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  • Letter
  • Open Access

Ultrafast modification of the electronic structure of a correlated insulator

O. Grånäs1,*, I. Vaskivskyi1,2, X. Wang1, P. Thunström1, S. Ghimire3, R. Knut1, J. Söderström1, L. Kjellsson1, D. Turenne1 et al.

R. Y. Engel4, M. Beye4, J. Lu3, D. J. Higley5, A. H. Reid5, W. Schlotter5, G. Coslovich5, M. Hoffmann5, G. Kolesov6, C. Schüßler-Langeheine7, A. Styervoyedov8, N. Tancogne-Dejean9, M. A. Sentef9, D. A. Reis3, A. Rubio9,10, S. S. P. Parkin8, O. Karis1, J.-E. Rubensson1, O. Eriksson1,11, and H. A. Dürr1

  • 1Department of Physics and Astronomy, Uppsala University, Regementsvägen 1, 752 37 Uppsala, Sweden
  • 2Center for Memory and Recording Research, University of California San Diego, 9500 Gilman Drive, La Jolla, California 92093-0401, USA
  • 3Stanford PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA
  • 4Department of Photon Science, DESY, Notkestraße 85, D-22607 Hamburg, Germany
  • 5SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA
  • 6John Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, USA
  • 7Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 12489 Berlin, Germany
  • 8Max-Planck Institut für Mikrostrukturphysik, Weinberg 2, Halle, Germany
  • 9Max Planck Institute for the Structure and Dynamics of Matter and Center for Free-Electron Laser Science, Luruper Chaussee 149, 22761 Hamburg, Germany
  • 10Center for Computational Quantum Physics, Flatiron Institute, New York, New York 10010 USA
  • 11School of Science and Technology, Örebro University, SE-701 82 Örebro, Sweden

  • *oscar.granas@physics.uu.se
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Phys. Rev. Research 4, L032030 – Published 16 August, 2022

DOI: https://doi.org/10.1103/PhysRevResearch.4.L032030

Abstract

A nontrivial balance between Coulomb repulsion and kinematic effects determines the electronic structure of correlated electron materials. The use of electromagnetic fields strong enough to rival these native microscopic interactions allows us to study the electronic response as well as the time scales and energies involved in using quantum effects for possible applications. We use element-specific transient x-ray absorption spectroscopy and high-harmonic generation to measure the response to ultrashort off-resonant optical fields in the prototypical correlated electron insulator NiO. Surprisingly, fields of up to 0.22 V/Å lead to no detectable changes in the correlated Ni 3d orbitals contrary to previous predictions. A transient directional charge transfer is uncovered, a behavior that is captured by first-principles theory. Our results highlight the importance of retardation effects in electronic screening and pinpoints a key challenge in functionalizing correlated materials for ultrafast device operation.

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Phys. Rev. Research 4, L032030– Published 16 August, 2022
  • Received 28 December 2021
  • Revised 22 June 2022
  • Accepted 27 June 2022
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