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Steering large magnetic exchange coupling in nanographenes near the closed-shell to open-shell transition

Kalyan Biswas1, Diego Soler2, Shantanu Mishra3,4, Qiang Chen5, Xuelin Yao5, Ana Sánchez-Grande1, Kristjan Eimre3, Pingo Mutombo2, Cristina Martín-Fuentes1, Koen Lauwaet1, José M. Gallego6, Pascal Ruffieux3, Carlo A. Pignedoli3*, Klaus Müllen5, Rodolfo Miranda1,7, José I. Urgel1, Akimitsu Narita5, Roman Fasel3,8, Pavel Jelínek2,9, David Écija1

1 IMDEA Nanoscience, C/ Faraday 9, Campus de Cantoblanco, 28049 Madrid, Spain

2 Institute of Physics of the Czech Academy of Science, 162 00 Praha, Czech Republic

3 Empa, Swiss Federal Laboratories for Materials Science and Technology, 8600 Dübendorf, Switzerland

4 IBM Research─Zurich, Säumerstrasse 4, 8803 Rüschlikon, Switzerland

5 Max Planck Institute for Polymer Research, 55128 Mainz, Germany

6 Instituto de Ciencia de Materiales de Madrid, CSIC, Cantoblanco, 28049 Madrid, Spain

7 Departamento de Física de la Materia Condensada, Universidad Autónoma de Madrid, 28049 Madrid, Spain

8 Department of Chemistry, Biochemistry and Pharmaceutical Sciences, University of Bern, 3012 Bern, Switzerland

9 Regional Centre of Advanced Technologies and Materials, Palacký University Olomouc, CZ-771 46 Olomouc, Czech Republic

* Corresponding authors emails: carlo.pignedoli@empa.ch
DOI10.24435/materialscloud:1j-43 [version v1]

Publication date: Oct 17, 2023

How to cite this record

Kalyan Biswas, Diego Soler, Shantanu Mishra, Qiang Chen, Xuelin Yao, Ana Sánchez-Grande, Kristjan Eimre, Pingo Mutombo, Cristina Martín-Fuentes, Koen Lauwaet, José M. Gallego, Pascal Ruffieux, Carlo A. Pignedoli, Klaus Müllen, Rodolfo Miranda, José I. Urgel, Akimitsu Narita, Roman Fasel, Pavel Jelínek, David Écija, Steering large magnetic exchange coupling in nanographenes near the closed-shell to open-shell transition, Materials Cloud Archive 2023.159 (2023), https://doi.org/10.24435/materialscloud:1j-43


The design of open-shell carbon-based nanomaterials is at the vanguard of materials science, steered by their beneficial magnetic properties like weaker spin–orbit coupling than that of transition metal atoms and larger spin delocalization, which are of potential relevance for future spintronics and quantum technologies. A key parameter in magnetic materials is the magnetic exchange coupling (MEC) between unpaired spins, which should be large enough to allow device operation at practical temperatures. In a recent work, we theoretically and experimentally explore three distinct families of nanographenes (NGs) (A, B, and C) featuring majority zigzag peripheries. Through many-body calculations, we identify a transition from a closed-shell ground state to an open-shell ground state upon an increase of the molecular size. Our predictions indicate that the largest MEC for open-shell NGs occurs in proximity to the transition between closed-shell and open-shell states. Such predictions are corroborated by the on-surface syntheses and structural, electronic, and magnetic characterizations of three NGs (A[3,5], B[4,5], and C[4,3]), which are the smallest open-shell systems in their respective chemical families and are thus located the closest to the transition boundary. Notably, two of the NGs (B[4,5] and C[4,3]) feature record values of MEC (close to 200 meV) measured on the Au(111) surface. Our strategy for maximizing the MEC provides perspectives for designing carbon nanomaterials with robust magnetic ground states. This record contains the data for the simulations discussed in our manuscript.

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External references

Journal reference (Manuscript where the results are discussed)
K. Biswas, D. Soler, S. Mishra, Q. Chen, X. Yao, A. Sánchez-Grande, K. Eimre, P. Mutombo, C. Martín-Fuentes, K. Lauwaet, J. M. Gallego, P. Ruffieux, C. A. Pignedoli, K. Müllen, R. Miranda, J. I. Urgel, A. Narita, R. Fasel, P. Jelínek, D. Écija, J. Am. Chem. Soc. 145, 5, 2968–2974 (2023) doi:10.1021/jacs.2c11431


nanographenes open-shell spectroscopy DFT MARVEL/P4 SNSF

Version history:

2023.159 (version v1) [This version] Oct 17, 2023 DOI10.24435/materialscloud:1j-43