G. Zvejnieks

Theory of non-equilibrium critical phenomena in three-dimensional condensed systems of charged mobile nanoparticles

A study of 3d electrostatic self-assembly (SA) in systems of charged nanoparticles (NPs) is one of the most difficult theoretical problems. In particular, the limiting case of negligible or very low polar media (e.g. salt) concentration, where the long-range NP interactions cannot be reduced to commonly used effective short-range (Yukawa) potentials, remains unstudied. Moreover, the present study has demonstrated that unlike the Debye-Hückel theory, a complete screening of the charges in SA kinetics (dynamic SA) is not always possible. Generally speaking, one has to take into account implicitly how each NP interacts with all other NPs (the true long-range interactions). Traditional theoretical methods allow us to monitor such electrostatic 3d system kinetics only for very short times, which is far from sufficient for understanding the dynamic SA. In this paper, combining an integrated analytical approach (the non-linear integro-differential kinetic equation for correlation functions) and reverse Monte Carlo in the 3d case, we have obtained a self-consistent solution of this challenging problem. We demonstrate, in particular, the existence of critical points and critical phenomena in the non-equilibrium kinetics in a 3d system of oppositely charged mobile NPs.

Electromechanical Properties of Ba(1-x)SrxTiO3 Perovskite Solid Solutions from First-Principles Calculations

An enhancement of the piezoelectric properties of lead-free materials, which allow conversion of mechanical energy into electricity, is a task of great importance and interest. Results of first-principles calculations of piezoelectric/electromechanical properties of the Ba(1-x)SrxTiO3 (BSTO) ferroelectric solid solution with a perovskite structure are presented and discussed. Calculations are performed within the linear combination of atomic orbitals (LCAO) approximation and periodic-boundary conditions, using the advanced hybrid functionals of density functional theory (DFT). A supercell model allows the investigation of multiple chemical compositions x. In particular, three BSTO solid solutions with x = 0, 0.125, 0.25 are considered within the experimental stability domain of the ferroelectric tetragonal phase of the solid solution (x < 0.3). The configurational disorder with x = 0.25 composition is also investigated explicitly considering the seven possible atomic configurations corresponding to this composition. It is predicted that Sr-doping of BaTiO3 makes it mechanically harder and enhances its electromechanical/piezoelectric properties, which are important for relevant applications.