Year: 2024
Type: article
Abstract: An analytical theory is developed for predicting the nonlinear susceptibility of ionic polarization to continuous electromagnetic waves in both bulk and strained thin film ferroelectrics. Using a perturbation method for solving the nonlinear equation of motion for ionic polarization within the framework of Landau-Ginzburg-Devonshire theory, the full second-order nonlinear susceptibility tensor is derived as a function of frequency, temperature, and strain. The theory predicts the coexistence of a significantly enhanced second-order dielectric susceptibility and a relatively low dielectric loss in ${\mathrm{BaTiO}}_{3}$ films with a strain-stabilized monoclinic ferroelectric phase and in a strained ${\mathrm{SrTiO}}_{3}$ film near its temperature-driven second-order ferroelectric-to-paraelectric phase transition. In this paper, we establish a theoretical framework for predicting and exploiting nonlinear interactions between terahertz waves and ferroelectric materials and, more generally, suggest exciting opportunities to strain-engineer nonlinear dynamical properties of ferroelectrics beyond the static and quasistatic limits.
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
Awards: G1292847278, G1453181110, G14554683, Track 4: Advanced CI Coordination Ecosystem: Monitoring and Measurement Services, G2022316211, G3265821332, G3406661761, G3562386289, G3898241218, G3927959030, G3993056153, Track 1: ACCESS Resource Allocations Marketplace and Platform Services (RAMPS), G4010157413, G4478963120, ACO: An Open CI Ecosystem to Advance Scientific Discovery (OpenCI), COMPUTATIONAL MESOSCALE SCIENCE AND OPEN SOFTWARE FOR QUANTUM MATERIALS, Track 3: COre National Ecosystem for CyberinfrasTructure (CONECT), G5098925467, G5212984984, G5367127336, G5464919783, G6021587051, G6025207788, G6121277264, G6247045938, G6473820372, G6965887028, G754761654, G8174472116, Track 2: Customized Multi-tier Assistance, Training, and Computational Help (MATCH) for End User ACCESS to CI, CAREER: Hidden Topological Polar Phases Created by Ultrafast Acoustic Excitation, COMPUTATIONAL MESOSCALE SCIENCE AND OPEN SOFTWARE FOR QUANTUM MATERIALS, Graduate Research Fellowship Program (GRFP), G8936547428
OpenAlex ID: W4401698561