Issue 3, 2016

Exciton–exciton annihilation and relaxation pathways in semiconducting carbon nanotubes

Abstract

We present a thorough analysis of one- and two-color transient absorption measurements performed on single- and double-walled semiconducting carbon nanotubes. By combining the currently existing models describing exciton–exciton annihilation—the coherent and the diffusion-limited ones—we are able to simultaneously reproduce excitation kinetics following both E11 and E22 pump conditions. Our simulations revealed the fundamental photophysical behavior of one-dimensional coherent excitons and non-trivial excitation relaxation pathways. In particular, we found that after non-linear annihilation a doubly-excited exciton relaxes directly to its E11 state bypassing the intermediate E22 manifold, so that after excitation resonant with the E11 transition, the E22 state remains unpopulated. A quantitative explanation for the observed much faster excitation kinetics probed at E22 manifold, comparing to those probed at the E11 band, is also provided.

Graphical abstract: Exciton–exciton annihilation and relaxation pathways in semiconducting carbon nanotubes

Article information

Article type
Paper
Submitted
03 Okt. 2015
Accepted
05 Dec. 2015
First published
07 Dec. 2015

Nanoscale, 2016,8, 1618-1626

Author version available

Exciton–exciton annihilation and relaxation pathways in semiconducting carbon nanotubes

J. Chmeliov, J. Narkeliunas, M. W. Graham, G. R. Fleming and L. Valkunas, Nanoscale, 2016, 8, 1618 DOI: 10.1039/C5NR06853C

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