Elastic excitations in BaTiO3 single crystals and ceramics: Mobile domain boundaries and polar nanoregions observed by resonant ultrasonic spectroscopy

Ekhard K. H. Salje, Michael A. Carpenter, Guillaume F. Nataf, Gunnar Picht, Kyle Webber, Jeevaka Weerasinghe, S. Lisenkov, and L. Bellaiche
Phys. Rev. B 87, 014106 – Published 14 January 2013

Abstract

The dynamic properties of elastic domain walls in BaTiO3 were investigated using resonance ultrasonic spectroscopy (RUS). The sequence of phase transitions is characterized by minima in the temperature dependence of RUS resonance frequencies and changes in Q factors (resonance damping). Damping is related to the friction of mobile twin boundaries (90° ferroelectric walls) and distorted polar nanoregions (PNRs) in the cubic phase. Damping is largest in the tetragonal phase of ceramic materials but very low in single crystals. Damping is also small in the low-temperature phases of the ceramic sample and slightly increases with decreasing temperature in the single crystal. The phase angle between the real and imaginary part of the dynamic response function changes drastically in the cubic and tetragonal phases and remains constant in the orthorhombic phase. Other phases show a moderate dependence of the phase angle on temperature showing systematic changes of twin microstructures. Mobile twin boundaries (or sections of twin boundaries such as kinks inside twin walls) contribute strongly to the energy dissipation of the forced oscillation while the reduction in effective modulus due to relaxing twin domains is weak. Single crystals and ceramics show strong precursor softening in the cubic phase related to polar nanoregions (PNRs). The effective modulus decreases when the transition point of the cubic-tetragonal transformation is approached from above. The precursor softening follows temperature dependence very similar to recent results from Brillouin scattering. Between the Burns temperature (≈586 K) and Tc at 405 K, we found a good fit of the squared RUS frequency [∼Δ (C11C12)] to a Vogel–Fulcher process with an activation energy of ∼0.2 eV. Finally, some first-principles-based effective Hamiltonian computations were carried out in BaTiO3 single domains to explain some of these observations in terms of the dynamics of the soft mode and central mode.

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  • Received 18 October 2012

DOI:https://doi.org/10.1103/PhysRevB.87.014106

©2013 American Physical Society

Authors & Affiliations

Ekhard K. H. Salje2,*, Michael A. Carpenter2, Guillaume F. Nataf1,2, Gunnar Picht3, Kyle Webber3, Jeevaka Weerasinghe4,5, S. Lisenkov6, and L. Bellaiche4

  • 1Department of Earth Sciences, Cambridge University, Cambridge CB2 3EQ, UK
  • 2Grenoble Institute of Technology, 46 Avenue Félix-Viallet Grenoble, France
  • 3Institute for Ceramics in Mechanical Engineering, Karlsruhe Institute of Technology, Haid-Und-Neu-Straße 7, D 76131 Karlsruhe, Germany
  • 4Department of Physics and Institute for Nanoscience and Engineering, University of Arkansas, Fayetteville, Arkansas 72701, USA
  • 5Department of Physics, University of North Texas, Denton, Texas 76205, USA
  • 6Department of Physics, University of South Florida, Tampa, Florida 33620, USA

  • *Corresponding author: ekhard@esc.cam.ac.uk

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Vol. 87, Iss. 1 — 1 January 2013

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