Intensity-dependent exciton dynamics of (6,5) single-walled carbon nanotubes: Momentum selection rules, diffusion, and nonlinear interactions

D. Mark Harrah, Jude R. Schneck, Alexander A. Green, Mark C. Hersam, Lawrence D. Ziegler, Anna K. Swan

Research output: Contribution to journalArticlepeer-review

29 Scopus citations

Abstract

The exciton dynamics for an ensemble of individual, suspended (6,5), single-walled carbon nanotubes revealed by single color E 22 resonant pump-probe spectroscopy for a wide range of pump fluences are reported. The optically excited initial exciton population ranges from approximately 5 to 120 excitons per ∼725 nm nanotube. At the higher fluences of this range, the pump-probe signals are no longer linearly dependent on the pump intensity. A single, predictive model is described that fits all data for two decades of pump fluences and three decades of delay times. The model introduces population loss from the optically active zero momentum E 22 state to the rest of the E 22 subband, which is dark due to momentum selection rules. In the single exciton limit, the E 11 dynamics are well described by a stretched exponential, which is a direct consequence of diffusion quenching from an ensemble of nanotubes of different lengths. The observed change in population relaxation dynamics as a function of increasing pump intensity is attributed to exciton-exciton Auger de-excitation in the E 11 subband and, to a lesser extent, in the E 22 subband. From the fit to the model, an average defect density 1/φ = 150 nm and diffusion constants D 11 = 4 cm 2/s and D 22 = 0.2 cm 2/s are determined.

Original languageEnglish (US)
Pages (from-to)9898-9906
Number of pages9
JournalACS nano
Volume5
Issue number12
DOIs
StatePublished - Dec 27 2011
Externally publishedYes

Keywords

  • diffusion
  • single-walled carbon nanotubes-pump-probe

ASJC Scopus subject areas

  • General Materials Science
  • General Engineering
  • General Physics and Astronomy

Fingerprint

Dive into the research topics of 'Intensity-dependent exciton dynamics of (6,5) single-walled carbon nanotubes: Momentum selection rules, diffusion, and nonlinear interactions'. Together they form a unique fingerprint.

Cite this