Revealing the Effect of Irradiation on Cement Hydrates: Evidence of a Topological Self-Organization.

Despite the crucial role of concrete in the construction of nuclear power plants, the effects of radiation exposure (i.e., in the form of neutrons) on the calcium-silicate-hydrate (C-S-H, i.e., the glue of concrete) remain largely unknown. Using molecular dynamics simulations, we systematically investigate the effects of irradiation on the structure of C-S-H across a range of compositions. Expectedly, although C-S-H is more resistant to irradiation than typical crystalline silicates, such as quartz, we observe that radiation exposure affects C-S-H's structural order, silicate mean chain length, and the amount of molecular water that is present in the atomic network. By topological analysis, we show that these "structural effects" arise from a self-organization of the atomic network of C-S-H upon irradiation. This topological self-organization is driven by the (initial) presence of atomic eigenstress in the C-S-H network and is facilitated by the presence of water in the network. Overall, we show that C-S-H exhibits an optimal resistance to radiation damage when its atomic network is isostatic (at Ca/Si = 1.5). Such an improved understanding of the response of C-S-H to irradiation can pave the way to the design of durable concrete for radiation applications.