Spectroscopic Studies of the Magnetic Excitation and Spin-Phonon Couplings in a Single-Molecule Magnet |
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Authors: | Shelby E. Stavretis Duncan H. Moseley Fan Fei Hui-Hui Cui Dr. Yongqiang Cheng Dr. Andrey A. Podlesnyak Dr. Xiaoping Wang Dr. Luke L. Daemen Dr. Christina M. Hoffmann Dr. Mykhaylo Ozerov Zhengguang Lu Prof. Komalavalli Thirunavukkuarasu Dr. Dmitry Smirnov Tieyan Chang Dr. Yu-Sheng Chen Dr. Anibal J. Ramirez-Cuesta Prof. Xue-Tai Chen Prof. Zi-Ling (Ben) Xue |
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Affiliation: | 1. Department of Chemistry, University of Tennessee, Knoxville, Tennessee, 37996 USA;2. State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023 China;3. Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee, 37831 USA;4. National High Magnetic Field Laboratory, Tallahassee, Florida, 32310 USA;5. Department of Physics, Florida A&M University, Tallahassee, Florida, 32307 USA;6. ChemMatCARS, Center for Advanced Radiation Sources, The University of Chicago, Argonne, Illinois, 60439 USA |
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Abstract: | Large separations between ground and excited magnetic states in single-molecule magnets (SMMs) are desirable to reduce the likelihood of spin reversal in the molecules. Spin-phonon coupling is a process leading to magnetic relaxation. Both the reversal and coupling, making SMMs lose magnetic moments, are undesirable. However, direct determination of large magnetic states separations (>45 cm−1) is challenging, and few detailed investigations of the spin-phonon coupling have been conducted. The magnetic separation in [Co(12-crown-4)2](I3)2(12-crown-4) ( 1 ) is determined and its spin-phonon coupling is probed by inelastic neutron scattering (INS) and far-IR spectroscopy. INS, using oriented single crystals, shows a magnetic transition at 49.4(1.0) cm−1. Far-IR reveals that the magnetic transition and nearby phonons are coupled, a rarely observed phenomenon, with spin-phonon coupling constants of 1.7–2.5 cm−1. The current work spectroscopically determines the ground–excited magnetic states separation in an SMM and quantifies its spin-phonon coupling, shedding light on the process causing magnetic relaxation. |
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Keywords: | cobalt magnetic transitions single-molecule magnets (SMMs) spin-phonon coupling vibrational spectroscopies |
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