Elia Turco^1*, Shantanu Mishra^1,2, Jason Melidonie³, Kristjan Eimre^1*, Sebastian Obermann³, Carlo A. Pignedoli¹, Roman Fasel^1,4*, Xinliang Feng^3,5, Pascal Ruffieux^1*

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

* Corresponding authors emails: elia.turco@empa.ch, kristjan.eimre@empa.ch, roman.fasel@empa.ch, pascal.ruffieux@empa.ch

DOI10.24435/materialscloud:j7-51 [version v1]

Publication date: Sep 20, 2021

How to cite this record

Elia Turco, Shantanu Mishra, Jason Melidonie, Kristjan Eimre, Sebastian Obermann, Carlo A. Pignedoli, Roman Fasel, Xinliang Feng, Pascal Ruffieux, On-surface synthesis and characterization of super-nonazethrene, Materials Cloud Archive 2021.151 (2021), doi: 10.24435/materialscloud:j7-51.

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.

Materials Cloud sections using this data

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ReadMe.yaml MD5md5:62837b9d84c3b77a0bc6c650355ee677	20.2 KiB	ReadMe file in yaml format listing the content of the record
data.tgz MD5md5:c5242c13c74419d3ed1ec4928a13be9a	19.2 MiB	Zipped tar file containing all files of the record
snz_ads-geometries.aiida MD5md5:14502e34686ed0a7d7aa97b74131945b Open this AiiDA archive on renkulab.io (https://renkulab.io/)	2.7 MiB	AiiDA archive containing the files for the geometry optimizations
snz_gw.aiida MD5md5:c63fc222857e62bc06bd4cdbc1d957e8 Open this AiiDA archive on renkulab.io (https://renkulab.io/)	1.0 MiB	AiiDA archive containing the files for the GW calculations

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External references

Keywords

MARVEL/DD3 nanographene ab initio simulations scanning tunneling microscopy zethrenes H2020 ERC Graphene flagship