Molecular Dynamics Simulations of Chemically Disordered Ferroelectric (Ba,Sr)TiO3 with a Semi-Empirical Effective Hamiltonian

Abstract

We present a semi-empirical effective Hamiltonian to capture effects of disorder associated with Ba and Sr cations occupying A sites in (BaxSr1-x)TiO3 on its ferroelectric phase transition. Averaging between the parameters of firstprinciples effective Hamiltonians of end members BaTiO3 and SrTiO3, we include a term with an empirical parameter to capture the local polarization and strains arising from the difference between ionic radii of Ba and Sr. Using mixed-space molecular dynamics of the effective Hamiltonian, we determine T-dependent ferroelectric phase transitions in (BaxSr1-x)TiO3 which are in good agreement with experiment. Our scheme of determination of semi-empirical parameters in effective Hamiltonian should be applicable to other perovskite-type ferroelectric solid solutions.