Oriented Attachment of ZnO Nanocrystals

TL;DR

This study investigates the oriented attachment of ZnO nanocrystals during deposition, finding that dipolar interactions are not the main driving force, and surface reduction likely plays a key role.

Contribution

It provides experimental evidence that dipolar interactions do not significantly influence ZnO nanocrystal attachment, highlighting surface reduction as the primary mechanism.

Findings

Electric field has no significant effect on nanocrystal organization.

Dipolar interactions are not the main driving force for attachment.

Surface reduction, possibly driven by Coulombic forces, is likely the key mechanism.

Abstract

Self-organization of nanoparticles is a major issue to synthesize mesoscopic structures. Among the possible mechanisms leading to self-organization, the oriented attachment is efficient yet not completely understood. We investigate here the oriented attachment process of ZnO nanocrystals preformed in the gas phase. During the deposition in high vacuum, about 60% of the particles, which are uncapped, form larger crystals through oriented attachment. In the present conditions of deposition, no selective direction for the oriented attachment is noticed. To probe the driving force of the oriented attachment, and more specifically the possible influence of the dipolar interaction between particles, we have deposited the same nanocrystals in the presence of a constant electric field. The expected effect was to enhance the fraction of domains resulting from the oriented attachment due to the increased interaction of the particle dipoles with the electric field. The multiscale analytical and statistical analysis (TEM coupled to XRD) shows no significant influence of the electric field on the organization of the particles. We therefore conclude that the dipolar interaction between nanocrystals is not the prominent driving force in the process. Consequently, we argue, in accordance with recent theoretical and experimental investigations, that the surface reduction, possibly driven by Coulombic interaction, may be the major mechanism for the oriented attachment process.