Correction Scheme for Comparison of Computed and Experimental Optical Transition Energies in Functionalized Single-Walled Carbon Nanotubes

doi:https://doi.org/10.1021/acs.jpclett.8b00653

Title: Correction Scheme for Comparison of Computed and Experimental Optical Transition Energies in Functionalized Single-Walled Carbon Nanotubes

Abstract

We present that covalent functionalization of single-walled carbon nanotubes (SWCNTs) introduces red-shifted emission features in the near-infrared spectral range due to exciton localization around the defect site. Such chemical modifications increase their potential use as near-infrared emitters and single-photon sources in telecommunications applications. Density functional theory (DFT) studies using finite-length tube models have been used to calculate their optical transition energies. Predicted energies are typically blue-shifted compared to experiment due to methodology errors including imprecise self-interaction corrections in the density functional and finite-size basis sets. Furthermore, artificial quantum confinement in finite models cannot be corrected by a constant-energy shift since they depend on the degree of exciton localization. Herein, we present a method that corrects the emission energies predicted by time-dependent DFT. Confinement and methodology errors are separately estimated using experimental data for unmodified tubes. Finally, corrected emission energies are in remarkable agreement with experiment, suggesting the value of this straightforward method toward predicting and interpreting the optical features of functionalized SWCNTs.

Authors:

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North Dakota State Univ., Fargo, ND (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of Southern California, Los Angeles, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
North Dakota State Univ., Fargo, ND (United States)

Publication Date:: 2018-04-20

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Office of Science (SC). Advanced Scientific Computing Research (ASCR) (SC-21)

OSTI Identifier:: 1481994

Report Number(s):: LA-UR-18-21776
Journal ID: ISSN 1948-7185

Grant/Contract Number:: AC52-06NA25396; AC02-05CH11231

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry Letters

Additional Journal Information:: Journal Volume: 9; Journal Issue: 10; Journal ID: ISSN 1948-7185

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats


                    Gifford, Brendan Joel, Sifain, Andrew E., Htoon, Han, Doorn, Stephen K., Kilina, Svetlana, and Tretiak, Sergei. Correction Scheme for Comparison of Computed and Experimental Optical Transition Energies in Functionalized Single-Walled Carbon Nanotubes.  United States: N. p., 2018. 
        Web.  doi:10.1021/acs.jpclett.8b00653.

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                    Gifford, Brendan Joel, Sifain, Andrew E., Htoon, Han, Doorn, Stephen K., Kilina, Svetlana, & Tretiak, Sergei. Correction Scheme for Comparison of Computed and Experimental Optical Transition Energies in Functionalized Single-Walled Carbon Nanotubes.  United States.  https://doi.org/10.1021/acs.jpclett.8b00653

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                    Gifford, Brendan Joel, Sifain, Andrew E., Htoon, Han, Doorn, Stephen K., Kilina, Svetlana, and Tretiak, Sergei. Fri .  
        "Correction Scheme for Comparison of Computed and Experimental Optical Transition Energies in Functionalized Single-Walled Carbon Nanotubes".  United States.  https://doi.org/10.1021/acs.jpclett.8b00653.  https://www.osti.gov/servlets/purl/1481994.

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@article{osti_1481994,

  title        = {Correction Scheme for Comparison of Computed and Experimental Optical Transition Energies in Functionalized Single-Walled Carbon Nanotubes},

  author       = {Gifford, Brendan Joel and Sifain, Andrew E. and Htoon, Han and Doorn, Stephen K. and Kilina, Svetlana and Tretiak, Sergei},

  abstractNote = {We present that covalent functionalization of single-walled carbon nanotubes (SWCNTs) introduces red-shifted emission features in the near-infrared spectral range due to exciton localization around the defect site. Such chemical modifications increase their potential use as near-infrared emitters and single-photon sources in telecommunications applications. Density functional theory (DFT) studies using finite-length tube models have been used to calculate their optical transition energies. Predicted energies are typically blue-shifted compared to experiment due to methodology errors including imprecise self-interaction corrections in the density functional and finite-size basis sets. Furthermore, artificial quantum confinement in finite models cannot be corrected by a constant-energy shift since they depend on the degree of exciton localization. Herein, we present a method that corrects the emission energies predicted by time-dependent DFT. Confinement and methodology errors are separately estimated using experimental data for unmodified tubes. Finally, corrected emission energies are in remarkable agreement with experiment, suggesting the value of this straightforward method toward predicting and interpreting the optical features of functionalized SWCNTs.},

  doi          = {10.1021/acs.jpclett.8b00653},

  url          = {https://www.osti.gov/biblio/1481994},
  journal      = {Journal of Physical Chemistry Letters},

  issn         = {1948-7185},

  number       = 10,

  volume       = 9,

  place        = {United States},

  year         = {2018},

  month        = {4}

}

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Works referencing / citing this record:

Narrow-band single-photon emission through selective aryl functionalization of zigzag carbon nanotubes
journal, September 2018

Saha, Avishek; Gifford, Brendan J.; He, Xiaowei
Nature Chemistry, Vol. 10, Issue 11
https://doi.org/10.1038/s41557-018-0126-4

Controlling the optical properties of carbon nanotubes with organic colour-centre quantum defects
journal, June 2019

Brozena, Alexandra H.; Kim, Mijin; Powell, Lyndsey R.
Nature Reviews Chemistry, Vol. 3, Issue 6
https://doi.org/10.1038/s41570-019-0103-5

Thermodynamic control of quantum defects on single-walled carbon nanotubes
journal, January 2019

Maeda, Yutaka; Murakoshi, Hiyori; Tambo, Haruto
Chemical Communications, Vol. 55, Issue 91
https://doi.org/10.1039/c9cc05623h

Optical properties of semiconducting zigzag carbon nanotubes with and without defects
journal, January 2019

Mu, Jinglin; Ma, Yuchen; Liu, Huichun
The Journal of Chemical Physics, Vol. 150, Issue 2
https://doi.org/10.1063/1.5055271

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Title: Correction Scheme for Comparison of Computed and Experimental Optical Transition Energies in Functionalized Single-Walled Carbon Nanotubes

Abstract

Citation Formats

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Controlling the optical properties of carbon nanotubes with organic colour-centre quantum defects journal, June 2019

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journal, June 2019

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journal, January 2019