RESUMO
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.
RESUMO
Hybrid organic-inorganic metal-halide perovskites have emerged as versatile materials for enabling low-cost, mechanically flexible optoelectronic applications. The progress has been commendable; however, technological breakthroughs have outgrown the basic understanding of processes occurring in bulk and at device interfaces. Here, we investigated the photocurrent at perovskite/organic semiconductor interfaces in relation to the microstructure of electronically active layers. We found that the photocurrent response is significantly enhanced in the bilayer structure as a result of a more efficient dissociation of the photogenerated excitons and trions in the perovskite layer. The increase in the grain size within the organic semiconductor layer results in reduced trapping and further enhances the photocurrent by extending the photocarriers' lifetime. The photodetector responsivity and detectivity have improved by 1 order of magnitude in the optimized samples, reaching values of 6.1 ± 1.1 A W-1, and 1.5 × 1011 ± 4.7 × 1010 Jones, respectively, and the current-voltage hysteresis has been eliminated. Our results highlight the importance of fine-tuning film microstructure in reducing the loss processes in thin-film optoelectronics based on metal-halide semiconductors and provide a powerful interfacial design method to consistently achieve high-performance photodetectors.
