Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate
Abstract
The ability to probe symmetry-breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-terahertz response of the model stripe compound La1.75Sr0.25NiO4, yielding novel insight into its electronic and structural dynamics following an ultrafast optical quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen—as witnessed by time-delayed suppression of zone-folded Ni–O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. As a result, the hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry-breaking dynamics in solids.
- Authors:
-
[1];
[2];
[4];
[3];
[3]
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); North Carolina State Univ., Raleigh, NC (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Tokyo Institute of Technology, Kanagawa (Japan)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1432217
- Alternate Identifier(s):
- OSTI ID: 1419320
- Grant/Contract Number:
- AC02-05CH11231; AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 11; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Coslovich, Giacomo, Kemper, Alexander F., Behl, Sascha, Huber, Bernhard, Bechtel, Hans A., Sasagawa, Takao, Martin, Michael C., Lanzara, Alessandra, and Kaindl, Robert A. Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate. United States: N. p., 2017.
Web. doi:10.1126/sciadv.1600735.
Coslovich, Giacomo, Kemper, Alexander F., Behl, Sascha, Huber, Bernhard, Bechtel, Hans A., Sasagawa, Takao, Martin, Michael C., Lanzara, Alessandra, & Kaindl, Robert A. Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate. United States. https://doi.org/10.1126/sciadv.1600735
Coslovich, Giacomo, Kemper, Alexander F., Behl, Sascha, Huber, Bernhard, Bechtel, Hans A., Sasagawa, Takao, Martin, Michael C., Lanzara, Alessandra, and Kaindl, Robert A. Fri .
"Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate". United States. https://doi.org/10.1126/sciadv.1600735. https://www.osti.gov/servlets/purl/1432217.
@article{osti_1432217,
title = {Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate},
author = {Coslovich, Giacomo and Kemper, Alexander F. and Behl, Sascha and Huber, Bernhard and Bechtel, Hans A. and Sasagawa, Takao and Martin, Michael C. and Lanzara, Alessandra and Kaindl, Robert A.},
abstractNote = {The ability to probe symmetry-breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-terahertz response of the model stripe compound La1.75Sr0.25NiO4, yielding novel insight into its electronic and structural dynamics following an ultrafast optical quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen—as witnessed by time-delayed suppression of zone-folded Ni–O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. As a result, the hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry-breaking dynamics in solids.},
doi = {10.1126/sciadv.1600735},
journal = {Science Advances},
number = 11,
volume = 3,
place = {United States},
year = {Fri Nov 24 00:00:00 EST 2017},
month = {Fri Nov 24 00:00:00 EST 2017}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 17 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Stripe order and vibrational properties of for : Measurements and ab initio calculations
journal, January 2007
- Homes, C. C.; Tranquada, J. M.; Buttrey, D. J.
- Physical Review B, Vol. 75, Issue 4
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Bond-Stretching-Phonon Anomalies in Stripe-Ordered
journal, January 2002
- Tranquada, J. M.; Nakajima, K.; Braden, M.
- Physical Review Letters, Vol. 88, Issue 7
Weak ferromagnetic spin and charge stripe order in
journal, September 2005
- Klingeler, R.; Büchner, B.; Cheong, S. -W.
- Physical Review B, Vol. 72, Issue 10
Ultrafast Electron Relaxation in Superconducting by Time-Resolved Photoelectron Spectroscopy
journal, November 2007
- Perfetti, L.; Loukakos, P. A.; Lisowski, M.
- Physical Review Letters, Vol. 99, Issue 19
Ultrafast changes in lattice symmetry probed by coherent phonons
journal, January 2012
- Wall, S.; Wegkamp, D.; Foglia, L.
- Nature Communications, Vol. 3, Issue 1
Broken translational and rotational symmetry via charge stripe order in underdoped YBa2Cu3O6+y
journal, March 2015
- Comin, R.; Sutarto, R.; da Silva Neto, E. H.
- Science, Vol. 347, Issue 6228
Phase fluctuations and the absence of topological defects in a photo-excited charge-ordered nickelate
journal, January 2012
- Lee, W. S.; Chuang, Y. D.; Moore, R. G.
- Nature Communications, Vol. 3, Issue 1
Light-Induced Superconductivity in a Stripe-Ordered Cuprate
journal, January 2011
- Fausti, D.; Tobey, R. I.; Dean, N.
- Science, Vol. 331, Issue 6014
From quantum matter to high-temperature superconductivity in copper oxides
journal, February 2015
- Keimer, B.; Kivelson, S. A.; Norman, M. R.
