Tuning Transition Metal‐Containing Molecular Magnets by On‐Surface Polymerization

Author:

Baranowski Daniel1ORCID,Cojocariu Iulia123,Schio Luca4,Bolaños Carolina Gutiérrez35,Floreano Luca4,Dreiser Jan5,Carlotto Silvia67,Casarin Maurizio7,Feyer Vitaliy18ORCID,Schneider Claus Michael189

Affiliation:

1. Peter Grünberg Institute (PGI‐6) Jülich Research Center 52428 Jülich Germany

2. Dipartimento di Fisica Università degli Studi di Trieste Trieste 34127 Italy

3. Elettra‐Sincrotrone S.C.p.A Trieste 34149 Italy

4. TASC Laboratory CNR‐IOM Trieste 34149 Italy

5. Photon Science Division Paul Scherrer Institute (PSI) Villigen 5232 Switzerland

6. Department of Chemical Sciences University of Padova Padova 35131 Italy

7. Institute of Condensed Matter Chemistry and Technologies for Energy (ICMATE) CNR c/o Department of Chemical Sciences University of Padova Padova 35131 Italy

8. Faculty of Physics and Center for Nanointegration Duisburg‐Essen (CENIDE) University of Duisburg‐Essen 47048 Duisburg Germany

9. Department of Physics, Astronomy University of California Davis Davis CA 95616 USA

Abstract

AbstractPorphyrins are promising multifunctional units particularly interesting for the realization of molecular nanodevices. Their structural variety allows to create precursors suitable for the on‐surface polymerization of porphyrin blocks. The corresponding increased stability and improved transport properties of the formed polymerized molecular nanostructures make them practically worthwhile. For the case of 2D porphyrin materials, the effect of polymerization on the magnetic properties of transition metal ions has not been reported yet. Therefore, details on the properties of an extended covalent nickel tetraphenylporphyrin network formed via Ullmann coupling on the Cu(111) surface are reported. By using photoelectron and absorption spectroscopies together with density functional theory calculations, it is systematically evolving how the functional properties of the Ni centers are changed within a polymerized molecular structure in comparison to single‐molecule nickel tetraphenylporphyrin derivatives that build the 2D molecular network. A model that explains the differences in the electronic and magnetic properties observed for the Ni centers in both structures based on the additional rigidity characteristic of the molecular layer after polymerization is drawn.

Publisher

Wiley

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