Surface Chemistry Matters. How Ligands Influence Excited State Interactions between CsPbBr3 and Methyl Viologen
Jeffrey DuBose a b, Prashant Kamat a b
a Department of Chemistry, University of Notre Dame, United States
b Radiation Laboratory, University of Notre Dame, US, United States
Proceedings of Internet Conference for Quantum Dots (iCQD)
Online, Spain, 2020 July 14th - 17th
Organizers: Quinten Akkerman, Raffaella Buonsanti, Zeger Hens and Maksym Kovalenko
Poster, Jeffrey DuBose, 066
Publication date: 3rd July 2020

The photocatalytic properties of cesium lead bromide (CsPbBr3) perovskite nanocrystals make them attractive for designing light harvesting assemblies. Often ignored, the surface chemistry can dictate the excited state interactions of these semiconductor nanocrystals with charge-shuttling redox molecules. We have now explored the impact of CsPbBr3 nanocrystal surface modification on the excited state interactions with methyl viologen (MV2+) for three different ligand environments: prototypical oleic acid/oleylamine (OA/OAm) ligands, PbSO4-oleate capping, and didodecyldimethylammonium bromide (DDAB) ligands. Native OA/OAm ligands and PbSO4-oleate capping exhibit the strongest complexation with MV2+, whereas the bulky DDAB ligand environment shows an order of magnitude weaker complexation. The electron transfer rate constants as measured from transient absorption spectroscopy vary in the range of 1.2–3.6 × 1011 s–1 for different ligand environments. For DDAB-CsPbBr3 NCs, the efficiency of electron transfer (Φet) is 73%. Despite a protective capping layer, PbSO4-oleate capped CsPbBr3 maintains a redox-active surface which is viable for photocatalytic applications. These results highlight the impact of surface chemistry on excited state interactions of CsPbBr3 NCs and photocatalytic applications.

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