Proceedings of nanoGe September Meeting 2015 (NFM15)
Publication date: 8th June 2015
Harvesting multiexcitons populating semiconductor quantum dots (generated by either solar concentration or carrier multiplication) could pave the way towards high efficient photovoltaic devices. In this work, using optical pump THz probe spectroscopy, we investigate interfacial biexciton transfer dynamics from PbS quantum dots directly nucleated onto mesoporous SnO2 film as a function of impinging photon flux and photon energy. We demonstrate that sub-picosecond dissociation of biexcitons populating the quantum dots can be achieved in sensitized systems. Furthermore, we show that the competition between interfacial biexciton dissociation and Auger recombination within the quantum dots dictates the efficiency of the process. For our sample geometry, we resolve that biexciton dissociation efficiency approach unity quantum yield by either delocalizing holes in the QD capping shell (which can reduce the electron-hole interactions within the QDs and then reduce Auger recombination rates) and/or when generating hot (non-relaxed) biexciton populations within the QDs (which can enhance donor-acceptor coupling strength and then boost interfacial biexciton dissociation). Implications of these results for solar energy conversion are discussed.
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