Dresden 2009 – wissenschaftliches Programm
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CPP: Fachverband Chemische Physik und Polymerphysik
CPP 23: Electronic and Optical Properties
CPP 23.10: Vortrag
Mittwoch, 25. März 2009, 16:30–16:45, ZEU 114
Three-Pulse Photon Echo beyond the Impulsive Limit — •Ines Mynttinen1, Wichard J. D. Beenken1, Tönu Pullerits2, and Erich Runge1 — 1Technische Universität Ilmenau, Germany — 2Lund University, Sweden
We present computational simulations of three-pulse photon echo (3PPE) experiments on Nile-blue as a reference. For the theoretical analysis, we go beyond the impulsive limit in order to simulate the effects of duration and chirp of the incoming laser pulses. In particular, we study the time-integrated intensity of the third order polarization, the frequency-resolved polarization, and the photon-echo peak shift. The latter is defined as the value of the first delay time where the maximum integrated signal intensity occurs for given second delay time. The peak shift is of general importance for the use of 3PPE in condensed-matter studies, since the time evolution of the peak shift was found earlier to reflect the time-correlation function of the system-bath interaction. We found that both, finite pulse duration and chirp, result in a distinct decay of the integrated intensity in dependence on the second delay time. Additionally, the chirp affects the decay of the peak shift. Our results make clear that it is necessary to control the chirp of the pulses in 3PPE experiments. In particular, the frequency-resolved third-order polarization signal allows to distinguish between the fundamental system-bath dynamics and the effects caused by the pulse chirp. Furthermore, careful analysis of the chirp dependence proves to be a tool to extract additional information from 3PPE experiments, which is usually hidden due to the finite pulse duration.