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


Ontology type: schema:ScholarlyArticle      Open Access: True


Article Info

DATE

2018-07-03

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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