Open AccessCharge Transfer into Organic Thin Films: A Deeper Insight through Machine‐Learning‐Assisted Structure Search
Author(s) -
Egger Alexander T.,
Hörmann Lukas,
Jeindl Andreas,
Scherbela Michael,
Obersteiner Veronika,
Todorović Milica,
Rinke Patrick,
Hofmann Oliver T.
Publication year - 2020
Publication title -
advanced science
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.388
H-Index - 100
ISSN - 2198-3844
DOI - 10.1002/advs.202000992
Subject(s) - tetracyanoethylene , monolayer , charge (physics) , organic molecules , chemical physics , density functional theory , materials science , interface (matter) , molecule , range (aeronautics) , nanotechnology , computer science , chemistry , computational chemistry , physics , organic chemistry , quantum mechanics , gibbs isotherm , composite material
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.