skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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; 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. 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. 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 = {2019},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Electronic Structure and Chemical Nature of Oxygen Dopant States in Carbon Nanotubes
journal, October 2014

  • Ma, Xuedan; Adamska, Lyudmyla; Yamaguchi, Hisato
  • ACS Nano, Vol. 8, Issue 10
  • DOI: 10.1021/nn504553y

Scaling of Excitons in Carbon Nanotubes
journal, June 2004


Efficient near-infrared up-conversion photoluminescence in carbon nanotubes
journal, November 2015

  • Akizuki, Naoto; Aota, Shun; Mouri, Shinichiro
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9920

Polarizable continuum model: Polarizable continuum model
journal, January 2012

  • Mennucci, Benedetta
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 3
  • DOI: 10.1002/wcms.1086

Long-Range Electronic-to-Vibrational Energy Transfer from Nanocrystals to Their Surrounding Matrix Environment
journal, February 2008


Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects
journal, September 2017


Theory of Electronic States and Transport in Carbon Nanotubes
journal, March 2005

  • Ando, Tsuneya
  • Journal of the Physical Society of Japan, Vol. 74, Issue 3
  • DOI: 10.1143/jpsj.74.777

Room-temperature single-photon generation from solitary dopants of carbon nanotubes
journal, July 2015

  • Ma, Xuedan; Hartmann, Nicolai F.; Baldwin, Jon K. S.
  • Nature Nanotechnology, Vol. 10, Issue 8
  • DOI: 10.1038/nnano.2015.136

Oxygen Doping Modifies Near-Infrared Band Gaps in Fluorescent Single-Walled Carbon Nanotubes
journal, November 2010


Molecularly Tunable Fluorescent Quantum Defects
journal, May 2016

  • Kwon, Hyejin; Furmanchuk, Al’ona; Kim, Mijin
  • Journal of the American Chemical Society, Vol. 138, Issue 21
  • DOI: 10.1021/jacs.6b03618

Brightening of excitons in carbon nanotubes on dimensionality modification
journal, July 2013

  • Miyauchi, Yuhei; Iwamura, Munechiyo; Mouri, Shinichiro
  • Nature Photonics, Vol. 7, Issue 9
  • DOI: 10.1038/nphoton.2013.179

Solvent- and Wavelength-Dependent Photoluminescence Relaxation Dynamics of Carbon Nanotube sp 3 Defect States
journal, July 2018


Torsional Characteristics of SingleWalled Carbon Nanotube with Water Interactions by Using Molecular Dynamics Simulation
journal, July 2014

  • Vijayaraghavan, V.; Wong, C. H.
  • Nano-Micro Letters, Vol. 6, Issue 3
  • DOI: 10.1007/bf03353791

COSMO: a new approach to dielectric screening in solvents with explicit expressions for the screening energy and its gradient
journal, January 1993


Brightening of carbon nanotube photoluminescence through the incorporation of sp3 defects
journal, July 2013

  • Piao, Yanmei; Meany, Brendan; Powell, Lyndsey R.
  • Nature Chemistry, Vol. 5, Issue 10
  • DOI: 10.1038/nchem.1711

Optical Probing of Local pH and Temperature in Complex Fluids with Covalently Functionalized, Semiconducting Carbon Nanotubes
journal, February 2015

  • Kwon, Hyejin; Kim, Mijin; Meany, Brendan
  • The Journal of Physical Chemistry C, Vol. 119, Issue 7
  • DOI: 10.1021/jp509546d

Impact of D 2 O/H 2 O Solvent Exchange on the Emission of HgTe and CdTe Quantum Dots: Polaron and Energy Transfer Effects
journal, March 2016


Diffusion Limited Photoluminescence Quantum Yields in 1-D Semiconductors: Single-Wall Carbon Nanotubes
journal, November 2010

  • Hertel, Tobias; Himmelein, Sabine; Ackermann, Thomas
  • ACS Nano, Vol. 4, Issue 12
  • DOI: 10.1021/nn101612b

Tunable room-temperature single-photon emission at telecom wavelengths from sp3 defects in carbon nanotubes
journal, July 2017


Exciton Localization and Optical Emission in Aryl-Functionalized Carbon Nanotubes
journal, November 2017

  • Gifford, Brendan J.; Kilina, Svetlana; Htoon, Han
  • The Journal of Physical Chemistry C, Vol. 122, Issue 3
  • DOI: 10.1021/acs.jpcc.7b09558

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

Photoluminescence Dynamics of Aryl sp 3 Defect States in Single-Walled Carbon Nanotubes
journal, August 2016

  • Hartmann, Nicolai F.; Velizhanin, Kirill A.; Haroz, Erik H.
  • ACS Nano, Vol. 10, Issue 9
  • DOI: 10.1021/acsnano.6b02986

Multi-exciton emission from solitary dopant states of carbon nanotubes
journal, January 2017

  • Ma, Xuedan; Hartmann, Nicolai F.; Velizhanin, Kirill A.
  • Nanoscale, Vol. 9, Issue 42
  • DOI: 10.1039/c7nr06661a

Photoluminescence Measurements and Molecular Dynamics Simulations of Water Adsorption on the Hydrophobic Surface of a Carbon Nanotube in Water Vapor
journal, April 2013


Fluorescent Carbon Nanotube Defects Manifest Substantial Vibrational Reorganization
journal, May 2016

  • Kim, Mijin; Adamska, Lyudmyla; Hartmann, Nicolai F.
  • The Journal of Physical Chemistry C, Vol. 120, Issue 20
  • DOI: 10.1021/acs.jpcc.6b02538

Phonon and Electronic Nonradiative Decay Mechanisms of Excitons in Carbon Nanotubes
journal, July 2008


Near infrared photoluminescence modulation of single-walled carbon nanotubes based on a molecular recognition approach
journal, January 2016

  • Shiraki, Tomohiro; Onitsuka, Hisashi; Shiraishi, Tomonari
  • Chemical Communications, Vol. 52, Issue 88
  • DOI: 10.1039/c6cc07287a

Infrared Spectrum and Structure of Liquid Water
journal, July 1966

  • Falk, Michael; Ford, T. A.
  • Canadian Journal of Chemistry, Vol. 44, Issue 14
  • DOI: 10.1139/v66-255

Trigonal warping effect of carbon nanotubes
journal, January 2000


    Works referencing / citing this record:

    Tailoring spontaneous infrared emission of HgTe quantum dots with laser-printed plasmonic arrays
    journal, February 2020

    • Sergeev, A. A.; Pavlov, D. V.; Kuchmizhak, A. A.
    • Light: Science & Applications, Vol. 9, Issue 1
    • DOI: 10.1038/s41377-020-0247-6