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

Journal Article · · Journal of Chemical Physics
DOI: https://doi.org/10.1063/1.4992785 · OSTI ID:1497873

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.

Research Organization:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1497873
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 3 Vol. 147; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (2)

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Singlet fission molecules among known compounds: finding a few needles in a haystack journal January 2019