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n-Type PbSe Quantum Dots via Post-Synthetic Indium Doping

Lu, Haipeng and Carroll, Gerard M. and Chen, Xihan and Amarasinghe, Dinesh K. and Neale, Nathan R. and Miller, Elisa M. and Sercel, Peter C. and Rabuffetti, Federico A. and Efros, Alexander L. and Beard, Matthew C. (2018) n-Type PbSe Quantum Dots via Post-Synthetic Indium Doping. Journal of the American Chemical Society, 140 (42). pp. 13753-13763. ISSN 0002-7863. http://resolver.caltech.edu/CaltechAUTHORS:20180926-082555531

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Abstract

We developed a postsynthetic treatment to produce impurity n-type doped PbSe QDs with In^(3+) as the substitutional dopant. Increasing the incorporated In content is accompanied by a gradual bleaching of the interband first-exciton transition and concurrently the appearance of a size-dependent, intraband absorption, suggesting the controlled introduction of delocalized electrons into the QD band edge states under equilibrium conditions. We compare the optical properties of our In-doped PbSe QDs to cobaltocene treated QDs, where the n-type dopant arises from remote reduction of the PbSe QDs and observe similar behavior. Spectroelectrochemical measurements also demonstrate characteristic n-type signatures, including both an induced absorption within the electrochemical bandgap and a shift of the Fermi-level toward the conduction band. Finally, we demonstrate that the In^(3+) dopants can be reversibly removed from the PbSe QDs, whereupon the first exciton bleach is recovered. Our results demonstrate that PbSe QDs can be controllably n-type doped via impurity aliovalent substitutional doping.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/jacs.8b07910DOIArticle
https://pubs.acs.org/doi/suppl/10.1021/jacs.8b07910PublisherSupporting Information
ORCID:
AuthorORCID
Lu, Haipeng0000-0003-0252-3086
Carroll, Gerard M.0000-0003-0195-8483
Chen, Xihan0000-0001-7907-2549
Neale, Nathan R.0000-0001-5654-1664
Miller, Elisa M.0000-0002-7648-5433
Rabuffetti, Federico A.0000-0001-8500-3427
Efros, Alexander L.0000-0003-1938-553X
Beard, Matthew C.0000-0002-2711-1355
Additional Information:© 2018 American Chemical Society. Received: July 25, 2018; Published: September 26, 2018. We acknowledge support at NREL from the Solar Photochemistry Program within the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, Office of Science within the U.S. Department of Energy. D.K.A. and F.A.R. acknowledge the support provided by Wayne State University and by the Research Corporation for Science Advancement through a Cottrell Scholar Award. A.L.E. acknowledges financial support of the Office of Naval Research (ONR) through the Naval Research Laboratory Basic Research Program. Part of this work was authored by the Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under Contract DE-AC36-08GO28308. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC36-08GO28308
Wayne State UniversityUNSPECIFIED
Research CorporationUNSPECIFIED
Office of Naval Research (ONR)UNSPECIFIED
Record Number:CaltechAUTHORS:20180926-082555531
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20180926-082555531
Official Citation:n-Type PbSe Quantum Dots via Post-Synthetic Indium Doping. Haipeng Lu, Gerard M. Carroll, Xihan Chen, Dinesh K. Amarasinghe, Nathan R. Neale, Elisa M. Miller, Peter C. Sercel, Federico A. Rabuffetti, Alexander L. Efros, and Matthew C. Beard. Journal of the American Chemical Society 2018 140 (42), 13753-13763. DOI: 10.1021/jacs.8b07910
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:89946
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:26 Sep 2018 17:52
Last Modified:25 Oct 2018 16:53

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