Thermodynamic Theory of Linear Optical and Electro-Optic Properties of Ferroelectrics
arXiv:2412.03459 · doi:10.1103/PhysRevB.111.085109
Abstract
Ferroelectric materials underlie key optical technologies in optical communications, integrated optics and quantum computing. Yet, there is a lack of a consistent thermodynamic framework to predict the optical properties of ferroelectrics and the mutual connections among ferroelectric polarization, optical properties, and optical dispersion. For example, there is no existing thermodynamic model for establishing the relationship between the ferroelectric polarization and the optical properties in the visible spectrum. Here we present a thermodynamic theory of the linear optical and electro-optic properties of ferroelectrics by separating the lattice and electronic contributions to the total polarization. We introduce a biquadratic coupling between the lattice and electronic contributions validated by both first-principles calculations and experimental measurements. As an example, we derive the temperature and wavelength-dependent anisotropic optical properties of BaTiO3, including the full linear optical dielectric tensor and the linear electro-optic (Pockels) effect through multiple ferroelectric phase transitions, which are in excellent agreement with existing experimental data and first principles calculations. This general framework incorporates essentially all optical properties of materials, including coupling between the ionic and electronic order parameters, as well as their dispersion and temperature dependence, and thus offers a powerful theoretical tool for analyzing light-matter interactions in ferroelectrics-based optical devices.
arXiv comment29 pages, 8 figures
References in corpus (15)
- Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
- Restoring the density-gradient expansion for exchange in solids and surfaces
- Generalized gradient approximation for solids and their surfaces
- Precision and efficiency in solid-state pseudopotential calculations
- The physics of dynamical atomic charges: the case of ABO3 compounds
- A First-Principles Approach to Insulators in Finite Electric Fields
- Extended DFT+U+V method with on-site and inter-site electronic interactions
- Phenomenological theory of a single domain wall in uniaxial trigonal ferroelectrics: lithium niobate and lithium tantalate
- Real-space approach to calculation of electric polarization and dielectric constants
- Devonshire-Landau free energy of BaTiO3 from first principles
- SHAARP: An Open-Source Package for Analytical and Numerical Modeling of Optical Second Harmonic Generation in Anisotropic Crystals
- Understanding the role of Hubbard corrections in the rhombohedral phase of BaTiO
- Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn1-xMgxO Thin Films through Engineering Electronic and Ionic Anharmonicities
- Modeling Temperature, Frequency, and Strain Effects on the Linear Electro-Optic Coefficients of Ferroelectric Oxides
- The Antisymmetry of Distortions