Published September 20, 2021 | Version v1
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On-surface synthesis and characterization of super-nonazethrene

  • 1. Empa - Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600 Dübendorf, Switzerland
  • 2. Present Address: IBM Research – Zurich, 8803 Rüschlikon, Switzerland
  • 3. Faculty of Chemistry and Food Chemistry, and Center for Advancing Electronics Dresden, Technical University of Dresden, 01069 Dresden, Germany
  • 4. Department of Chemistry, Biochemistry and Pharmaceutical Sciences, University of Bern, 3012 Bern, Switzerland
  • 5. Department of Synthetic Materials and Functional Devices, Max Planck Institute of Microstructure Physics, 06120 Halle, Germany

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Description

This record contains data to support the findings discussed in our recent work on the synthesis and characterization of super-nonazethrene. Beginning with the early work of Clar et al. in 1955, zethrenes and their laterally-extended homologues, super-zethrenes, have been intensively studied in the solution phase, and are widely investigated as optical and charge transport materials. Super-zethrenes are also considered to exhibit an open-shell ground state. Zethrenes may thus serve as model compounds to investigate nanoscale π-magnetism. However, their synthesis is extremely challenging due to their high reactivity. In the work we report here a combined in-solution and on-surface synthesis of the hitherto largest zethrene homologue – super-nonazethrene – on Au(111). Using single-molecule scanning tunneling microscopy and spectroscopy, we show that super-nonazethrene exhibits an open-shell singlet ground state featuring a large spin polarization-driven electronic gap of 1 eV. We obtain real-space maps of the frontier molecular orbitals, and find that they correspond to singly occupied molecular orbitals. In consistence with the emergence of an open-shell ground state, high-resolution tunneling spectroscopy reveals inelastic singlet-triplet spin excitations in super-nonazethrene, characterized by a strong intramolecular magnetic exchange coupling of 51 meV. Further insights are gained by mean-field and many-body perturbation theory calculations. Given the paucity of zethrene chemistry on surfaces, our results therefore provide unprecedented access to large open-shell zethrene compounds amenable to scanning probe measurements, with potential application in molecular spintronics.

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References

Journal reference (Manuscript where the results are presented)
E. Turco, S. Mishra, J. Melidonie, K. Eimre, S. Obermann, C. A. Pignedoli, R. Fasel, X. Feng, P. Ruffieux J. Phys. Chem. Lett. 12, 34, 8314–8319 (2021), doi: 10.1021/acs.jpclett.1c02381