Two-dimensional electronic spectroscopy reveals the dynamics of phonon-mediated excitation pathways in semiconducting single-walled carbon nanotubes

Matt W. Graham, Tessa R. Calhoun, Alexander A. Green, Mark C Hersam, Graham R. Fleming

Research output: Contribution to journalArticle

25 Citations (Scopus)

Abstract

Electronic two-dimensional Fourier transform (2D-FT) spectroscopy is applied to semiconducting single-walled carbon nanotubes and provides a spectral and time-domain map of exciton-phonon assisted excitations. Using 12 fs long pulses, we resolve side-bands above the E 22 transition that correspond with the RBM, G, G′, 2G and other multiphonon modes. The appearance of 2D-FT spectral cross-peaks explicitly resolves discrete phonon assisted population transfer that scatters excitations to the E 22 (γ-pt) state, often through a second-order exciton-phonon coupling process. All 2D-FT peaks exhibit a strong peak amplitude modulation at the G-band period (21 fs) which we show originates from an impulsive stimulated Raman process that populates a ground-state G-band vibrational coherence over a 1.3 ps phonon lifetime.

Original languageEnglish
Pages (from-to)813-819
Number of pages7
JournalNano Letters
Volume12
Issue number2
DOIs
Publication statusPublished - Feb 8 2012

Fingerprint

Single-walled carbon nanotubes (SWCN)
Excitons
carbon nanotubes
Spectroscopy
Amplitude modulation
electronics
excitons
Ground state
spectroscopy
excitation
Fourier transforms
life (durability)
ground state
pulses
LDS 751

Keywords

  • carbon nanotubes
  • femtosecond dynamics
  • multidimensional spectroscopy
  • multiphonon assisted transition
  • phonon side-band
  • ultrafast

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Mechanical Engineering

Cite this

Two-dimensional electronic spectroscopy reveals the dynamics of phonon-mediated excitation pathways in semiconducting single-walled carbon nanotubes. / Graham, Matt W.; Calhoun, Tessa R.; Green, Alexander A.; Hersam, Mark C; Fleming, Graham R.

In: Nano Letters, Vol. 12, No. 2, 08.02.2012, p. 813-819.

Research output: Contribution to journalArticle

Graham, Matt W. ; Calhoun, Tessa R. ; Green, Alexander A. ; Hersam, Mark C ; Fleming, Graham R. / Two-dimensional electronic spectroscopy reveals the dynamics of phonon-mediated excitation pathways in semiconducting single-walled carbon nanotubes. In: Nano Letters. 2012 ; Vol. 12, No. 2. pp. 813-819.
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