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Perovskite quantum dots (QDs) have efficient optical absorption and emission in the visible range, and show a strong quantum confinement effect and high external quantum efficiency. They have been at the forefront of next‐generation photovoltaics and optoelectronics applications. However, two major challenges associated with perovskites and their nanomaterials are poor stability (such as against moisture and polar solvents), as well as the lack of efficient nanopatterning methods. In this work, a promising approach is provided to address both of those major challenges by molecular engineering and integration of QDs with block copolymers (BCP). The BCP thermoplastic elastomers not only substantially improve the stability of perovskite QDs by encapsulating them in a highly stable and soft matrix, but also enable molecular‐level control of the alignment and assembly of perovskite QDs in the microphase‐separated BCP matrix. It is demonstrated that designing and synthesis of compatible polymer ligands for perovskite QDs is key to enabling their selective and strong interaction with the BCP matrix. The structure and molecular weight of the BCP also play an important role in the interfacial structure and optical properties of the QDs‐BCP nanocomposites. Such soft and flexible optical nanocomposites have potential applications in flexible optoelectronics, optical storage, and displays.

This series of publications describes research rendering soft polyisobutylene (PIB)‐based thermoplastic elastomers 3D printable by blending with rigid chemically compatible thermoplastics. The molecular structure, morphology, physical properties, and 3D printability of such blends have been systematically investigated. The authors' first report was concerned with the rendering of soft poly(styrene‐b‐isobutylene‐b‐styrene) (SIBS) 3D printable by blending with rigid polystyrene (PS). Here they report the macromolecular engineering of SIBS/polyphenylene oxide (PPO) blends for 3D printing. PPO, a rigid high‐performance thermoplastic, is compatible with the hard PS block in SIBS; however, neither PPO nor SIBS can be directly 3D printed. The microphase‐separated structures and physical properties of SIBS/PPO blends are systematically tuned by controlling blending ratios and molecular weights. Suitable composition ranges and desirable properties of SIBS/PPO blends for 3D printing are optimized. The morphology and properties of SIBS/PPO blends are characterized by an ensemble of techniques, including atomic force microscopy, small‐angle X‐ray scattering, and thermal and mechanical properties testing. The elucidation of processing‐structure‐property relationship of SIBS/PPO blends is essential for 3D printing and advanced manufacturing of high‐performance polymer systems.