Neutron study of non-Gaussian self dynamics in liquid parahydrogen

Abstract

A time-honoured approach to single-molecule, or self, dynamics of liquids is based on the so-called Gaussian approximation (GA), where it is assumed that, in the whole dynamical range between hydrodynamic diffusion and free-particle streaming, the motion of a particle is fully determined by a unique function of time directly related to the velocity autocorrelation function. An evident support to the GA is offered by the fact that the approximation becomes exact in both above limit conditions. Yet, experimental inquiries into the presence of non-Gaussian dynamics are very scarce, particularly in liquid parahydrogen in spite of its importance as the prototype of a "quantum Boltzmann liquid" which has also served as a benchmark for the development of quantum dynamics simulation algorithms. Though experimental evidence of the breakdown of the GA was obtained by some of the authors a few years ago, the localization in Q space of non-Gaussian behaviour was still undetermined, and no quantitative assessment of the effect was ever obtained. These issues have been tackled and solved by a new neutron investigation, which provides the first determination of non-Gaussian behaviour in the framework of the well-known theoretical approach by Rahman, Singwi and Sjölander.