The interparticle distance limit for multiple exciton dissociation in PbS quantum dot solid films.

Understanding the behaviour of multiple exciton dissociation in quantum dot (QD) solid films is of fundamental interest and paramount importance for improving the performance of quantum dot solar cells (QDSCs). Unfortunately, the charge transfer behaviour of photogenerated multiple exciton in QD solid films is not clear to date. Herein, we systematically investigate the multiple exciton charge transfer behaviour in PbS QD solid films by using ultrafast transient absorption spectroscopy. We observe that the multiple exciton charge transfer rate within QD ensembles is exponentially enhanced as the interparticle distance between the QDs decreases. Biexciton and triexciton dissociation between adjacent QDs occurs via a charge transfer tunneling effect just like single exciton, and the charge tunneling constants of the single exciton (ß1: 0.67 ± 0.02 nm-1), biexciton (ß2: 0.68 ± 0.05 nm-1) and triexciton (ß3: 0.71 ± 0.01 nm-1) are obtained. More importantly, for the first time, the interparticle distance limit (≤4.3 nm) for multiple exciton charge transfer between adjacent QDs is found for the extraction of multiple excitons rapidly before the occurrence of Auger recombination. This result points out a vital and necessary condition for the use of multiple excitons produced in PbS QD films, especially for their applications in QDSCs.

Interface Passivation Effects on the Photovoltaic Performance of Quantum Dot Sensitized Inverse Opal TiO2 Solar Cells.

Quantum dot (QD)-sensitized solar cells (QDSSCs) are expected to achieve higher energy conversion efficiency than traditional single-junction silicon solar cells due to the unique properties of QDs. An inverse opal (IO)-TiO2 (IO-TiO2) electrode is useful for QDSSCs because of its three-dimensional (3D) periodic nanostructures and better electrolyte penetration compared to the normal nanoparticles (NPs)-TiO2 (NPs-TiO2) electrode. We find that the open-circuit voltages Voc of the QDSSCs with IO-TiO2 electrodes are higher than those of QDSSCs with NPs-TiO2 electrodes. One important strategy for enhancing photovoltaic conversion efficiency of QDSSCs with IO-TiO2 electrodes is surface passivation of photoanodes using wide-bandgap semiconducting materials. In this study, we have proposed surface passivation on IO-TiO2 with ZnS coating before QD deposition. The efficiency of QDSSCs with IO-TiO2 electrodes is largely improved (from 0.74% to 1.33%) because of the enhancements of Voc (from 0.65 V to 0.74 V) and fill factor (FF) (from 0.37 to 0.63). This result indicates that ZnS passivation can reduce the interfacial recombination at the IO-TiO2/QDs and IO-TiO2/electrolyte interfaces, for which two possible explanations can be considered. One is the decrease of recombination at IO-TiO2/electrolyte interfaces, and the other one is the reduction of the back-electron injection from the TiO2 electrode to QDs. All of the above results are effective for improving the photovoltaic properties of QDSSCs.