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Discovery of a dysprosium metallocene single-molecule magnet with two high-temperature orbach processes

DOI: 10.1021/acs.inorgchem.1c03980 DOI Help

Authors: Fu-Sheng Guo (University of Sussex) , Mian He (University of Sussex) , Guo-Zhang Huang (Sun-Yat Sen University) , Sean R. Giblin (Cardiff University) , David Billington (Cardiff University) , Frank W. Heinemann (Friedrich-Alexander-University Erlangen-Nürnberg) , Ming-Liang Tong (Sun-Yat Sen University) , Akseli Mansikkamäki (University of Oulu) , Richard A. Layfield (University of Sussex)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Inorganic Chemistry , VOL 69

State: Published (Approved)
Published: April 2022
Diamond Proposal Number(s): 29466

Open Access Open Access

Abstract: Magnetic 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.

Journal Keywords: Phonons; Magnetic properties; Hysteresis; Ligands; Energy

Diamond Keywords: Data Storage

Subject Areas: Chemistry, Physics, Information and Communication Technology

Instruments: I11-High Resolution Powder Diffraction

Added On: 18/04/2022 11:25


Discipline Tags:

Physics Physical Chemistry Components & Micro-systems Information & Communication Technologies Chemistry Magnetism Materials Science Inorganic Chemistry

Technical Tags:

Diffraction X-ray Powder Diffraction