Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI3 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 CsPbI3 nanocrystal arrays is confirmed via infrared and photoelectron spectroscopies. Untreated CsPbI3 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 (F4TCNQ) 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 F4TCNQ doping of the nanocrystal arrays. The improved hole mobility in photoexcited p-type arrays leads to a pronounced enhancement in phototransistors.
- Authors:
-
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- California Inst. of Technology (CalTech), Pasadena, CA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Solar Photochemistry Program; USDOE National Renewable Energy Laboratory (NREL), Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1514850
- Alternate Identifier(s):
- OSTI ID: 1511887
- Report Number(s):
- NREL/JA-5K00-73496
Journal ID: ISSN 0935-9648
- Grant/Contract Number:
- AC36-08GO28308; AC36‐08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Volume: 31; Journal Issue: 27; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; detectors; doping; nanocrystals; perovskites; transport
Citation Formats
Gaulding, Elizabeth, Hao, Ji, Kang, Hyun Suk, Link, Elisa M., Habisreutinger, Severin N., Zhao, Qian, Hazarika, Abhijit, Sercel, Peter C., Luther, Joseph M., and Blackburn, Jeffrey L. Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI3 Nanocrystal Films. United States: N. p., 2019.
Web. doi:10.1002/adma.201902250.
Gaulding, Elizabeth, Hao, Ji, Kang, Hyun Suk, Link, Elisa M., Habisreutinger, Severin N., Zhao, Qian, Hazarika, Abhijit, Sercel, Peter C., Luther, Joseph M., & Blackburn, Jeffrey L. Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI3 Nanocrystal Films. United States. https://doi.org/10.1002/adma.201902250
Gaulding, Elizabeth, Hao, Ji, Kang, Hyun Suk, Link, Elisa M., Habisreutinger, Severin N., Zhao, Qian, Hazarika, Abhijit, Sercel, Peter C., Luther, Joseph M., and Blackburn, Jeffrey L. Fri .
"Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI3 Nanocrystal Films". United States. https://doi.org/10.1002/adma.201902250. https://www.osti.gov/servlets/purl/1514850.
@article{osti_1514850,
title = {Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI3 Nanocrystal Films},
author = {Gaulding, Elizabeth and Hao, Ji and Kang, Hyun Suk and Link, Elisa M. and Habisreutinger, Severin N. and Zhao, Qian and Hazarika, Abhijit and Sercel, Peter C. and Luther, Joseph M. and Blackburn, Jeffrey L.},
abstractNote = {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 CsPbI3 nanocrystal arrays is confirmed via infrared and photoelectron spectroscopies. Untreated CsPbI3 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 (F4TCNQ) 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 F4TCNQ doping of the nanocrystal arrays. The improved hole mobility in photoexcited p-type arrays leads to a pronounced enhancement in phototransistors.},
doi = {10.1002/adma.201902250},
journal = {Advanced Materials},
number = 27,
volume = 31,
place = {United States},
year = {Fri May 10 00:00:00 EDT 2019},
month = {Fri May 10 00:00:00 EDT 2019}
}
Web of Science
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