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Correlation-Driven d-Band Modifications Promote Chemical Bonding at 3d-Ferromagnetic Surfaces.

David Maximilian Janas1, Andreas Windischbacher2, Alessandro Sala3

  • 1Department of Physics, TU Dortmund University, 44227, Dortmund, Germany.

Small (Weinheim an Der Bergstrasse, Germany)
|December 4, 2025
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Summary
This summary is machine-generated.

This study reveals how electronic correlations in oxygen-passivated iron surfaces enhance chemical bonding with pentacene molecules. This understanding is key for designing advanced catalysts and organic electronic devices.

Keywords:
chemisorptiond‐band modelelectron correlationferromagnetic surfacemetal/organic interface

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Area of Science:

  • Surface Science
  • Materials Chemistry
  • Condensed Matter Physics

Background:

  • Understanding molecule-metal interfaces is crucial for catalysis, spintronics, and organic electronics.
  • Existing models like Newns-Anderson and d-band theory have limitations with complex organic molecules and correlated metals.

Purpose of the Study:

  • Investigate the chemical bonding between pentacene (5A) and an oxygen-passivated Fe(100) surface (Fe-O).
  • Explore the role of strong electronic correlations induced by oxygen chemisorption.
  • Extend chemisorption models to incorporate many-body effects at correlated surfaces.

Main Methods:

  • Employed photoemission orbital tomography and scanning tunneling spectroscopy.
  • Utilized electronic structure calculations, including a tailored DFT+U approach.
  • Validated findings with dynamical mean-field theory (DMFT).

Main Results:

  • Observed significant hybridization between pentacene frontier orbitals and Fe d-states.
  • Demonstrated that DFT+U with negative Ueff accurately models d-band narrowing and reduced spin splitting.
  • Showed that correlation effects promote a transition from physisorption to strong chemisorption.

Conclusions:

  • Developed an extended d-band model incorporating spatially modulated adsorbate-substrate coupling.
  • Provided a method for integrating many-body effects into chemisorption models.
  • Enabled predictive insights for designing 3d-metal catalysts and organic spintronic interfaces.