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Published July 5, 2019 | Supplemental Material
Journal Article Open

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

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.

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.

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August 22, 2023
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