Iron-based trinuclear metal-organic nanostructures on a surface with local charge accumulation

Cornelius Krull, Marina Castelli, Prokop Hapala, Dhaneesh Kumar, Anton Tadich, Martina Capsoni, Mark T. Edmonds, Jack Hellerstedt, Sarah A. Burke, Pavel Jelinek () and Agustin Schiffrin ()
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Cornelius Krull: Monash University
Marina Castelli: Monash University
Prokop Hapala: Institute of Physics of the CAS
Dhaneesh Kumar: Monash University
Anton Tadich: Australian Synchrotron
Martina Capsoni: Department of Physics and Astronomy, University of British Columbia
Mark T. Edmonds: Monash University
Jack Hellerstedt: Monash University
Sarah A. Burke: Department of Physics and Astronomy, University of British Columbia
Pavel Jelinek: Institute of Physics of the CAS
Agustin Schiffrin: Monash University

Nature Communications, 2018, vol. 9, issue 1, 1-7

Abstract: Abstract Coordination chemistry relies on harnessing active metal sites within organic matrices. Polynuclear complexes—where organic ligands bind to several metal atoms—are relevant due to their electronic/magnetic properties and potential for functional reactivity pathways. However, their synthesis remains challenging; few geometries and configurations have been achieved. Here, we synthesise—via supramolecular chemistry on a noble metal surface—one-dimensional metal-organic nanostructures composed of terpyridine (tpy)-based molecules coordinated with well-defined polynuclear iron clusters. Combining low-temperature scanning probe microscopy and density functional theory, we demonstrate that the coordination motif consists of coplanar tpyʼs linked via a quasi-linear tri-iron node in a mixed (positive-)valence metal–metal bond configuration. This unusual linkage is stabilised by local accumulation of electrons between cations, ligand and surface. The latter, enabled by bottom-up on-surface synthesis, yields an electronic structure that hints at a chemically active polynuclear metal centre, paving the way for nanomaterials with novel catalytic/magnetic functionalities.

Date: 2018
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DOI: 10.1038/s41467-018-05543-4

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