Spin–phonon couplings in transition metal complexes with slow magnetic relaxation View Full Text


Ontology type: schema:ScholarlyArticle      Open Access: True


Article Info

DATE

2018-12

AUTHORS

Duncan H. Moseley, Shelby E. Stavretis, Komalavalli Thirunavukkuarasu, Mykhaylo Ozerov, Yongqiang Cheng, Luke L. Daemen, Jonathan Ludwig, Zhengguang Lu, Dmitry Smirnov, Craig M. Brown, Anup Pandey, A. J. Ramirez-Cuesta, Adam C. Lamb, Mihail Atanasov, Eckhard Bill, Frank Neese, Zi-Ling Xue

ABSTRACT

Spin-phonon coupling plays an important role in single-molecule magnets and molecular qubits. However, there have been few detailed studies of its nature. Here, we show for the first time distinct couplings of g phonons of CoII(acac)2(H2O)2 (acac = acetylacetonate) and its deuterated analogs with zero-field-split, excited magnetic/spin levels (Kramers doublet (KD)) of the S = 3/2 electronic ground state. The couplings are observed as avoided crossings in magnetic-field-dependent Raman spectra with coupling constants of 1-2 cm-1. Far-IR spectra reveal the magnetic-dipole-allowed, inter-KD transition, shifting to higher energy with increasing field. Density functional theory calculations are used to rationalize energies and symmetries of the phonons. A vibronic coupling model, supported by electronic structure calculations, is proposed to rationalize the behavior of the coupled Raman peaks. This work spectroscopically reveals and quantitates the spin-phonon couplings in typical transition metal complexes and sheds light on the origin of the spin-phonon entanglement. More... »

PAGES

2572

Identifiers

URI

http://scigraph.springernature.com/pub.10.1038/s41467-018-04896-0

DOI

http://dx.doi.org/10.1038/s41467-018-04896-0

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1105180684

PUBMED

https://www.ncbi.nlm.nih.gov/pubmed/29968702


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