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Title: Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate

Journal Article · · Science Advances
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)

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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231; AC02-76SF00515
OSTI ID:
1432217
Alternate ID(s):
OSTI ID: 1419320
Journal Information:
Science Advances, Vol. 3, Issue 11; ISSN 2375-2548
Publisher:
AAASCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 17 works
Citation information provided by
Web of Science

References (46)

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
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
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
Light-Induced Superconductivity in a Stripe-Ordered Cuprate journal January 2011
From quantum matter to high-temperature superconductivity in copper oxides journal February 2015
First principles phonon calculations in materials science journal November 2015
Direct observation of dynamic charge stripes in La2–xSrxNiO4 journal March 2014
Classification of charge density waves based on their nature journal February 2015
Fluctuating stripes at the onset of the pseudogap in the high-Tc superconductor Bi2Sr2CaCu2O8+x journal December 2010
Real-Time Manifestation of Strongly Coupled Spin and Charge Order Parameters in Stripe-Ordered La 1.75 Sr 0.25 NiO 4 Nickelate Crystals Using Time-Resolved Resonant X-Ray Diffraction journal March 2013
Theory for determination of the low-frequency time-dependent response function in liquids using time-resolved terahertz pulse spectroscopy journal May 1999
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
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
Snapshots of cooperative atomic motions in the optical suppression of charge density waves journal November 2010
Kramers–Kronig constrained variational analysis of optical spectra journal August 2005
Principles of Optics book January 1999
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
On the dynamics of polaron formation in a deformable medium journal February 1986
Ultrafast charge localization in a stripe-phase nickelate journal October 2013
Coherent effects in pump–probe spectroscopy of excitons journal January 1988
Conductivity artifacts in optical-pump THz-probe measurements of YBa_2Cu_3O_7 journal January 2000
A time-dependent order parameter for ultrafast photoinduced phase transitions journal August 2014
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
The theory of ultrafast vibrational spectroscopy journal April 1995
Spin Correlations among the Charge Carriers in an Ordered Stripe Phase journal December 2003
Disentangling the electronic and phononic glue in a high-Tc superconductor text January 2012
Relaxation dynamics of the Holstein polaron text January 2012
Comment on "Terahertz time-domain spectroscopy of transient metallic and superconducting states" (arXiv:1506.06758) preprint January 2015
First principles phonon calculations in materials science preprint January 2015
Kramers-Kronig constrained variational analysis of optical spectra text January 2005

Cited By (3)

Phonon dispersion evolution in uniaxially strained aluminum crystal journal April 2018
Theory of Time-Resolved Optical Conductivity of Superconductors: Comparing Two Methods for Its Evaluation journal August 2019
Theory of time-resolved optical conductivity of superconductors:comparing two methods for its evaluation text January 2019

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