Abstract
Third-order nonlinear optical response in single-walled carbon nanotubes (SWNTs) has been investigated by means of femtosecond pump–probe spectroscopy. The imaginary part of nonlinear susceptibility Im χ (3) measured under the nonresonant excitation conditions shows the resonant enhancement at each optical transition of the specific ( n, m) tube in miscelle-suspended SWNTs. With the selective excitation of the E 22 exciton transition for the (7,6) tube, the value of Im χ (3) is increased by an order of magnitude compared with the nonresonant excitation case. The nonlinear response signal at the E 22 transition energy for the (8,7) tube has been also enhanced for the excitation at ∼0.22 eV above the E 22 transition energy. This result is interpreted in terms of the phonon-assisted E 22 transition for the (8,7) tube, indicating strong exciton–phonon coupling.
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