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Title: Multiple exciton generation in chiral carbon nanotubes: Density functional theory based computation

Abstract

We use a Boltzmann transport equation (BE) to study time evolution of a photo-excited state in a nanoparticle including phonon-mediated exciton relaxation and the multiple exciton generation (MEG) processes, such as exciton-to-biexciton multiplication and biexciton-to-exciton recombination. BE collision integrals are computed using Kadanoff-Baym-Keldysh many-body perturbation theory based on density functional theory simulations, including exciton effects. We compute internal quantum efficiency (QE), which is the number of excitons generated from an absorbed photon in the course of the relaxation. We apply this approach to chiral single-wall carbon nanotubes (SWCNTs), such as (6,2) and (6,5). We predict efficient MEG in the (6,2) and (6,5) SWCNTs within the solar spectrum range starting at the 2Eg energy threshold and with QE reaching ~1.6 at about 3Eg, where Eg is the electronic gap.

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:
1497879
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 15; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Kryjevski, Andrei, Mihaylov, Deyan, Kilina, Svetlana, and Kilin, Dmitri. Multiple exciton generation in chiral carbon nanotubes: Density functional theory based computation. United States: N. p., 2017. Web. doi:10.1063/1.4997048.
Kryjevski, Andrei, Mihaylov, Deyan, Kilina, Svetlana, & Kilin, Dmitri. Multiple exciton generation in chiral carbon nanotubes: Density functional theory based computation. United States. https://doi.org/10.1063/1.4997048
Kryjevski, Andrei, Mihaylov, Deyan, Kilina, Svetlana, and Kilin, Dmitri. Fri . "Multiple exciton generation in chiral carbon nanotubes: Density functional theory based computation". United States. https://doi.org/10.1063/1.4997048. https://www.osti.gov/servlets/purl/1497879.
@article{osti_1497879,
title = {Multiple exciton generation in chiral carbon nanotubes: Density functional theory based computation},
author = {Kryjevski, Andrei and Mihaylov, Deyan and Kilina, Svetlana and Kilin, Dmitri},
abstractNote = {We use a Boltzmann transport equation (BE) to study time evolution of a photo-excited state in a nanoparticle including phonon-mediated exciton relaxation and the multiple exciton generation (MEG) processes, such as exciton-to-biexciton multiplication and biexciton-to-exciton recombination. BE collision integrals are computed using Kadanoff-Baym-Keldysh many-body perturbation theory based on density functional theory simulations, including exciton effects. We compute internal quantum efficiency (QE), which is the number of excitons generated from an absorbed photon in the course of the relaxation. We apply this approach to chiral single-wall carbon nanotubes (SWCNTs), such as (6,2) and (6,5). We predict efficient MEG in the (6,2) and (6,5) SWCNTs within the solar spectrum range starting at the 2Eg energy threshold and with QE reaching ~1.6 at about 3Eg, where Eg is the electronic gap.},
doi = {10.1063/1.4997048},
url = {https://www.osti.gov/biblio/1497879}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 15,
volume = 147,
place = {United States},
year = {2017},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 6 works
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Figures / Tables:

Figure 1 Figure 1: Typical Feynman diagrams for the Σ$$^{+-}$$ describing exciton-phonon coupling. Shown in (a) and (b) are the one- and two-phonon processes, respectively. Thin solid lines stand for the KS state propagators, thick solid lines depict excitons, and dashed lines depict phonons. The +- contributions obtain when + and aremore » interchanged.« less

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    Works referencing / citing this record:

    Molecular dynamics of reactions between (4,0) zigzag carbon nanotube and hydrogen peroxide under extreme conditions
    journal, January 2018


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


      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.