Self-assembled nanoparticle superlattices (NPSLs) are an emergent class of self-architected nanocomposite materials that possess promising properties arising from precise nanoparticle ordering. Their multiple coupled properties make them desirable as functional components in devices where mechanical robustness is critical. However, questions remain about NPSL mechanical properties and how shaping them affects their mechanical response. Here, we perform in situ nanomechanical experiments that evidence up to an 11-fold increase in stiffness (∼1.49 to 16.9 GPa) and a 5-fold increase in strength (∼88 to 426 MPa) because of surface stiffening/strengthening from shaping these nanomaterials via focused-ion-beam milling. To predict the mechanical properties of shaped NPSLs, we present discrete element method (DEM) simulations and an analytical core-shell model that capture the FIB-induced stiffening response. This work presents a route for tunable mechanical responses of self-architected NPSLs and provides two frameworks to predict their mechanical response and guide the design of future NPSL-containing devices.
Keywords: FIB shaping; in situ nanomechanics; nanoparticle superlattices; self-architected materials; surface stiffening.