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Vibrational real-time spectra of poly-[2-methoxy-5-(2'-ethyl-hexyloxy)-p-phenylene vinylene] (MEH-PPV) were measured in a 5 fs pump–probe experiment simultaneously at 128 probe wavelengths with a multichannel detection system. The spectral dependence of the coherent vibrational amplitudes obtained from the Fourier transform (FT) on the probe wavelength detected was found to be given by the sum of the ground-state absorption spectrum and its first and second derivatives. This indicates that the change of the transition probability caused by a wave packet motion can be explained as induced by both the non-Condon effect (non-Condon (NC) mechanism) and the time-dependent Franck–Condon factor (Frank-Condon (FC) mechanism). The FC mechanism can contribute to the first and second derivatives' dependence. On the other hand, the NC mechanism is dominant in the zeroth-order derivative. This result proves that the 11Bu exciton is strongly coupled with the excited 1 Ag state, which is known to be essential in third-order optical nonlinearity. The amounts of shift of the absorption peaks and changes in the bandwidth due to the wave packet motions were determined for the four most prominent modes in the FT power spectra. The shift due to the FC mechanism was about 1.3–1.1% of the peak transition energy and the broadening of the vibronic transition due to the NC mechanism was about 8.0–7.6% of the bandwidth for the four modes. A novel ultrafast optical switch utilizing the modulation of electronic transition probability by molecular vibration through vibronic coupling and the interference of the wave packets is proposed.

Non-Condon vibronic coupling of coherent molecular vibration in MEH-PPV induced by a visible few-cycle pulse laser