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

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 and Zi-Ling Xue ()
Additional contact information
Duncan H. Moseley: University of Tennessee
Shelby E. Stavretis: University of Tennessee
Komalavalli Thirunavukkuarasu: Florida A&M University
Mykhaylo Ozerov: National High Magnetic Field Laboratory
Yongqiang Cheng: Oak Ridge National Laboratory
Luke L. Daemen: Oak Ridge National Laboratory
Jonathan Ludwig: National High Magnetic Field Laboratory
Zhengguang Lu: National High Magnetic Field Laboratory
Dmitry Smirnov: National High Magnetic Field Laboratory
Craig M. Brown: National Institute of Standards and Technology
Anup Pandey: Oak Ridge National Laboratory
A. J. Ramirez-Cuesta: Oak Ridge National Laboratory
Adam C. Lamb: University of Tennessee
Mihail Atanasov: Max Planck Institute for Coal Research
Eckhard Bill: Max Planck Institute for Chemical Energy Conversion
Frank Neese: Max Planck Institute for Coal Research
Zi-Ling Xue: University of Tennessee

Nature Communications, 2018, vol. 9, issue 1, 1-11

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-018-04896-0

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