Proceedings of nanoGe September Meeting 2015 (NFM15)
Publication date: 8th June 2015
This presentation describes the permeability of PbS QD ligand shells consisting of mixed monolayers of 1H,1H,2H,2H-perfluorodecanethiol (PFDT) and decanethiol (DT) to substituted benzoquinone molecules (s-BQs), as probed by monitoring the photo-oxidation of the QDs by benzoquinone via photoluminescence and transient absorption spectroscopies. We demonstrate that increasing the fraction of PFDT in the PbS QD ligand shell reduces the efficiency of collisional photoinduced electron transfer between the nanocrystal and 2,3,4,5-tetramethyl-p-benzoquinone (Me4BQ) in solution corresponding to a decrease in the permeability of the alkylthiolate monolayer upon partial fluorination. Replacing only 23% of the total thiols in the PbS ligand shell with PFDT reduced the collisional quenching efficiency of Me4BQ by 80%, which we interpret as indicating that the fluorinated ligand is dispersed rather than phase separated within the alkylthiolate adlayer. We also find that the extent to which fluorinated ligands can reduce collisional charge transfer efficiency between PbS QDs and s-BQ molecules is correlated with the molecular volume of the quencher, despite the fact that all tested s-BQ molecules are poorly solubilized by fluorocarbon solvents. This result indicates that the PFDT ligands reduce the permeability of the alkylthiolate ligand shell primarily due to their steric bulk rather than their oleophobic nature.
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