RESUMEN
Recent advances in quantum dot surface passivation have led to a rapid development of high-efficiency solar cells. Another critical element for achieving efficient power conversion is the charge neutrality of quantum dots, as charge imbalances induce electronic states inside the energy gap. Here we investigate how the simultaneous introduction of metal cations and halide anions modifies the charge balance and enhances the solar cell efficiency. The addition of metal salts between QD deposition and ligand exchange with 1,3-BDT results in an increase in the short-circuit current and fill factor, accompanied by a distinct reduction in a crossover between light and dark current density-voltage characteristics.
RESUMEN
Quantum dot photovoltaics (QDPV) offer the potential for low-cost solar cells. To develop strategies for continued improvement in QDPVs, a better understanding of the factors that limit their performance is essential. Here, we study carrier recombination processes that limit the power conversion efficiency of PbS QDPVs. We demonstrate the presence of radiative sub-bandgap states and sub-bandgap state filling in operating devices by using photoluminescence (PL) and electroluminescence (EL) spectroscopy. These sub-bandgap states are most likely the origin of the high open-circuit-voltage (VOC) deficit and relatively limited carrier collection that have thus far been observed in QDPVs. Combining these results with our perspectives on recent progress in QDPV, we conclude that eliminating sub-bandgap states in PbS QD films has the potential to show a greater gain than may be attainable by optimization of interfaces between QDs and other materials. We suggest possible future directions that could guide the design of high-performance QDPVs.
Asunto(s)
Plomo/química , Puntos Cuánticos , Energía Solar , Sulfuros/química , Suministros de Energía Eléctrica , Oro/química , Espectrometría de FluorescenciaRESUMEN
In this Letter, we present transient optoelectronic experimental studies of the recombination processes limiting the fill factor (FF) in three conjugated polymer:fullerene systems, poly(3-hexylthiophene) (P3HT) and two lower-band-gap polymers that exhibit lower FFs poly[2,6-(4,4-bis-(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b']dithiophene)-alt-4,7-(2,1,3-benzothiadiazole) (PCPDTBT) and poly(2,7-(9,9-dioctylfluorene)-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)) (APFO-3). Using transient absorption spectroscopy, charge extraction, and transient photovoltage experiments, we show that the lower FF observed for the PCPDTBT-based device results from enhanced nongeminate recombination even at short circuit, In contrast, we show that for APFO-3 devices, the FF is primarily limited by a voltage-dependent free charge generation, which we assign to a geminate recombination process.