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Ultrafast modification of the electronic structure of a correlated insulator

MPS-Authors
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Tancogne-Dejean,  N.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

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Sentef,  M. A.
Theoretical Description of Pump-Probe Spectroscopies in Solids, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

/persons/resource/persons22028

Rubio,  A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Center for Computational Quantum Physics, Flatiron Institute;

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Fulltext (public)

PhysRevResearch.4.L032030.pdf
(Publisher version), 3MB

Supplementary Material (public)

Supplemental_Material.pdf
(Supplementary material), 2MB

Citation

Grånäs, O., Vaskivskyi, I., Wang, X., Thunström, P., Ghimire, S., Knut, R., et al. (2022). Ultrafast modification of the electronic structure of a correlated insulator. Physical Review Research, 4(3): L032030. doi:10.1103/PhysRevResearch.4.L032030.


Cite as: https://hdl.handle.net/21.11116/0000-000A-DDD2-0
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.