A critical review and perspectives on atomistic models of non-crystalline cementitious materials

Abstract

The use of atomic-scale modelling in the study of cement-related materials has grown steadily. However, the complexity of the systems under investigation and disparities in length and time scales between simulations and real-world processes, has hindered a clear demonstration of simulation-driven design of cement properties. The presence of multiple components, with intricate atomic and nanoscale structures and high degrees of amorphicity, makes the construction of realistic atomic-scale models the major challenge. This paper presents a critical review of state-of-the-art models of non-crystalline cementitious materials. Special attention is given to calcium silicate hydrate (C–S–H), where recent advances in bulk and interface models, disorder quantification, and novel formation mechanisms are assessed. The review also covers other key phases, including amorphous aluminosilicates, amorphous carbonates, and magnesium silicate hydrates (M–S–H). By outlining current methodologies and limitations, this work aims to inspire new approaches and tools for advancing predictive modelling of increasingly complex cementitious systems.