Kalyan Biswas¹, Diego Soler², Shantanu Mishra^3,4, Qiang Chen⁵, Xuelin Yao⁵, Ana Sánchez-Grande¹, Kristjan Eimre³, Pingo Mutombo², Cristina Martín-Fuentes¹, Koen Lauwaet¹, José M. Gallego⁶, Pascal Ruffieux³, Carlo A. Pignedoli^3*, Klaus Müllen⁵, Rodolfo Miranda^1,7, José I. Urgel¹, Akimitsu Narita⁵, Roman Fasel^3,8, Pavel Jelínek^2,9, 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

Description

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.

Materials Cloud sections using this data

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gw.aiida MD5md5:cfb8f05dad3c05727fae0c9a9fa91555 Open this AiiDA archive on renkulab.io (https://renkulab.io/)	2.0 MiB	AiiDA archive file containing aiida nodes to reproduce calculations that support the results published
gaussian.aiida MD5md5:07b18f015b783fe1571ac20c3dfaad07 Open this AiiDA archive on renkulab.io (https://renkulab.io/)	793.9 MiB	AiiDA archive file containing aiida nodes to reproduce calculations that support the results published
ReadMe.txt MD5md5:4c607ac96f37a555cc085264d2bd533b	411 Bytes	ReadMe file recalling the manuscript to which data belong

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External references

Keywords

nanographenes open-shell spectroscopy DFT MARVEL/P4 SNSF