TY - JOUR
T1 - Ligand-Directed Self-Assembly of Organic-Semiconductor/Quantum-Dot Blend Films Enables Efficient Triplet Exciton-Photon Conversion
AU - Gray, Victor
AU - Toolan, Daniel T.W.
AU - Dowland, Simon
AU - Allardice, Jesse R.
AU - Weir, Michael P.
AU - Zhang, Zhilong
AU - Xiao, James
AU - Klimash, Anastasia
AU - Winkel, Jurjen F.
AU - Holland, Emma K.
AU - Fregoso, Garrett M.
AU - Anthony, John E.
AU - Bronstein, Hugo
AU - Friend, Richard
AU - Ryan, Anthony J.
AU - Jones, Richard A.L.
AU - Greenham, Neil C.
AU - Rao, Akshay
N1 - Publisher Copyright:
© 2024 The Authors. Published by American Chemical Society
PY - 2024/3/20
Y1 - 2024/3/20
N2 - 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.
AB - 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.
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U2 - 10.1021/jacs.4c00125
DO - 10.1021/jacs.4c00125
M3 - Article
C2 - 38456418
AN - SCOPUS:85187374409
SN - 0002-7863
VL - 146
SP - 7763
EP - 7770
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 11
ER -