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Exchange Interactions and Intermolecular Hybridization in a Spin-1/2 Nanographene Dimer


Krane, Nils; Turco, Elia; Bernhardt, Annika; Jacob, David; Gandus, Guido; Passerone, Daniele; Luisier, Mathieu; Juricek, Michal; Fasel, Roman; Fernández-Rossier, Joaquin; Ruffieux, Pascal (2023). Exchange Interactions and Intermolecular Hybridization in a Spin-1/2 Nanographene Dimer. Nano letters, 23(20):9353-9359.

Abstract

Phenalenyl is a radical nanographene with a triangular shape hosting an unpaired electron with spin S = 1/2. The open-shell nature of the phenalenyl is expected to be retained in covalently bonded networks. As a first step, we report synthesis of the phenalenyl dimer by combining in-solution synthesis and on-surface activation and its characterization on Au(111) and on a NaCl decoupling layer by means of inelastic electron tunneling spectroscopy (IETS). IETS shows inelastic steps that are identified as singlet–triplet excitation arising from interphenalenyl exchange. Spin excitation energies with and without the NaCl decoupling layer are 48 and 41 meV, respectively, indicating significant renormalization due to exchange with Au(111) electrons. Furthermore, third-neighbor hopping-induced interphenalenyl hybridization is fundamental to explaining the position-dependent bias asymmetry of the inelastic steps and activation of kinetic interphenalenyl exchange. Our results pave the way for bottom-up synthesis of S = 1/2 spin-lattices with large exchange interactions.

Abstract

Phenalenyl is a radical nanographene with a triangular shape hosting an unpaired electron with spin S = 1/2. The open-shell nature of the phenalenyl is expected to be retained in covalently bonded networks. As a first step, we report synthesis of the phenalenyl dimer by combining in-solution synthesis and on-surface activation and its characterization on Au(111) and on a NaCl decoupling layer by means of inelastic electron tunneling spectroscopy (IETS). IETS shows inelastic steps that are identified as singlet–triplet excitation arising from interphenalenyl exchange. Spin excitation energies with and without the NaCl decoupling layer are 48 and 41 meV, respectively, indicating significant renormalization due to exchange with Au(111) electrons. Furthermore, third-neighbor hopping-induced interphenalenyl hybridization is fundamental to explaining the position-dependent bias asymmetry of the inelastic steps and activation of kinetic interphenalenyl exchange. Our results pave the way for bottom-up synthesis of S = 1/2 spin-lattices with large exchange interactions.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > Bioengineering
Physical Sciences > General Chemistry
Physical Sciences > General Materials Science
Physical Sciences > Condensed Matter Physics
Physical Sciences > Mechanical Engineering
Uncontrolled Keywords:Mechanical Engineering, Condensed Matter Physics, General Materials Science, General Chemistry, Bioengineering
Language:English
Date:25 October 2023
Deposited On:20 Feb 2024 08:37
Last Modified:30 Jun 2024 03:32
Publisher:American Chemical Society (ACS)
ISSN:1530-6984
OA Status:Closed
Publisher DOI:https://doi.org/10.1021/acs.nanolett.3c02633
PubMed ID:37819646
Project Information:
  • : FunderWerner Siemens-Stiftung
  • : Grant ID
  • : Project Title
  • : FunderH2020
  • : Grant ID716139
  • : Project TitleINSPIRAL - Spin-Delocalization with a Twist: Chiral Open-Shell Helices
  • : FunderSNSF
  • : Grant ID205602
  • : Project TitleNCCR MARVEL: Materials’ Revolution: Computational Design and Discovery of Novel Materials (phase III)
  • : FunderH2020
  • : Grant ID813036
  • : Project TitleULTIMATE - Bottom-Up generation of atomicalLy precise syntheTIc 2D MATerials for high performance in energy and Electronic applications â�� A multi-site innovative training action
  • : FunderSNSF
  • : Grant ID205987
  • : Project TitleBottom-up design and exploration of p-electron quantum magnetism
  • : FunderSNSF
  • : Grant ID182015
  • : Project TitleOn-surface synthesis of low-dimensional nanomaterials (OSSY)
  • : FunderSNSF
  • : Grant ID170534
  • : Project TitleControl of Spin Interactions in Helical Systems
  • : FunderSNSF
  • : Grant ID198900
  • : Project TitleA “Closer Look” at Open-Shell Nanographenes Through Bond and Space
  • : FunderSNSF
  • : Grant ID187617
  • : Project TitleExploring synthetic approaches to non-alternant ring topologies in graphene nanostructures