Issue 41, 2020

Simultaneous manifestation of metallic conductivity and single-molecule magnetism in a layered molecule-based compound

Abstract

Single-molecule magnets (SMMs) show superparamagnetic behaviour below blocking temperature at the molecular scale, so they exhibit large magnetic density compared to the conventional magnets. Combining SMMs and molecular conductors in one compound will bring about new physical phenomena, however, the synergetic effects between them still remain unexplored. Here we present a layered molecule-based compound, β′′-(BEDO-TTF)4 [Co(pdms)2]·3H2O (BO4), (BEDO-TTF (BO) and H2pdms are bis(ethylenedioxy)tetrathiafulvalene and 1,2-bis(methanesulfonamido)benzene, respectively), which was synthesized by using an electrochemical approach and studied by using crystal X-ray diffraction. This compound simultaneously exhibited metallic conductivity and SMM behaviour up to 11 K for the first time. The highest electrical conductivity was 400–650 S cm−1 at 6.5 K, which is the highest among those reported so far for conducting SMM materials. Furthermore, antiferromagnetic ordering occurred below 6.5 K, along with a decrease in conductivity, and the angle-independent negative magnetoresistance suggested an effective electron correlation between the conducting BO and Co(pdms)2 SMM layers (d–π interactions). The strong magnetic anisotropy and two-dimensional conducting plane play key roles in the low-temperature antiferromagnetic semiconducting state. BO4 is the first compound exhibiting antiferromagnetic ordering among SMMs mediated by π-electrons, demonstrating the synergetic effects between SMMs and molecular conductors.

Graphical abstract: Simultaneous manifestation of metallic conductivity and single-molecule magnetism in a layered molecule-based compound

Supplementary files

Article information

Article type
Edge Article
Submitted
24 Jūl. 2020
Accepted
25 Aug. 2020
First published
01 Sept. 2020
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2020,11, 11154-11161

Simultaneous manifestation of metallic conductivity and single-molecule magnetism in a layered molecule-based compound

Y. Shen, H. Ito, H. Zhang, H. Yamochi, S. Katagiri, S. K. Yoshina, A. Otsuka, M. Ishikawa, G. Cosquer, K. Uchida, C. Herrmann, T. Yoshida, B. K. Breedlove and M. Yamashita, Chem. Sci., 2020, 11, 11154 DOI: 10.1039/D0SC04040A

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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