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Title: Exciton relaxation in carbon nanotubes via electronic-to-vibrational energy transfer

Abstract

Covalent functionalization of semiconducting single-wall carbon nanotubes (CNTs) introduces new photoluminescent emitting states. These states are spatially localized around functionalization sites and strongly red-shifted relative to the emission commonly observed from the CNT band-edge exciton state. A particularly important feature of these localized exciton states is that because the exciton is no longer free to diffusively sample photoluminescent quenching sites along the CNT length, its lifetime is significantly extended. We have recently demonstrated that an important relaxation channel of such localized excitons is the electronic-to-vibrational energy transfer (EVET). This process is analogous to the Förster resonance energy transfer except the final state of this process is not electronically, but vibrationally excited molecules of the surrounding medium (e.g., solvent). In this work, we develop a theory of EVET for a nanostructure of arbitrary shape and apply it to the specific case of EVET-mediated relaxation of defect-localized excitons in a covalently functionalized CNT. Here, the resulting EVET relaxation times are in good agreement with experimental data.

Authors:
ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1572329
Report Number(s):
LA-UR-19-22301
Journal ID: ISSN 0021-9606
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 14; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbon nanotubes; exciton; resonance energy transfer

Citation Formats

Velizhanin, Kirill A. Exciton relaxation in carbon nanotubes via electronic-to-vibrational energy transfer. United States: N. p., 2019. Web. doi:10.1063/1.5121300.
Velizhanin, Kirill A. Exciton relaxation in carbon nanotubes via electronic-to-vibrational energy transfer. United States. doi:10.1063/1.5121300.
Velizhanin, Kirill A. Tue . "Exciton relaxation in carbon nanotubes via electronic-to-vibrational energy transfer". United States. doi:10.1063/1.5121300.
@article{osti_1572329,
title = {Exciton relaxation in carbon nanotubes via electronic-to-vibrational energy transfer},
author = {Velizhanin, Kirill A.},
abstractNote = {Covalent functionalization of semiconducting single-wall carbon nanotubes (CNTs) introduces new photoluminescent emitting states. These states are spatially localized around functionalization sites and strongly red-shifted relative to the emission commonly observed from the CNT band-edge exciton state. A particularly important feature of these localized exciton states is that because the exciton is no longer free to diffusively sample photoluminescent quenching sites along the CNT length, its lifetime is significantly extended. We have recently demonstrated that an important relaxation channel of such localized excitons is the electronic-to-vibrational energy transfer (EVET). This process is analogous to the Förster resonance energy transfer except the final state of this process is not electronically, but vibrationally excited molecules of the surrounding medium (e.g., solvent). In this work, we develop a theory of EVET for a nanostructure of arbitrary shape and apply it to the specific case of EVET-mediated relaxation of defect-localized excitons in a covalently functionalized CNT. Here, the resulting EVET relaxation times are in good agreement with experimental data.},
doi = {10.1063/1.5121300},
journal = {Journal of Chemical Physics},
number = 14,
volume = 151,
place = {United States},
year = {2019},
month = {10}
}

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Works referenced in this record:

Band Gap Fluorescence from Individual Single-Walled Carbon Nanotubes
journal, July 2002

  • O'Connell, Michael J.; Bachilo, Sergei M.; Huffman, Chad B.
  • Science, Vol. 297, Issue 5581, p. 593-596
  • DOI: 10.1126/science.1072631