Dynamic Reconfiguration of Compressed 2D Nanoparticle Monolayers

A Gibbs monolayer of jammed, or nearly jammed, spherical nanoparticles was imaged at a liquid surface in real time by in-situ scanning electron microscopy performed at the single-particle level. At nanoparticle areal fractions above that for the onset of two-dimensional crystallization, structural reorganizations of the mobile polymer-coated particles were visualized after a stepwise areal compression. When the compression was small, slow shearing near dislocations and reconfigured nanoparticle bonding were observed at crystal grain boundaries. At larger scales, domains grew as they rotated into registry by correlated but highly intermittent motions. Simultaneously, the areal density in the middle of the monolayer increased. When the compression was large, the jammed monolayers exhibited out-of-plane deformations such as wrinkles and bumps. Due to their large interfacial binding energy, few (if any) of the two-dimensionally mobile nanoparticles returned to the liquid subphase. Compressed long enough (several hours or more), monolayers transformed into solid nanoparticle films, as evidenced by their cracking and localized rupturing upon subsequent areal expansion. These observations provide mechanistic insights into the dynamics of a simple model system that undergoes jamming/unjamming in response to mechanical stress.