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Field-induced oscillation of magnetization blocking barrier in a holmium metallacrown single-molecule magnet

Authors :
Gheorghe Taran
Guo-Zhang Huang
Jie-Yu Zheng
Si-Guo Wu
Liviu F. Chibotaru
Jin Wang
Wolfgang Wernsdorfer
Veacheslav Vieru
Le Tuan Anh Ho
Yan-Cong Chen
Xiao-Ming Chen
Ming-Liang Tong
Ze-Yu Ruan
Jun-Liang Liu
RS: FSE MSP
Maastricht Science Programme
Source :
Chem, 7(4), 982-992. Elsevier Inc.
Publication Year :
2021
Publisher :
Elsevier BV, 2021.

Abstract

Summary Single-molecule magnets (SMMs) exhibit magnetization blocking in the presence of strong magnetic anisotropy. By employing molecular engineering, the blocking barrier can be significantly modified, remaining independent from other external factors, such as magnetic field. Taking advantage of hyperfine coupling of electronic and nuclear spins further highlights their unique functionality. However, a poor understanding of relaxation mechanisms limits the exploitation of nuclear-spin molecular qubits. Here, we report the first observation of field-dependent oscillation of the magnetization blocking barrier in a holmium metallacrown magnet driven by the switch of relaxation mechanisms involving hyperfine interaction. First-principles calculations reveal an activated temperature dependence of magnetic relaxation, dominated either by incoherent quantum tunneling of magnetization at anti-crossing points or by Orbach-like processes at crossing points. This mechanism demonstrates that these relaxation barriers can be consecutively switched by increasing the external field, which paves a way for manipulating magnetization dynamics of SMMs using hyperfine interaction.

Details

ISSN :
24519294
Volume :
7
Database :
OpenAIRE
Journal :
Chem
Accession number :
edsair.doi.dedup.....40e9cb014c4dd260a1e2f7df34165aca