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

Title: Singlet fission in chiral carbon nanotubes: Density functional theory based computation

Abstract

Singlet fission (SF) process, where a singlet exciton decays into a pair of spin one exciton states which are in the total spin singlet state, is one of the possible channels for multiple exciton generation (MEG). In chiral single-wall carbon nanotubes (SWCNTs), efficient SF is present within the solar spectrum energy range which is shown by the many-body perturbation theory calculations based on the density functional theory simulations. We calculate SF exciton-to-biexciton decay rates R1→2 and biexciton-to-exciton rates R2→1 in the (6,2), (6,5), (10,5) SWCNTs, and in the (6,2) SWCNT functionalized with Cl atoms. Within the solar energy range, we predict R 1→2~10 14-10 15 s -1, while biexciton-to-exciton recombination is weak with R 2→1/R 1→2≤10 -2. SF MEG strength in pristine SWCNTs varies strongly with the excitation energy, which is due to highly non-uniform density of states at low energy. However, our results for the (6,2) SWCNT with chlorine atoms adsorbed to the surface suggest that MEG in the chiral SWCNTs can be enhanced by altering the low-energy electronic states via surface functionalization.

Authors:
ORCiD logo [1];  [1];  [1];  [1]
  1. North Dakota State Univ., Fargo, ND (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1497873
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 3; 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

Citation Formats

Kryjevski, Andrei, Mihaylov, Deyan, Gifford, Brendan, and Kilin, Dmitri. Singlet fission in chiral carbon nanotubes: Density functional theory based computation. United States: N. p., 2017. Web. doi:10.1063/1.4992785.
Kryjevski, Andrei, Mihaylov, Deyan, Gifford, Brendan, & Kilin, Dmitri. Singlet fission in chiral carbon nanotubes: Density functional theory based computation. United States. doi:10.1063/1.4992785.
Kryjevski, Andrei, Mihaylov, Deyan, Gifford, Brendan, and Kilin, Dmitri. Wed . "Singlet fission in chiral carbon nanotubes: Density functional theory based computation". United States. doi:10.1063/1.4992785. https://www.osti.gov/servlets/purl/1497873.
@article{osti_1497873,
title = {Singlet fission in chiral carbon nanotubes: Density functional theory based computation},
author = {Kryjevski, Andrei and Mihaylov, Deyan and Gifford, Brendan and Kilin, Dmitri},
abstractNote = {Singlet fission (SF) process, where a singlet exciton decays into a pair of spin one exciton states which are in the total spin singlet state, is one of the possible channels for multiple exciton generation (MEG). In chiral single-wall carbon nanotubes (SWCNTs), efficient SF is present within the solar spectrum energy range which is shown by the many-body perturbation theory calculations based on the density functional theory simulations. We calculate SF exciton-to-biexciton decay rates R1→2 and biexciton-to-exciton rates R2→1 in the (6,2), (6,5), (10,5) SWCNTs, and in the (6,2) SWCNT functionalized with Cl atoms. Within the solar energy range, we predict R1→2~1014-1015 s-1, while biexciton-to-exciton recombination is weak with R2→1/R1→2≤10-2. SF MEG strength in pristine SWCNTs varies strongly with the excitation energy, which is due to highly non-uniform density of states at low energy. However, our results for the (6,2) SWCNT with chlorine atoms adsorbed to the surface suggest that MEG in the chiral SWCNTs can be enhanced by altering the low-energy electronic states via surface functionalization.},
doi = {10.1063/1.4992785},
journal = {Journal of Chemical Physics},
number = 3,
volume = 147,
place = {United States},
year = {2017},
month = {7}
}

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

Save / Share:

Works referenced in this record:

Highly Efficient Multiple Exciton Generation in Colloidal PbSe and PbS Quantum Dots
journal, May 2005

  • Ellingson, Randy J.; Beard, Matthew C.; Johnson, Justin C.
  • Nano Letters, Vol. 5, Issue 5, p. 865-871
  • DOI: 10.1021/nl0502672

Detailed Balance Limit of Efficiency of p?n Junction Solar Cells
journal, March 1961

  • Shockley, William; Queisser, Hans J.
  • Journal of Applied Physics, Vol. 32, Issue 3, p. 510-519
  • DOI: 10.1063/1.1736034