Hamburg 2009 – scientific programme
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MO: Fachverband Molekülphysik
MO 9: Femtosekundenspektroskopie 3
MO 9.6: Talk
Tuesday, March 3, 2009, 17:45–18:00, VMP 6 HS-F
Three-Pulse Photon Echo beyond the Impulsive Limit - For Example Nile-Blue — Ines Mynttinen1, •Wichard J.D. Beenken1, Tönu Pullerits2, and Erich Runge1 — 1Technische Universität Ilmenau, Germany — 2Lund University, Sweden
We performed computational study of the three pulse photon echo experiments with Nile-blue as a reference molecule. Our aim is to go beyond the impulsive limit and simulate the effect of spectral properties of the incoming laser pulses. We calculated the time-integrated intensity of the third-order polarization generated by three laser pulses. The signal was analysed in terms of the photon-echo peak-shift and the frequency-resolved echo signal. Both, finite pulse duration and chirp of the incoming pulses lead to a faster decay of the integrated intensity in dependency on the second delay time. This influences the photon-echo peak-shift considerably. However, only the chirp affects the time-scales of the peak-shift decay. This means that one has to be extra careful in interpreting the photon echo peak shift as the time-correlation function of the system-bath interaction. The presence of chirp can be checked via the frequency-resolved third-order polarization. The advantage of this method is that in frequency-resolved plots one can easily distinguish the characteristics occurring due to the chirp of the incoming pulses from effects resulting from the molecular system and its interaction with the surrounding bath.