Dysprosium(III)-containing single-molecule magnets (SMMs) show blocking of the molecular magnetization and hysteresis effects in one molecule. They belong to the class of the best performing SMMs at present. Here, we present first results of 161Dy-Nuclear Resonance Vibrational Spectroscopy (NRVS) experiments on the dysprosium(III) complex [Dy(H2dapp)(NO3)2](NO3) with H2dapp being 2,6-bis((E)-1-(2-(pyridine-2-yl)-hydrazineylidene)ethyl)pyridine. For the 161Dy-NRVS experiments a compact novel He flow cryostat was used at the Advanced Photon Source, Argonne National Laboratories, which enables low temperature NRVS experiments in helium vapour circumventing the often-observed difference between sensor read and "real" sample temperature in mostly used LHe and/or closed cycle cryostats with the NRVS sample being in vacuum. To explore the vibrational modes of the molecule simulations based on first density functional theory (DFT) calculations are presented. [ABSTRACT FROM AUTHOR]