Article
Femtosecond spectroscopy of optical excitations in single-walled carbon nanotubes: evidence for exciton-exciton annihilation.
Department of Chemistry, University of California, Berkeley, California 94720-1460, USA.
Physical Review Letters (impact factor:
7.37).
05/2005;
94(15):157402.
pp.157402
Source: PubMed
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Citations (0)
- Cited In (3)
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Article: Cross-polarized excitons in carbon nanotubes.
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ABSTRACT: Polarization of low-lying excitonic bands in finite-size semiconducting single-walled carbon nanotubes (SWNTs) is studied by using quantum-chemical methodologies. Our calculations elucidate properties of cross-polarized excitons, which lead to the transverse optical absorption of nanotubes and presumably couple to intermediate-frequency modes recently observed in resonance Raman excitation spectroscopy. We identify up to 12 distinct excitonic transitions below the second fundamental band associated with the E(22) van Hove singularity. Calculations for several chiral SWNTs distinguish the optically active "bright" excitonic band polarized parallel to the tube axis and several optically "weak" cross-polarized excitons. The rest are optically (near) forbidden "dark" transitions. An analysis of the transition density matrices related to excitonic bands provides detailed information about delocalization of excitonic wavefunction along the tube. Utilization of the natural helical coordinate system accounting for the tube chirality allows one to disentangle longitudinal and circumferential components. The distribution of the transition density matrix along a tube axis is similar for all excitons. However, four parallel-polarized excitons associated with the E(11) transition are more localized along the circumference of a tube, compared with others related to the E(12) and E(21) cross-polarized transitions. Calculated splitting between optically active parallel- and cross-polarized transitions increases with tube diameter, which compares well with experimental spectroscopic data.Proceedings of the National Academy of Sciences 06/2008; 105(19):6797-802. · 9.68 Impact Factor -
Article: Electron correlation effects on the femtosecond dephasing dynamics of E22 excitons in (6,5) carbon nanotubes.
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ABSTRACT: Highly nonlinear pump fluence dependence was observed in the ultrafast one-color pump-probe responses excited by 38 fs pulses resonant with the E(22) transition in a room-temperature solution of (6,5) carbon nanotubes. The differential probe transmission (ΔT/T) at the peak of the pump-probe response (τ = 20 fs) was measured for pump fluences from ∼10(13) to 10(17) photons/pulse cm(2). The onset of saturation is observed at ∼2 × 10(15) photons/pulse cm(2) (∼8 × 10(5) excitons/cm). At pump fluences >4 × 10(16) photons/pulse cm(2) (∼1.6 × 10(6) excitons/cm), ΔT/T decreases as the pump fluence increases. Analogous signal saturation behavior was observed for all measured probe delays. Despite the high exciton density at saturation, no change in the E(22) population decay rate was observed at short times (<300 fs). The pump probe signal was modeled by a third-order perturbation theory treatment that includes the effects of inhomogeneous broadening. The observed ΔT/T signal is well-fit by a pump-fluence-dependent dephasing rate linearly dependent on the number of excitons created by the pump pulse. Therefore, the observed nonlinear pump intensity dependence is attributed to the effects of quasi-elastic exciton-exciton interactions on the dephasing rates of single carbon nanotubes. The low fluence total dephasing time is 36 fs, corresponding to a homogeneous width of 36 meV (290 cm(-1)), and the derived E(22) inhomogeneous width is 68 meV (545 cm(-1)). These results are contrasted with photon-echo-derived parameters for the E(11) transition.The Journal of Physical Chemistry A 01/2011; 115(16):3917-23. · 2.95 Impact Factor -
Article: Single-walled carbon nanotubes as base material for THz photoconductive switching: a theoretical study from input power to output THz emission.
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ABSTRACT: This paper studies the relation between photoexcitation of a single-walled carbon nanotube (SWNT) based device, and its THz output power in the context of THz photoconductive (PC) switching and THz photomixing. A detailed approach of calculating output THz power for such a device describes the effect of each parameter on the performance of the THz PC switch and highlights the design dependent achievable limits. A numerical assessment, with typical values for each parameter, shows that-subject to thermal stability of the device-SWNT based PC switch can improve the output power by almost two orders of magnitudes compared to conventional materials such as LT-GaAs.Optics Express 08/2011; 19(16):15077-89. · 3.59 Impact Factor
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Keywords
distinct amplitude dependence
excitonic origin
first electronic transitions
Frequency-resolved femtosecond transient absorption spectra
nonlinear exciton annihilation
optical excitation
spectra
transitions
