Exploring Silicon-Based Ca2TiSiO6 Ordered Double Perovskite Oxides: a Comprehensive DFT Investigation of Structural, Dynamical, Mechanical Stability, and Optoelectronic Properties

A cross-platform program,VESTA, has been developed to visualize both structural and volumetric data in multiple windows with tabs.VESTArepresents crystal structures by ball-and-stick, space-filling, polyhedral, wireframe, stick, dot-surface and thermal-ellipsoid models. A variety of crystal-chemical information is extractable from fractional coordinates, occupancies and oxidation states of sites. Volumetric data such as electron and nuclear densities, Patterson functions, and wavefunctions are displayed as isosurfaces, bird's-eye views and two-dimensional maps. Isosurfaces can be colored according to other physical quantities. Translucent isosurfaces and/or slices can be overlapped with a structural model. Collaboration with external programs enables the user to locate bonds and bond angles in the `graphics area', simulate powder diffraction patterns, and calculate site potentials and Madelung energies. Electron densities determined experimentally are convertible into their Laplacians and electronic energy densities.

Optical conductivity measurements on the perovskite-related oxide CaCu3Ti4O12 provide a hint of the physics underlying the observed giant dielectric effect in this material. A low-frequency vibration displays anomalous behavior, implying that there is a redistribution of charge within the unit cell at low temperature. At infrared frequencies (terahertz), the value for the dielectric constant is approximately 80 at room temperature, which is far smaller than the value of approximately 10(5) obtained at lower radio frequencies (kilohertz). This discrepancy implies the presence of a strong absorption at very low frequencies due to dipole relaxation. At room temperature, the characteristic relaxation times are fast (less than or approximately 500 nanoseconds) but increase dramatically at low temperature, suggesting that the large change in dielectric constant may be due to a relaxor-like dynamical slowing down of dipolar fluctuations in nanosize domains.