Publication date: 1st July 2014
The direct nucleation of QD nanocrystals onto mesoporous oxide matrices by successive ionic layer adsorption and reaction (SILAR) represents a promising route towards the development of novel architectures for solar energy conversion. This low-cost solution process approach has shown considerable potential for controlling nanocrystal size (as evidenced by a red shift of the absorption threshold as a function of dipping steps) and providing high sensitizer loadings per oxide unit area; features that have allowed the development of sensitized solar cells with efficiencies above 5%. Despite the potential of SILAR systems, little research effort has been devoted to unravel the donor-acceptor electron transfer dynamics, a key aspect for optimum photovoltaic performance. In this work, photo-induced electron transfer (ET) processes in PbS/SnO2 SILAR based electrodes are investigated using optical pump-THz probe (OPTP) spectroscopy. The ET dynamics are correlated with QD structure determined using HRTEM analysis. ET rates are found to be independent of QD size, dielectric environment and temperature, suggesting Fermi level pinning at the QD/oxide interface and tunnelling as the ET related mechanism. On the other hand, ET rates in SILAR based QD sensitized oxides are found to be highly dependent on photo-excitation energy. This observation provides unambiguous proof that hot electron transfer processes take place at the intimate QD/oxide interface. The implications of these results for solar cell design are discussed.
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