Rationalizing charge transfer: a single-molecule case study across three distinct surfaces

Abstract

Organic molecules are versatile building blocks for the formation of complex low-dimensional nanostructures on surfaces. Recently, interest has grown in translating on-surface synthetic protocols from noble metal surfaces to insulating surfaces, which offer technological relevance, and to magnetic or superconducting surfaces, which offer new routes to correlated phases. It is important, therefore, to understand how these alternative surfaces may alter the properties of adsorbates through processes like charge transfer and screening. Evidence for charge transfer is often obtained experimentally via scanning tunneling microscopy (STM) and spectroscopy (STS), and theoretically via density functional theory (DFT). In this work, we systematically compare the properties of isolated macrocyclic emeraldine (Me₆) molecules on three different surfaces: metallic Au(111), a semiconducting ferromagnetic monolayer of FeCl₂, and a cleaved superconducting surface of bulk 2H-NbSe₂. We show that STS and DFT alone are insufficient to quantify charge transfer for these cases. Instead, we complement these methods with Kelvin probe force microscopy (KPFM) measurements and model Hamiltonian calculations to demonstrate that on Au(111) and FeCl₂, Me₆ molecules donate a single electron to the substrate, whereas on NbSe₂ two electrons are transferred from molecule to substrate. Our work provides insight into the interplay of charge transfer, screening, and molecule-substrate coupling, and develops experimental and theoretical methods for comparing the properties of adsorbates across different surfaces for future studies.

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BibTeX RIS

BibTeX

@misc{lowe2026rationalizing,
  title = {{Rationalizing charge transfer: a single-molecule case study across three distinct surfaces}},
  author = {Benjamin Lowe and Jan Berger and Martin Ondráček and Oleksandr Stetsovych and Shayan Louie and Marco Lozano and Diego Soler-Polo and Shiladitya Karmarkar and Andrés Pinar Solé and Iva Plutnarová and Pingo Mutombo and Manish Kumar and Michael Píro and Ali Cem Demirok and Michael L. Steigerwald and Zdeněk Sofer and Colin Nuckolls and Pavel Jelínek},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2610.32903},
  eprint = {2610.32903},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2610.32903},
  note = {CC BY 4.0},
}

RIS

TY  - UNPB
TI  - Rationalizing charge transfer: a single-molecule case study across three distinct surfaces
AU  - Benjamin Lowe
AU  - Jan Berger
AU  - Martin Ondráček
AU  - Oleksandr Stetsovych
AU  - Shayan Louie
AU  - Marco Lozano
AU  - Diego Soler-Polo
AU  - Shiladitya Karmarkar
AU  - Andrés Pinar Solé
AU  - Iva Plutnarová
AU  - Pingo Mutombo
AU  - Manish Kumar
AU  - Michael Píro
AU  - Ali Cem Demirok
AU  - Michael L. Steigerwald
AU  - Zdeněk Sofer
AU  - Colin Nuckolls
AU  - Pavel Jelínek
PY  - 2026
DA  - 2026/10/23
PB  - arXiv
DO  - 10.48550/arxiv.2610.32903
UR  - https://arxiv.org/abs/2610.32903
AB  - Organic molecules are versatile building blocks for the formation of complex low-dimensional nanostructures on surfaces. Recently, interest has grown in translating on-surface synthetic protocols from noble metal surfaces to insulating surfaces, which offer technological relevance, and to magnetic or superconducting surfaces, which offer new routes to correlated phases. It is important, therefore, to understand how these alternative surfaces may alter the properties of adsorbates through processes like charge transfer and screening. Evidence for charge transfer is often obtained experimentally via scanning tunneling microscopy (STM) and spectroscopy (STS), and theoretically via density functional theory (DFT). In this work, we systematically compare the properties of isolated macrocyclic emeraldine (Me_6) molecules on three different surfaces: metallic Au(111), a semiconducting ferromagnetic monolayer of FeCl_2, and a cleaved superconducting surface of bulk 2H-NbSe_2. We show that STS and DFT alone are insufficient to quantify charge transfer for these cases. Instead, we complement these methods with Kelvin probe force microscopy (KPFM) measurements and model Hamiltonian calculations to demonstrate that on Au(111) and FeCl_2, Me_6 molecules donate a single electron to the substrate, whereas on NbSe_2 two electrons are transferred from molecule to substrate. Our work provides insight into the interplay of charge transfer, screening, and molecule-substrate coupling, and develops experimental and theoretical methods for comparing the properties of adsorbates across different surfaces for future studies.
ER  -

Abstract

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