Optical Absorbance Enhancement in PbS QD/Cinnamate Ligand Complexes

Kroupa, Daniel M.; Voros, Marton; Brawand, Nicholas P.; Bronstein, Noah; McNichols, Brett W.; Castaneda, Chloe V.; Nozik, Arthur J.; Sellinger, Alan; Galli, Giulia; Beard, Matthew C.

doi:10.1021/acs.jpclett.8b01451

Title: Optical Absorbance Enhancement in PbS QD/Cinnamate Ligand Complexes

Journal Article · 31 May 2018 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.8b01451 · OSTI ID:1457664

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^[4]; McNichols, Brett W. ^[5]; Castaneda, Chloe V. ^[4];

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

We studied the optical absorption enhancement in colloidal suspensions of PbS quantum dots (QD) upon ligand exchange from oleate to a series of cinnamate ligands. By combining experiments and ab initio simulations, we elucidate physical parameters that govern the optical absorption enhancement. We find that within the cinnamate/PbS QD system the optical absorption enhancement scales linearly with the electronic gap of the ligand, indicating that the ligand/QD coupling occurs equally efficient between the QD and ligand HOMO and their respective LUMO levels. Disruption of the conjugation that connects the aromatic ring and its substituents to the QD core causes a reduction of the electronic coupling. Our results further support the notion that the ligand/QD complex should be considered as a distinct chemical system with emergent behavior rather than a QD core with ligands whose sole purpose is to passivate surface dangling bonds and prevent agglomeration.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1457664

Report Number(s):: NREL/JA-5900-70974

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 12 Vol. 9; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Optical Absorbance Enhancement in PbS QD/Cinnamate Ligand Complexes

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