Journal
NATURE COMMUNICATIONS
Volume 9, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-018-04896-0
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Funding
- US National Science Foundation [CHE1633870]
- U.S. Department of Navy HBCU/MI program
- Deutsche Forschungsgemeinschaft and Max-Planck-Gesellschaft
- Shull Wollan Center Graduate Research Fellowship
- American Chemical Society Petroleum Research Fund
- Laboratory Directed Research and Development at Oak Ridge National Laboratory
- NSF [NSF-DMR-0084173]
- State of Florida
- University of Tennessee's Open Publishing Support Fund
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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 Co-II(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.
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