Exciton-exciton annihilation in single-walled carbon nanotubes

Leonas Valkunas, Ying-Zhong Ma, and Graham R. Fleming

Phys. Rev. B 73, 115432 – Published 30 March 2006

Abstract

The femtosecond fluorescence and transient absorption kinetics recorded on selected semiconducting single-walled carbon nanotubes exhibit pronounced excitation-intensity-dependent decays as the result of exciton-exciton annihilation. A satisfactory description of the decays obtained at various excitation intensities, however, requires a time-independent annihilation rate that is valid only for extended systems with dimensionality greater than 2 in conjunction with diffusive migration of excitons. We resolved this apparent contradiction by developing a stochastic model, in which we assumed that the exciton states in semiconducting nanotubes are coherent, and the multiexciton manifolds are resonantly coupled with other excited states, which decay by subsequent linear relaxation due to electron-phonon coupling. The formalism derived from this model enables a qualitative description of the experimental results for the (9,5), (8,3), and (6,5) semiconducting single-walled carbon nanotubes.

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Received 20 December 2005

DOI:https://doi.org/10.1103/PhysRevB.73.115432

Authors & Affiliations

Leonas Valkunas

Department of Chemistry, University of California, Berkeley, Berkeley, California 94720-1460, USA; Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720-1460, USA; Institute of Physics, Savanoriu Ave. 231, 02300 Vilnius, Lithuania; and Theoretical Physics Department, Faculty of Physics of Vilnius University, Sauletekio Ave. 9, building 3, 10222 Vilnius, Lithuania

Ying-Zhong Ma and Graham R. Fleming^*

Department of Chemistry, University of California, Berkeley, Berkeley, California 94720-1460, USA and Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720-1460, USA

^*Author to whom correspondence should be addressed. Electronic address: grfleming@lbl.gov

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Vol. 73, Iss. 11 — 15 March 2006

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