Ultrafast terahertz-field-driven ionic response in ferroelectric
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.
- Authors:
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- 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)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Univ. of Pennsylvania, Philadelphia, PA (United States). Makineni Theoretical Lab., Dept. of Chemistry; Carnegie Inst. of Washington, Argonne, IL (United States). Geophysical Lab.
- Univ. of Pennsylvania, Philadelphia, PA (United States). Makineni Theoretical Lab., Dept. of Chemistry
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
- Univ. of Duisburg-Essen, Duisburg (Germany). Faculty of Physics and Center for Nanointegration Duisburg-Essen (CENIDE)
- Lund Univ. (Sweden). MAX IV Lab.
- 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
- 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)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
- Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
- Univ. of Wisconsin, Madison, WI (United States). Dept. of Materials Science and Engineering
- Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
- Stanford Univ., CA (United States). Geballe Lab. for Advanced Materials
- Lund Univ. (Sweden). Dept. of Physics
- 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
- 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)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- 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)
- OSTI Identifier:
- 1360175
- Alternate Identifier(s):
- OSTI ID: 1333328; OSTI ID: 1468336
- 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
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 94; Journal Issue: 18; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Chen, F., Zhu, Y., Liu, S., Qi, Y., Hwang, H. Y., Brandt, N. C., Lu, J., Quirin, F., Enquist, H., Zalden, P., Hu, T., Goodfellow, J., Sher, M. -J., Hoffmann, M. C., Zhu, D., Lemke, H., Glownia, J., Chollet, M., Damodaran, A. R., Park, J., Cai, Z., Jung, I. W., Highland, M. J., Walko, D. A., Freeland, J. W., Evans, P. G., Vailionis, A., Larsson, J., Nelson, K. A., Rappe, A. M., Sokolowski-Tinten, K., Martin, L. W., Wen, H., and Lindenberg, A. M. Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3. United States: N. p., 2016.
Web. doi:10.1103/PhysRevB.94.180104.
Chen, F., Zhu, Y., Liu, S., Qi, Y., Hwang, H. Y., Brandt, N. C., Lu, J., Quirin, F., Enquist, H., Zalden, P., Hu, T., Goodfellow, J., Sher, M. -J., Hoffmann, M. C., Zhu, D., Lemke, H., Glownia, J., Chollet, M., Damodaran, A. R., Park, J., Cai, Z., Jung, I. W., Highland, M. J., Walko, D. A., Freeland, J. W., Evans, P. G., Vailionis, A., Larsson, J., Nelson, K. A., Rappe, A. M., Sokolowski-Tinten, K., Martin, L. W., Wen, H., & Lindenberg, A. M. Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3. United States. https://doi.org/10.1103/PhysRevB.94.180104
Chen, F., Zhu, Y., Liu, S., Qi, Y., Hwang, H. Y., Brandt, N. C., Lu, J., Quirin, F., Enquist, H., Zalden, P., Hu, T., Goodfellow, J., Sher, M. -J., Hoffmann, M. C., Zhu, D., Lemke, H., Glownia, J., Chollet, M., Damodaran, A. R., Park, J., Cai, Z., Jung, I. W., Highland, M. J., Walko, D. A., Freeland, J. W., Evans, P. G., Vailionis, A., Larsson, J., Nelson, K. A., Rappe, A. M., Sokolowski-Tinten, K., Martin, L. W., Wen, H., and Lindenberg, A. M. Tue .
"Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3". United States. https://doi.org/10.1103/PhysRevB.94.180104. https://www.osti.gov/servlets/purl/1360175.
@article{osti_1360175,
title = {Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3},
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, J. and Nelson, K. A. and Rappe, A. M. and Sokolowski-Tinten, K. and Martin, L. W. and Wen, H. and Lindenberg, A. M.},
abstractNote = {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.},
doi = {10.1103/PhysRevB.94.180104},
journal = {Physical Review B},
number = 18,
volume = 94,
place = {United States},
year = {Tue Nov 22 00:00:00 EST 2016},
month = {Tue Nov 22 00:00:00 EST 2016}
}
Web of Science
Works referenced in this record:
Ultrafast polarization switching in thin-film ferroelectrics
journal, February 2004
- Li, J.; Nagaraj, B.; Liang, H.
