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Adv Sci (Weinh) ; 6(20): 1901352, 2019 Oct 16.
Artigo em Inglês | MEDLINE | ID: mdl-31637168


A new class of single-molecule magnets (SMMs) based on Dy-oxide clusterfullerenes is synthesized. Three isomers of Dy2O@C82 with C s(6), C 3v(8), and C 2v(9) cage symmetries are characterized by single-crystal X-ray diffraction, which shows that the endohedral Dy-(µ2-O)-Dy cluster has bent shape with very short Dy-O bonds. Dy2O@C82 isomers show SMM behavior with broad magnetic hysteresis, but the temperature and magnetization relaxation depend strongly on the fullerene cage. The short Dy-O distances and the large negative charge of the oxide ion in Dy2O@C82 result in the very strong magnetic anisotropy of Dy ions. Their magnetic moments are aligned along the Dy-O bonds and are antiferromagnetically (AFM) coupled. At low temperatures, relaxation of magnetization in Dy2O@C82 proceeds via the ferromagnetically (FM)-coupled excited state, giving Arrhenius behavior with the effective barriers equal to the AFM-FM energy difference. The AFM-FM energy differences of 5.4-12.9 cm-1 in Dy2O@C82 are considerably larger than in SMMs with {Dy2O2} bridges, and the Dy∙∙∙Dy exchange coupling in Dy2O@C82 is the strongest among all dinuclear Dy SMMs with diamagnetic bridges. Dy-oxide clusterfullerenes provide a playground for the further tuning of molecular magnetism via variation of the size and shape of the fullerene cage.

J Phys Condens Matter ; 31(42): 425401, 2019 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-31226695


For solid-state phase transitions, the alterations of electronic structure driven by the band Jahn-Teller effect would play an essential role in the structural phase transitions and in switching the resistivity or magnetization states for potential applications. However, this evolution of the electronic structure and electronic transport during the martensitic transformations (MT) still lacks comprehensive investigations, especially in magnetic martensitic materials studied in recent years. In this work, we report a study on the electronic behaviors during the MT in a kind of all-d-metal Ni50-x Fe x Mn35Ti15 Heusler magnetic shape memory alloys, by combining x-ray diffraction, calorimetric, magnetic, transport measurements and calculations. Based on the magnetic MTs, the system shows large magnetocaloric effect and magnetoresistance. In the whole temperature range, the system is dominated by hole carriers in both parent and martensite phases. A sharp increase in carrier concentration is observed across the transformations. Meanwhile, the mobility of holes is depressed due to the lattice distortion. A picture of the characteristics of MTs has been proposed for general understanding and clues of the potential spintronic applications based on the magnetostructural phase transitions.