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Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI_3 Nanocrystal Films

Gaulding, E. Ashley and Hao, Ji and Kang, Hyun Suk and Miller, Elisa M. and Habisreutinger, Severin N. and Zhao, Qian and Hazarika, Abhijit and Sercel, Peter C. and Luther, Joseph M. and Blackburn, Jeffrey L. (2019) Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI_3 Nanocrystal Films. Advanced Materials, 31 (27). Art. No. 1902250. ISSN 0935-9648. https://resolver.caltech.edu/CaltechAUTHORS:20190513-104335650

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Abstract

Doping of semiconductors enables fine control over the excess charge carriers, and thus the overall electronic properties, crucial to many technologies. Controlled doping in lead‐halide perovskite semiconductors has thus far proven to be difficult. However, lower dimensional perovskites such as nanocrystals, with their high surface‐area‐to‐volume ratio, are particularly well‐suited for doping via ground‐state molecular charge transfer. Here, the tunability of the electronic properties of perovskite nanocrystal arrays is detailed using physically adsorbed molecular dopants. Incorporation of the dopant molecules into electronically coupled CsPbI_3 nanocrystal arrays is confirmed via infrared and photoelectron spectroscopies. Untreated CsPbI_3 nanocrystal films are found to be slightly p‐type with increasing conductivity achieved by incorporating the electron‐accepting dopant 2,3,5,6‐tetrafluoro‐7,7,8,8‐tetracyanoquinodimethane (F_4TCNQ) and decreasing conductivity for the electron‐donating dopant benzyl viologen. Time‐resolved spectroscopic measurements reveal the time scales of Auger‐mediated recombination in the presence of excess electrons or holes. Microwave conductance and field‐effect transistor measurements demonstrate that both the local and long‐range hole mobility are improved by F_4TCNQ doping of the nanocrystal arrays. The improved hole mobility in photoexcited p‐type arrays leads to a pronounced enhancement in phototransistors.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1002/adma.201902250DOIArticle
ORCID:
AuthorORCID
Miller, Elisa M.0000-0002-7648-5433
Zhao, Qian0000-0001-6939-3568
Hazarika, Abhijit0000-0003-0391-2163
Sercel, Peter C.0000-0002-1734-3793
Luther, Joseph M.0000-0002-4054-8244
Blackburn, Jeffrey L.0000-0002-9237-5891
Alternate Title:Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI3 Nanocrystal Films
Additional Information:© 2019 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim. Received: April 8, 2019; Published online: May 10, 2019. J.L.B., J.M.L., J.H., Q.Z., and A.H. were supported by the Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE), an Energy Frontier Research Center funded by the Office of Science, Office of Basic Energy Sciences within the U.S. Department of Energy. For photoelectron spectroscopy measurements and transient absorption measurements, EMM and HSK, respectively, acknowledge support from the Solar Photochemistry Program, Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy. EAG and SNH acknowledge support from the Director's Fellowship within NREL's Laboratory Directed Research and Development (LDRD) program. Part of this work was authored by Alliance for Sustainable Energy, Limited Liability Company, the manager and operator of the National Renewable Energy Laboratory under Contract No. DE‐AC36‐08GO28308. The views expressed in the article do not necessarily represent the views of the Department of Energy 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 conflict of interest.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE‐AC36‐08GO28308
Subject Keywords:detectors; doping; nanocrystals; perovskites; transport
Issue or Number:27
Record Number:CaltechAUTHORS:20190513-104335650
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20190513-104335650
Official Citation:Gaulding, E. A., Hao, J., Kang, H. S., Miller, E. M., Habisreutinger, S. N., Zhao, Q., Hazarika, A., Sercel, P. C., Luther, J. M., Blackburn, J. L., Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI3 Nanocrystal Films. Adv. Mater. 2019, 31, 1902250. https://doi.org/10.1002/adma.201902250
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:95431
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:13 May 2019 18:41
Last Modified:09 Mar 2020 13:19

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