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International Conference on Ultrafast Phenomena

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

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

Published Jan 1, 1996• 0 citations
Publisher

Abstract

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.

DOI
10.1364/up.1996.fe.55

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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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The Journal of Chemical Physics•May 7, 2010•16 citations
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.
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.
Optical dephasing of a cyanine dye chromophore in solution is investigated by time-gated photon echo spectroscopy in a three-pulse scattering geometry. The third-order polarization response is gated by up-conversion with a reference pulse in a nonlinear optical crystal. Time gating establishes two controllable periods of system evolution in an optical coherence. The measurements are compared with numerical simulations employing the measured OKE spectrum of solvent (butanol, DMSO) fluctuations. The time-shift of the time-gated echo signals for several gating forming pulse time delays agrees with simulation while the narrower simulated widths suggest a frequency-dependent solute-solvent interaction and the consideration of chromophore vibronic transitions.
The dependence of the electronic absorption spectrum of a dye molecule on the time of delay between the excitation of the molecule by a pump-laser pulse and the probing of the absorption by a test-laser pulse is studied. The effect of dephasing of the molecular transition arising from the interaction with dissipative systems is described by a stochastic modulation of the electronic transition frequency. It is shown that in the case when the two laser pulses are short compared with the correlation time of the frequency modulation and when the spectral linewidth of the pump-laser light is smaller than the bandwidth of the equilibrium absorption spectrum, hole burning appears although the molecules have equal mean transition frequencies. This effect arises from non-Markovian correlations between the dephasings of the molecule during the actions of the pump- and the test-laser pulse. With increasing delay time the holes are smoothed out and disappear when the delay time exceeds the correlation time. Such effects were found in recent femtosecond absorption experiments by Shank et al. [in Ultrafast Phenomena V, dited by G. R. Fleming and A. E. Siegman (Springer, Berlin, 1986), p. 179].
The role of weakly chirped pulses (time bandwidth product, DeltanuDeltatau<0.61) on three-pulse photon echo signals has been systematically studied. Pulses with varying chirp were characterized with frequency resolved optical gating (FROG) and used to measure spectrally resolved three-pulse photon echoes of a dye in solution. The weakly chirped pulses give rise to markedly different echo signals for population times below approximately 100 fs. The chirped pulses can decrease or enhance spectral signatures of an excited state absorption transition in the echo signal. Furthermore, the observed dephasing dynamics depend on the phase of the electric fields. Simulations based on a three-level model and the electric fields retrieved from the FROG traces give a good agreement for photon echo experiments with both transform limited and chirped pulses. The simulations also allow for a numerical investigation of effects of chirp in two-dimensional spectroscopy. For a two-level system, the chirped pulses result in nonelliptical two-dimensional spectra that can erroneously be interpreted as spectral heterogeneity with frequency dependent dephasing dynamics. Furthermore, chirped pulses can give rise to "false" cross peaks when strong vibrational modes are involved in the system-bath interaction.