Can Non-Kramers Tm(III) Mononuclear Molecules be Single-Molecule Magnets (SMMs)?

Chemistry : a European Journal
Bing-Wu WangSong Gao

Abstract

In recent years, plentiful lanthanide-based (Tb(III) , Dy(III) , and Er(III) ) single-molecule magnets (SMMs) were studied, while examples of other lanthanides, for example, Tm(III) are still unknown. Herein, for the first time, we show that by rationally manipulating the coordination sphere, two thulium compounds, 1[(Tp)Tm(COT)] and 2[(Tp*)Tm(COT)] (Tp=hydrotris(1-pyrazolyl)borate; COT=cyclooctatetraenide; Tp*=hydrotris(3,5-dimethyl-1-pyrazolyl)borate), can adopt the structure of non-Kramers SMMs and exhibit their behaviors. Dynamic magnetic studies indicated that both compounds showed slow magnetic relaxation under dc field and a relatively high effective energy barrier (111 K for 1, 46 K for 2). Magnetic diluted 1 a[(Tp)Tm0.05 Y0.95 (COT)] and 2 a[(Tp*)Tm0.05 Y0.95 (COT)] even exhibited magnetic relaxation under zero dc field. Relativistic ab initio calculations combined with single-crystal angular-resolved magnetometry measurements revealed the strong easy axis anisotropy and nearly degenerated ground doublet states. The comparison of 1 and 2 highlights the importance of local symmetry for obtaining Tm SMMs.

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Citations

Oct 22, 2016·Accounts of Chemical Research·Yin-Shan MengSong Gao
May 17, 2017·Angewandte Chemie·Janek RauschFrank T Edelmann
Mar 23, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·A AmjadL Sorace
Feb 1, 2018·Chemistry : a European Journal·Min Feng, Ming-Liang Tong
Aug 29, 2018·Chemical Communications : Chem Comm·Volker LorenzFrank T Edelmann
Jan 9, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Jin WangMing-Liang Tong
Oct 1, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·A ArauzoE Bartolomé
Oct 16, 2018·Chemical Science·Shi-Ming ChenSong Gao
Jan 19, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Mei-Xing XuSong Gao
May 14, 2021·Nature Communications·Sheng-Qun SuOsamu Sato
Jul 2, 2021·Chemistry : a European Journal·Maxime TricoireGrégory Nocton
May 7, 2019·Chemical Reviews·Fu-Sheng GuoRichard A Layfield

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