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Kroupa DM, Pach GF, Vörös M, et al. Enhanced Multiple Exciton Generation in PbS|CdS Janus-like Heterostructured Nanocrystals. ACS Nano. 2018;12(10):10084-10094doi: 10.1021/acsnano.8b04850.
Kroupa, D. M., Pach, G. F., Vörös, M., Giberti, F., Chernomordik, B. D., Crisp, R. W., Nozik, A. J., Johnson, J. C., Singh, R., Klimov, V. I., Galli, G., & Beard, M. C. (2018). Enhanced Multiple Exciton Generation in PbS|CdS Janus-like Heterostructured Nanocrystals. ACS nano, 12(10), 10084-10094. https://doi.org/10.1021/acsnano.8b04850
Kroupa, Daniel M, et al. "Enhanced Multiple Exciton Generation in PbS|CdS Janus-like Heterostructured Nanocrystals." ACS nano vol. 12,10 (2018): 10084-10094. doi: https://doi.org/10.1021/acsnano.8b04850
Kroupa DM, Pach GF, Vörös M, Giberti F, Chernomordik BD, Crisp RW, Nozik AJ, Johnson JC, Singh R, Klimov VI, Galli G, Beard MC. Enhanced Multiple Exciton Generation in PbS|CdS Janus-like Heterostructured Nanocrystals. ACS Nano. 2018 Oct 23;12(10):10084-10094. doi: 10.1021/acsnano.8b04850. Epub 2018 Sep 21. PMID: 30216045.
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ACS Nano. 2018 Oct 23;12(10):10084-10094. doi: 10.1021/acsnano.8b04850. Epub 2018 Sep 21.

Enhanced Multiple Exciton Generation in PbS|CdS Janus-like Heterostructured Nanocrystals.

ACS nano

Daniel M Kroupa, Gregory F Pach, Márton Vörös, Federico Giberti, Boris D Chernomordik, Ryan W Crisp, Arthur J Nozik, Justin C Johnson, Rohan Singh, Victor I Klimov, Giulia Galli, Matthew C Beard

Affiliations

  1. Chemistry & Nanoscience Center , National Renewable Energy Laboratory , Golden , Colorado 80401 , United States.
  2. Department of Chemistry and Biochemistry , University of Colorado , Boulder , Colorado 80309 , United States.
  3. Materials Science Division , Argonne National Laboratory , Lemont , Illinois 60439 , United States.
  4. Institute for Molecular Engineering , University of Chicago , Chicago , Illinois 60637 , United States.
  5. Department of Physics , Colorado School of Mines , Golden , Colorado 80401 , United States.
  6. Chemistry Division , Los Alamos National Laboratory , Los Alamos , New Mexico 87545 , United States.
  7. Department of Chemistry , University of Chicago , Chicago , Illinois 60637 , United States.

PMID: 30216045 DOI: 10.1021/acsnano.8b04850

Abstract

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.

Keywords: carrier multiplication; multiple excition generation; nanocrystal; quantum dot; solar cell; transient absorption spectroscopy

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