  Hybrid structures formed between organic molecules and inorganic quantum dots
can accomplish unique photophysical transformations by taking advantage of
their disparate properties. The electronic coupling between these materials is
typically weak, leading photoexcited charge carriers to spatially localize to a
dot or a molecule at its surface. However, we show that by converting a
chemical linker that covalently binds anthracene molecules to silicon quantum
dots from a carbon-carbon single bond to a double bond, we access a
strong-coupling regime where excited carriers spatially delocalize across both
anthracene and silicon. By pushing the system to delocalize, we design a photon
upconversion system with a higher efficiency (17.2%) and lower threshold
intensity (0.5 W/cm^2) than that of a corresponding weakly-coupled system. Our
results show that strong coupling between molecules and nanostructures achieved
through targeted linking chemistry provides a new route for tailoring
properties in materials for light-driven applications.
