This thesis is about new ways to experimentally realise materials with desired nano-structures for solution-processable optoelectronic devices such as solar cells and light-emitting diodes (LEDs), and examine structure-performance relationships in these devices.

Short exciton diffusion length limits the efficiency of most exciton-based solar cells. By introducing nano-structured architectures to solar cells, excitons can be separated more effectively, leading to an enhancement of the cell’s power conversion efficiency. We use diblock copolymer lithography combined with solvent-vapour-assisted imprinting to fabricate nano-structures with 20-80 nm feature sizes. We demonstrate nanostructured solar cell incorporating the high-performance polymer PBDTTT-CT. Furthermore, we demonstrated the patterning of singlet fission materials, including a TIPS-pentacene solar cell based on ZnO nanopillars.

Recently perovskites have emerged as a promising semiconductor for optoelectronic applications. We demonstrate a perovskite light-emitting diode that employs perovskite nanoparticles embedded in a dielectric polymer matrix as the emissive layer. The emissive layer is spin-coated from perovskite precursor/polymer blend solution. The resultant polymer-perovskite composites effectively block shunt pathways within the LED, thus leading to an external quantum efficiency of 1.2%, one order of magnitude higher than previous reports.

We demonstrate formations of stably emissive perovskite nanoparticles in an alumina nanoparticle matrix. These nanoparticles have much higher photoluminescence quantum efficiency (25%) than bulk perovskite and the emission is found to be stable over several months.

Finally, we demonstrate a new vapour-phase crosslinking method to construct full-colour perovskite nanocrystal LEDs. With detailed structural and compositional analysis we are able to pinpoint the aluminium-based crosslinker that resides between the nanocrystals, which enables remarkably high EQE of 5.7% in CsPbI3 LEDs.