Impact resistance of nanocellulose films with bioinspired Bouligand microstructures

solvent processing. Taking CNC films as a model Bouligand system, we present atomistically-informed coarse-grained molecular dynamics simulations to measure the ballistic performance of thin films with helicoidally assembled nanocrystals by subjecting them to loading similar to laser-induced projectile impact tests. The effect of pitch angle on the impact performance of CNC films was quantified in the context of their specific ballistic limit velocity and energy absorption. Bouligand structures with low pitch angles (18-42°) were found to display the highest ballistic resistance, significantly outperforming other pitch angle and quasi-isotropic baseline structures. Improved energy dissipation through greater interfacial sliding, larger in-plane crack openings, and through-thickness twisting cracks resulted in improved impact performance of optimal pitch angle Bouligand CNC films. Intriguingly, decreasing interfacial interactions enhanced the impact performance by readily admitting dissipative inter-fibril and inter-layer sliding events without severe fibril fragmentation. This work helps reveal structural and chemical factors that govern the optimal mechanical design of Bouligand microstructures made from high aspect ratio nanocrystals, paving the way for sustainable, impact resistant, and multi-functional films.