Despite advances in nanomaterials synthesis, the bottom-up preparation of nanopatterned films as templates for spatially confined surface reactions remains a challenge. We report an approach to fabricating nanoscale thin film surface structures with periodicities on the order of 20 nm and with the capacity to localize reactions with small molecules and nanoparticles. A block copolymer (BCP) of polystyrene-block-poly[(allyl glycidyl ether)-co-(ethylene oxide)] (PS-b-P(AGE-co-EO)) is used to prepare periodically ordered, reactive thin films. As proof-of-principle demonstrations of the versatility of the chemical functionalization, a small organic molecule, an amino acid, and ultrasmall silica nanoparticles are selectively attached via thiol−ene click chemistry to the exposed P(AGE-co-EO) domains of the BCP thin film. Our approach employing click chemistry on the spatially confined reactive surfaces of a BCP thin film overcomes solvent incompatibilities typically encountered when synthetic polymers are functionalized with watersoluble molecules. Moreover, this post-assembly functionalization of a reactive thin film surface preserves the original patterning reduces the amount of required reactant, and leads to short reaction times. The demonstrated approach is expected to provide a new materials platform in applications including sensing, catalysis, pattern recognition, or microelectronics.
In recent years, high-resolution optical imaging in the far field has provided opportunities for alternative approaches to nanocharacterization traditionally dominated by electron and scanning probe microscopies. Here, we report the optical super-resolution imaging of model block copolymer (BCP) thin film surface nanostructures through stochastic optical reconstruction microscopy (STORM). We compare a set of surface-functionalized fluorescent core–shell silica nanoparticles encapsulating two different organic dyes, Cy3 and Cy5, with the corresponding free dyes in STORM. Using various click-type chemistries, these probes are covalently attached to the surface of specific blocks of BCP thin films, enabling selective block labeling and optical visualization. We demonstrate that the enhanced brightness of these particle probes offers distinct advantages over conventional dye labeling, outperforming one of the best STORM dyes available (Cy5).
While patterning the nucleation of crystalline inorganics at the nanometer length scale via low temperature, aqueous growth methods is highly desirable, it remains synthetically challenging. We report a generalizable approach for fabricating crystalline nanostructured inorganics at temperatures below 60 °C with periodicities on the order of 50 nm. A block copolymer (BCP) of polystyrene-block-poly[(allyl glycidyl ether)-co-(ethylene oxide)] (PS-b-P(AGE-co-EO)) is used to prepare periodically ordered, reactive thin film templates that are functionalized postassembly with an amino acid, cysteine, via thiol–ene click chemistry, exclusively at the sites of the exposed P(AGE-co-EO) domains. These functionalized areas subsequently template the confined crystallization of copper(I) oxide (Cu2O) and zinc oxide (ZnO) with high fidelity, from aqueous solutions at low temperatures. The demonstrated method provides a versatile materials platform to control the growth of nanostructured crystalline materials via the introduction of a plethora of surface functional groups by means of facile thiol–ene click chemistry. The resulting organic substrates can be used to template the growth of multiple different crystalline inorganic materials on surfaces nanostructured via BCP self-assembly.
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