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

• DOI: 10.1038/s41467-018-04896-0
• Publication Date: 2018-06-27T08:21:22Z
• Authors: Duncan H. Moseley; Shelby E. Stavretis; Komalavalli Thiru...; 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
• Keywords: Science; Q; 01 natural sciences; Article; 0104 chemical sciences

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 g phonons CoII(acac)2(H2O)2 (acac = acetylacetonate) deuterated analogs with zero-field-split, excited magnetic/spin levels (Kramers doublet (KD)) S 3/2 electronic ground state. The are observed as avoided crossings magnetic-field-dependent Raman spectra constants 1-2 cm-1. Far-IR reveal magnetic-dipole-allowed, inter-KD transition, shifting to higher energy increasing field. Density functional theory calculations used rationalize energies symmetries phonons. A vibronic model, supported by structure calculations, is proposed behavior coupled peaks. This work spectroscopically reveals quantitates spin-phonon typical transition metal complexes sheds light on origin entanglement.