Perovskite Nanocrystals Initiate One‐Step Oxygen Tolerant PET‐RAFT Polymerization of Highly Loaded, Efficient Plastic Nanocomposites

Abstract Lead halide perovskite nanocrystals (LHP‐NCs) incorporated within polymer matrices have emerged as promising materials for various photonic applications. However, challenges persist in achieving high‐quality nanocomposites due to low monomer conversion yields, restricted LHP‐NCs loadings, and difficulty in maintaining NCs integrity post‐polymerization. A novel protocol for synthesizing LHP‐NCs/poly(methyl methacrylate) nanocomposites in a single step via the NC‐initiated photoinduced electron transfer‐reversible addition‐fragmentation chain transfer (PET‐RAFT) method is presented. Polymerization initiation mediated by NCs surfaces under blue light enables the fabrication of homogeneous nanocomposites with NCs loadings up to 7% w/w and ≈90% monomer conversion even in the presence of oxygen. This process preserves the optical quality of the NCs and passivates NCs surface defects, resulting in nanocomposites exhibiting near unity luminescence efficiencies. The potential of this approach for producing highly loaded nanocomposites for radiation detection is validated by radioluminescence measurements showing light yield values of 6000 ph MeV −1 and fast scintillation dynamics with effective lifetime of 490 ps, showing promise for time‐of‐flight radiometry.