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Semiconducting, core-shell nanocrystals (NCs) are promising building blocksfor the construction of higher dimensional artificial nanostructures usingoriented attachment. However, the assembly and epitaxial attachment stepscritical to this construction introduce disorder and defects which inhibit theobservation of desirable emergent electronic phenomena. Consequently,understanding defect formation and remediation in these systems as a functionof dimensionality is a crucial step to perfecting their synthesis. In thiswork, we use in situ high resolution transmission electron microscopy toexamine the role of chloride ligands as remediator agents for imperfectattachment interfaces between CdSe/CdS core-shell NCs for both 1D and 2Dattachment cases. In the 1D case, we find that the presence of chlorideadditives in imperfectly attached NC dimers can result in defect removal speedsnearly twice as large as those found in their plain, non-chloride treatedcounterparts. However, when we increased the dimensionality of the system andexamined 2D NC arrays, we found no statistically significant difference inattachment interface quality between the chloride and non-chloride treatedsamples. We propose that this discongruity arises from fundamental differencesbetween 1D and 2D NC attachment and discuss synthetic guidelines to informfuture nanomaterial superlattice design.

Examining the Role of Chloride Ligands on Defect Removal in Imperfectly Attached Semiconductor Nanocrystals for 1D and 2D Attachment Cases