Defect Self-Elimination in Nanocube Superlattices Through the Interplay of Brownian, van der Waals, and Ligand-Based Forces and Torques
Year: 2024
Type: article
Abstract: 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.
Source: ACS Nano
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
Funders: National Science Foundation, U.S. Department of Energy, Battelle, National Energy Research Scientific Computing Center, Office of Science, Division of Chemical, Bioengineering, Environmental, and Transport Systems, Basic Energy Sciences, Biological and Environmental Research, Pacific Northwest National Laboratory, Division of Materials Sciences and Engineering
Awards: G1147001989, G1202769797, G122673668, G125460123, G1286236842, G1286251239, G1337544421, G138090931, G1677143136, G1851334662, G1863003419, G1899721271, G198587779, G223002938, G2320984915, G237429762, G2506945562, G2510423872, G2605861094, G2810384502, G2820049545, G2963654190, G2988778103, G30714459, G3083819904, G3476726851, Mechanistic Understanding of Oriented Attachment Crystallization Processes for Lead-Halide Perovskite Nanocrystals, G391136020, G414219354, G419881185, G42916606, G4501827968, G498139845, G5044650253, G5076365615, G5321382714, G5373841109, G5640612048, G5653134238, G5726405315, G613759197, G6437394012, G650090426, G7073172499, G7560550554, G7787287669, G7897470476, G791371132, G821644656, G969889393
OpenAlex ID: W4404229523