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Study of Two Xanthene Dyes Using Spectrally Resolved Three-Pulse Photon Echo Spectroscopy

Ajitesh Kumar, Satyendra Kumar, Sumit Singhal, Debabrata Goswami

Published May 25, 2015• 0 citations
Publisher

Abstract

Comparative study of the molecular dynamics of two xanthene dye derivatives (Rhodamine-6G and Fluorescein-548) is reported using spectrally resolved three-pulse photon echo spectroscopy. An appreciable change in the coherence and population dynamics was observed between the two xanthene derivatives due to the presence of different functional groups. Solution of Rhodamine-6G in methanol behaves in a more coherent fashion compared to that of Fluorescein-548 dye.

DOI
10.18520/cs/v108/i10/1801-1803

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Comparative study of the molecular dynamics of two xanthene dye derivatives (Rhodamine-6G and Fluorescein-548) is reported using spectrally resolved three-pulse photon echo spectroscopy. An appreciable change in the coherence and population dynamics was observed between the two xanthene derivatives due to the presence of different functional groups. Solution of Rhodamine-6G in methanol behaves in a more coherent fashion compared to that of Fluorescein-548 dye.
Wavelength dependent study of a laser dye: Rhodamine-6G (Rh6G) by using spectrally resolved photon-echo spectroscopy is presented. The coherence and population dynamics of Rh6G solution in methanol changes as the excitation wavelength is tuned near its absorption maxima of 528 nm. Specifically, the central wavelength of the femtosecond laser pulse was set to 535 nm and to 560 nm while the respective spectra of the photon-echo signals were collected. This gives information on how the ultrafast dynamics of the Rh6G molecule changes with a change in the excitation wavelength.
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.
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.
Optical two-dimensional photon-echo spectroscopy is realized with shaped excitation pulses, allowing coherent control of twodimensional spectra. This development enables probing of state-selective quantum decoherence and phase/time sensitive couplings between states. The coherently-controlled two-dimensional photon-echo spectrometer with two pulse shapers is based on a passively stabilized four-beam interferometer with diffractive optic, and allows heterodyne detection of signals with a long-term phase stability of approximately Lambda/100. The two-dimensional spectra of Rhodamine 101 in a methanol solution, measured with unshaped and shaped pulses, exhibit significant differences. We observe in particular, the appearance of fine structure in the spectra obtained using shaped excitation pulses.