DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 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:
ORCiD logo [1];  [2]; ORCiD logo [3];  [1];  [1]; ORCiD logo [3];  [4];  [1]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [1]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)
  3. Univ. of Fribourg, Fribourg (Switzerland)
  4. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  5. 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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 83 works
Citation information provided by
Web of Science

Save / Share:

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
  • DOI: 10.1038/nature06119

Electric-Field-Induced Soft-Mode Hardening in SrTiO 3 Films
journal, May 2000


Crystal stability and the theory of ferroelectricity
journal, October 1960


Dielectric, infrared, and Raman response of undoped SrTiO 3 ceramics: Evidence of polar grain boundaries
journal, October 2001


Soft-mode hardening in SrTiO3 thin films
journal, March 2000

  • Sirenko, A. A.; Bernhard, C.; Golnik, A.
  • Nature, Vol. 404, Issue 6776
  • DOI: 10.1038/35006023

Elastic strain engineering of ferroic oxides
journal, February 2014

  • Schlom, Darrell G.; Chen, Long-Qing; Fennie, Craig J.
  • MRS Bulletin, Vol. 39, Issue 2
  • DOI: 10.1557/mrs.2014.1

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
  • DOI: 10.1088/0953-8984/21/39/395502

Far-Infrared Ferroelectric Vibration Mode in SrTi O 3
journal, March 1962


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
  • DOI: 10.1063/1.4977088

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
  • DOI: 10.1063/1.4983153

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
  • DOI: 10.1038/nature25484

Ferroelectric quantum criticality
journal, March 2014

  • Rowley, S. E.; Spalek, L. J.; Smith, R. P.
  • Nature Physics, Vol. 10, Issue 5
  • DOI: 10.1038/nphys2924

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


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
  • DOI: 10.1073/pnas.1809725115

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
  • DOI: 10.1038/nature13894

Collective Coherent Control: Synchronization of Polarization in Ferroelectric PbTiO 3 by Shaped THz Fields
journal, June 2009


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
  • DOI: 10.1063/1.4940976

Reversal of Ferroelectric Domains by Ultrashort Optical Pulses
journal, August 1994


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
  • DOI: 10.1143/JPSJ.26.396

Nonlinear phononics as an ultrafast route to lattice control
journal, August 2011

  • Först, M.; Manzoni, C.; Kaiser, S.
  • Nature Physics, Vol. 7, Issue 11
  • DOI: 10.1038/nphys2055

Temperature Dependence of a Transverse Optic Mode in Strontium Titanate
journal, August 1962


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
  • DOI: 10.1364/UP.2016.UW4A.11

Far Infrared Dielectric Dispersion in BaTi O 3 , SrTi O 3 , and Ti O 2
journal, June 1962


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
  • DOI: 10.1021/j100112a043

Femtosecond Structural Dynamics in VO 2 during an Ultrafast Solid-Solid Phase Transition
journal, November 2001


Magnetic-field-induced metal-insulator phenomena in Pr 1 x Ca x Mn O 3 with controlled charge-ordering instability
journal, January 1996


Room-temperature ferroelectricity in strained SrTiO3
journal, August 2004

  • Haeni, J. H.; Irvin, P.; Chang, W.
  • Nature, Vol. 430, Issue 7001, p. 758-761
  • DOI: 10.1038/nature02773

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
  • DOI: 10.1063/1.2734374

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
  • DOI: 10.1073/pnas.1604145113

Laser-induced ultrafast spin reorientation in the antiferromagnet TmFeO3
journal, June 2004

  • Kimel, A. V.; Kirilyuk, A.; Tsvetkov, A.
  • Nature, Vol. 429, Issue 6994
  • DOI: 10.1038/nature02659

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
  • DOI: 10.1103/RevModPhys.73.515

Ultrafast Strain Engineering in Complex Oxide Heterostructures
journal, March 2012


Quantum Critical Origin of the Superconducting Dome in SrTiO 3
journal, December 2015


Observation of coherent phonons in strontium titanate: Structural phase transition and ultrafast dynamics of the soft modes
journal, August 2006


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
  • DOI: 10.1038/nature09293

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
  • DOI: 10.1103/PhysRevB.13.5188

Ultrafast terahertz field control of electronic and structural interactions in vanadium dioxide
journal, July 2018


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
  • DOI: 10.1006/adnd.1993.1013

Crystal Stability and the Theory of Ferroelectricity
journal, November 1959


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
  • DOI: 10.1016/j.nima.2013.01.057

Lattice Dynamics and Phase Transitions of Strontium Titanate
journal, May 1964


Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces
journal, April 2008


Mode-Selective Control of the Crystal Lattice
journal, January 2015

  • Först, M.; Mankowsky, R.; Cavalleri, A.
  • Accounts of Chemical Research, Vol. 48, Issue 2
  • DOI: 10.1021/ar500391x

Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5
journal, December 2014


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
  • DOI: 10.1107/S1600577515005135

Ferroelectric Soft Mode in a SrTiO 3 Thin Film Impulsively Driven to the Anharmonic Regime Using Intense Picosecond Terahertz Pulses
journal, February 2012


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
  • DOI: 10.1063/1.4880724

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
  • DOI: 10.1364/OE.19.021855

SrTi O 3 : An intrinsic quantum paraelectric below 4 K
journal, April 1979


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
  • DOI: 10.1002/jrs.1250140413

Polar phonons in some compressively stressed epitaxial and polycrystalline SrTiO3 thin films
journal, April 2008


Coherent phonons in a Bi 2 Se 3 film generated by an intense single-cycle THz pulse
journal, June 2018


Sum-frequency ionic Raman scattering
journal, May 2018


Infrared dispersion in SrTi O 3 at high temperature
journal, December 1980


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
  • DOI: 10.1038/nmat4046

Large-Amplitude Spin Dynamics Driven by a THz Pulse in Resonance with an Electromagnon
journal, March 2014


Quantum Critical Origin of the Superconducting Dome in SrTiO₃
text, January 2015

  • Aschauer, Ulrich Johannes; Balatsky, Alexander V.; Spaldin, Nicola A.
  • American Physical Society
  • DOI: 10.7892/boris.85274

Interfacial mode coupling as the origin of the enhancement of Tc in FeSe films on SrTiO3
text, January 2013


Terahertz ellipsometry study of the soft mode behavior in ultrathin SrTiO3 films
text, January 2015


Probing the Interatomic Potential of Solids by Strong-Field Nonlinear Phononics
text, January 2017


Parametric amplification of optical phonons
preprint, January 2017


Works referencing / citing this record:

Light control of surface–bulk coupling by terahertz vibrational coherence in a topological insulator
journal, February 2020


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
  • DOI: 10.1088/1361-6463/ab6ccc

Ultrafast reversal of the ferroelectric polarization by a midinfrared pulse
journal, January 2020


Terahertz field–induced ferroelectricity in quantum paraelectric SrTiO 3
journal, June 2019


Investigation of Phonon Scattering on the Tunable Mechanisms of Terahertz Graphene Metamaterials
journal, December 2019


Ultrafast transient increase of oxygen octahedral rotations in a perovskite
text, January 2019


Ultrafast transient increase of oxygen octahedral rotations in a perovskite
text, January 2019