Discovery of a Dysprosium Metallocene Single-Molecule Magnet with Two High-Temperature Orbach Processes.pdf (2.37 MB)
Discovery of a dysprosium metallocene single-molecule magnet with two high-temperature Orbach processes
journal contribution
posted on 2023-06-10, 04:54 authored by Fu-Shen Guo, Mian He, Guo-Zhang Huang, Sean R Giblin, David Billington, Frank W Heinemann, Ming-Liang Tong, Akseli Mansikkamäki, Richard LayfieldRichard LayfieldMagnetic bistability in single-molecule magnets (SMMs) is a potential basis for new types of nanoscale information storage material. The standard model for thermally activated relaxation of the magnetization in SMMs is based on the occurrence of a single Orbach process. Here, we show that incorporating a phosphorus atom into the framework of the dysprosium metallocene [(CpiPr5)Dy(CpPEt4)]+[B(C6F5)4]- (CpiPr5 is penta-isopropylcyclopentadienyl, CpPEt4 is tetraethylphospholyl) leads to the occurrence of two distinct high-temperature Orbach processes, with energy barriers of 1410(10) and 747(7) cm-1, respectively. These barriers provide experimental evidence for two different spin-phonon coupling regimes, which we explain with the aid of ab initio calculations. The strong and highly axial crystal field in this SMM also allows magnetic hysteresis to be observed up to 70 K, using a scan rate of 25 Oe s-1. In characterizing this SMM, we show that a conventional Debye model and consideration of rotational contributions to the spin-phonon interaction are insufficient to explain the observed phenomena.
History
Publication status
- Published
File Version
- Published version
Journal
Inorganic ChemistryISSN
0020-1669Publisher
American Chemical Society (ACS)External DOI
Issue
16Volume
61Page range
6017-6025Event location
United StatesDepartment affiliated with
- Chemistry Publications
Full text available
- Yes
Peer reviewed?
- Yes
Legacy Posted Date
2022-09-29First Open Access (FOA) Date
2022-09-29First Compliant Deposit (FCD) Date
2022-09-28Usage metrics
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