Ab initio inversion of structure and the lattice dynamics of a metallic glass: the case of Pd40Ni40P20

In this paper we infer the structure of Pd40Ni40P20 from experimental diffraction data and ab initio interactions using 'force enhanced atomic refinement'. Our model accurately reproduces known experimental signatures of the system and is more efficient than conventional melt-quench schemes. We critically evaluate the local order, carry out detailed comparisons to extended x-ray absorption fine structure experiments and also discuss the electronic structure. We thoroughly explore the lattice dynamics of the system, and describe a vibrational localized-to-extended transition and discuss the special role of P dynamics. At low energies P is fully contributing to extended modes, but at higher frequencies executes local motion reminiscent of a 'rattler' inside a cage of metal atoms. These highly localized vibrational states suggest a possible utility of these materials for thermoelectric applications.