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Title: Efficiency of Charge-Transfer Doping in Organic Semiconductors Probed with Quantitative Microwave and Direct-Current Conductance

Abstract

Although molecular charge-transfer doping is widely used to manipulate carrier density in organic semiconductors, only a small fraction of charge carriers typically escape the Coulomb potential of dopant counterions to contribute to electrical conductivity. Here, we utilize microwave and direct-current (DC) measurements of electrical conductivity to demonstrate that a high percentage of charge carriers in redox-doped semiconducting single-walled carbon nanotube (s-SWCNT) networks is delocalized as a free carrier density in the p-electron system (estimated as >46% at high doping densities). The microwave and four-point probe conductivities of hole-doped s-SWCNT films quantitatively match over almost 4 orders of magnitude in conductance, indicating that both measurements are dominated by the same population of delocalized carriers. We address the relevance of this surprising one-to-one correspondence by discussing the degree to which local environmental parameters (e.g., tube-tube junctions, Coulombic stabilization, and local bonding environment) may impact the relative magnitudes of each transport measurement.

Authors:
 [1];  [2];  [1];  [1];  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1484594
Report Number(s):
NREL/JA-5K00-72779
Journal ID: ISSN 1948-7185
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 23; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Citation Formats

Ferguson, Andrew J., Reid, Obadiah G., Nanayakkara, Sanjini U., Ihly, Rachelle, and Blackburn, Jeffrey L.. Efficiency of Charge-Transfer Doping in Organic Semiconductors Probed with Quantitative Microwave and Direct-Current Conductance. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b03074.
Ferguson, Andrew J., Reid, Obadiah G., Nanayakkara, Sanjini U., Ihly, Rachelle, & Blackburn, Jeffrey L.. Efficiency of Charge-Transfer Doping in Organic Semiconductors Probed with Quantitative Microwave and Direct-Current Conductance. United States. https://doi.org/10.1021/acs.jpclett.8b03074
Ferguson, Andrew J., Reid, Obadiah G., Nanayakkara, Sanjini U., Ihly, Rachelle, and Blackburn, Jeffrey L.. 2018. "Efficiency of Charge-Transfer Doping in Organic Semiconductors Probed with Quantitative Microwave and Direct-Current Conductance". United States. https://doi.org/10.1021/acs.jpclett.8b03074. https://www.osti.gov/servlets/purl/1484594.
@article{osti_1484594,
title = {Efficiency of Charge-Transfer Doping in Organic Semiconductors Probed with Quantitative Microwave and Direct-Current Conductance},
author = {Ferguson, Andrew J. and Reid, Obadiah G. and Nanayakkara, Sanjini U. and Ihly, Rachelle and Blackburn, Jeffrey L.},
abstractNote = {Although molecular charge-transfer doping is widely used to manipulate carrier density in organic semiconductors, only a small fraction of charge carriers typically escape the Coulomb potential of dopant counterions to contribute to electrical conductivity. Here, we utilize microwave and direct-current (DC) measurements of electrical conductivity to demonstrate that a high percentage of charge carriers in redox-doped semiconducting single-walled carbon nanotube (s-SWCNT) networks is delocalized as a free carrier density in the p-electron system (estimated as >46% at high doping densities). The microwave and four-point probe conductivities of hole-doped s-SWCNT films quantitatively match over almost 4 orders of magnitude in conductance, indicating that both measurements are dominated by the same population of delocalized carriers. We address the relevance of this surprising one-to-one correspondence by discussing the degree to which local environmental parameters (e.g., tube-tube junctions, Coulombic stabilization, and local bonding environment) may impact the relative magnitudes of each transport measurement.},
doi = {10.1021/acs.jpclett.8b03074},
url = {https://www.osti.gov/biblio/1484594}, journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 23,
volume = 9,
place = {United States},
year = {2018},
month = {11}
}

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Cited by: 9 works
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Works referenced in this record:

The Disperse Charge-Carrier Kinetics in Regioregular Poly(3-hexylthiophene)
journal, November 2004


Quantitative analysis of time-resolved microwave conductivity data
journal, November 2017


Temperature-Dependent Charge Transport in Polymer-Sorted Semiconducting Carbon Nanotube Networks with Different Diameter Distributions
journal, July 2018


Extracting the field-effect mobilities of random semiconducting single-walled carbon nanotube networks: A critical comparison of methods
journal, November 2017


Homogeneous dispersion of organic p-dopants in an organic semiconductor as an origin of high charge generation efficiency
journal, April 2011


Aggregates Promote Efficient Charge Transfer Doping of Poly(3-hexylthiophene)
journal, August 2013


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Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI 3 Nanocrystal Films
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Effect of nanotube coupling on exciton transport in polymer-free monochiral semiconducting carbon nanotube networks
journal, January 2019