Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification

Nature Communications
Daniel M KroupaMatthew C Beard

Abstract

Band edge positions of semiconductors determine their functionality in many optoelectronic applications such as photovoltaics, photoelectrochemical cells and light emitting diodes. Here we show that band edge positions of lead sulfide (PbS) colloidal semiconductor nanocrystals, specifically quantum dots (QDs), can be tuned over 2.0 eV through surface chemistry modification. We achieved this remarkable control through the development of simple, robust and scalable solution-phase ligand exchange methods, which completely replace native ligands with functionalized cinnamate ligands, allowing for well-defined, highly tunable chemical systems. By combining experiments and ab initio simulations, we establish clear relationships between QD surface chemistry and the band edge positions of ligand/QD hybrid systems. We find that in addition to ligand dipole, inter-QD ligand shell inter-digitization contributes to the band edge shifts. We expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications.

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Citations

Sep 8, 2018·Physical Chemistry Chemical Physics : PCCP·Melody L KesslerJillian L Dempsey
Jan 16, 2019·Nanoscale·Rafael AbarguesJuan P Martínez-Pastor
Mar 21, 2020·Advanced Materials·Margherita BiondiEdward H Sargent
Jul 27, 2017·Analytical and Bioanalytical Chemistry·Hani Nasser AbdelhamidHui-Fen Wu
Nov 30, 2019·The Journal of Chemical Physics·Haipeng LuMatthew C Beard
Aug 14, 2020·Physical Chemistry Chemical Physics : PCCP·James B DerrValentine I Vullev
Sep 25, 2020·Nature Communications·Seungjin LeeEdward H Sargent
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Oct 21, 2020·Small·Taewan KimJongmin Choi
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Jun 3, 2018·The Journal of Physical Chemistry Letters·Daniel M KroupaMatthew C Beard
Jul 26, 2018·Journal of the American Chemical Society·Lance M WheelerJoseph M Luther

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Methods Mentioned

BETA
infrared spectroscopy
nuclear magnetic resonance
PCR
X-ray
NMR

Software Mentioned

ESPRESSO
Quantum

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