Letter | Published:

Optically excited structural transition in atomic wires on surfaces at the quantum limit

Nature volume 544, pages 207211 (13 April 2017) | Download Citation

Abstract

Transient control over the atomic potential-energy landscapes of solids could lead to new states of matter and to quantum control of nuclear motion on the timescale of lattice vibrations. Recently developed ultrafast time-resolved diffraction techniques1 combine ultrafast temporal manipulation with atomic-scale spatial resolution and femtosecond temporal resolution. These advances have enabled investigations of photo-induced structural changes in bulk solids that often occur on timescales as short as a few hundred femtoseconds2,3,4,5,6. In contrast, experiments at surfaces and on single atomic layers such as graphene report timescales of structural changes that are orders of magnitude longer7,8,9. This raises the question of whether the structural response of low-dimensional materials to femtosecond laser excitation is, in general, limited. Here we show that a photo-induced transition from the low- to high-symmetry state of a charge density wave in atomic indium (In) wires supported by a silicon (Si) surface takes place within 350 femtoseconds. The optical excitation breaks and creates In–In bonds, leading to the non-thermal excitation of soft phonon modes, and drives the structural transition in the limit of critically damped nuclear motion through coupling of these soft phonon modes to a manifold of surface and interface phonons that arise from the symmetry breaking at the silicon surface. This finding demonstrates that carefully tuned electronic excitations can create non-equilibrium potential energy surfaces that drive structural dynamics at interfaces in the quantum limit (that is, in a regime in which the nuclear motion is directed and deterministic)8. This technique could potentially be used to tune the dynamic response of a solid to optical excitation, and has widespread potential application, for example in ultrafast detectors10,11.

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Acknowledgements

This work was supported by the Deutsche Forschungsgemeinschaft through SFB616 ‘Energy dissipation at surfaces’, FOR1700 ‘Metallic nanowires on the atomic scale: electronic and vibrational coupling in real world systems’, SFB1242 ‘Non-equilibrium dynamics of condensed matter in the time domain’, FOR1405 ‘Dynamics of electron transfer processes within transition metal sites in biological and bioinorganic systems’ and the High Performance Computing Center Stuttgart and the Paderborn Center for Parallel Computing. We acknowledge discussions with R. Ernstorfer and K. Sokolowski-Tinten.

Author information

Affiliations

  1. Fakultät für Physik und Center for Nanointegration (CENIDE), Universität Duisburg-Essen, Lotharstrasse 1, 47057 Duisburg, Germany

    • T. Frigge
    • , B. Hafke
    • , T. Witte
    • , B. Krenzer
    • , C. Streubühr
    • , A. Samad Syed
    • , V. Mikšić Trontl
    • , I. Avigo
    • , P. Zhou
    • , M. Ligges
    • , D. von der Linde
    • , U. Bovensiepen
    •  & M. Horn-von Hoegen
  2. Max-Planck-Institut für Eisenforschung, Max-Planck-Straße 1, 40237 Düsseldorf, Germany

    • S. Wippermann
  3. Lehrstuhl für Theoretische Materialphysik, Universität Paderborn, 33095 Paderborn, Germany

    • A. Lücke
    • , S. Sanna
    • , U. Gerstmann
    •  & W. G. Schmidt

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Contributions

T.F., B.H. and T.W. performed the ultrafast electron diffraction measurements and data analysis. The tilted pulse front scheme was set up by C.S., T.F., P.Z., M.L. and D.v.d.L. The trARPES measurements were performed by A.S.S., M.L., V.M.T. and I.A. and M.L. analysed the data. DFT calculations were performed by A.L., S.W., U.G., S.S. and W.G.S. B.K., M.H.-v.H., M.L. and U.B. conceived the experiments. The manuscript was written by B.K., T.F., M.L., U.B., M.H.-v.H. and W.G.S. All authors discussed the results and commented on the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to M. Horn-von Hoegen.

Reviewer Information Nature thanks J. Freericks, J. Ortega and the other anonymous reviewer(s) for their contribution to the peer review of this work.

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DOI

https://doi.org/10.1038/nature21432

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