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Title: 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 La 1.75Sr 0.25NiO 4, 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:
ORCiD logo [1]; ORCiD logo [2];  [3];  [3];  [3]; ORCiD logo [4]; ORCiD logo [3];  [5]; ORCiD logo [3]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); North Carolina State Univ., Raleigh, NC (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Tokyo Institute of Technology, Kanagawa (Japan)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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. doi: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. doi: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 = {2017},
month = {11}
}

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Works referenced in this record:

Stripe order and vibrational properties of La 2 Ni O 4 + δ for δ = 2 15 : Measurements and ab initio calculations
journal, January 2007


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
  • DOI: 10.1103/PhysRevLett.77.3865

Bond-Stretching-Phonon Anomalies in Stripe-Ordered La 1.69 Sr 0.31 NiO 4
journal, January 2002


Weak ferromagnetic spin and charge stripe order in La 5 3 Sr 1 3 Ni O 4
journal, September 2005


Ultrafast Electron Relaxation in Superconducting Bi 2 Sr 2 CaCu 2 O 8 + δ by Time-Resolved Photoelectron Spectroscopy
journal, November 2007


Ultrafast changes in lattice symmetry probed by coherent phonons
journal, January 2012

  • Wall, S.; Wegkamp, D.; Foglia, L.
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms1719

Broken translational and rotational symmetry via charge stripe order in underdoped YBa2Cu3O6+y
journal, March 2015


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
  • DOI: 10.1038/ncomms1837

Light-Induced Superconductivity in a Stripe-Ordered Cuprate
journal, January 2011


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
  • DOI: 10.1038/nature14165

First principles phonon calculations in materials science
journal, November 2015


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
  • DOI: 10.1038/ncomms4467

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
  • DOI: 10.1073/pnas.1424791112

The theory of ultrafast vibrational spectroscopy
journal, April 1995


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
  • DOI: 10.1038/nature09597

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
  • DOI: 10.1063/1.478766

Structural, magnetic and dielectric properties of La2−xCaxNiO4+δ (x=0, 0.1, 0.2, 0.3)
journal, January 2011


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
  • DOI: 10.1038/ncomms7772

Long-Range Incommensurate Charge Fluctuations in (Y,Nd)Ba2Cu3O6+x
journal, July 2012


Relaxation Dynamics of the Holstein Polaron
journal, December 2012


Analysis of Femtosecond Dynamic Absorption Spectra of Nonstationary States
journal, October 1992


Dynamics and Control in Complex Transition Metal Oxides
journal, July 2014


Spin Correlations among the Charge Carriers in an Ordered Stripe Phase
journal, December 2003


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
  • DOI: 10.1038/nature09539

Kramers–Kronig constrained variational analysis of optical spectra
journal, August 2005

  • Kuzmenko, A. B.
  • Review of Scientific Instruments, Vol. 76, Issue 8
  • DOI: 10.1063/1.1979470

Electron–phonon coupling reflecting dynamic charge inhomogeneity in copper oxide superconductors
journal, April 2006


Terahertz time-domain spectroscopy of transient metallic and superconducting states
journal, October 2015


Coherent effects in femtosecond infrared spectroscopy
journal, November 1995


Disentangling the Electronic and Phononic Glue in a High-Tc Superconductor
journal, March 2012


How to detect fluctuating stripes in the high-temperature superconductors
journal, October 2003


Femtochemistry:  Atomic-Scale Dynamics of the Chemical Bond
journal, June 2000

  • Zewail, Ahmed H.
  • The Journal of Physical Chemistry A, Vol. 104, Issue 24
  • DOI: 10.1021/jp001460h

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
  • DOI: 10.1063/1.450502

Ultrafast charge localization in a stripe-phase nickelate
journal, October 2013

  • Coslovich, G.; Huber, B.; Lee, W. -S.
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3643

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
  • DOI: 10.1364/OL.13.000276

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
  • DOI: 10.1364/JOSAB.17.000327

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

Optical conductivity studies of La 3 / 2 Sr 1 / 2 NiO 4 : Lattice effect on charge ordering
journal, September 2001


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


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
  • DOI: 10.1038/nmat4042