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

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. As a result, we expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [5] ; ORCiD logo [1] ;  [6] ;  [2] ;  [5]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chicago, Chicago, IL (United States)
  3. Univ. of Chicago, Chicago, IL (United States)
  4. Colorado School of Mines, Golden, CO (United States)
  5. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  6. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
Publication Date:
Report Number(s):
NREL/JA-5900-66738
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC36-08GO28308; AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Energy Frontier Research Center; Center for Advanced Solar Photophysics; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences, and Biosciences Division
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; quantum dots; band edge positions; ligand exchange; electronic properties and materials; organic-inorganic nanostructures; chemical synthesis
OSTI Identifier:
1357948
Alternate Identifier(s):
OSTI ID: 1373584