Easy-plane to easy-axis anisotropy switching in a Co(ii) single-ion magnet triggered by the diamagnetic lattice

Joscha Nehrkorn, Igor A. Valuev, Mikhail A. Kiskin, Artem S. Bogomyakov, Elizaveta A. Suturina, Alena M. Sheveleva, Victor I. Ovcharenko, Karsten Holldack, Carmen Herrmann, Matvey V. Fedin, Alexander Schnegg, Sergey L. Veber

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Abstract

Single-ion magnets (SIMs) with large magnetic anisotropy are promising candidates for realization of single-molecule based magnetic memory and qubits. Creation of materials with magnetically uncoupled spatially separated SIMs requires dilution in a diamagnetic matrix. Herein, we report that progressive dilution of paramagnetic Co(ii) by diamagnetic Zn(ii) in the SIM ([CoxZn(1−x)(piv)2(2-NH2-Py)2], x = 1 ÷ 0) beyond a threshold of 50% reveals an abrupt structural change, where the distorted tetrahedral Zn coordination structure is superimposed on the remaining Co ions, which were initially in a distorted octahedral environment. Dilution-induced structure modification switches the magnetic anisotropy from easy-plane (D = 36.7 cm−1) to easy-axis type (D = −23.9 cm−1), accompanied by a fivefold increase of the magnetic relaxation time at 2 K. Changes of the static and dynamic magnetic properties are monitored by electron paramagnetic resonance spectroscopy and AC susceptibility measurements. Complementary quantum chemical ab initio calculations quantify the influence of structural changes on the electronic structure and the magnetic anisotropy. Thus, magnetic dilution hits two goals at once, the creation of isolated magnetic centres and an improvement of their SIM properties.
Original languageEnglish
Pages (from-to)9446-9452
Number of pages7
JournalJournal of Materials Chemistry C
Volume9
Issue number30
Early online date8 Jun 2021
DOIs
Publication statusPublished - 14 Aug 2021

Bibliographical note

Publisher Copyright:
© The Royal Society of Chemistry 2021.

Funding

Financial support by the Russian Science Foundation through grant no. 17-13-01412 (X-band EPR measurements) and by the Deutsche Forschungsgemeinschaft (DFG) through priority program SPP 1601 and a Research Fellowship to J. N. (grant no. NE 2064/1-1 FOR) is thankfully acknowledged. J. N., I. A. V., and S. L. V. thankfully acknowledge the financial support from HZB. J. N. and A. S. acknowledge funding through the Max Planck Society. M. A. K. is grateful for financial support from the State Assignment on Fundamental Research of the Kurna-kov Institute of General and Inorganic Chemistry of RAS (IGIC RAS) and thank the User Facilities Centers of IGIC RAS for the facility to do X-ray, IR and elemental analysis measurements. V. I. O. and A. S. B. acknowledge Russian Science Foundation (project 18-13-00380) for support of the SQUID measurements. E. A. S. acknowledges Russian Science Foundation (project 16-13-10155) and Supercomputer center of the Novosibirsk State University for support of the computational part of this work. J. N. and C. H. thank the University of Hamburg High Performance Computing Centre (RRZ) for computational resources. We thank Dirk Ponwitz (HZB) for technical support, Dr Ekaterina Zorina-Tikhonova (IGIC RAS) for IR data interpretation and Dr Alexander Baranchikov (IGIC RAS) for EDX analysis. Financial support by the Russian Science Foundation through grant no. 17-13-01412 (X-band EPR measurements) and by the Deutsche Forschungsgemeinschaft (DFG) through priority program SPP 1601 and a Research Fellowship to J. N. (grant no. NE 2064/1-1 FOR) is thankfully acknowledged. J. N., I. A. V., and S. L. V. thankfully acknowledge the financial support from HZB. J. N. and A. S. acknowledge funding through the Max Planck Society. M. A. K. is grateful for financial support from the State Assignment on Fundamental Research of the Kurnakov Institute of General and Inorganic Chemistry of RAS (IGIC RAS) and thank the User Facilities Centers of IGIC RAS for the facility to do X-ray, IR and elemental analysis measurements. V. I. O. and A. S. B. acknowledge Russian Science Foundation (project 18-13-00380) for support of the SQUID measurements. E. A. S. acknowledges Russian Science Foundation (project 16-13-10155) and Supercomputer center of the Novosibirsk State University for support of the computational part of this work. J. N. and C. H. thank the University of Hamburg High Performance Computing Centre (RRZ) for computational resources. We thank Dirk Ponwitz (HZB) for technical support, Dr Ekaterina Zorina-Tikhonova (IGIC RAS) for IR data interpretation and Dr Alexander Baranchikov (IGIC RAS) for EDX analysis.

FundersFunder number
Kurna-kov Institute of General and Inorganic Chemistry of RAS16-13-10155, 18-13-00380
Kurnakov Institute of General and Inorganic Chemistry of RAS
Novosibirsk State University
Deutsche ForschungsgemeinschaftSPP 1601, NE 2064/1-1 FOR
Max Planck Society
Universität Hamburg
Russian Science Foundation17-13-01412

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