Theory of nonlinear terahertz susceptibility in ferroelectrics

Zhu, Yujie; Chen, Taorui; Ross, Aiden; Wang, Bo; Guo, Xiangwei; Gopalan, Venkatraman; Chen, Long-Qing; Hu, Jia-Mian

doi:10.1103/physrevb.110.054311

Theory of nonlinear terahertz susceptibility in ferroelectrics

Journal Article · Mon Aug 19 00:00:00 EDT 2024 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.110.054311· OSTI ID:2426422

^[1]; Chen, Taorui ^[2]; Ross, Aiden ^[3]; ^[4]; ^[2]; ^[3]; Chen, Long-Qing ^[3]; ^[2]

University of Wisconsin-Madison; Penn State University
University of Wisconsin-Madison
The Pennsylvania State University
Lawrence Livermore National Laboratory

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. Here, the theory predicts the coexistence of a significantly enhanced second-order dielectric susceptibility and a relatively low dielectric loss in BaTiO₃ films with a strain-stabilized monoclinic ferroelectric phase and in a strained SrTiO₃ 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC52-07NA27344; SC0020145

OSTI ID:: 2426422

Alternate ID(s):: OSTI ID: 2440335
OSTI ID: 2474167

Report Number(s):: LLNL--JRNL-862697

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 5 Vol. 110; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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