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.
| Original language | English |
|---|---|
| Pages (from-to) | 7763-7770 |
| Number of pages | 8 |
| Journal | Journal of the American Chemical Society |
| Volume | 146 |
| Issue number | 11 |
| DOIs | |
| State | Published - Mar 20 2024 |
Bibliographical note
Publisher Copyright:© 2024 The Authors. Published by American Chemical Society
Funding
The authors acknowledge funding through the Winton Programme for the Physics of Sustainability and the Engineering and Physical Sciences Research Council (U.K.). The authors acknowledge beamtime awarded at the ISIS Pulsed Neutron and Muon Source through experiment number RB1810513 (DOI: 10.5286/ISIS.E.RB1810513). V.G. acknowledges funding from the Swedish Research Council, Vetenskapsrådet 2018-00238. J.R.A. acknowledges the Cambridge Commonwealth European and International Trust for financial support. J.X. acknowledges EPSRC Cambridge NanoDTC, EP/L015978/1, for financial support. J.E.A. acknowledges the U.S. National Science Foundation (DMREF-1627428) for support of organic semiconductor synthesis. Z.Z. acknowledges funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Actions grant (No. 842271─TRITON project). This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement number 758826). Part of the paper has been adapted from a PhD thesis.
| Funders | Funder number |
|---|---|
| Horizon 2020 Framework Programme | |
| Gates Cambridge Trust | |
| H2020 European Research Council | 758826 |
| UK Medical Research Council, Engineering and Physical Sciences Research Council | EP/P027741/1, EP/L015978/1 |
| Vetenskapsrådet | 2018-00238 |
| National Science Foundation Arctic Social Science Program | DMREF-1627428 |
| H2020 Marie Skłodowska-Curie Actions | 842271 |
| ISIS Pulsed Neutron and Muon Source | RB1810513 |
ASJC Scopus subject areas
- Catalysis
- Biochemistry
- General Chemistry
- Colloid and Surface Chemistry