Proton vibrational dynamics in lithium imide investigated through incoherent inelastic and Compton neutron scattering

In the present study we report neutron spectroscopic measurements on polycrystalline lithium imide, namely, incoherent inelastic neutron scattering at 20 K, and neutron Compton scattering from 10 K up to room temperature. From the former technique the H-projected density of phonon states up to 100 meV is derived, while the latter works out the spherically averaged single-particle (i.e., H, Li, and N) momentum distributions and, from this, the mean kinetic energies. Only for H at the lowest investigated temperature, non-Gaussian components of its momentum distribution are detected. However, these components do not seem directly connected to the system anharmonicity, being fully compatible with the simple N-H bond anisotropy. Neutron data are also complemented by ab initio lattice dynamics simulations, both harmonic and, at room temperature, carried out in the framework of the so-called quantum colored noise thermostat method. The single-particle mean kinetic energies in lithium imide as a function of temperature show a quite peculiar behavior at the moment not reproduced by ab initio lattice dynamics methods, at least as far as H and Li are concerned. As matter of fact, neither their low temperature values nor their temperature trends can be precisely explained in terms of standard phonon calculations.