Terahertz-driven phonon upconversion in SrTiO3
Abstract
Direct manipulation of the atomic lattice using intense long-wavelength laser pulses has become a viable approach to create new states of matter in complex materials. Conventionally, a high-frequency vibrational mode is driven resonantly by a mid-infrared laser pulse and the lattice structure is modified through indirect coupling of this infrared-active phonon to other, lower-frequency lattice modulations. Here, we drive the lowest-frequency optical phonon in the prototypical transition metal oxide SrTiO3 well into the anharmonic regime with an intense terahertz field. We show that it is possible to transfer energy to higher-frequency phonon modes through nonlinear coupling. Lastly, our observations are carried out by directly mapping the lattice response to the coherent drive field with femtosecond X-ray pulses, enabling direct visualization of the atomic displacements.
- Authors:
-
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)
- Univ. of Fribourg, Fribourg (Switzerland)
- Paul Scherrer Inst. (PSI), Villigen (Switzerland)
- Stockholm Univ., Stockholm (Sweden)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1528889
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Physics
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 4; Journal ID: ISSN 1745-2473
- Publisher:
- Nature Publishing Group (NPG)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 74 ATOMIC AND MOLECULAR PHYSICS
Citation Formats
Kozina, M., Fechner, M., Marsik, P., van Driel, T., Glownia, J. M., Bernhard, C., Radovic, M., Zhu, D., Bonetti, S., Staub, U., and Hoffmann, M. C. Terahertz-driven phonon upconversion in SrTiO3. United States: N. p., 2019.
Web. doi:10.1038/s41567-018-0408-1.
Kozina, M., Fechner, M., Marsik, P., van Driel, T., Glownia, J. M., Bernhard, C., Radovic, M., Zhu, D., Bonetti, S., Staub, U., & Hoffmann, M. C. Terahertz-driven phonon upconversion in SrTiO3. United States. https://doi.org/10.1038/s41567-018-0408-1
Kozina, M., Fechner, M., Marsik, P., van Driel, T., Glownia, J. M., Bernhard, C., Radovic, M., Zhu, D., Bonetti, S., Staub, U., and Hoffmann, M. C. Mon .
"Terahertz-driven phonon upconversion in SrTiO3". United States. https://doi.org/10.1038/s41567-018-0408-1. https://www.osti.gov/servlets/purl/1528889.
@article{osti_1528889,
title = {Terahertz-driven phonon upconversion in SrTiO3},
author = {Kozina, M. and Fechner, M. and Marsik, P. and van Driel, T. and Glownia, J. M. and Bernhard, C. and Radovic, M. and Zhu, D. and Bonetti, S. and Staub, U. and Hoffmann, M. C.},
abstractNote = {Direct manipulation of the atomic lattice using intense long-wavelength laser pulses has become a viable approach to create new states of matter in complex materials. Conventionally, a high-frequency vibrational mode is driven resonantly by a mid-infrared laser pulse and the lattice structure is modified through indirect coupling of this infrared-active phonon to other, lower-frequency lattice modulations. Here, we drive the lowest-frequency optical phonon in the prototypical transition metal oxide SrTiO3 well into the anharmonic regime with an intense terahertz field. We show that it is possible to transfer energy to higher-frequency phonon modes through nonlinear coupling. Lastly, our observations are carried out by directly mapping the lattice response to the coherent drive field with femtosecond X-ray pulses, enabling direct visualization of the atomic displacements.},
doi = {10.1038/s41567-018-0408-1},
journal = {Nature Physics},
number = 4,
volume = 15,
place = {United States},
year = {2019},
month = {1}
}
Web of Science
Works referenced in this record:
Control of the electronic phase of a manganite by mode-selective vibrational excitation
journal, September 2007
- Rini, Matteo; Tobey, Ra'anan; Dean, Nicky
- Nature, Vol. 449, Issue 7158
Electric-Field-Induced Soft-Mode Hardening in Films
journal, May 2000
- Akimov, I. A.; Sirenko, A. A.; Clark, A. M.
- Physical Review Letters, Vol. 84, Issue 20
Crystal stability and the theory of ferroelectricity
journal, October 1960
- Cochran, W.
- Advances in Physics, Vol. 9, Issue 36
Dielectric, infrared, and Raman response of undoped ceramics: Evidence of polar grain boundaries
journal, October 2001
- Petzelt, J.; Ostapchuk, T.; Gregora, I.
- Physical Review B, Vol. 64, Issue 18
Soft-mode hardening in SrTiO3 thin films
journal, March 2000
- Sirenko, A. A.; Bernhard, C.; Golnik, A.
