Probing weak chemical interactions of metal surface atoms with CO-terminated AFM tips identifies molecular adsorption sites

Abstract Metal surfaces play a key role in on-surface synthesis as they provide a two-dimensional catalytic reaction environment that stimulates activation, diffusion, and coupling of molecular reactants. Fundamental understanding of the interactions between surface atoms and reactants is very limit...

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Main Authors: Jalmar Tschakert, Qigang Zhong, Alexander Sekels, Pascal Henkel, Jannis Jung, K. Linus H. Pohl, Hermann A. Wegner, Doreen Mollenhauer, André Schirmeisen, Daniel Ebeling
Format: Article
Language:English
Published: Nature Portfolio 2025-08-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-63159-x
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author Jalmar Tschakert
Qigang Zhong
Alexander Sekels
Pascal Henkel
Jannis Jung
K. Linus H. Pohl
Hermann A. Wegner
Doreen Mollenhauer
André Schirmeisen
Daniel Ebeling
author_facet Jalmar Tschakert
Qigang Zhong
Alexander Sekels
Pascal Henkel
Jannis Jung
K. Linus H. Pohl
Hermann A. Wegner
Doreen Mollenhauer
André Schirmeisen
Daniel Ebeling
author_sort Jalmar Tschakert
collection DOAJ
description Abstract Metal surfaces play a key role in on-surface synthesis as they provide a two-dimensional catalytic reaction environment that stimulates activation, diffusion, and coupling of molecular reactants. Fundamental understanding of the interactions between surface atoms and reactants is very limited but would enable controlling on-surface reaction processes for designing functional nanomaterials. Here, we measure chemical interactions between CO-terminated tips and Cu(111), Ag(111), and Au(111) surface atoms in all spatial directions with picometer resolution via low temperature atomic force microscopy. This allows a site-specific quantification of the weak chemical interactions of densely packed metal surface atoms and provides a picture of the potential energy landscape experienced by adsorbed reactants. Accompanying density functional theory calculations and the crystal orbital overlap population method reveal small covalent binding contributions from orbital overlap of the corresponding p- and d-states of the CO tip and the metal surface atoms as the cause for the site-specific interactions. Accessing such small covalent bonding contributions in the background of the dispersion-dominated interaction enables revealing insights into the nature of chemical bond formation with metal surface atoms and a reliable determination of molecular adsorption sites. The latter can serve both as a starting point and as a direct comparison with theoretical studies.
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issn 2041-1723
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spelling doaj-art-b984641c660b48bda2b3aa12b3acbf122025-08-24T11:38:59ZengNature PortfolioNature Communications2041-17232025-08-0116111010.1038/s41467-025-63159-xProbing weak chemical interactions of metal surface atoms with CO-terminated AFM tips identifies molecular adsorption sitesJalmar Tschakert0Qigang Zhong1Alexander Sekels2Pascal Henkel3Jannis Jung4K. Linus H. Pohl5Hermann A. Wegner6Doreen Mollenhauer7André Schirmeisen8Daniel Ebeling9Institute of Applied Physics (IAP), Justus Liebig University GiessenInstitute of Applied Physics (IAP), Justus Liebig University GiessenInstitute of Applied Physics (IAP), Justus Liebig University GiessenCenter for Materials Research (LaMa), Justus Liebig University GiessenCenter for Materials Research (LaMa), Justus Liebig University GiessenCenter for Materials Research (LaMa), Justus Liebig University GiessenCenter for Materials Research (LaMa), Justus Liebig University GiessenCenter for Materials Research (LaMa), Justus Liebig University GiessenInstitute of Applied Physics (IAP), Justus Liebig University GiessenInstitute of Applied Physics (IAP), Justus Liebig University GiessenAbstract Metal surfaces play a key role in on-surface synthesis as they provide a two-dimensional catalytic reaction environment that stimulates activation, diffusion, and coupling of molecular reactants. Fundamental understanding of the interactions between surface atoms and reactants is very limited but would enable controlling on-surface reaction processes for designing functional nanomaterials. Here, we measure chemical interactions between CO-terminated tips and Cu(111), Ag(111), and Au(111) surface atoms in all spatial directions with picometer resolution via low temperature atomic force microscopy. This allows a site-specific quantification of the weak chemical interactions of densely packed metal surface atoms and provides a picture of the potential energy landscape experienced by adsorbed reactants. Accompanying density functional theory calculations and the crystal orbital overlap population method reveal small covalent binding contributions from orbital overlap of the corresponding p- and d-states of the CO tip and the metal surface atoms as the cause for the site-specific interactions. Accessing such small covalent bonding contributions in the background of the dispersion-dominated interaction enables revealing insights into the nature of chemical bond formation with metal surface atoms and a reliable determination of molecular adsorption sites. The latter can serve both as a starting point and as a direct comparison with theoretical studies.https://doi.org/10.1038/s41467-025-63159-x
spellingShingle Jalmar Tschakert
Qigang Zhong
Alexander Sekels
Pascal Henkel
Jannis Jung
K. Linus H. Pohl
Hermann A. Wegner
Doreen Mollenhauer
André Schirmeisen
Daniel Ebeling
Probing weak chemical interactions of metal surface atoms with CO-terminated AFM tips identifies molecular adsorption sites
Nature Communications
title Probing weak chemical interactions of metal surface atoms with CO-terminated AFM tips identifies molecular adsorption sites
title_full Probing weak chemical interactions of metal surface atoms with CO-terminated AFM tips identifies molecular adsorption sites
title_fullStr Probing weak chemical interactions of metal surface atoms with CO-terminated AFM tips identifies molecular adsorption sites
title_full_unstemmed Probing weak chemical interactions of metal surface atoms with CO-terminated AFM tips identifies molecular adsorption sites
title_short Probing weak chemical interactions of metal surface atoms with CO-terminated AFM tips identifies molecular adsorption sites
title_sort probing weak chemical interactions of metal surface atoms with co terminated afm tips identifies molecular adsorption sites
url https://doi.org/10.1038/s41467-025-63159-x
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