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

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

doi:10.1021/acsnano.8b04850

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

Journal Article · Fri Sep 14 00:00:00 EDT 2018 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.8b04850· OSTI ID:1471985

Kroupa, Daniel M. ^[1]; Pach, Gregory F. ^[2]; ^[3]; ^[4]; Chernomordik, Boris D. ^[2]; Crisp, Ryan W. ^[1]; ^[1]; ^[2]; Singh, Rohan ^[5]; ^[5]; Galli, Giulia ^[3]; ^[2]

National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Chicago, IL (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

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 hetero-nanostructures 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 hetero-nanostructure 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 by 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); 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:: AC02-06CH11357; AC36-08GO28308

OSTI ID:: 1471985

Alternate ID(s):: OSTI ID: 1489380

Report Number(s):: NREL/JA--5900-71834

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 10 Vol. 12; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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