- Nature, Vol. 404, Issue 6776
Elastic strain engineering of ferroic oxides
journal, February 2014
- Schlom, Darrell G.; Chen, Long-Qing; Fennie, Craig J.
- MRS Bulletin, Vol. 39, Issue 2
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009
- Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
- Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
Far-Infrared Ferroelectric Vibration Mode in SrTi
journal, March 1962
- Barker, A. S.; Tinkham, M.
- Physical Review, Vol. 125, Issue 5
Local terahertz field enhancement for time-resolved x-ray diffraction
journal, February 2017
- Kozina, M.; Pancaldi, M.; Bernhard, C.
- Applied Physics Letters, Vol. 110, Issue 8
Ultrafast X-ray diffraction probe of terahertz field-driven soft mode dynamics in SrTiO 3
journal, September 2017
- Kozina, M.; van Driel, T.; Chollet, M.
- Structural Dynamics, Vol. 4, Issue 5
Real-Time Manifestation of Strongly Coupled Spin and Charge Order Parameters in Stripe-Ordered Nickelate Crystals Using Time-Resolved Resonant X-Ray Diffraction
journal, March 2013
- Chuang, Y. D.; Lee, W. S.; Kung, Y. F.
- Physical Review Letters, Vol. 110, Issue 12
Probing the interatomic potential of solids with strong-field nonlinear phononics
journal, February 2018
- von Hoegen, A.; Mankowsky, R.; Fechner, M.
- Nature, Vol. 555, Issue 7694
Ferroelectric quantum criticality
journal, March 2014
- Rowley, S. E.; Spalek, L. J.; Smith, R. P.
- Nature Physics, Vol. 10, Issue 5
Femtosecond time-resolved measurements of optic phonon dephasing by impulsive stimulated raman scattering in α-perylene crystal from 20 to 300 K
journal, May 1985
- De Silvestri, S.; Fujimoto, J. G.; Ippen, E. P.
- Chemical Physics Letters, Vol. 116, Issue 2-3
Parametric amplification of optical phonons
journal, November 2018
- Cartella, A.; Nova, T. F.; Fechner, M.
- Proceedings of the National Academy of Sciences, Vol. 115, Issue 48
Interfacial mode coupling as the origin of the enhancement of Tc in FeSe films on SrTiO3
journal, November 2014
- Lee, J. J.; Schmitt, F. T.; Moore, R. G.
- Nature, Vol. 515, Issue 7526
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
Terahertz ellipsometry study of the soft mode behavior in ultrathin SrTiO 3 films
journal, February 2016
- Marsik, P.; Sen, K.; Khmaladze, J.
- Applied Physics Letters, Vol. 108, Issue 5
Reversal of Ferroelectric Domains by Ultrashort Optical Pulses
journal, August 1994
- Fahy, S.; Merlin, R.
- Physical Review Letters, Vol. 73, Issue 8
Neutron Scattering and Nature of the Soft Optical Phonon in SrTiO 3
journal, February 1969
- Yamada, Yasusada; Shirane, Gen
- Journal of the Physical Society of Japan, Vol. 26, Issue 2
Nonlinear phononics as an ultrafast route to lattice control
journal, August 2011
- Först, M.; Manzoni, C.; Kaiser, S.
- Nature Physics, Vol. 7, Issue 11
Temperature Dependence of a Transverse Optic Mode in Strontium Titanate
journal, August 1962
- Cowley, R. A.
- Physical Review Letters, Vol. 9, Issue 4
High-Field THz Lattice Control Via Anharmonic Vibrational Coupling
conference, January 2016
- Johnson, Jeremy A.; Salmans, Parker D.; Ellsworth, Nicholas R.
- International Conference on Ultrafast Phenomena
Far Infrared Dielectric Dispersion in BaTi , SrTi , and Ti
journal, June 1962
- Spitzer, W. G.; Miller, Robert C.; Kleinman, D. A.
- Physical Review, Vol. 126, Issue 5
Structures of the ferroelectric phases of barium titanate
journal, March 1993
- Kwei, G. H.; Lawson, A. C.; Billinge, S. J. L.
- The Journal of Physical Chemistry, Vol. 97, Issue 10
Femtosecond Structural Dynamics in during an Ultrafast Solid-Solid Phase Transition
journal, November 2001
- Cavalleri, A.; Tóth, Cs.; Siders, C. W.
- Physical Review Letters, Vol. 87, Issue 23
Magnetic-field-induced metal-insulator phenomena in with controlled charge-ordering instability
journal, January 1996
- Tomioka, Y.; Asamitsu, A.; Kuwahara, H.
