Electrochemically n-Doped CsPbBr3 Nanocrystal Thin Films

Sungyeon Heo; Kwangdong Roh; Fengyu Zhang; Steven E. Tignor; Andrew B. Bocarsly; Antoine Kahn; Barry P. Rand

doi:10.1021/acsenergylett.1c02554

Electrochemically n-Doped CsPbBr₃ Nanocrystal Thin Films

Sungyeon Heo, Kwangdong Roh, Fengyu Zhang, Steven E. Tignor, Andrew B. Bocarsly, Antoine Kahn, Barry P. Rand

Department of Physics

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

Electrochemical doping is a promising strategy to dope halide perovskites without introducing impurities into the lattice. However, n-type doping of halide perovskites remains challenging due to intrinsically limited electrochemical stability. Herein, we report electrochemically n-doped CsPbBr₃ nanocrystal (NC) films within electrochemically stable potential windows (−0.9–0.5 V vs Ag/AgNO₃). Compared to bulk films with limited accessible surface area for cation charge compensation, NC films show more efficient n-doping properties due to their porous nature. Electrochemically doped NC films exhibit Fermi level shifts, confirmed via electrochemical measurements, vacuum-Kelvin probe contact potential difference, and photoelectron spectroscopy. As a result, in situ conductivity measurements show increases when films are p- or n-doped. Furthermore, n-doped films show a photoluminescence intensity increase. Given that we remain within the electrochemically stable window, we suspect this is due to an alleviation of electron traps, likely a result of altering the charge state of the interstitial Br population.

Original language	English
Pages (from-to)	211-216
Number of pages	6
Journal	ACS Energy Letters
Volume	7
Issue number	1
DOIs	https://doi.org/10.1021/acsenergylett.1c02554
State	Published - 14 Jan 2022

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Cite this

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title = "Electrochemically n-Doped CsPbBr3 Nanocrystal Thin Films",

abstract = "Electrochemical doping is a promising strategy to dope halide perovskites without introducing impurities into the lattice. However, n-type doping of halide perovskites remains challenging due to intrinsically limited electrochemical stability. Herein, we report electrochemically n-doped CsPbBr3 nanocrystal (NC) films within electrochemically stable potential windows (−0.9–0.5 V vs Ag/AgNO3). Compared to bulk films with limited accessible surface area for cation charge compensation, NC films show more efficient n-doping properties due to their porous nature. Electrochemically doped NC films exhibit Fermi level shifts, confirmed via electrochemical measurements, vacuum-Kelvin probe contact potential difference, and photoelectron spectroscopy. As a result, in situ conductivity measurements show increases when films are p- or n-doped. Furthermore, n-doped films show a photoluminescence intensity increase. Given that we remain within the electrochemically stable window, we suspect this is due to an alleviation of electron traps, likely a result of altering the charge state of the interstitial Br population.",

author = "Sungyeon Heo and Kwangdong Roh and Fengyu Zhang and Tignor, {Steven E.} and Bocarsly, {Andrew B.} and Antoine Kahn and Rand, {Barry P.}",

note = "Funding Information: This work was supported by ExxonMobil through its membership in the Princeton E-filliates Partnership of the Andlinger Center for Energy and the Environment. S.E.T. and A.B.B. acknowledge financial support by the National Science Foundation under grant CHE-1800400. A.K. acknowledges support from the US-Israel Binational Science Foundation (BSF grant #2018349). K.R. acknowledges support from DARPA Award no. N66001-20-1-4052. S.H. thanks Prof. Jeffrey Schwartz for allowing the use of a glovebox and Dr. Ross Kerner for helpful discussions. The authors acknowledge the use of Princeton{\textquoteright}s Imaging and Analysis Center, which is partially supported by the Princeton Center for Complex Materials, a National Science Foundation (NSF)-MRSEC program (DMR1420541). Publisher Copyright: {\textcopyright} 2021 American Chemical Society",

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T1 - Electrochemically n-Doped CsPbBr3 Nanocrystal Thin Films

AU - Heo, Sungyeon

AU - Roh, Kwangdong

AU - Zhang, Fengyu

AU - Tignor, Steven E.

AU - Bocarsly, Andrew B.

AU - Kahn, Antoine

AU - Rand, Barry P.

N1 - Funding Information: This work was supported by ExxonMobil through its membership in the Princeton E-filliates Partnership of the Andlinger Center for Energy and the Environment. S.E.T. and A.B.B. acknowledge financial support by the National Science Foundation under grant CHE-1800400. A.K. acknowledges support from the US-Israel Binational Science Foundation (BSF grant #2018349). K.R. acknowledges support from DARPA Award no. N66001-20-1-4052. S.H. thanks Prof. Jeffrey Schwartz for allowing the use of a glovebox and Dr. Ross Kerner for helpful discussions. The authors acknowledge the use of Princeton’s Imaging and Analysis Center, which is partially supported by the Princeton Center for Complex Materials, a National Science Foundation (NSF)-MRSEC program (DMR1420541). Publisher Copyright: © 2021 American Chemical Society

PY - 2022/1/14

Y1 - 2022/1/14

N2 - Electrochemical doping is a promising strategy to dope halide perovskites without introducing impurities into the lattice. However, n-type doping of halide perovskites remains challenging due to intrinsically limited electrochemical stability. Herein, we report electrochemically n-doped CsPbBr3 nanocrystal (NC) films within electrochemically stable potential windows (−0.9–0.5 V vs Ag/AgNO3). Compared to bulk films with limited accessible surface area for cation charge compensation, NC films show more efficient n-doping properties due to their porous nature. Electrochemically doped NC films exhibit Fermi level shifts, confirmed via electrochemical measurements, vacuum-Kelvin probe contact potential difference, and photoelectron spectroscopy. As a result, in situ conductivity measurements show increases when films are p- or n-doped. Furthermore, n-doped films show a photoluminescence intensity increase. Given that we remain within the electrochemically stable window, we suspect this is due to an alleviation of electron traps, likely a result of altering the charge state of the interstitial Br population.

AB - Electrochemical doping is a promising strategy to dope halide perovskites without introducing impurities into the lattice. However, n-type doping of halide perovskites remains challenging due to intrinsically limited electrochemical stability. Herein, we report electrochemically n-doped CsPbBr3 nanocrystal (NC) films within electrochemically stable potential windows (−0.9–0.5 V vs Ag/AgNO3). Compared to bulk films with limited accessible surface area for cation charge compensation, NC films show more efficient n-doping properties due to their porous nature. Electrochemically doped NC films exhibit Fermi level shifts, confirmed via electrochemical measurements, vacuum-Kelvin probe contact potential difference, and photoelectron spectroscopy. As a result, in situ conductivity measurements show increases when films are p- or n-doped. Furthermore, n-doped films show a photoluminescence intensity increase. Given that we remain within the electrochemically stable window, we suspect this is due to an alleviation of electron traps, likely a result of altering the charge state of the interstitial Br population.

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