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Direct imaging of the massive 3d orbital switching across the metal-insulator transition in VO2

Paulius Dolmantas1,*, Chun-Fu Chang1, Martin Sundermann1,2, Andrea Marino1, Andrea Amorese1,†, Hlynur Gretarsson2, Marcus Schmidt1, Thomas Christoph Koethe3, Maurits W. Haverkort4 et al.

Liu Hao Tjeng1,‡

  • *Contact author: Paulius.Dolmantas@cpfs.mpg.de
  • †Present address: ASML Netherlands B.V., De Run 6501, 5504 DR Veldhoven, The Netherlands.
  • ‡Contact author: Hao.Tjeng@cpfs.mpg.de
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Phys. Rev. Research 8, 023164 – Published 14 May, 2026

DOI: https://doi.org/10.1103/dvsr-8ft7

Abstract

We carried out nonresonant inelastic x-ray scattering measurements at the V L1 edge to probe the local V 3d charge density in VO2 across the metal-insulator transition (MIT). Without relying on spectral calculations, we were able to integrate directly from the orientational dependence an image of the occupied 3d shell and extract quantitatively the orbital occupations of the V ions. We found that in the low-temperature insulating M1 phase the V is highly polarized toward the σ configuration. The orbital occupation undergoes significant redistribution upon transition into the metallic R phase, leading to a more isotropic charge density. The massiveness of the orbital switching promotes the scenario in which electron correlations and lattice degrees of freedom are strongly coupled, so that the contribution of the lattice and the electronic part to the energetics must be treated on equal footing to model the MIT quantitatively.

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Phys. Rev. Research 8, 023164– Published 14 May, 2026
  • Received 22 November 2025
  • Accepted 18 April 2026
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Open access publication funded by Max Planck Society.

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