- Physical Review B, Vol. 53, Issue 4
Room-temperature ferroelectricity in strained SrTiO3
journal, August 2004
- Haeni, J. H.; Irvin, P.; Chang, W.
- Nature, Vol. 430, Issue 7001, p. 758-761
Generation of 10μJ ultrashort terahertz pulses by optical rectification
journal, April 2007
- Yeh, K. -L.; Hoffmann, M. C.; Hebling, J.
- Applied Physics Letters, Vol. 90, Issue 17
Phonon mechanism in the most dilute superconductor n -type SrTiO 3
journal, April 2016
- Gor’kov, Lev P.
- Proceedings of the National Academy of Sciences, Vol. 113, Issue 17
Laser-induced ultrafast spin reorientation in the antiferromagnet TmFeO3
journal, June 2004
- Kimel, A. V.; Kirilyuk, A.; Tsvetkov, A.
- Nature, Vol. 429, Issue 6994
Phonons and related crystal properties from density-functional perturbation theory
journal, July 2001
- Baroni, Stefano; de Gironcoli, Stefano; Dal Corso, Andrea
- Reviews of Modern Physics, Vol. 73, Issue 2
Ultrafast Strain Engineering in Complex Oxide Heterostructures
journal, March 2012
- Caviglia, A. D.; Scherwitzl, R.; Popovich, P.
- Physical Review Letters, Vol. 108, Issue 13
Quantum Critical Origin of the Superconducting Dome in
journal, December 2015
- Edge, Jonathan M.; Kedem, Yaron; Aschauer, Ulrich
- Physical Review Letters, Vol. 115, Issue 24
Observation of coherent phonons in strontium titanate: Structural phase transition and ultrafast dynamics of the soft modes
journal, August 2006
- Kohmoto, T.; Tada, K.; Moriyasu, T.
- Physical Review B, Vol. 74, Issue 6
Enhancement of superconductivity by pressure-driven competition in electronic order
journal, August 2010
- Chen, Xiao-Jia; Struzhkin, Viktor V.; Yu, Yong
- Nature, Vol. 466, Issue 7309
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Ultrafast terahertz field control of electronic and structural interactions in vanadium dioxide
journal, July 2018
- Gray, A. X.; Hoffmann, M. C.; Jeong, J.
- Physical Review B, Vol. 98, Issue 4
X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92
journal, July 1993
- Henke, B. L.; Gullikson, E. M.; Davis, J. C.
- Atomic Data and Nuclear Data Tables, Vol. 54, Issue 2, p. 181-342
Crystal Stability and the Theory of Ferroelectricity
journal, November 1959
- Cochran, W.
- Physical Review Letters, Vol. 3, Issue 9
CSPAD-140k: A versatile detector for LCLS experiments
journal, August 2013
- Herrmann, Sven; Boutet, Sébastien; Duda, Brian
- Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 718
Lattice Dynamics and Phase Transitions of Strontium Titanate
journal, May 1964
- Cowley, R. A.
- Physical Review, Vol. 134, Issue 4A
Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces
journal, April 2008
- Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I.
- Physical Review Letters, Vol. 100, Issue 13
Temperature Dependence of the Transverse and Longitudinal Optic Mode Frequencies and Charges in SrTi and BaTi
journal, May 1966
- Barker, A. S.
- Physical Review, Vol. 145, Issue 2
Mode-Selective Control of the Crystal Lattice
journal, January 2015
- Först, M.; Mankowsky, R.; Cavalleri, A.
- Accounts of Chemical Research, Vol. 48, Issue 2
Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5
journal, December 2014
- Mankowsky, R.; Subedi, A.; Först, M.
- Nature, Vol. 516, Issue 7529
The X-ray Pump–Probe instrument at the Linac Coherent Light Source
journal, April 2015
- Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco
- Journal of Synchrotron Radiation, Vol. 22, Issue 3
Dynamical matrices, Born effective charges, dielectric permittivity tensors, and interatomic force constants from density-functional perturbation theory
journal, April 1997
- Gonze, Xavier; Lee, Changyol
- Physical Review B, Vol. 55, Issue 16
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
Performance of a beam-multiplexing diamond crystal monochromator at the Linac Coherent Light Source
journal, June 2014
- Zhu, Diling; Feng, Yiping; Stoupin, Stanislav
- Review of Scientific Instruments, Vol. 85, Issue 6, Article No. 063106
Spectral encoding of x-ray/optical relative delay
journal, January 2011
- Bionta, Mina R.; Lemke, H. T.; Cryan, J. P.
