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

Lu, Haipeng; Carroll, Gerard M.; Chen, Xihan; Amarasinghe, Dinesh K.; Neale, Nathan R.; Miller, Elisa M.; Sercel, Peter C.; Rabuffetti, Federico A.; Efros, Alexander L.; Beard, Matthew C.

doi:10.1021/jacs.8b07910

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

Journal Article · Wed Sep 26 00:00:00 EDT 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b07910· OSTI ID:1487326

Lu, Haipeng ^[1]; Carroll, Gerard M. ^[1]; Chen, Xihan ^[1]; Amarasinghe, Dinesh K. ^[2]; Neale, Nathan R. ^[1]; Miller, Elisa M. ^[1]; Sercel, Peter C. ^[3]; Rabuffetti, Federico A. ^[2]; Efros, Alexander L. ^[4]; Beard, Matthew C. ^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States)
Wayne State Univ., Detroit, MI (United States)
California Inst. of Technology (CalTech), Pasadena, CA (United States)
Naval Research Lab. (NRL), Washington, DC (United States)

We developed a postsynthetic treatment to produce impurity n-type doped PbSe QDs with In³⁺ 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 In³⁺ 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.

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Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

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

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1487326

Report Number(s):: NREL/JA-5900-72021

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 42; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 24 works

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