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Title: Photoinduced Spontaneous Free-Carrier Generation in Semiconducting Single-Walled Carbon Nanotubes

Abstract

The strong quantum confinement and low dielectric screening impart single-walled carbon nanotubes with exciton-binding energies substantially exceeding kBT at room temperature. Despite these large binding energies, reported photoluminescence quantum yields are typically low and some studies suggest that photoexcitation of carbon nanotube excitonic transitions can produce free charge carriers. Here we report the direct measurement of long-lived free-carrier generation in chirality-pure, single-walled carbon nanotubes in a low dielectric solvent. Time-resolved microwave conductivity enables contactless and quantitative measurement of the real and imaginary photoconductance of individually suspended nanotubes. We found that the conditions of the microwave conductivity measurement allow us to avoid the complications of most previous measurements of nanotube free-carrier generation, including tube–tube/tube–electrode contact, dielectric screening by nearby excitons and many-body interactions. At low photon fluence (approximately 0.05 excitons per μm length of tubes), we directly observe free carriers on excitation of the first and second carbon nanotube exciton transitions.

Authors:
 [1];  [2];  [1];  [2]
+ Show Author Affiliations
  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 Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1227714
Report Number(s):
NREL/JA-5900-64645
Journal ID: ISSN 2041-1723; MainId:11995;UUID:08b8fde6-4a20-e511-8e4e-d89d67132a6d;MainAdminID:475
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY; quantum confinement; carbon nanotubes; binding energies; photoluminescence

Citation Formats

Park, Jaehong, Reid, Obadiah G., Blackburn, Jeffrey L., and Rumbles, Garry. Photoinduced Spontaneous Free-Carrier Generation in Semiconducting Single-Walled Carbon Nanotubes. United States: N. p., 2015. Web. doi:10.1038/ncomms9809.
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Park, Jaehong, Reid, Obadiah G., Blackburn, Jeffrey L., & Rumbles, Garry. Photoinduced Spontaneous Free-Carrier Generation in Semiconducting Single-Walled Carbon Nanotubes. United States. https://doi.org/10.1038/ncomms9809
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Park, Jaehong, Reid, Obadiah G., Blackburn, Jeffrey L., and Rumbles, Garry. Wed . "Photoinduced Spontaneous Free-Carrier Generation in Semiconducting Single-Walled Carbon Nanotubes". United States. https://doi.org/10.1038/ncomms9809. https://www.osti.gov/servlets/purl/1227714.
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@article{osti_1227714,
title = {Photoinduced Spontaneous Free-Carrier Generation in Semiconducting Single-Walled Carbon Nanotubes},
author = {Park, Jaehong and Reid, Obadiah G. and Blackburn, Jeffrey L. and Rumbles, Garry},
abstractNote = {The strong quantum confinement and low dielectric screening impart single-walled carbon nanotubes with exciton-binding energies substantially exceeding kBT at room temperature. Despite these large binding energies, reported photoluminescence quantum yields are typically low and some studies suggest that photoexcitation of carbon nanotube excitonic transitions can produce free charge carriers. Here we report the direct measurement of long-lived free-carrier generation in chirality-pure, single-walled carbon nanotubes in a low dielectric solvent. Time-resolved microwave conductivity enables contactless and quantitative measurement of the real and imaginary photoconductance of individually suspended nanotubes. We found that the conditions of the microwave conductivity measurement allow us to avoid the complications of most previous measurements of nanotube free-carrier generation, including tube–tube/tube–electrode contact, dielectric screening by nearby excitons and many-body interactions. At low photon fluence (approximately 0.05 excitons per μm length of tubes), we directly observe free carriers on excitation of the first and second carbon nanotube exciton transitions.},
doi = {10.1038/ncomms9809},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Wed Nov 04 00:00:00 EST 2015},
month = {Wed Nov 04 00:00:00 EST 2015}
}
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https://doi.org/10.1038/ncomms9809
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Contactless Determination of the Photoconductivity Action Spectrum, Exciton Diffusion Length, and Charge Separation Efficiency in Polythiophene-Sensitized TiO 2 Bilayers
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Prolonging Charge Separation in P3HT−SWNT Composites Using Highly Enriched Semiconducting Nanotubes
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Photogenerated Free Carrier Dynamics in Metal and Semiconductor Single-Walled Carbon Nanotube Films
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Ultrafast Excitation Energy Transfer in Small Semiconducting Carbon Nanotube Aggregates
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Photocurrent Spectroscopy of ( n , m ) Sorted Solution-Processed Single-Walled Carbon Nanotubes
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Highly selective dispersion of single-walled carbon nanotubes using aromatic polymers
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