- Optics Express, Vol. 19, Issue 22
SrTi : An intrinsic quantum paraelectric below 4 K
journal, April 1979
- Müller, K. A.; Burkard, H.
- Physical Review B, Vol. 19, Issue 7
Hyper-Raman spectra and frequency dependence of soft mode damping in SrTiO3
journal, August 1983
- Denisov, V. N.; Mavrin, B. N.; Podobedov, V. B.
- Journal of Raman Spectroscopy, Vol. 14, Issue 4
Polar phonons in some compressively stressed epitaxial and polycrystalline SrTiO3 thin films
journal, April 2008
- Nuzhnyy, D.; Petzelt, J.; Kamba, S.
- Journal of Electroceramics, Vol. 22, Issue 1-3
Coherent phonons in a film generated by an intense single-cycle THz pulse
journal, June 2018
- Melnikov, A. A.; Boldyrev, K. N.; Selivanov, Yu. G.
- Physical Review B, Vol. 97, Issue 21
Sum-frequency ionic Raman scattering
journal, May 2018
- Juraschek, Dominik M.; Maehrlein, Sebastian F.
- Physical Review B, Vol. 97, Issue 17
Infrared dispersion in SrTi at high temperature
journal, December 1980
- Servoin, J. L.; Luspin, Y.; Gervais, F.
- Physical Review B, Vol. 22, Issue 11
A time-dependent order parameter for ultrafast photoinduced phase transitions
journal, August 2014
- Beaud, P.; Caviezel, A.; Mariager, S. O.
- Nature Materials, Vol. 13, Issue 10
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
Quantum Critical Origin of the Superconducting Dome in SrTiO₃
text, January 2015
- Aschauer, Ulrich Johannes; Balatsky, Alexander V.; Spaldin, Nicola A.
- American Physical Society
Polar phonons in some compressively stressed epitaxial and polycrystalline SrTiO3 thin films
text, January 2009
- Nuzhnyy, D.; Petzelt, J.; Kamba, S.
- arXiv
Interfacial mode coupling as the origin of the enhancement of Tc in FeSe films on SrTiO3
text, January 2013
- Lee, J. J.; Schmitt, F. T.; Moore, R. G.
- arXiv
Terahertz ellipsometry study of the soft mode behavior in ultrathin SrTiO3 films
text, January 2015
- Marsik, Premysl; Sen, Kaushik; Khmaladze, Jarji
- arXiv
Ultrafast THz Field Control of Electronic and Structural Interactions in Vanadium Dioxide
text, January 2016
- Gray, A. X.; Hoffmann, M. C.; Jeong, J.
- arXiv
Probing the Interatomic Potential of Solids by Strong-Field Nonlinear Phononics
text, January 2017
- von Hoegen, Alexander; Mankowsky, Roman; Fechner, Michael
- arXiv
Parametric amplification of optical phonons
preprint, January 2017
- Cartella, Andrea; Nova, Tobia Federico; Fechner, Michael
- arXiv
Works referencing / citing this record:
Light control of surface–bulk coupling by terahertz vibrational coherence in a topological insulator
journal, February 2020
- Yang, Xu; Luo, Liang; Vaswani, Chirag
- npj Quantum Materials, Vol. 5, Issue 1
Tunable strontium titanate terahertz all-dielectric metamaterials
journal, February 2020
- He, Xiaoyong; Lin, Fangting; Liu, Feng
- Journal of Physics D: Applied Physics, Vol. 53, Issue 15
Ultrafast reversal of the ferroelectric polarization by a midinfrared pulse
journal, January 2020
- Abalmasov, Veniamin A.
- Physical Review B, Vol. 101, Issue 1
Terahertz field–induced ferroelectricity in quantum paraelectric SrTiO 3
journal, June 2019
- Li, Xian; Qiu, Tian; Zhang, Jiahao
- Science, Vol. 364, Issue 6445
Investigation of Phonon Scattering on the Tunable Mechanisms of Terahertz Graphene Metamaterials
journal, December 2019
- He, Xiaoyong; Lin, Fangting; Liu, Feng
- Nanomaterials, Vol. 10, Issue 1
Ultrafast transient increase of oxygen octahedral rotations in a perovskite
text, January 2019
- Porer, Michael; Fechner, M.; Kubli, M.
- Universität Regensburg
Ultrafast transient increase of oxygen octahedral rotations in a perovskite
text, January 2019
- Porer, M.; Fechner, M.; Kubli, M.
- arXiv
Ultrafast reversal of the ferroelectric polarization by a midinfrared pulse
text, January 2019
- Abalmasov, Veniamin A.
- arXiv