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:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (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; TRN: US2001238
- 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. https://doi.org/10.1063/1.5121300
Velizhanin, Kirill A. Tue .
"Exciton relaxation in carbon nanotubes via electronic-to-vibrational energy transfer". United States. https://doi.org/10.1063/1.5121300. https://www.osti.gov/servlets/purl/1572329.
@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 = {Tue Oct 08 00:00:00 EDT 2019},
month = {Tue Oct 08 00:00:00 EDT 2019}
}
Web of Science
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