Discovery of a Dysprosium Metallocene Single-Molecule Magnet with Two High-Temperature Orbach Processes

Guo FS, He M, Huang GZ, Giblin SR, Billington D, Heinemann FW, Tong ML, Mansikkamäki A, Layfield RA (2022)

Publication Type: Journal article

Publication year: 2022

Journal

Inorganic Chemistry American Chemical Society

Book Volume: 61

Pages Range: 6017-6025

Journal Issue: 16

DOI: 10.1021/acs.inorgchem.1c03980

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.

Authors with CRIS profile

Frank Wilhelm Heinemann Lehrstuhl für Anorganische und Allgemeine Chemie

Involved external institutions

Cardiff University GB United Kingdom (GB) University of Sussex GB United Kingdom (GB) Sun Yat-Sen University CN China (CN) Oulun Yliopisto / University of Oulo FI Finland (FI)

How to cite

APA:

Guo, F.S., He, M., Huang, G.Z., Giblin, S.R., Billington, D., Heinemann, F.W.,... Layfield, R.A. (2022). Discovery of a Dysprosium Metallocene Single-Molecule Magnet with Two High-Temperature Orbach Processes. Inorganic Chemistry, 61(16), 6017-6025. https://dx.doi.org/10.1021/acs.inorgchem.1c03980

MLA:

Guo, Fu Sheng, et al. "Discovery of a Dysprosium Metallocene Single-Molecule Magnet with Two High-Temperature Orbach Processes." Inorganic Chemistry 61.16 (2022): 6017-6025.

BibTeX: Download