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    Enhanced Multiple Exciton Generation in PbS|CdS Janus-like Heterostructured Nanocrystals
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    • Daniel M. Kroupa
      Daniel M. Kroupa
      Chemistry & Nanoscience Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States
      Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado 80309, United States
      More by Daniel M. Kroupa
    • Gregory F. Pach
      Gregory F. Pach
      Chemistry & Nanoscience Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States
      More by Gregory F. Pach
    • Márton Vörös
      Márton Vörös
      Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
      Institute for Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States
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      Orcidhttp://orcid.org/0000-0003-1321-9207
    • Federico Giberti
      Federico Giberti
      Institute for Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States
      More by Federico Giberti
      Orcidhttp://orcid.org/0000-0003-0830-8141
    • Boris D. Chernomordik
      Boris D. Chernomordik
      Chemistry & Nanoscience Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States
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    • Ryan W. Crisp
      Ryan W. Crisp
      Chemistry & Nanoscience Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States
      Department of Physics, Colorado School of Mines, Golden, Colorado 80401, United States
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    • Arthur J. Nozik
      Arthur J. Nozik
      Chemistry & Nanoscience Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States
      Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado 80309, United States
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      Orcidhttp://orcid.org/0000-0001-7176-7645
    • Justin C. Johnson
      Justin C. Johnson
      Chemistry & Nanoscience Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States
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      Orcidhttp://orcid.org/0000-0002-8874-6637
    • Rohan Singh
      Rohan Singh
      Chemistry Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States
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    • Victor I. Klimov
      Victor I. Klimov
      Chemistry Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States
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      Orcidhttp://orcid.org/0000-0003-1158-3179
    • Giulia Galli
      Giulia Galli
      Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
      Institute for Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States
      Department of Chemistry, University of Chicago, Chicago, Illinois 60637, United States
      More by Giulia Galli
    • Matthew C. Beard*
      Matthew C. Beard
      Chemistry & Nanoscience Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States
      *E-mail: [email protected]
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      Orcidhttp://orcid.org/0000-0002-2711-1355
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    ACS Nano

    Cite this: ACS Nano 2018, 12, 10, 10084–10094
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    https://doi.org/10.1021/acsnano.8b04850
    Published September 14, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    Generating multiple excitons by a single high-energy photon is a promising third-generation solar energy conversion strategy. We demonstrate that multiple exciton generation (MEG) in PbS|CdS Janus-like heteronanostructures is enhanced over that of single-component and core/shell nanocrystal architectures, with an onset close to two times the PbS band gap. We attribute the enhanced MEG to the asymmetric nature of the heteronanostructure that results in an increase in the effective Coulomb interaction that drives MEG and a reduction of the competing hot exciton cooling rate. Slowed cooling occurs through effective trapping of hot-holes by a manifold of valence band interfacial states having both PbS and CdS character, as evidenced by photoluminescence studies and ab initio calculations. Using transient photocurrent spectroscopy, we find that the MEG characteristics of the individual nanostructures are maintained in conductive arrays and demonstrate that these quasi-spherical PbS|CdS nanocrystals can be incorporated as the main absorber layer in functional solid-state solar cell architectures. Finally, based upon our analysis, we provide design rules for the next generation of engineered nanocrystals to further improve the MEG characteristics.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.8b04850.

    • Absorbance, PL, PLE, and XRD of Janus-like nanocrystals with varying Pb:Cd ratios, hyperspectral transient absorption surface plots and representative transient absorption data with MEG analysis, structural model and computational results detailing energy alignment, exciton quantum yield plotted for systems of differing MEG efficiency, computed MEG rates for Janus-like nanocrystals with and without interface states as well as a varying electric field, additional TRPL plots with time-integrated PL spectra, EQE from the device shown in Figure 7b (PDF)

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    Cited By

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    This article is cited by 59 publications.

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    ACS Nano

    Cite this: ACS Nano 2018, 12, 10, 10084–10094
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.8b04850
    Published September 14, 2018
    Copyright © 2018 American Chemical Society
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