Charger transfer at interfaces studied with non-linear infrared probes

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In this project, funded by the Chemical Structure, Dynamics and Mechanisms program of the NSF Chemistry Division, Professor Martin Zanni from the University of Wisconsin-Madison will utilize two-dimensional infrared (2D IR) and heterodyned sum-frequency generation (SFG) spectroscopies to study electron transfer across molecule/semiconductor interfaces. This process is one of the most fundamental aspects of solar-to-electrical and solar-to-fuel conversion processes, but is still not fully understood largely due to the difficulties in characterizing molecular structures at interfaces. These techniques will be used to resolve multiple dye conformations, map their individual kinetics by measuring the time-dependence of their respective cross peaks, and determine their conformations by measuring the angles of molecular bonds on single crystal interfaces. The broader impacts of this proposal include the training of undergraduates and graduate students in this multi-disciplinary field, the dissemination of our results at national ACS meetings and through refereed publications, and the development of a website to make it easy and efficient to keep up-to-date on developments in multidimensional spectroscopy. The goal is to provide a level of molecular detail not previously attainable for interfacial charge transfer, thereby leading to a better understanding of charge separation and transfer at molecule-semiconductor interfaces that is necessary for the rational design of organic dye- and quantum-dot sensitized solar and fuel cells.