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Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3

Chen, F. ; Zhu, Y. ; Liu, S. ; Qi, Y. ; Hwang, H. Y. ; Brandt, N. C. ; Lu, J. ; Quirin, F. ; Enquist, H. LU orcid and Zalden, P. , et al. (2016) In Physical Review B 94(18).
Abstract

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and... (More)

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review B
volume
94
issue
18
article number
180104
publisher
American Physical Society
external identifiers
  • wos:000388465200001
  • scopus:84999018288
ISSN
1098-0121
DOI
10.1103/PhysRevB.94.180104
language
English
LU publication?
yes
id
231087c2-6642-4737-8ff2-2370d85cfb43
date added to LUP
2016-12-20 09:59:56
date last changed
2025-03-10 02:23:17
@article{231087c2-6642-4737-8ff2-2370d85cfb43,
  abstract     = {{<p>The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.</p>}},
  author       = {{Chen, F. and Zhu, Y. and Liu, S. and Qi, Y. and Hwang, H. Y. and Brandt, N. C. and Lu, J. and Quirin, F. and Enquist, H. and Zalden, P. and Hu, T. and Goodfellow, J. and Sher, M. J. and Hoffmann, M. C. and Zhu, D. and Lemke, H. and Glownia, J. and Chollet, M. and Damodaran, A. R. and Park, J. and Cai, Z. and Jung, I. W. and Highland, M. J. and Walko, D. A. and Freeland, J. W. and Evans, P. G. and Vailionis, A. and Larsson, Jörgen and Nelson, K. A. and Rappe, A. M. and Sokolowski-Tinten, K. and Martin, L. W. and Wen, H. and Lindenberg, A. M.}},
  issn         = {{1098-0121}},
  language     = {{eng}},
  month        = {{11}},
  number       = {{18}},
  publisher    = {{American Physical Society}},
  series       = {{Physical Review B}},
  title        = {{Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3}},
  url          = {{http://dx.doi.org/10.1103/PhysRevB.94.180104}},
  doi          = {{10.1103/PhysRevB.94.180104}},
  volume       = {{94}},
  year         = {{2016}},
}