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Title: Giant electromechanical coupling of relaxor ferroelectrics controlled by polar nanoregion vibrations

Relaxor-based ferroelectrics are prized for their giant electromechanical coupling and have revolutionized sensor and ultrasound applications. A long-standing challenge for piezoelectric materials has been to understand how these ultrahigh electromechanical responses occur when the polar atomic displacements underlying the response are partially broken into polar nanoregions (PNRs) in relaxor-based ferroelectrics. Given the complex inhomogeneous nanostructure of these materials, it has generally been assumed that this enhanced response must involve complicated interactions. By using neutron scattering measurements of lattice dynamics and local structure, we show that the vibrational modes of the PNRs enable giant coupling by softening the underlying macrodomain polarization rotations in relaxor-based ferroelectric PMN-xPT {(1 x)[Pb(Mg1/3Nb2/3)O3] xPbTiO3} (x = 30%). The mechanism involves the collective motion of the PNRs with transverse acoustic phonons and results in two hybrid modes, one softer and one stiffer than the bare acoustic phonon. The softer mode is the origin of macroscopic shear softening. Furthermore, a PNR mode and a component of the local structure align in an electric field; this further enhances shear softening, revealing a way to tune the ultrahigh piezoelectric response by engineering elastic shear softening.
 [1] ;  [2] ;  [3] ;  [4] ;  [4] ;  [2] ;  [1] ;  [1] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
  3. TRS Technologies, State College, PA (United States)
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). NIST Center for Neutron Research
Publication Date:
OSTI Identifier:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 2; Journal Issue: 9; Journal ID: ISSN 2375-2548
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR); Spallation Neutron Source
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
36 MATERIALS SCIENCE relaxor ferroelectric; piezoelectricity; local modes; neutron scattering