First-principles thermodynamics and kinetics of multi-component solids

Anton Van der Ven, University of Michigan Ann Arbor, DMR 0748516

Energy surface of ZrO2 as a function of c/a ratio and the degree of oxygen distortion

Prediction of high temperature thermodynamic propertiesThe properties of materials at high temperature depend

sensitively on features of the energy of their crystal structure as a function of atomic distortions

Atomic transport in the solid state determines the rate with which (i) batteries can be charged, (ii)

solids transform during processing and (iii) materials corrode.

Diffusion in multi-component solids is a complex many-body process involving atomic rearrangements due to a succession of thermally activated atomic hops. In non-dilute solids, interactions among diffusing atoms becomes important and atomic transport becomes sensitive to the local state of short- and/or long-range order.

We have developed first-principles statistical mechanical tools to predict diffusion coefficients in

alloys and complex alloys used in Li-batteries.

Qingchuan Xu, A Van der Ven, “The effect of large vacancy concentration on intrinsic and interdiffusion coefficients: A first-principles study of B2-NiAl”, Acta Materialia 59, 1095-1104 (2011).

First-principles thermodynamics and kinetics of multi-component solids

Anton Van der Ven, University of Michigan Ann Arbor, DMR 0748516

We have development an automated software package CASM (a clusters approach to statistical mechanics) to predict diffusion coefficients in multi-component solids from first principles. The code is geared for research and education.

CASM was used in a graduate thermodynamics course helping students explore statistical mechanical concepts and predict thermodynamic properties of realistic alloys from first principles.

Graduate and undergraduate students as well as a high school intern participate in code development

General first-principles framework for predicting diffusion coefficients in multi-

component solids and formulation of metrics to characterize transport behavior and their

relation to electronic structure and bonding