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The Journal of Chemical Physics

Mode suppression in the non-Markovian limit by time-gated stimulated photon echo

Wim P. de Boeij, Maxim S. Pshenichnikov, Douwe A. Wiersma

Published Aug 22, 1996• 42 citations
Publisher

Abstract

It is demonstrated that enhanced mode suppression in stimulated photon echo experiments can be obtained by diagonal time gating of the echo. This technique is especially important when the optical dynamics of the system is non-Markovian. A two-mode Brownian oscillator model is used to analyze the effect of time gating on the stimulated photon echo. The method is demonstrated on a dye solution of DTTCI in ethylene glycol at room temperature. Experimentally, time gating of the echo is accomplished by means of femtosecond phase-locked heterodyne detected stimulated photon echo. The vibrational dynamics in this system are explored by conventional stimulated photon echo experiments. Especially stimulated photon echo-maximum shift measurements are found to be particularly useful.

DOI
10.1063/1.472812

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European Quantum Electronics Conference (EQEC)•Jan 1, 1996•0 citations
It is demonstrated that enhanced mode suppression in stimulated photon echo experiments can be obtained by diagonal time gating of the echo. This technique is especially important when the optical dynamics of the system is non-Markovian. A two-mode Brownian oscillator model is used to analyze the effect of time gating on the stimulated photon echo. The method is demonstrated on a dye solution of DTTCI in ethylene glycol at room temperature. Experimentally, time gating of the echo is accomplished by means of femtosecond phase-locked heterodyne detected stimulated photon echo. The vibrational dynamics in this system are explored by conventional stimulated photon echo experiments. Especially stimulated photon echo-maximum shift measurements are found to be particularly useful.
Numerous studies to date are aimed at a better understanding of the optical dynamics of dissolved dye molecules. Most dyes exhibit prominent vibronic features in their absorption spectra. For impulsive excitation the initially excited state is a vibronic wave packet, that strongly influences the observed dynamics. Shank and co-workers were the first to recognize the importance of vibrational mode suppression towards optical dephasing measurements.[1,2] However, mode suppression based on time-integrated stimulated photon echo works only in systems that exhibit Bloch-like dynamics.
We show how in the framework of the multimode Brownian oscillator model the system−bath correlation function can be derived from conventional and time-gated stimulated photon echo experiments and consideration of the linear optical spectra. Experiments are performed on the infrared dye DTTCI in room temperature solutions of ethylene glycol, methanol, and acetonitrile. The obtained correlation function is the sum of several Brownian oscillators, of which four are attributed to intrachromophore vibrational dynamics and the other three to solute−solvent dynamics. The ultrafast part of the correlation function on the time scale of the excitation pulses is interpreted as a free induction decay-like effect due to impulsive excitation of spectrally broad underlying vibrational structure in the dye's electronic transition. The slower parts are assigned to multiple time scale solute−solvent dynamics. The effect of vibrational coherences on the echo measurements is also analyzed; this analysis permits the dissection of the correlation function into a part due to intrachromophore dynamics and a part due to solvation dynamics. The spectral densities associated with these latter oscillators are located in the far infrared, in the same spectral region as probed by the optical Kerr effect. The measurements, however, provide no definite answer to the question of whether these spectral densities are the same.
By using stochastic theory, we analyze the non-Markovian temporal behavior in four types of photon echoes, including the two-pulse echo, stimulated echo, accumulated echo, and heterodyne-detected accumulated echo. In particular, the origin of the exp(-ct3{\mathit{ct}}^{3}ct3) dependence of the two-pulse echo in the limit of slow modulation is discussed in detail. It is also pointed out that, at the slow-modulation limit, the temporal behavior of the stimulated echo changes from exp(-ct3{\mathit{ct}}^{3}ct3) dependence to exp(-ct2{\mathit{ct}}^{2}ct2) dependence as the waiting time (the time interval between the second and the third excitation pulses) is varied.
Phase-locked optical coherence experiments were performed on the 10 fs time scale. A 13 fs cavity-dumped Ti:sapphire laser was considered as an ideal source to extend these experiments to the 10 fs time scale due to extremely high amplitude and spectral stability. Femtosecond phase-locked heterodyne detected femtosecond stimulated photon echo (PL-HSPE) proved to be very useful for exploring the details of the optical dynamics of the optical system. The PL-HSPE involves a six-dimensional experiment governed by three times between four fs pulses, two relative phases between paired pulses, and signal amplitude.