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Colloidal quantum dots (QDs) exhibit highly desirable size- andshape-dependent properties for applications from electronic devices to imaging.Indium phosphide QDs have emerged as a primary candidate to replace the moretoxic CdSe QDs, but production of InP QDs with the desired properties lagsbehind other QD materials due to a poor understanding of how to tune the growthprocess. Using high-temperature ab initio molecular dynamics (AIMD)simulations, we report the first direct observation of the early stageintermediates and subsequent formation of an InP cluster from separated indiumand phosphorus precursors. In our simulations, indium agglomeration precedesformation of In-P bonds. We observe a predominantly intercomplex pathway inwhich In-P bonds form between one set of precursor copies while the carboxylateligand of a second indium precursor in the agglomerated indium abstracts aligand from the phosphorus precursor. This process produces an indium-richcluster with structural properties comparable to those in bulk zinc-blende InPcrystals. Minimum energy pathway characterization of the AIMD-sampled reactionevents confirms these observations and identifies that In-carboxylatedissociation energetics solely determine the barrier along the In-P bondformation pathway, which is lower for intercomplex (13 kcal/mol) thanintracomplex (21 kcal/mol) mechanisms. The phosphorus precursor chemistry, onthe other hand, controls the thermodynamics of the reaction. Our observationsof the differing roles of precursors in controlling QD formation stronglysuggests that the challenges thus far encountered in InP QD synthesisoptimization may be attributed to an overlooked need for a cooperative tuningstrategy that simultaneously addresses the chemistry of both indium andphosphorus precursors.

Direct Observation of Early-stage Quantum Dot Growth Mechanisms with High-temperature Ab Initio Molecular Dynamics