This work demonstrates a facile and versatile method for generating low scattering cross-linked quantum dot (QD)-polymer composite films and patterned highly emissive structures with ultrahigh QD loading, minimal phase separation, and tunable mechanical properties. Uniform QD-polymer films are fabricated using thiol-ene chemistry, in which cross-linked polymer networks are rapidly produced in ambient conditions via fast UV polymerization in bulk to suppress QD aggregation. UV-controlled thiol-ene chemistry limits phase separation through producing highly QD loaded cross-linked composites with loadings above majority of those reported in the literature (<1%) and approaching 30%. As the QD loading is increased, the thiol and ene conversion decreases, resulting in nanocomposites with widely variable and tailorable mechanical properties as a function of UV irradiation time with an elastic modulus decreasing to 1 GPa being characteristic of reinforced elastomeric materials, in contrast to usually observed stiff and brittle materials under these loading conditions. Furthermore, we demonstrate that the thiol-ene chemistry is compatible with soft-imprint lithography, making it possible to pattern highly loaded QD films while preserving the optical properties essential for high gain and low optical loss devices. The versatility of thiol-ene chemistry to produce high-dense QD-polymer films potentially makes it an important technique for polymer-based elastomeric optical metamaterials, where efficient light propagation is critical, like peculiar waveguides, sensors, and optical gain films.
Keywords: photoluminescence; polymer nanocomposite; quantum dots; quantum yield; soft lithography; thiol−ene; thiol−ene chemistry.