Fully Atomistic Understanding of the Electronic and Optical Properties of a Prototypical Doped Charge-Transfer Interface

Anu Baby, Marco Gruenewald, Christian Zwick, Felix Otto, Roman Forker, Gerben Van Straaten, Markus Franke, Benjamin Stadtmüller, Christian Kumpf, Gian Paolo Brivio, Guido Fratesi, Torsten Fritz, Egbert Zojer

Publikation: Beitrag in einer FachzeitschriftArtikelForschungBegutachtung

Abstract

The current study generates profound atomistic insights into doping-induced changes of the optical and electronic properties of the prototypical PTCDA/Ag(111) interface. For doping K atoms are used, as KxPTCDA/Ag(111) has the distinct advantage of forming well-defined stoichiometric phases. To arrive at a conclusive, unambiguous, and fully atomistic understanding of the interface properties, we combine state-of-the-art density-functional theory calculations with optical differential reflectance data, photoelectron spectra, and X-ray standing wave measurements. In combination with the full structural characterization of the KxPTCDA/Ag(111) interface by low-energy electron diffraction and scanning tunneling microscopy experiments (ACS Nano 2016, 10, 2365-2374), the present comprehensive study provides access to a fully characterized reference system for a well-defined metal-organic interface in the presence of dopant atoms, which can serve as an ideal benchmark for future research and applications. The combination of the employed complementary techniques allows us to understand the peculiarities of the optical spectra of K2PTCDA/Ag(111) and their counterintuitive similarity to those of neutral PTCDA layers. They also clearly describe the transition from a metallic character of the (pristine) adsorbed PTCDA layer on Ag(111) to a semiconducting state upon doping, which is the opposite of the effect (degenerate) doping usually has on semiconducting materials. All experimental and theoretical efforts also unanimously reveal a reduced electronic coupling between the adsorbate and the substrate, which goes hand in hand with an increasing adsorption distance of the PTCDA molecules caused by a bending of their carboxylic oxygens away from the substrate and toward the potassium atoms.

Originalspracheenglisch
Seiten (von - bis)10495-10508
Seitenumfang14
FachzeitschriftACS Nano
Jahrgang11
Ausgabenummer10
DOIs
PublikationsstatusVeröffentlicht - 24 Okt 2017

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Electronic properties
Charge transfer
Optical properties
charge transfer
Doping (additives)
optical properties
electronics
Atoms
atoms
reference systems
standing waves
Low energy electron diffraction
optical spectrum
scanning tunneling microscopy
Scanning tunneling microscopy
Substrates
Adsorbates
potassium
Photoelectrons
photoelectrons

Schlagwörter

    ASJC Scopus subject areas

    • !!Materials Science(all)
    • !!Engineering(all)
    • !!Physics and Astronomy(all)

    Fields of Expertise

    • Advanced Materials Science

    Treatment code (Nähere Zuordnung)

    • Basic - Fundamental (Grundlagenforschung)

    Dies zitieren

    Fully Atomistic Understanding of the Electronic and Optical Properties of a Prototypical Doped Charge-Transfer Interface. / Baby, Anu; Gruenewald, Marco; Zwick, Christian; Otto, Felix; Forker, Roman; Van Straaten, Gerben; Franke, Markus; Stadtmüller, Benjamin; Kumpf, Christian; Brivio, Gian Paolo; Fratesi, Guido; Fritz, Torsten; Zojer, Egbert.

    in: ACS Nano, Jahrgang 11, Nr. 10, 24.10.2017, S. 10495-10508.

    Publikation: Beitrag in einer FachzeitschriftArtikelForschungBegutachtung

    Baby, A, Gruenewald, M, Zwick, C, Otto, F, Forker, R, Van Straaten, G, Franke, M, Stadtmüller, B, Kumpf, C, Brivio, GP, Fratesi, G, Fritz, T & Zojer, E 2017, 'Fully Atomistic Understanding of the Electronic and Optical Properties of a Prototypical Doped Charge-Transfer Interface' ACS Nano, Jg. 11, Nr. 10, S. 10495-10508. https://doi.org/10.1021/acsnano.7b05828
    Baby, Anu ; Gruenewald, Marco ; Zwick, Christian ; Otto, Felix ; Forker, Roman ; Van Straaten, Gerben ; Franke, Markus ; Stadtmüller, Benjamin ; Kumpf, Christian ; Brivio, Gian Paolo ; Fratesi, Guido ; Fritz, Torsten ; Zojer, Egbert. / Fully Atomistic Understanding of the Electronic and Optical Properties of a Prototypical Doped Charge-Transfer Interface. in: ACS Nano. 2017 ; Jahrgang 11, Nr. 10. S. 10495-10508.
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    AU - Forker, Roman

    AU - Van Straaten, Gerben

    AU - Franke, Markus

    AU - Stadtmüller, Benjamin

    AU - Kumpf, Christian

    AU - Brivio, Gian Paolo

    AU - Fratesi, Guido

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