In stark contrast to conventional organic ligand-capped counterparts, the ability to create stable metal halide perovskite nanocrystals strongly tethered with conjugated polymers (CPs) represents an important endeavor towards tailoring charge carrier dynamics at their interface that critically underpins applications of this unique class of all semiconducting, organic-inorganic nanomaterials for optoelectronics. This, however, has yet to be largely explored. Herein, we report, for the first time, the unravelling of efficient charge separation at judiciously designed CP/perovskite quantum dot (QD) interface for photo-induced atom transfer radical polymerization (p-ATRP). Such scrutiny is rendered by in-situ crafting an array of monodisperse, highly stable, CP-ligated perovskite QDs with precisely controlled dimensions of each constituent via capitalizing on unimolecular, amphiphilic star-like block copolymers as nanoreactors. The intimate and permanent surface-tethering of CPs imparts remarkable thermal, photo, and polar-solvent stabilities of CP-ligated perovskite QDs. More importantly, they manifest efficient interfacial charge separation with a profound dependence on the length of ligated CPs and size of perovskite QDs. The outstanding structural stabilities and charge separation characteristic enable CP-ligated perovskite QDs as robust photocatalysts for p-ATRP of a wide selection of monomers with stable and controllable reaction kinetics, also depending crucially on the length of CPs and size of perovskite QDs. In principle, an exciting variety of CP-ligated, uniform perovskite QDs with virtually unlimited material choice of both, markedly improved stabilities, and tunable electronic band alignments can be readily accessed by exploiting amphiphilic star-like block copolymer nanoreactor strategy for use in photodetectors, sensors, LEDs, and solar cells, among other areas.

Tailoring charge separation at meticulously engineered conjugated polymer/perovskite quantum dot interface for photocatalyzing atom transfer radical polymerization

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ACS Fall 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.