Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.003
Publication date: 18th July 2019
Indium phosphide quantum dots (QDs) have emerged as a promising candidate to replace more toxic II–VI CdSe QDs, but production of high-quality III–V InP QDs with targeted properties requires a better understanding of their growth. I will describe our work in developing a first-principles-derived model that unifies InP QD formation from isolated precursor and early stage cluster reactions to 1.3 nm magic sized clusters and rationalize experimentally observed properties of full sized >3 nm QDs. Our first-principles study on realistic QD models reveals large surface-dependent reactivity for all elementary growth process steps, including In-ligand bond cleavage and P precursor addition. I will describe the correlation of thermodynamic trends to kinetic properties at all stages of growth. This analysis suggests the presence of labile and stable spots on cluster and QD surfaces. Correlation of electronic or geometric properties to energetics identifies surprising sources for these variations: short In···In separation on the surface produces the most reactive sites, at odds with conventional understanding of strain (i.e., separation) in bulk metallic surfaces increasing reactivity and models for ionic II–VI QD growth. We rationalize these differences by the covalent, directional nature of bonding in III–V QDs and explained by descriptors derived directly from the In–O bond density. The unique constraints of carboxylate and P precursor bonding to In atoms rationalize why all sizes of InP clusters and QDs are In-rich but become less so as QDs mature. Time permitting, I will discuss how these observations could be used to suggest alternate growth recipes that take into account strong surface-dependence of kinetics as well as the shapes of both In and P precursors for better control of kinetics and surface morphology in III–V QDs.
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