Modeling Temperature, Frequency, and Strain Effects on the Linear Electro-Optic Coefficients of Ferroelectric Oxides

An electro-optic modulator offers the function of modulating the propagation of light in a material with electric field and enables seamless connection between electronics-based computing and photonics-based communication. The search for materials with large electro-optic coefficients and low optical loss is critical to increase the efficiency and minimize the size of electro-optic devices. We present a semi-empirical method to compute the electro-optic coefficients of ferroelectric materials by combining first-principles density-functional theory calculations with Landau-Devonshire phenomenological modeling. We apply the method to study the electro-optic constants, also called Pockels coefficients, of three paradigmatic ferroelectric oxides: BaTiO3, LiNbO3, and LiTaO3. We present their temperature-, frequency- and strain-dependent electro-optic tensors calculated using our method. The predicted electro-optic constants agree with the experimental results, where available, and provide benchmarks for experimental verification.Comment: 30 pages, 6 figures, 2 tables and 2 boxe

Crystal growth and structural analysis of perovskite chalcogenide BaZrS3_3 and Ruddlesden-Popper phase Ba3_3Zr2_2S7_7

Perovskite chalcogenides are gaining substantial interest as an emerging class of semiconductors for optoelectronic applications. High quality samples are of vital importance to examine their inherent physical properties. We report the successful crystal growth of the model system, BaZrS$_3$ and its Ruddlesden-Popper phase Ba$_3$Zr$_2$S$_7$ by flux method. X-ray diffraction analyses showed space group of $Pnma$ with lattice constants of $a$ = 7.056(3) \AA\/, $b$ = 9.962(4) \AA\/, $c$ = 6.996(3) \AA\/ for BaZrS$_3$ and $P4_2/mnm$ with $a$ = 7.071(2) \AA\/, $b$ = 7.071(2) \AA\/, $c$ = 25.418(5) \AA\/ for Ba$_3$Zr$_2$S$_7$. Rocking curves with full-width-at-half-maximum of 0.011$^\circ$ for BaZrS$_3$ and 0.027$^\circ$ for Ba$_3$Zr$_2$S$_7$ were observed. Pole figure analysis, scanning transmission electron microscopy images and electron diffraction patterns also establish high quality of grown crystals. The octahedra tilting in the corner-sharing octahedra network are analyzed by extracting the torsion angles.Comment: 4 Figures, 2 Table

A hybrid pulsed laser deposition approach to grow thin films of chalcogenides

Vapor-pressure mismatched materials such as transition metal chalcogenides have emerged as electronic, photonic, and quantum materials with scientific and technological importance. However, epitaxial growth of vapor-pressure mismatched materials are challenging due to differences in the reactivity, sticking coefficient, and surface adatom mobility of the mismatched species constituting the material, especially sulfur containing compounds. Here, we report a novel approach to grow chalcogenides - hybrid pulsed laser deposition - wherein an organosulfur precursor is used as a sulfur source in conjunction with pulsed laser deposition to regulate the stoichiometry of the deposited films. Epitaxial or textured thin films of sulfides with variety of structure and chemistry such as alkaline metal chalcogenides, main group chalcogenides, transition metal chalcogenides and chalcogenide perovskites are demonstrated, and structural characterization reveal improvement in thin film crystallinity, and surface and interface roughness compared to the state-of-the-art. The growth method can be broadened to other vapor-pressure mismatched chalcogenides such as selenides and tellurides. Our work opens up opportunities for broader epitaxial growth of chalcogenides, especially sulfide-based thin film technological applications.Comment: 27 page