@article{35a24f2d4483446da698046d245c81d0,
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 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. 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.",
author = "Giacomo Coslovich and Kemper, {Alexander F.} and Sascha Behl and Bernhard Huber and Bechtel, {Hans A.} and Takao Sasagawa and Martin, {Michael C.} and Alessandra Lanzara and Kaindl, {Robert A.}",
note = "Funding Information: We thank W.-S. Lee and Z.-X. Shen for discussions and contributions in the early stage of this work, as well as A. Cavalleri and M. Trigo for stimulating scientific discussions. Funding: This work was primarily funded by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract no. DE-AC02-05CH11231 (Ultrafast Materials Science program KC2203), covering ultrafast and equilibrium terahertz spectroscopy and data analysis (G.C., S.B., B.H., A.L., and R.A.K.). For equilibrium FTIR characterization, the research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility supported under contract no. DE-AC02-05CH11231 (H.A.B. and M.C.M.). B.H. and S.B. acknowledge student fellowships from the German Academic Exchange Service. Author contributions: G.C. and R.A.K. conceived and performed the ultrafast terahertz study; A.F.K. performed the DFT calculations; G.C., B.H., H.A.B., and M.C.M. implemented the FTIR spectroscopy; T.S. synthesized the crystals; and G.C. and R.A.K. analyzed the data and wrote the manuscript. All the authors contributed to the discussion and interpretation of the experimental data. Competing interests: The authors declare that they have no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials. Additional data related to this paper may be requested from the authors. Publisher Copyright: Copyright {\textcopyright} 2017 The Authors.",
year = "2017",
doi = "10.1126/sciadv.1600735",
language = "English (US)",
volume = "3",
journal = "Science Advances",
issn = "2375-2548",
publisher = "American Association for the Advancement of Science",
number = "11",
}