Modeling of Compositionally Graded Barium Strontium Titanate From First Principles

Barium Strontium Titanate (BaxSr1-xTiO3 or BST) is a Perovskite alloy of interest for both technological and intellectual reasons. Its ferroelectric and piezoelectric properties make it useful in a variety of electric components such as transducers and actuators, and BST in particular is a material of interest for the development of a ferroelectric RAM for computers. The inclusion of SrTiO3, an incipient ferroelectric, and the fact that the properties of a BST system depend strongly on its relative composition of BaTiO3 and SrTiO3 (ST), make also this a material of high interest. Compositionally graded systems are of further interest , partly because their compositional grading leads to a built-in polarization gradient. Due to this, these systems could act as transcapacitors, devices which act as charge amplifiers in much the same way that transistors act as current amplifiers. Here, compositionally graded BST systems were modeled using a first-principles derived effective Hamiltonian method within Monte-Carlo simulation. (6) The graded systems under consideration had an average Ba composition of 70%. These systems were modeled under stress-free conditions, as well as, under epitaxial strain due to a SrTiO3 substrate

Geometric frustration in compositionally modulated ferroelectrics

Geometric frustration is a broad phenomenon that results from an intrinsic incompatibility between some fundamental interactions and the underlying lattice geometry1-7. Geometric frustration gives rise to new fundamental phenomena and is known to yield intriguing effects, such as the formation of exotic states like spin ice, spin liquids and spin glasses1-7. It has also led to interesting findings of fractional charge quantization and magnetic monopoles5,6. Geometric frustration related mechanisms have been proposed to understand the origins of relaxor behavior in some multiferroics, colossal magnetocapacitive coupling and unusual and novel mechanisms of high Tc superconductivity1-5. Although geometric frustration has been particularly well studied in magnetic systems in the last 20 years or so, its manifestation in the important class formed by ferroelectric materials (that are compounds exhibiting electric rather than magnetic dipoles) is basically unknown. Here, we show, via the use of a first-principles-based technique, that compositionally graded ferroelectrics possess the characteristic "fingerprints" associated with geometric frustration. These systems have a highly degenerate energy surface and exhibit original critical phenomena. They further reveal exotic orderings with novel stripe phases involving complex spatial organization. These stripes display spiral states, topological defects and curvature. Compositionally graded ferroelectrics can thus be considered as the "missing" link that brings ferroelectrics into the broad category of materials able to exhibit geometric frustration. Our ab-initio calculations allow a deep microscopic insight into this novel geometrically frustrated system.Comment: 14 pages, 5 Figures; http://www.nature.com/nature/journal/v470/n7335/full/nature09752.htm