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Title: Ultrafast Exciton Trapping at sp 3 Quantum Defects in Carbon Nanotubes

Abstract

Semiconducting single-walled carbon nanotubes (SWCNTs) constitute an ideal platform for developing near-infrared biosensors, single photon sources, and nanolasers due to their distinct optical and electrical properties. Covalent doping of SWCNTs has recently been discovered as an efficient approach in enhancing their emission intensities. We perform pump–probe studies of SWCNTs that are covalently doped with sp 3 quantum defects and reveal strikingly different exciton formation dynamics and decay mechanisms in the presence of the defect sites. We show that, in highly doped SWCNTs, ultrafast trapping of excitons at the defect sites can outpace other photodynamic processes and lead to ground-state photobleaching of the quantum defects. Our fitting of the transient data with a kinetic model also reveals an upper limit in the quantum defect density for obtaining highly luminescent SWCNTs without causing irreversible damage. In conclusion, these findings not only deepen our understanding of the photodynamics in covalently doped SWCNTs but also reveal critical information for the design of bright near-infrared emitters that can be utilized in biological, quantum information, and nanophotonic applications.

Authors:
 [1];  [2];  [2];  [1];  [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
  2. Univ. of Maryland, College Park, MD (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1607370
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 13; Journal Issue: 11; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; single-walled carbon nanotubes; quantum defects; pump-probe spectroscopy; ground-state photobleaching; stimulated emission; exciton trapping

Citation Formats

Sykes, Matthew E., Kim, Mijin, Wu, Xiaojian, Wiederrecht, Gary P., Peng, Lintao, Wang, YuHuang, Gosztola, David J., and Ma, Xuedan. Ultrafast Exciton Trapping at sp3 Quantum Defects in Carbon Nanotubes. United States: N. p., 2019. Web. doi:10.1021/acsnano.9b06279.
Sykes, Matthew E., Kim, Mijin, Wu, Xiaojian, Wiederrecht, Gary P., Peng, Lintao, Wang, YuHuang, Gosztola, David J., & Ma, Xuedan. Ultrafast Exciton Trapping at sp3 Quantum Defects in Carbon Nanotubes. United States. https://doi.org/10.1021/acsnano.9b06279
Sykes, Matthew E., Kim, Mijin, Wu, Xiaojian, Wiederrecht, Gary P., Peng, Lintao, Wang, YuHuang, Gosztola, David J., and Ma, Xuedan. Tue . "Ultrafast Exciton Trapping at sp3 Quantum Defects in Carbon Nanotubes". United States. https://doi.org/10.1021/acsnano.9b06279. https://www.osti.gov/servlets/purl/1607370.
@article{osti_1607370,
title = {Ultrafast Exciton Trapping at sp3 Quantum Defects in Carbon Nanotubes},
author = {Sykes, Matthew E. and Kim, Mijin and Wu, Xiaojian and Wiederrecht, Gary P. and Peng, Lintao and Wang, YuHuang and Gosztola, David J. and Ma, Xuedan},
abstractNote = {Semiconducting single-walled carbon nanotubes (SWCNTs) constitute an ideal platform for developing near-infrared biosensors, single photon sources, and nanolasers due to their distinct optical and electrical properties. Covalent doping of SWCNTs has recently been discovered as an efficient approach in enhancing their emission intensities. We perform pump–probe studies of SWCNTs that are covalently doped with sp3 quantum defects and reveal strikingly different exciton formation dynamics and decay mechanisms in the presence of the defect sites. We show that, in highly doped SWCNTs, ultrafast trapping of excitons at the defect sites can outpace other photodynamic processes and lead to ground-state photobleaching of the quantum defects. Our fitting of the transient data with a kinetic model also reveals an upper limit in the quantum defect density for obtaining highly luminescent SWCNTs without causing irreversible damage. In conclusion, these findings not only deepen our understanding of the photodynamics in covalently doped SWCNTs but also reveal critical information for the design of bright near-infrared emitters that can be utilized in biological, quantum information, and nanophotonic applications.},
doi = {10.1021/acsnano.9b06279},
url = {https://www.osti.gov/biblio/1607370}, journal = {ACS Nano},
issn = {1936-0851},
number = 11,
volume = 13,
place = {United States},
year = {2019},
month = {10}
}

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