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Diagonal time gating of stimulated photon echo: vibrational mode suppression in the non-Markovian limit

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

Published Jan 1, 1996• 0 citations
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Abstract

In this contribution we show that enhanced mode suppression can be obtained by time-gating the stimulated photon echo (SPE) at the conventional echo time and in phase with the wave packet dynamics. This novel technique is demonstrated on a dye solution of DTTCI in ethylene glycol. As it was directly shown recently, the dynamics of such a system is distinctly non-Markovian.

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

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

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.

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Vibrational Mode Suppression in the Non-Markovian Limit: Diagonal Time-Gating of the Stimulated Photon Echo

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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.

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Stimulated photon echoes (SPEs) with time duration comparable to the coherent lifetime and Rabi period have been investigated theoretically and experimentally with an angled beam configuration. The Rabi oscillation effects on both the transmitted field (optical nutation) and the SPE fields are explained by analytic solutions of Maxwell-Bloch equations. The theory also predicts that an echo can exist in the noncausal direction, and this was confirmed by experiments with Tm:YAG crystal.

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

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.

The Journal of Physical Chemistry•Jan 1, 1996•223 citations
In this contribution we show that enhanced mode suppression can be obtained by time-gating the stimulated photon echo (SPE) at the conventional echo time and in phase with the wave packet dynamics. This novel technique is demonstrated on a dye solution of DTTCI in ethylene glycol. As it was directly shown recently, the dynamics of such a system is distinctly non-Markovian.
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.
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.
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.