ABSTRACT Indium phosphide (InP) quantum dots (QDs) are promising cadmium‐free emitters for next‐generation optoelectronic devices, yet their synthesis remains challenging due to rapid precursor reactivity, uncontrolled nucleation, and surface defect formation. Conventional approaches that regulate either phosphorus or indium precursor kinetics often fall short under high‐temperature synthesis conditions, failing to address early‐stage surface energy stabilization and passivation. Here, we introduce a versatile strategy using 1H,1H,2H,2H‐perfluorodecyltriethoxysilane (denoted FTS), which simultaneously moderates both phosphorus and indium precursor reactivities while enabling in situ passivation and surface energy control. Upon hydrolysis, FTS releases ethanol to transiently coordinate with indium precursors, slowing nucleation, while its perfluorinated chain imposes steric hindrance and forms a hydrophobic shell. This reduces surface energy, suppresses Ostwald ripening, and promotes uniform size growth. Density functional theory calculations confirm that FTS‐derived silanol groups reduce surface phosphorus reactivity and passivate P‐terminated InP surfaces, eliminating mid‐gap states, passivating dangling bonds and stabilizing the surface. Using this integrated approach, we achieve green‐emitting InP QDs with a PLQY of 93% and a narrow emission FWHM of 38 nm. This work provides a scalable route for producing monodisperse, oxidation‐resistant InP QDs through simultaneous control of nucleation, surface chemistry, and energy stabilization.
Malo et al. (Thu,) studied this question.