Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3

F. Chen, Y. Zhu, S. Liu, Y. Qi, H. Y. Hwang, Nathaniel C Brandt, J. Lu, F. Quirin, H. Enquist, P. Zalden, T. Hu, J. Goodfellow, M. J. Sher, M. C. Hoffmann, D. Zhu, H. Lemke, J. Glownia, M. Chollet, A. R. Damodaran, J. ParkZ. Cai, I. W. Jung, M. J. Highland, D. A. Walko, J. W. Freeland, P. G. Evans, A. Vailionis, J. Larsson, K. A. Nelson, A. M. Rappe, K. Sokolowski-Tinten, L. W. Martin, H. Wen, A. M. Lindenberg

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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 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.

Original languageEnglish (US)
Article number180104
JournalPhysical Review B
Volume94
Issue number18
DOIs
StatePublished - Nov 22 2016
Externally publishedYes

Bibliographical note

Funding Information:
This work was supported by the Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division. A.R.D. acknowledges support from the Army Research Office under Grant No. W911NF-14-1-0104. H.W. and L.W.M. acknowledge support from the Department of Energy under Grant No. DE-SC0012375. Work at Argonne was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. S.L. acknowledges support from the U.S. Department of Energy, Office of Basic Energy Sciences, under Grant No. DE-FG02-07ER15920, as well as the Carnegie Institution for Science. Y.Q. acknowledges support from the National Science Foundation under Grant No. CMMI-1334241. A.M.R. acknowledges support from the Office of Naval Research under Grant No. N00014-12-1-1033. Research by the MIT group was supported in part by Office of Naval Research Grant No. N00014-13-1-0509 and National Science Foundation Grant No. CHE-1111557. Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.

Publisher Copyright:
© 2016 American Physical Society.

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