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Singlet fission (SF), an exciton multiplication process occurring in organicsemiconductors, offers a way to break the Shockley-Queisser limit insingle-bandgap photovoltaics (PV). If the triplet excitons generated by SF canbe transferred to inorganic quantum dots (QDs), where they radiativelyrecombine, SF based photon multiplication is achieved, converting a singlehigh-energy photon into two low-energy photons. Such a SF photon multiplicationfilm (SF-PMF) could raise the efficiency of the best Si-PV from 26.7% to 32.5%.But a precise nanoscale morphology is required within such a film consisting ofthe appropriate morphology for the organic phase, allowing for efficient SF,within which the QD emitters are well dispersed on a tens of nm length scale toenable efficient harvesting of the triplets. However, it has been along-standing problem that the individual components in organic-QD blends havea tendency to aggregate and phase separate, due to a mismatch of their size,shape and surface energies. Here, we demonstrate a QD surface engineeringapproach using an electronically active, highly soluble semiconductor ligandthat is matched to the SF material, which allows us to direct the self-assemblyprocess yielding solution processed films with well-dispersed QDs and minimalaggregation, as characterised by X-ray and neutron scattering and electronmicroscopy. Steady state and time-resolved optical spectroscopy show that thefilms support efficient SF (190% yield) in the organic phase and quantitativetriplet energy transfer across the organic-QD interface, resulting in 95% ofthe triplet excitons being harvested by the QDs. Our results establish theSF-PMF as a highly promising architecture to harness the SF process to enhancePV efficiencies, and also provide a highly versatile approach to overcomechallenges in the blending of organic semiconductors with QDs.

Ligand Directed Self-Assembly of Bulk Organic-Semiconductor/Quantum-Dot Blend Films Enables Near Quantitative Harvesting of Triplet Excitons