We have assembled hybrid nanostructures that couple light harvesting II-VI nanocrystals with redox catalysts that perform proton reduction and water oxidation. The functionality of such hybrid structures depends strongly on the charge transfer kinetics between the photoexcited nanocrystal and the catalyst. We utilize ultrafast transient absorption spectroscopy to examine the dynamics of nanocrystal-catalyst charge transfer and the competitiveness of this process with the energy-wasting charge recombination. Our recent findings identifying kinetic bottlenecks for photochemistry will be discussed. Our ongoing efforts to design nanocrystal structure and surface chemistry to enhance the kinetic competitiveness of the photochemical pathways will be described. References: 1. M. B. Wilker, K. E. Shinopoulos, K. A. Brown, D. W. Mulder, P. W. King, G. Dukovic. “Electron transfer kinetics in CdS nanorod-[FeFe] hydrogenase complexes an implications for photochemical H2 generation.” Journal of the American Chemical Society, 2014, 136, 4316-4364. 2. H-W. Tseng, M. B. Wilker, N. H. Damrauer, G. Dukovic. “Charge Transfer Dynamics between Photoexcited CdS Nanorods and Mononuclear Ru Water-Oxidation Catalysts” Journal of the American Chemical Society, 2013, 135, 3383-3386. 3. K. A. Brown, M. B. Wilker, M. Boehm, G. Dukovic, P. W. King. “Characterization of photochemical processes for H2 production by CdS nanorod-[FeFe] hydrogenase complexes.” Journal of the American Chemical Society, 2012, 134, 5627–5636.

Photochemical reactions of semiconductor nanocrystals coupled with redox catalysts

249th National Meeting (2015)

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