- Nature, Vol. 518, Issue 7538
First principles phonon calculations in materials science
journal, November 2015
- Togo, Atsushi; Tanaka, Isao
- Scripta Materialia, Vol. 108
Direct observation of dynamic charge stripes in La2–xSrxNiO4
journal, March 2014
- Anissimova, S.; Parshall, D.; Gu, G. D.
- Nature Communications, Vol. 5, Issue 1
Classification of charge density waves based on their nature
journal, February 2015
- Zhu, Xuetao; Cao, Yanwei; Zhang, Jiandi
- Proceedings of the National Academy of Sciences, Vol. 112, Issue 8
Fluctuating stripes at the onset of the pseudogap in the high-Tc superconductor Bi2Sr2CaCu2O8+x
journal, December 2010
- Parker, Colin V.; Aynajian, Pegor; da Silva Neto, Eduardo H.
- Nature, Vol. 468, Issue 7324
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
Theory for determination of the low-frequency time-dependent response function in liquids using time-resolved terahertz pulse spectroscopy
journal, May 1999
- Kindt, James T.; Schmuttenmaer, Charles A.
- The Journal of Chemical Physics, Vol. 110, Issue 17
Structural, magnetic and dielectric properties of La2−xCaxNiO4+δ (x=0, 0.1, 0.2, 0.3)
journal, January 2011
- Shi, Chen-Yang; Hu, Zhong-Bo; Hao, Yong-Mei
- Journal of Alloys and Compounds, Vol. 509, Issue 4
Ultrafast myoglobin structural dynamics observed with an X-ray free-electron laser
journal, April 2015
- Levantino, Matteo; Schirò, Giorgio; Lemke, Henrik Till
- Nature Communications, Vol. 6, Issue 1
Long-Range Incommensurate Charge Fluctuations in (Y,Nd)Ba2Cu3O6+x
journal, July 2012
- Ghiringhelli, G.; Le Tacon, M.; Minola, M.
- Science, Vol. 337, Issue 6096
Relaxation Dynamics of the Holstein Polaron
journal, December 2012
- Golež, Denis; Bonča, Janez; Vidmar, Lev
- Physical Review Letters, Vol. 109, Issue 23
Analysis of Femtosecond Dynamic Absorption Spectra of Nonstationary States
journal, October 1992
- Pollard, W. T.; Mathies, R. A.
- Annual Review of Physical Chemistry, Vol. 43, Issue 1
Dynamics and Control in Complex Transition Metal Oxides
journal, July 2014
- Zhang, J.; Averitt, R. D.
- Annual Review of Materials Research, Vol. 44, Issue 1
Snapshots of cooperative atomic motions in the optical suppression of charge density waves
journal, November 2010
- Eichberger, Maximilian; Schäfer, Hanjo; Krumova, Marina
- Nature, Vol. 468, Issue 7325
Kramers–Kronig constrained variational analysis of optical spectra
journal, August 2005
- Kuzmenko, A. B.
- Review of Scientific Instruments, Vol. 76, Issue 8
Principles of Optics
book, January 1999
- Born, Max; Wolf, Emil; Bhatia, A. B.
- Cambridge University Press
Electron–phonon coupling reflecting dynamic charge inhomogeneity in copper oxide superconductors
journal, April 2006
- Reznik, D.; Pintschovius, L.; Ito, M.
- Nature, Vol. 440, Issue 7088
Terahertz time-domain spectroscopy of transient metallic and superconducting states
journal, October 2015
- Orenstein, J.; Dodge, J. S.
- Physical Review B, Vol. 92, Issue 13
Coherent effects in femtosecond infrared spectroscopy
journal, November 1995
- Hamm, P.
- Chemical Physics, Vol. 200, Issue 3
Disentangling the Electronic and Phononic Glue in a High-Tc Superconductor
journal, March 2012
- Dal Conte, S.; Giannetti, C.; Coslovich, G.
- Science, Vol. 335, Issue 6076
How to detect fluctuating stripes in the high-temperature superconductors
journal, October 2003
- Kivelson, S. A.; Bindloss, I. P.; Fradkin, E.
- Reviews of Modern Physics, Vol. 75, Issue 4
Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond †
journal, June 2000
- Zewail, Ahmed H.
- The Journal of Physical Chemistry A, Vol. 104, Issue 24
On the dynamics of polaron formation in a deformable medium
journal, February 1986
- Brown, David W.; Lindenberg, Katja; West, Bruce J.
- The Journal of Chemical Physics, Vol. 84, Issue 3
Ultrafast charge localization in a stripe-phase nickelate
journal, October 2013
- Coslovich, G.; Huber, B.; Lee, W. -S.
