Ligand-Directed Self-Assembly of Organic-Semiconductor/Quantum-Dot Blend Films Enables Efficient Triplet Exciton-Photon Conversion

Gray, Victor; Toolan, Daniel T. W.; Dowland, Simon; Allardice, Jesse R.; Weir, Michael P.; Zhang, Zhilong; Xiao, James; Klimash, Anastasia; Winkel, Jurjen F.; Holland, Emma K.; Fregoso, Garrett M.; Anthony, John E.; Bronstein, Hugo; Friend, Richard; Ryan, Anthony J.; Jones, Richard A. L.; Greenham, Neil C.; Rao, Akshay

Abstract

Blends comprising organic semiconductors and inorganic quantum dots (QDs) are relevant for many optoelectronic applications and devices. However, the individual components in organic-QD blends have a strong tendency to aggregate and phase-separate during film processing, compromising both their structural and electronic properties. Here, we demonstrate a QD surface engineering approach using electronically active, highly soluble semiconductor ligands that are matched to the organic semiconductor host material to achieve well-dispersed inorganic–organic blend films, as characterized by X-ray and neutron scattering, and electron microscopies. This approach preserves the electronic properties of the organic and QD phases and also creates an optimized interface between them. We exemplify this in two emerging applications, singlet-fission-based photon multiplication (SF-PM) and triplet–triplet annihilation-based photon upconversion (TTA-UC). Steady-state and time-resolved optical spectroscopy shows that triplet excitons can be transferred with near unity efficiently across the organic–inorganic interface, while the organic films maintain efficient SF (190% yield) in the organic phase. By changing the relative energy between organic and inorganic components, yellow upconverted emission is observed upon 790 nm NIR excitation. Overall, we provide a highly versatile approach to overcome longstanding challenges in the blending of organic semiconductors with QDs that have relevance for many optical and optoelectronic applications.

Citation

Gray, V., Toolan, D. T. W., Dowland, S., Allardice, J. R., Weir, M. P., Zhang, Z., …Rao, A. (2024). Ligand-Directed Self-Assembly of Organic-Semiconductor/Quantum-Dot Blend Films Enables Efficient Triplet Exciton-Photon Conversion. Journal of the American Chemical Society, 146(11), 7763-7770. https://doi.org/10.1021/jacs.4c00125

• Journal Article Type: Article
• Acceptance Date: Feb 14, 2024
• Online Publication Date: Mar 8, 2024
• Publication Date: Mar 20, 2024
• Deposit Date: Mar 26, 2024
• Publicly Available Date: Mar 27, 2024
• Journal: Journal of the American Chemical Society
• Print ISSN: 0002-7863
• Electronic ISSN: 1520-5126
• Publisher: American Chemical Society
• Peer Reviewed: Peer Reviewed
• Volume: 146
• Issue: 11
• Pages: 7763-7770
• DOI: https://doi.org/10.1021/jacs.4c00125
• Keywords: Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis
• Public URL: https://nottingham-repository.worktribe.com/output/32736254
• Publisher URL: https://pubs.acs.org/doi/10.1021/jacs.4c00125