Exploring the Vibrational Side of Spin-Phonon Coupling in Single-Molecule Magnets via Dy-161 Nuclear Resonance Vibrational Spectroscopy

摘要

Synchrotron-based nuclear resonance vibrational spectroscopy (NRVS) using the Mossbauer isotope Dy-161 has been employed for the first time to study the vibrational properties of a single-molecule magnet (SMM) incorporating Dy-III, namely [Dy(Cy3PO)(2)(H2O)(5)]Br-3.2 (Cy3PO).2 H2O .2 EtOH. The experimental partial phonon density of states (pDOS), which includes all vibrational modes involving a displacement of the Dy-III ion, was reproduced by means of simulations using density functional theory (DFT), enabling the assignment of all intramolecular vibrational modes. This study proves that Dy-161 NRVS is a powerful experimental tool with significant potential to help to clarify the role of phonons in SMMs.