Scherthan Lena, Pfleger Rouven F, Auerbach Hendrik, Hochdörffer Tim, Wolny Juliusz A, Bi Wenli, Zhao Jiyong, Hu Michael Y, Alp E Ercan, Anson Christopher E, Diller Rolf, Powell Annie K, Schünemann Volker
Department of Physics, Technische Universität Kaiserslautern, Erwin-Schrödinger-Str. 46, 67663, Kaiserslautern, Germany.
Institute of Inorganic Chemistry, Karlsruhe Institute of Technology, Engesserstr. 15, 76131, Karlsruhe, Germany.
Angew Chem Int Ed Engl. 2020 Jun 2;59(23):8818-8822. doi: 10.1002/anie.201914728. Epub 2020 Apr 24.
Synchrotron-based nuclear resonance vibrational spectroscopy (NRVS) using the Mössbauer isotope Dy has been employed for the first time to study the vibrational properties of a single-molecule magnet (SMM) incorporating Dy , namely [Dy(Cy PO) (H O) ]Br ⋅2 (Cy PO)⋅2 H O ⋅2 EtOH. The experimental partial phonon density of states (pDOS), which includes all vibrational modes involving a displacement of the Dy 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 NRVS is a powerful experimental tool with significant potential to help to clarify the role of phonons in SMMs.
首次采用基于同步加速器的核共振振动光谱（NRVS），利用穆斯堡尔同位素镝来研究包含镝的单分子磁体（SMM）的振动特性，即[Dy(CyPO) (H₂O) ]Br₂·2（CyPO）·2H₂O·2EtOH。通过使用密度泛函理论（DFT）进行模拟，再现了包括所有涉及镝离子位移的振动模式的实验部分声子态密度（pDOS），从而能够对所有分子内振动模式进行归属。这项研究证明，镝NRVS是一种强大的实验工具，在帮助阐明声子在单分子磁体中的作用方面具有巨大潜力。
