Temperature-dependent permeability of the ligand shell of PbS quantum dots probed by electron transfer to benzoquinone

Kenneth O. Aruda, Miriam Bohlmann Kunz, Mario Tagliazucchi, Emily A Weiss

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

This paper describes an increase in the yield of collisionally gated photoinduced electron transfer (electron transfer events per collision) from oleate-capped PbS quantum dots (QDs) to benzoquinone (BQ) with increasing temperature (from 0 to 50 °C), due to increased permeability of the oleate adlayer of the QDs to BQ. The same changes in intermolecular structure of the adlayer that increase its permeability to BQ also increase its permeability to the solvent, toluene, resulting in a decrease in viscous drag and an apparent increase in the diffusion coefficient of the QDs, as measured by diffusion-ordered spectroscopy (DOSY) NMR. Comparison of NMR and transient absorption spectra of QDs capped with flexible oleate with those capped with rigid methylthiolate provides evidence that the temperature dependence of the permeability of the oleate ligand shell is due to formation of transient gaps in the adlayer through conformational fluctuations of the ligands.

Original languageEnglish
Pages (from-to)2841-2846
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume6
Issue number14
DOIs
Publication statusPublished - Jul 16 2015

Fingerprint

quinones
Oleic Acid
Semiconductor quantum dots
permeability
electron transfer
Ligands
quantum dots
ligands
Electrons
viscous drag
Temperature
nuclear magnetic resonance
temperature
Toluene
Nuclear magnetic resonance spectroscopy
Drag
toluene
Absorption spectra
diffusion coefficient
Nuclear magnetic resonance

Keywords

  • quantum dots

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

Temperature-dependent permeability of the ligand shell of PbS quantum dots probed by electron transfer to benzoquinone. / Aruda, Kenneth O.; Bohlmann Kunz, Miriam; Tagliazucchi, Mario; Weiss, Emily A.

In: Journal of Physical Chemistry Letters, Vol. 6, No. 14, 16.07.2015, p. 2841-2846.

Research output: Contribution to journalArticle

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