Chapter 1 - Disclosing the hierarchical structure of ionic liquid mixtures by multiscale computational methods

This chapter deals with the structural analysis of ionic liquid-containing mixtures through multiscale computational methods. The chapter is divided into two sections, dealing with a basic introduction to the topic, and a more in-depth presentation of four different computational methods typically used to simulate the structural and dynamical properties of complex liquid systems. Initially, the concept of the structure of a liquid is discussed, providing definitions and some examples. Subsequently, the main features of the experimental technique based on X-ray scattering are presented, which allow accessing structural information of amorphous systems. A short introduction of the laws governing the scattering phenomenon, and how scattered photons can provide information about the structure of a system is also presented. A significant part of this chapter is devoted to introducing four of the most used state-of-the-art computational methods, namely density functional theory “static” optimization, semiempirical molecular dynamics, classical molecular dynamics, and coarse-grained molecular dynamics. The starting point is the quantastic treatment of the system, in which only minimal approximations are used. The reader is then guided toward successive approximations enabling to explore different system sizes and timescales. The intricate system ethylammonium nitrate:acetonitrile 1:9 binary mixture is taken as a case study to show what the four obtained models can return in terms of characterization. The final picture describes how the various methods are fundamentally complementary to each other, meaning that there is nothing as a “best” method.