Recent research has pushed the efficiency of colloidal quantum dot solar cells toward a level that spurs commercial interest. Quantum dot/metal oxide bilayers form the most efficient colloidal quantum dot solar cells, and most studies have advanced the understanding of the quantum dot component. We study the interfacial recombination process in depleted heterojunction colloidal quantum dot (QD) solar cells formed with ZnO as the oxide by varying (i) the carrier concentration of the ZnO layer and (ii) the density of intragap recombination sites in the QD layer. We find that the open-circuit voltage and efficiency of PbS QD/ZnO devices can be improved by 50% upon doping of the ZnO with nitrogen to reduce its carrier concentration. In contrast, doping the ZnO did not change the performance of PbSe QD/ZnO solar cells. We use X-ray photoemission spectroscopy, ultraviolet photoemission spectroscopy, transient photovoltage decay measurements, transient absorption spectroscopy, and intensity-dependent photocurrent measurements to investigate the origin of this effect. We find a significant density of intragap states within the band gap of the PbS quantum dots. These states facilitate recombination at the PbS/ZnO interface, which can be suppressed by reducing the density of occupied states in the ZnO. For the PbSe QD/ZnO solar cells, where fewer intragap states are observed in the quantum dots, the interfacial recombination channel does not limit device performance. Our study sheds light on the mechanisms of interfacial recombination in colloidal quantum dot solar cells and emphasizes the influence of quantum dot intragap states and metal oxide properties on this loss pathway.

We demonstrate that solution-processible silver-nanowire films coated with zinc-oxide-nanoparticles (ZnO-NPs) can be used as transparent electrodes in organic photovoltaic devices. The ZnO-NP coating acts as electron extraction layer and as encapsulating agent, protecting the wires from oxidation and improving their mechanical stability. Scanning photocurrent microscopy showed photocurrent generation to be more efficient at the active material surrounding the wires. Ultra-violet illumination as present in the solar spectrum was found to enhance photocurrent by improving the ZnO in-layer conductivity through the photoconductive effect. Inverted polythiophene:fullerene devices using ZnO-NP coated silver-nanowires or indium-tin-oxide as transparent electrode reached power conversion efficiencies of 2.4%.

Hybrid nanocrystal–polymer systems are promising candidates for photovoltaic applications, but the processes controlling charge generation are poorly understood. Here, we disentangle the energy- and charge-transfer processes occurring in a model system based on blends of cadmium selenide nanocrystals (CdSe-NC) with poly[2-methoxy-5-(3′,7′-dimethyloctyloxy)-1,4-phenylene vinylene] (MDMO-PPV) using a combination of time-resolved absorption and luminescence measurements. The use of different capping ligands (n-butylamine, oleic acid) as well as thermal annealing allows tuning of the polymer–nanocrystal interaction. We demonstrate that energy transfer from MDMO-PPV to CdSe-NCs is the dominant exciton quenching mechanism in nonannealed blends and occurs on ultrafast time scales (<1 ps). Upon thermal annealing electron transfer becomes competitive with energy transfer, with a transfer rate of 800 fs independent of the choice of the ligand. Interestingly, we find hole transfer to be much less efficient than electron transfer and to extend over several nanoseconds. Our results emphasize the importance of tuning the organic–nanocrystal interaction to achieve efficient charge separation and highlight the unfavorable hole-transfer dynamics in these blends.

We investigate charge dynamics in solar cells constructed using solution-processed layers of CuInS2 (CIS) nanocrystals (NCs) as the electron donor and CdS as the electron acceptor. By using time-resolved spectroscopic techniques, we are able to observe photoinduced absorptions that we attribute to the mobile hole carriers in the NC film. In combination with transient photocurrent and photovoltage measurements, we monitor charge dynamics on time scales from 300 fs to 1 ms. Carrier dynamics are investigated for devices with CIS layers composed of either colloidally synthesized 1,3-benzenedithiol-capped nanocrystals or in situ sol-gel synthesized thin films as the active layer. We find that deep trapping of holes in the colloidal NC cells is responsible for decreases in the open-circuit voltage and fill factor as compared to those of the sol-gel synthesized CIS/CdS cell.

Recently, we demonstrated that small-molecule azomethines are promising candidates as electron donating materials for organic photovoltaic devices. Azomethines can be prepared via well-known condensation chemistry with water being the sole by-product. Here we present a record power conversion efficiency for azomethine-based small-molecule OPV of 2.2%. To understand the underlying physics limiting device performance, TPA-TBT-TPA devices were characterized using a range of spectroscopic and electro-optical techniques. Light intensity dependent current-density measurement showed the presence of non-geminate charge recombination, which is most likely the result of poor charge mobility. In addition, transient absorption measurements showed a relatively short life time of the exciton (120 ps). However, due to the very fast charge dissociation (<300 fs) charge separation is relatively efficient. This knowledge presents a guideline for preparing subsequent generations of compounds with improved device performance.