By using time-of-flight neutron spectroscopy with polarization analysis, we have separated coherent and incoherent contributions to the scattering of deuterated tetrahydrofuran in a wide scattering vector (Q)-range from meso- to inter-molecular length scales. The results are compared with those recently reported for water to address the influence of the nature of inter-molecular interactions (van der Waals vs hydrogen bond) on the dynamics. The phenomenology found is qualitatively similar in both systems. Both collective and self-scattering functions are satisfactorily described in terms of a convolution model that considers vibrations, diffusion, and a Q-independent mode. We observe a crossover in the structural relaxation from being dominated by the Q-independent mode at the mesoscale to being dominated by diffusion at inter-molecular length scales. The characteristic time of the Q-independent mode is the same for collective and self-motions and, contrary to water, faster and with a lower activation energy (≈1.4 Kcal/mol) than the structural relaxation time at inter-molecular length scales. This follows the macroscopic viscosity behavior. The collective diffusive time is well described by the de Gennes narrowing relation proposed for simple monoatomic liquids in a wide Q-range entering the intermediate length scales, in contraposition to the case of water.
© 2023 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).