution

It introduces a numerical algorithm to identify minima and transition pathways in silica clusters, linking landscape topology to physical properties and tunneling systems.

Findings

Identified numerous adjacent minima and transition pathways.

Analyzed the cooperativity of transitions and their relation to physical properties.

Calculated quantum tunneling splittings for two-level systems.

Abstract

Relaxation phenomena in glasses can be related to jump processes between different minima of the potential energy in the configuration space. These transitions play a key role in the low temperature regime, giving rise to tunneling systems responsible for the anomalous specific heat and thermal conductivity in disordered solids with respect to crystals. By using a recently developed numerical algorithm, we study the potential energy landscape of silica clusters, taking as a starting point the location of first order saddle points. This allows us to find a great number of adjacent minima. We analyze the degree of cooperativity of these transitions and the connection of physical properties with the topology of the configuration space. We also identify two-level systems (pairs of minima constituting a tunneling system) and calculate the quantum mechanical ground state splitting by means of the WKB approximation.