- Nature Communications, Vol. 4, Issue 1
Coherent effects in pump–probe spectroscopy of excitons
journal, January 1988
- Joffre, M.; la Guillaume, C. Benoit à; Peyghambarian, N.
- Optics Letters, Vol. 13, Issue 4
Conductivity artifacts in optical-pump THz-probe measurements of YBa_2Cu_3O_7
journal, January 2000
- Averitt, Richard D.; Rodriguez, George; Siders, Jennifer L. W.
- Journal of the Optical Society of America B, Vol. 17, Issue 2
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
Optical conductivity studies of Lattice effect on charge ordering
journal, September 2001
- Jung, J. H.; Kim, D. -W.; Noh, T. W.
- Physical Review B, Vol. 64, Issue 16
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
Non-thermal separation of electronic and structural orders in a persisting charge density wave
journal, July 2014
- Porer, M.; Leierseder, U.; Ménard, J. -M.
- Nature Materials, Vol. 13, Issue 9
The theory of ultrafast vibrational spectroscopy
journal, April 1995
- Wynne, Klaas; Hochstrasser, R. M.
- Chemical Physics, Vol. 193, Issue 3
From quantum matter to high-temperature superconductivity in copper oxides
journal, February 2015
- Keimer, B.; Kivelson, S. A.; Norman, M. R.
- Nature, Vol. 518, Issue 7538
Phase fluctuations and the absence of topological defects in a photo-excited charge-ordered nickelate
journal, January 2012
- Lee, W. S.; Chuang, Y. D.; Moore, R. G.
- Nature Communications, Vol. 3, Issue 1
Direct observation of dynamic charge stripes in La2–xSrxNiO4
journal, March 2014
- Anissimova, S.; Parshall, D.; Gu, G. D.
- Nature Communications, Vol. 5, Issue 1
Non-thermal separation of electronic and structural orders in a persisting charge density wave
journal, July 2014
- Porer, M.; Leierseder, U.; Ménard, J. -M.
- Nature Materials, Vol. 13, Issue 9
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
On the dynamics of polaron formation in a deformable medium
journal, February 1986
- Brown, David W.; Lindenberg, Katja; West, Bruce J.
- The Journal of Chemical Physics, Vol. 84, Issue 3
Spin Correlations among the Charge Carriers in an Ordered Stripe Phase
journal, December 2003
- Boothroyd, A. T.; Freeman, P. G.; Prabhakaran, D.
- Physical Review Letters, Vol. 91, Issue 25
Analysis of Femtosecond Dynamic Absorption Spectra of Nonstationary States
journal, October 1992
- Pollard, W. T.; Mathies, R. A.
- Annual Review of Physical Chemistry, Vol. 43, Issue 1
Disentangling the electronic and phononic glue in a high-Tc superconductor
text, January 2012
- Conte, Stefano Dal; Giannetti, Claudio; Coslovich, Giacomo
- arXiv
Relaxation dynamics of the Holstein polaron
text, January 2012
- Golež, Denis; Bonča, Janez; Vidmar, Lev
- arXiv
Comment on "Terahertz time-domain spectroscopy of transient metallic and superconducting states" (arXiv:1506.06758)
preprint, January 2015
- Nicoletti, D.; Mitrano, M.; Cantaluppi, A.
- arXiv
First principles phonon calculations in materials science
preprint, January 2015
- Togo, Atsushi; Tanaka, Isao
- arXiv
Kramers-Kronig constrained variational analysis of optical spectra
text, January 2005
- Kuzmenko, A. B.
- arXiv
Works referencing / citing this record:
Phonon dispersion evolution in uniaxially strained aluminum crystal
journal, April 2018
- Parthasarathy, Ranganathan; Misra, Anil; Aryal, Sitaram
- Continuum Mechanics and Thermodynamics, Vol. 30, Issue 5
Theory of Time-Resolved Optical Conductivity of Superconductors: Comparing Two Methods for Its Evaluation
journal, August 2019
- Revelle, John P.; Kumar, Ankit; Kemper, Alexander F.
- Condensed Matter, Vol. 4, Issue 3
Theory of time-resolved optical conductivity of superconductors:comparing two methods for its evaluation
text, January 2019
- Revelle, John P.; Kumar, Ankit; Kemper, Alexander F.
- arXiv
Theory of time-resolved optical conductivity of superconductors:comparing two methods for its evaluation
text, January 2019
- Revelle, John P.; Kumar, Ankit; Kemper, Alexander F.
- arXiv