Revealing Structure and Crystallographic Orientation of Soft Epitaxial Assembly of Nanocrystals by Grazing Incidence X-ray Scattering.

Abstract

We study the structural coherence of a self-assembled overlayer of PbS nanocrystal (NC) superlattice onto an underlying PbS NC monolayer, which acts as a template. We explore the effect of the templating layer on the structure of the overlayer asemblies by varying interfacial strain and determine the impact of new ligands on their superlattice structure. The overlayers and templates are analyzed by grazing-incidence X-ray scattering and microscopy. We find that differences in the lattice parameters of 7.7% between the two layers are tolerated in terms of a "soft epitaxial" assembly into the body-centered tetragonal superstucture and lead to structural registry within the overlayer. Conversely, at the interface, a lattice mismatch of 24.4% is too large for soft epitaxy and invokes a change in the superlattice. Upon ligand treatment, the overlayer superlattices transform their orientation axis and the NCs orient preferentially. These results provide new insights into mitigating defects in layered, heterostructured NC assemblies.