Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks
JC Ondry and JP Philbin and M Lostica and E Rabani and AP Alivisatos, ACS NANO, 13, 12322-12344 (2019).
The goal of this work is to identify favored pathways for preparation of defect-resilient attached wurtzite CdX (X = S, Se, Te) nanocrystals. We seek guidelines for oriented attachment of faceted nanocrystals that are most likely to yield pairs of nanocrystals with either few or no electronic defects or electronic defects that are in and of themselves desirable and stable. Using a combination of in situ high -resolution transmission electron microscopy (HRTEM) and electronic structure calculations, we evaluate the relative merits of atomic attachment of wurtzite CdSe nanocrystals on the 1 (1) over bar 00 or 11 (2) over bar0 family of facets. Pairwise attachment on either facet can lead to perfect interfaces, provided the nanocrystal facets are perfectly flat and the angles between the nanocrystals can adjust during the assembly. Considering defective attachment, we observe for 1 (1) over bar 00 facet attachment that only one type of edge dislocation forms, creating deep hole traps. For 11 (2) over bar0 facet attachment, we observe that four distinct types of extended defects form, some of which lead to deep hole traps whereas others only to shallow hole traps. HRTEM movies of the dislocation dynamics that dislocations at 1 (1) over bar 00 interfaces can be removed, albeit slowly. Whereas only some extended defects at 11 (2) over bar0 interfaces could be removed, others were trapped at the interface. Based on these insights, we identify the most resilient pathways to atomic attachment of pairs of wurtzite CdX nanocrystals and consider how these insights can translate to the creation of electronically useful materials from quantum dots with other crystal structures.
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