Imaging Inelastic Fracture Processes in Biomimetic Nanocomposites and Nacre by Laser Speckle for Better Toughness

Abstract Mollusk nacre is a prototypical biological inorganic–organic composite that combines high toughness, stiffness, and strength by its brick‐and‐mortar microstructure, which has inspired several synthetic mimics. Its remarkable fracture toughness relies on inelastic deformations at the process zone at the crack tip that dissolve stress concentrations and stop cracks. The micrometer‐scale structure allows resolving the size and shape of the process zone to understand the fracture processes. However, for better scalability, nacre‐mimetic nanocomposites with aligned inorganic or graphene nanosheets are extensively pursued, to avoid the packing problems of mesoscale sheets like in nacre or slow in situ biomineralization. This calls for novel methods to explore the process zone of biomimetic nanocomposites. Here the fracture of nacre and nacre‐inspired clay/polymer nanocomposite is explored using laser speckle imaging that reveals the process zone even in absence of changes in optical scattering. To demonstrate the diagnostic value, compared to nacre, the nacre‐inspired nanocomposite develops a process zone more abruptly with macroscopic crack deflection shown by a flattened process zone. In situ scanning electron microscopy suggests similar toughening mechanisms in nanocomposite and nacre. These new insights guide the design of nacre‐inspired nanocomposites toward better mechanical properties to reach the level of synergy of their biological model.