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Title: Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO 3

Journal Article · · Physical Review B
 [1];  [2];  [3];  [4];  [5];  [5];  [5];  [6];  [7];  [8];  [9];  [9];  [10];  [11];  [11];  [11];  [11];  [11];  [12];  [13] more »;  [2];  [14];  [15];  [2];  [2];  [13];  [16];  [17];  [5];  [4];  [6];  [18];  [2];  [19] « less
  1. Stanford Univ., CA (United States). Dept. of Electrical Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  3. Univ. of Pennsylvania, Philadelphia, PA (United States). Makineni Theoretical Lab., Dept. of Chemistry; Carnegie Inst. of Washington, Argonne, IL (United States). Geophysical Lab.
  4. Univ. of Pennsylvania, Philadelphia, PA (United States). Makineni Theoretical Lab., Dept. of Chemistry
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
  6. Univ. of Duisburg-Essen, Duisburg (Germany). Faculty of Physics and Center for Nanointegration Duisburg-Essen (CENIDE)
  7. Lund Univ. (Sweden). MAX IV Lab.
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  9. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  10. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  11. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  12. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  13. Univ. of Wisconsin, Madison, WI (United States). Dept. of Materials Science and Engineering
  14. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
  15. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  16. Stanford Univ., CA (United States). Geballe Lab. for Advanced Materials
  17. Lund Univ. (Sweden). Dept. of Physics
  18. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  19. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); Stanford Univ., CA (United States). Dept. of Materials Science and Engineering,; SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)

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.

Research Organization:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Army Research Office (ARO); National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR)
Grant/Contract Number:
SC0012375; AC02-06CH11357; FG02-07ER15920; AC02-76SF00515; W911NF-14-1-0104; CMMI-1334241; CHE-1111557; N00014-12-1-1033; N00014-13-1-0509; AC02-05CH11231
OSTI ID:
1360175
Alternate ID(s):
OSTI ID: 1333328; OSTI ID: 1468336
Journal Information:
Physical Review B, Vol. 94, Issue 18; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 63 works
Citation information provided by
Web of Science

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Cited By (12)

Probing dynamics in quantum materials with femtosecond X-rays journal June 2018
Enhanced optical-to-THz conversion efficiency of photoconductive antenna using dielectric nano-layer encapsulation journal May 2018
Soft-mode driven polarity reversal in ferroelectrics mapped by ultrafast x-ray diffraction journal March 2018
Terahertz waveform considerations for nonlinearly driving lattice vibrations journal April 2019
Non-thermal fluence threshold for femtosecond pulsed x-ray radiation damage in perovskite complex oxide epitaxial heterostructures journal December 2019
Vibronic (pseudo Jahn-Teller) theory of ferroelectricity: Novel aspects and applications journal November 2018
Ultrafast polarization switching in ferroelectrics journal November 2019
Experimental station Bernina at SwissFEL: condensed matter physics on femtosecond time scales investigated by X-ray diffraction and spectroscopic methods journal April 2019
Scientific instrument Femtosecond X-ray Experiments (FXE): instrumentation and baseline experimental capabilities journal August 2019
Anti-reflection coating design for metallic terahertz meta-materials journal January 2018
Anti-reflection coating design for metallic terahertz meta-materials conference January 2018
Ultrafast polarization switching in ferroelectrics text January 2020

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