- Applied Physics Letters, Vol. 84, Issue 7
Sub-Picosecond Processes of Ferroelectric Domain Switching from Field and Temperature Experiments
journal, November 2011
- Jiang, An Quan; Lee, Hyun Ju; Hwang, Cheol Seong
- Advanced Functional Materials, Vol. 22, Issue 1
Femtosecond time-resolved spectroscopy of soft modes in structural phase transitions of perovskites
journal, October 1994
- Dougherty, Thomas P.; Wiederrecht, Gary P.; Nelson, Keith A.
- Physical Review B, Vol. 50, Issue 13
Ultrafast Photovoltaic Response in Ferroelectric Nanolayers
journal, February 2012
- Daranciang, Dan; Highland, Matthew J.; Wen, Haidan
- Physical Review Letters, Vol. 108, Issue 8
Mesoscopic structural phase progression in photo-excited VO2 revealed by time-resolved x-ray diffraction microscopy
journal, February 2016
- Zhu, Yi; Cai, Zhonghou; Chen, Pice
- Scientific Reports, Vol. 6, Issue 1
Ultrafast lattice response of photoexcited thin films studied by X-ray diffraction
journal, November 2014
- Schick, Daniel; Herzog, Marc; Bojahr, André
- Structural Dynamics, Vol. 1, Issue 6
Atomic-Scale Visualization of Inertial Dynamics
journal, April 2005
- Lindenberg, A. M.
- Science, Vol. 308, Issue 5720
Light-induced size changes in BiFeO3 crystals
journal, July 2010
- Kundys, B.; Viret, M.; Colson, D.
- Nature Materials, Vol. 9, Issue 10
The chain structure of BaTiO3 and KNbO3
journal, October 1968
- Comes, R.; Lambert, M.; Guinier, A.
- Solid State Communications, Vol. 6, Issue 10
Rotator and extender ferroelectrics: Importance of the shear coefficient to the piezoelectric properties of domain-engineered crystals and ceramics
journal, March 2007
- Davis, Matthew; Budimir, Marko; Damjanovic, Dragan
- Journal of Applied Physics, Vol. 101, Issue 5
THz time domain spectroscopy of pulsed laser deposited BaTiO3 thin films
journal, October 2004
- Misra, M.; Kotani, K.; Kiwa, T.
- Applied Surface Science, Vol. 237, Issue 1-4
Electronic Origin of Ultrafast Photoinduced Strain in
journal, January 2013
- Wen, Haidan; Chen, Pice; Cosgriff, Margaret P.
- Physical Review Letters, Vol. 110, Issue 3
Thermodynamics of an eight-site order-disorder model for ferroelectrics
journal, January 1976
- Chaves, A. S.; Barreto, F. C. S.; Nogueira, R. A.
- Physical Review B, Vol. 13, Issue 1
Picosecond acoustic response of a laser-heated gold-film studied with time-resolved x-ray diffraction
journal, May 2011
- Nicoul, Matthieu; Shymanovich, Uladzimir; Tarasevitch, Alexander
- Applied Physics Letters, Vol. 98, Issue 19
Terahertz dielectric response of single-domain BaTiO 3 measured by far-infrared spectroscopic ellipsometry
journal, September 2014
- Hoshina, Takuya; Kanehara, Kazuki; Takeda, Hiroaki
- Japanese Journal of Applied Physics, Vol. 53, Issue 9S
Efficient real-time detection of terahertz pulse radiation based on photoacoustic conversion by carbon nanotube nanocomposite
journal, May 2014
- Chen, Sung-Liang; Chang, You-Chia; Zhang, Cheng
- Nature Photonics, Vol. 8, Issue 7
Extraordinary carrier multiplication gated by a picosecond electric field pulse
journal, September 2011
- Hirori, H.; Shinokita, K.; Shirai, M.
- Nature Communications, Vol. 2, Issue 1
Nucleation and growth mechanism of ferroelectric domain-wall motion
journal, October 2007
- Shin, Young-Han; Grinberg, Ilya; Chen, I-Wei
- Nature, Vol. 449, Issue 7164
Dynamic Structural Response and Deformations of Monolayer MoS 2 Visualized by Femtosecond Electron Diffraction
journal, September 2015
- Mannebach, Ehren M.; Li, Renkai; Duerloo, Karel-Alexander
- Nano Letters, Vol. 15, Issue 10
Giant bulk photovoltaic effect in thin ferroelectric films
journal, October 2014
- Zenkevich, A.; Matveyev, Yu.; Maksimova, K.
