Highly Luminescent Shell-Less Indium Phosphide Quantum Dots Enabled by Atomistically Tailored Surface States.

Contrary to the prevailing notion that shell structures arise from the intricate chemistry and surface defects of InP quantum dots (QDs), an innovative strategy that remarkably enhances the luminescence efficiency of core-only InP QDs to over 90% is introduced. This paradigm shift is achieved through the concurrent utilization of group 2 and 3 metal-derived ligands, providing an effective remedy for surface defects and facilitating charge recombination. Specifically, a combination of Zn carboxylate and Ga chloride is employed to address the undercoordination issues associated with In and P atoms, leading to the alleviation of in-gap trap states. The intricate interplay and proportional ratio between Ga- and Zn-containing ligands play pivotal roles in attaining record-high luminescence efficiency in core-only InP QDs, as successfully demonstrated across various sizes and color emissions. Moreover, the fabrication of electroluminescent devices relying solely on InP core emission opens a new direction in optoelectronics, demonstrating the potential of the approach not only in optoelectronic applications but also in catalysis or energy conversion by charge transfer.

Colloidal Synthesis of P-Type Zn3As2 Nanocrystals.

Zinc pnictides, particularly Zn3As2, hold significant promise for optoelectronic applications owing to their intrinsic p-type behavior and appropriate bandgaps. However, despite the outstanding properties of colloidal Zn3As2 nanocrystals, research in this area is lacking because of the absence of suitable precursors, occurrence of surface oxidation, and intricacy of the crystal structures. In this study, a novel and facile solution-based synthetic approach is presented for obtaining highly crystalline p-type Zn3As2 nanocrystals with accurate stoichiometry. By carefully controlling the feed ratio and reaction temperature, colloidal Zn3As2 nanocrystals are successfully obtained. Moreover, the mechanism underlying the conversion of As precursors in the initial phases of Zn3As2 synthesis is elucidated. Furthermore, these nanocrystals are employed as active layers in field-effect transistors that exhibit inherent p-type characteristics with native surface ligands. To enhance the charge transport properties, a dual passivation strategy is introduced via phase-transfer ligand exchange, leading to enhanced hole mobilities as high as 0.089 cm2 V-1 s-1. This study not only contributes to the advancement of nanocrystal synthesis, but also opens up new possibilities for previously underexplored p-type nanocrystal research.

Ligand-Crosslinking Strategy for Efficient Quantum Dot Light-Emitting Diodes via Thiol-Ene Click Chemistry.

While solution-processable colloidal quantum dots (QDs) offer cost-effective and large-scale manufacturing, they can be susceptible to subsequent solution processes, making continuous processing challenging. To enable complex and integrated device architectures, robust QD films with subsequent patterning are necessary. Here, we report a facile ligand-crosslinking strategy based on thiol-ene click chemistry. Thiol molecules added to QD films react with UV light to form radicals that crosslink with QD ligands containing carbon double bonds, enabling microscale photo-patterning of QD films and enhancing their solvent resistance. This strategy can also be extended to other ligand-capped nanocrystals. It is found that the swelling of QD films during the process of binding with the thiol molecules placed between the ligands contributes to the improvement of photoluminescence and electroluminescence properties. These results suggest that the thiol-ene crosslinking modifies the optoelectronic properties and enables direct optical patterning, expanding the potential applications of QDs.