Understanding defect healing is necessary to control the electronic and optoelectronic performance of devices based on nanoparticle (NP) superlattices. However, a key challenge remains to understand how NP interactions and the resulting dynamics are coupled to defect self-elimination during assembly processes. Additional degrees of freedom that account for the anisotropic nature of NPs associated with rotational dynamics and torques further complicate the challenge. Here, we investigate nanocube (NC) superlattices by employing liquid-phase transmission electron microscopy, continuum theory, and molecular dynamics simulations. Our detailed analyses reveal that interparticle forces and torques due to ligand interactions dominate those from Brownian motions and van der Waals interactions. More importantly, NC translations and rotations induced by unbalanced forces and torques are transmitted to neighboring NCs, prompting "chain interactions" in a two-dimensional (2D) network and expediting self-elimination. The mechanistic understanding will further enable the design and fabrication of defect-free superlattices as well as those with tailored defects via assembly of anisotropic particles.
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