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Entropy-structure relations in amorphous materials

It is suggested that a generalisation of a variational relation between the equilibrium free energy and the pair potential also holds for changes of the system along paths of non-equilibrium states. Combined with a parametrised model for the radial distribution function, this relation leads to an expression for the configurational entropy of an amorphous phase in terms of empirically determined radial distributions and a given pair potential. It is applied in combination with the 'structural diffusion' model to computer simulated amorphous aluminium, using recently determined model parameters from the normal liquid down to the amorphous solid at 273 K. The entropy difference between the liquid at melting point and the amorphous solid is estimated to be of the order of the entropy of melting, implying a negligible residual entropy. The temperature dependence of the structural diffusion coefficient, as determined from structural data, exhibits a glass transition of the amorphous system.