- Physical Review B, Vol. 90, Issue 16
The ferroelectric and cubic phases in BaTiO3 ferroelectrics are also antiferroelectric
journal, September 2006
- Zhang, Q.; Cagin, T.; Goddard, W. A.
- Proceedings of the National Academy of Sciences, Vol. 103, Issue 40
Coupled Ultrafast Lattice and Polarization Dynamics in Ferroelectric Nanolayers
journal, June 2007
- Korff Schmising, C. v.; Bargheer, M.; Kiel, M.
- Physical Review Letters, Vol. 98, Issue 25
Ultrafast large-amplitude relocation of electronic charge in ionic crystals
journal, March 2012
- Zamponi, F.; Rothhardt, P.; Stingl, J.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 14
Perovskite oxides for visible-light-absorbing ferroelectric and photovoltaic materials
journal, November 2013
- Grinberg, Ilya; West, D. Vincent; Torres, Maria
- Nature, Vol. 503, Issue 7477, p. 509-512
Switchable Ferroelectric Diode and Photovoltaic Effect in BiFeO 3
journal, February 2009
- Choi, T.; Lee, S.; Choi, Y. J.
- Science, Vol. 324, Issue 5923
First Principles Calculation of the Shift Current Photovoltaic Effect in Ferroelectrics
journal, September 2012
- Young, Steve M.; Rappe, Andrew M.
- Physical Review Letters, Vol. 109, Issue 11, Article No. 116601
Collective Coherent Control: Synchronization of Polarization in Ferroelectric by Shaped THz Fields
journal, June 2009
- Qi, Tingting; Shin, Young-Han; Yeh, Ka-Lo
- Physical Review Letters, Vol. 102, Issue 24
Ferroelectric Soft Mode in a Thin Film Impulsively Driven to the Anharmonic Regime Using Intense Picosecond Terahertz Pulses
journal, February 2012
- Katayama, I.; Aoki, H.; Takeda, J.
- Physical Review Letters, Vol. 108, Issue 9
Crystal Structure and the Paraelectric-to-Ferroelectric Phase Transition of Nanoscale BaTiO 3
journal, June 2008
- Smith, Millicent B.; Page, Katharine; Siegrist, Theo
- Journal of the American Chemical Society, Vol. 130, Issue 22
Above-bandgap voltages from ferroelectric photovoltaic devices
journal, January 2010
- Yang, S. Y.; Seidel, J.; Byrnes, S. J.
- Nature Nanotechnology, Vol. 5, Issue 2
Ultrafast modulation of polarization amplitude by terahertz fields in electronic-type organic ferroelectrics
journal, October 2013
- Miyamoto, Tatsuya; Yada, Hiroyuki; Yamakawa, Hiromichi
- Nature Communications, Vol. 4, Issue 1
Ultrafast Terahertz Gating of the Polarization and Giant Nonlinear Optical Response in BiFeO 3 Thin Films
journal, September 2015
- Chen, Frank; Goodfellow, John; Liu, Shi
- Advanced Materials, Vol. 27, Issue 41
Dynamical x‐ray diffraction from nonuniform crystalline films: Application to x‐ray rocking curve analysis
journal, June 1986
- Wie, C. R.; Tombrello, T. A.; Vreeland, T.
- Journal of Applied Physics, Vol. 59, Issue 11
Molecular Dynamics Study of Dielectric Response in a Relaxor Ferroelectric
journal, November 2009
- Grinberg, Ilya; Shin, Young-Han; Rappe, Andrew M.
- Physical Review Letters, Vol. 103, Issue 19
Atomistic description for temperature-driven phase transitions in
journal, October 2016
- Qi, Y.; Liu, S.; Grinberg, I.
- Physical Review B, Vol. 94, Issue 13
Resonant and nonresonant control over matter and light by intense terahertz transients
journal, August 2013
- Kampfrath, Tobias; Tanaka, Koichiro; Nelson, Keith A.
