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

Kroupa, Daniel M.; Vörös, Márton; Brawand, Nicholas P.; McNichols, Brett W.; Miller, Elisa M.; Gu, Jing; Nozik, Arthur J.; Sellinger, Alan; Galli, Giulia; Beard, Matthew C.

doi:10.1038/ncomms15257

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

Journal Article · Tue May 16 00:00:00 EDT 2017 · Nature Communications

DOI:https://doi.org/10.1038/ncomms15257· OSTI ID:1357948

Kroupa, Daniel M. ^[1]; Vörös, Márton ^[2]; Brawand, Nicholas P. ^[3]; McNichols, Brett W. ^[4]; Miller, Elisa M. ^[5]; Gu, Jing ^[5];

^[1]; Sellinger, Alan ^[6]; Galli, Giulia ^[2]; Beard, Matthew C. ^[5]

National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chicago, Chicago, IL (United States)
Univ. of Chicago, Chicago, IL (United States)
Colorado School of Mines, Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)

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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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC36-08GO28308; AC02-06CH11357

OSTI ID:: 1357948

Alternate ID(s):: OSTI ID: 1373584

Report Number(s):: NREL/JA-5900-66738

Journal Information:: Nature Communications, Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 183 works

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

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