JOURNAL ARTICLE
RESEARCH SUPPORT, NON-U.S. GOV'T
RESEARCH SUPPORT, U.S. GOV'T, NON-P.H.S.
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Noncovalent Control of the Electrostatic Potential of Quantum Dots through the Formation of Interfacial Ion Pairs.

This paper describes the role of tetraalkylammonium counterions [NR4 + , R = -CH3 , -CH2 CH3 , -(CH2 )2 CH3 , or -(CH2 )3 CH3 ] in gating the electrostatic potential at the interface between the 6-mercaptohexanoate (MHA) ligand shell of a PbS quantum dot (QD) and water. The permeability of this ligand shell to a negatively charged anthraquinone derivative (AQ), measured from the yield of electron transfer (eT) from the QD core to AQ, increases as the steric bulk of NR4 + increases (for a given concentration of NR4 + ). This result indicates that bulkier counterions screen repulsive interactions at the ligand/solvent interface more effectively than smaller counterions. Free energy scaling analysis and molecular dynamics simulations suggest that ion pairing between the ligand shell of the QD and NR4 + results from a combination of electrostatic and van der Waals components, and that the van der Waals interaction promotes ion pairing with longer-chain counterions and more effective screening. This work provides molecular-level details that dictate a nanoparticle's electrostatic potential and demonstrates the sensitivity of the yield of photoinduced charge transfer between a QD and a molecular probe to even low-affinity binding events at the QD/solvent interface.

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