- Nature Photonics, Vol. 7, Issue 9
Local structure and the phase transitions of BaTiO 3
journal, February 1998
- Ravel, B.; Stern, E. A.; Vedrinskii, R. I.
- Ferroelectrics, Vol. 206, Issue 1
X‐ray study of lattice strain in boron implanted laser annealed silicon
journal, June 1980
- Larson, B. C.; Barhorst, J. F.
- Journal of Applied Physics, Vol. 51, Issue 6
Large-Amplitude Spin Dynamics Driven by a THz Pulse in Resonance with an Electromagnon
journal, March 2014
- Kubacka, T.; Johnson, J. A.; Hoffmann, M. C.
- Science, Vol. 343, Issue 6177
Nanosecond Domain Wall Dynamics in Ferroelectric Thin Films
journal, May 2006
- Grigoriev, Alexei; Do, Dal-Hyun; Kim, Dong Min
- Physical Review Letters, Vol. 96, Issue 18
Dynamics of the laser-induced ferroelectric excitation in BaTiO3 studied by x-ray diffraction
journal, January 2007
- Istomin, Konstantin; Kotaidis, Vassilios; Plech, Anton
- Applied Physics Letters, Vol. 90, Issue 2
Works referencing / citing this record:
Probing dynamics in quantum materials with femtosecond X-rays
journal, June 2018
- Buzzi, Michele; Först, Michael; Mankowsky, Roman
- Nature Reviews Materials, Vol. 3, Issue 9
Enhanced optical-to-THz conversion efficiency of photoconductive antenna using dielectric nano-layer encapsulation
journal, May 2018
- Gupta, Abhishek; Rana, Goutam; Bhattacharya, Arkabrata
- APL Photonics, Vol. 3, Issue 5
Soft-mode driven polarity reversal in ferroelectrics mapped by ultrafast x-ray diffraction
journal, March 2018
- Hauf, Christoph; Hernandez Salvador, Antonio-Andres; Holtz, Marcel
- Structural Dynamics, Vol. 5, Issue 2
Terahertz waveform considerations for nonlinearly driving lattice vibrations
journal, April 2019
- Knighton, Brittany E.; Tanner Hardy, R.; Johnson, Courtney L.
- Journal of Applied Physics, Vol. 125, Issue 14
Non-thermal fluence threshold for femtosecond pulsed x-ray radiation damage in perovskite complex oxide epitaxial heterostructures
journal, December 2019
- Lee, Hyeon Jun; Ahn, Youngjun; Marks, Samuel D.
- Applied Physics Letters, Vol. 115, Issue 25
Vibronic (pseudo Jahn-Teller) theory of ferroelectricity: Novel aspects and applications
journal, November 2018
- Bersuker, I. B.
- Ferroelectrics, Vol. 536, Issue 1
Ultrafast polarization switching in ferroelectrics
journal, November 2019
- Yukalov, V. I.; Yukalova, E. P.
- Physical Review Research, Vol. 1, Issue 3
Experimental station Bernina at SwissFEL: condensed matter physics on femtosecond time scales investigated by X-ray diffraction and spectroscopic methods
journal, April 2019
- Ingold, Gerhard; Abela, Rafael; Arrell, Christopher
- Journal of Synchrotron Radiation, Vol. 26, Issue 3
Scientific instrument Femtosecond X-ray Experiments (FXE): instrumentation and baseline experimental capabilities
journal, August 2019
- Galler, Andreas; Gawelda, Wojciech; Biednov, Mykola
- Journal of Synchrotron Radiation, Vol. 26, Issue 5
Anti-reflection coating design for metallic terahertz meta-materials
journal, January 2018
- Pancaldi, Matteo; Freeman, Ryan; Hudl, Matthias
- Optics Express, Vol. 26, Issue 3
Anti-reflection coating design for metallic terahertz meta-materials
conference, January 2018
- Pancaldi, Matteo; Freeman, Ryan; Hudl, Matthias
- CLEO: Applications and Technology, Conference on Lasers and Electro-Optics
Ultrafast polarization switching in ferroelectrics
text, January 2020
- Yukalov, V. I.; Yukalova, E. P.
- arXiv