Quantum yield regeneration: influence of neutral ligand binding on photophysical properties in colloidal core/shell quantum dots

ACS Nano
Yi ShenAndrew B Greytak

Abstract

This article describes an experiment designed to identify the role of specific molecular ligands in maintaining the high photoluminescence (PL) quantum yield (QY) observed in as-synthesized CdSe/CdZnS and CdSe/CdS quantum dots (QDs). Although it has been possible for many years to prepare core/shell quantum dots with near-unity quantum yield through high-temperature colloidal synthesis, purification of such colloidal particles is frequently accompanied by a reduction in quantum yield. Here, a recently established gel permeation chromatography (GPC) technique is used to remove weakly associated ligands without a change in solvent: a decrease in ensemble QY and average PL lifetime is observed. Minor components of the initial mixture that were removed by GPC are then added separately to purified QD samples to determine whether reintroduction of these components can restore the photophysical properties of the initial sample. We show that among these putative ligands trioctylphosphine and cadmium oleate can regenerate the initial high QY of all samples, but only the "L-type" ligands (trioctyphosphine and oleylamine) can restore the QY without changing the shapes of the optical spectra. On the basis of the PL decay analysis, we confi...Continue Reading

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Citations

Jun 25, 2015·Chemical Reviews·Graham H CareyEdward H Sargent
Jun 18, 2016·Journal of the American Chemical Society·Chaodan Pu, Xiaogang Peng
Jul 1, 2016·Physical Chemistry Chemical Physics : PCCP·R SchneiderA Eychmüller
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Dec 30, 2020·Chemical Reviews·Cherie R KaganSarah M Thompson
Jun 1, 2021·Chemistry of Materials : a Publication of the American Chemical Society·Indy du FosséArjan J Houtepen
Jul 20, 2021·Chemical Science·Constantin D SahmErwin Reisner
Feb 9, 2017·Journal of the American Chemical Society·Chaodan PuXiaogang Peng
Mar 7, 2020·Nano Letters·Danielle A HenckelBrandi M Cossairt
Jul 6, 2019·Chemistry of Materials : a Publication of the American Chemical Society·Indy du FosséArjan J Houtepen
Aug 14, 2020·Nano Letters·Orian ElimelechUri Banin
Jan 15, 2021·Journal of the American Chemical Society·Carolyn L HartleyJillian L Dempsey

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