Charge Transfer into Organic Thin Films: A Deeper Insight through Machine‐Learning‐Assisted Structure Search

Alexander Egger, Lukas Hörmann, Andreas Jeindl, Michael Scherbela, Veronika Obersteiner, Milica Todorović, Patrick Rinke, Oliver Hofmann*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review


Density functional theory calculations are combined with machine learning to investigate the coverage-dependent charge transfer at the tetracyanoethylene/Cu(111) hybrid organic/inorganic interface. The study finds two different monolayer phases, which exhibit a qualitatively different charge-transfer behavior. Our results refute previous theories of long-range charge transfer to molecules not in direct contact with the surface. Instead, they demonstrate that experimental evidence supports our hypothesis of a coverage-dependent structural reorientation of the first monolayer. Such phase transitions at interfaces may be more common than currently envisioned, beckoning a thorough reevaluation of organic/inorganic interfaces.

Original languageEnglish
Article number2000992
JournalAdvanced Science
Issue number15
Publication statusPublished - 28 Jun 2020


  • Bayesian inference
  • charge transfer
  • density functional theory
  • hybrid interfaces
  • machine learning
  • organic electronics
  • structure search
  • vibrations

ASJC Scopus subject areas

  • Engineering(all)
  • Physics and Astronomy(all)
  • Chemical Engineering(all)
  • Biochemistry, Genetics and Molecular Biology (miscellaneous)
  • Materials Science(all)
  • Medicine (miscellaneous)

Fields of Expertise

  • Advanced Materials Science


  • NAWI Graz

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