title: Desolvation-Driven 100-Fold Slow-down of Tunneling Relaxation Rate in Co(II)-Dy(III) Single-Molecule Magnets through a Single-Crystal-to-Single-Crystal Process.
abstract: Single-molecule magnets (SMMs) are regarded as a class of promising materials for spintronic and ultrahigh-density storage devices. Tuning the magnetic dynamics of single-molecule magnets is a crucial challenge for chemists. Lanthanide ions are not only highly magnetically anisotropic but also highly sensitive to the changes in the coordination environments. We developed a feasible approach to understand parts of the magneto-structure correlations and propose to regulate the relaxation behaviors via rational design. A series of Co(II)-Dy(III)-Co(II) complexes were obtained using in situ synthesis; in this system of complexes, the relaxation dynamics can be greatly improved, accompanied with desolvation, via single-crystal to single-crystal transformation. The effective energy barrier can be increased from 293 cm(-1) (422 K) to 416 cm(-1) (600 K), and the tunneling relaxation time can be grown from 8.5 × 10(-4) s to 7.4 × 10(-2) s. These remarkable improvements are due to the change in the coordination environments of Dy(III) and Co(II). Ab initio calculations were performed to better understand the magnetic dynamics.
authors.affiliation: Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, 510275 Guangzhou, Guangdong, P. R. China.
authors.forename: Jun-Liang
authors.initials: JL
authors.lastname: Liu
authors.affiliation: Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, 510275 Guangzhou, Guangdong, P. R. China.
authors.forename: Jie-Yi
authors.initials: JY
authors.lastname: Wu
authors.affiliation: Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, 510275 Guangzhou, Guangdong, P. R. China.
authors.forename: Guo-Zhang
authors.initials: GZ
authors.lastname: Huang
authors.affiliation: Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, 510275 Guangzhou, Guangdong, P. R. China.
authors.forename: Yan-Cong
authors.initials: YC
authors.lastname: Chen
authors.affiliation: Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, 510275 Guangzhou, Guangdong, P. R. China.
authors.forename: Jian-Hua
authors.initials: JH
authors.lastname: Jia
authors.affiliation: Theory of Nanomaterials Group and INPAC - Institute of Nanoscale Physics and Chemistry, Katholieke Universiteit Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium.
authors.forename: Liviu
authors.initials: L
authors.lastname: Ungur
authors.affiliation: Theory of Nanomaterials Group and INPAC - Institute of Nanoscale Physics and Chemistry, Katholieke Universiteit Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium.
authors.forename: Liviu F
authors.initials: LF
authors.lastname: Chibotaru
authors.affiliation: Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, 510275 Guangzhou, Guangdong, P. R. China.
authors.forename: Xiao-Ming
authors.initials: XM
authors.lastname: Chen
authors.affiliation: Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, 510275 Guangzhou, Guangdong, P. R. China.
authors.forename: Ming-Liang
authors.initials: ML
authors.lastname: Tong