Exploitation of solution-processed quantum dots in solid-state devices requires formation of robust interfaces that facilitate transport of photo- or electro-generated carriers. Sol-gel assembly is a powerful method for integrating nanoparticles into 2-D (films) and 3-D (porous) architectures. While traditional sol-gel methods are focused on oxides and involve the use of molecular precursors, such as metal alkoxides, that dictate the architecture by tuning rates of hydrolysis and condensation, we have developed a nanoparticle oxidative assembly route that produces thin films and aerogels, and does so with metal chalcogenides. The resultant quantum dot nanostructures retain the inherent quantum confinement effects of the discrete particles, while enabling carrier transport throughout the macrostructure assembly. However, the oxidized nature of the interfaces makes them subject to reductive dispersion; i.e., they are not redox-stable. In the present contribution, we will show that the interfacial chemistry can be dictated by varying the mechanism of assembly, or modified by chemical treatment post-assembly. These results will be discussed in the context of designing robust materials with optimized carrier transport properties for photovoltaics and solar fuels generation.

Sol-gel assembly of quantum dots: Creating and modifying interfaces for redox stability and facilitated carrier transport

2019 Spring National Meeting

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