Quantum dots enabling all-in-one controllable polymerization through triplet energy transfer.

Colloidal quantum dots (QDs) have recently emerged as a class of initiators or activators for photopolymerization, typically relying on photoinduced charge transfer from QDs to co-additives. Here we report efficient photopolymerization of acrylates using QDs alone without any co-additives, triggered by energy transfer from photoexcited QDs to the triplet excited-states of acrylates on sub-nanosecond timescales. The diradical-like triplets are converted to free radicals through interaction with QDs' surface dangling bonds, thereby initiating chain propagation. The radical-surface interaction enables controlled polymerization with narrow polydispersity and block copolymerization capability. This study demonstrates how the interior excitons and surface atoms of QDs can synergistically drive controllable photopolymerization, distinguishing QDs from conventional molecular initiators. Practical advantages of this all-in-one approach include its streamlined reaction system, well-preserved emission of QDs, and enhanced stability of QDs in nanocomposites that are well suited for display and optical waveguiding applications.