Modelling stacking disorder in graphite

Graphite is a layered material with applications in nuclear reactors, electronics, and batteries. As a consequence of the weak van der Waals interactions between the layers, their stacking arrangement is often disordered which in turn affects the mechanical, electronic and optical properties of graphite. In this work, we develop an atomistic approach to predict the structure of graphite and capture its stacking disorder. We first perform ab initio density-functional theory to determine the potential energy surface of graphite, which is then used to parametrize an effective model. Using this model, we perform large-scale Monte-Carlo simulations to predict the atomic structure of graphite at finite temperatures. We compare the resulting structures to those produced by an Ising model and show that our approach produces X-ray diffraction patterns in closer agreement with experimental measurements. In the future, this approach can be straightforwardly applied to other layered materials, such as covalent organic frameworks or transition metal dichalcogenides.