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Spectrally resolved photon-echo spectroscopy of Rhodamine-6G.

Ajitesh Kumar, S. K. Karthick, Debabrata Goswami

Published Feb 1, 2013• 2 citations
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Abstract

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.

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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.
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.
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.
We explore how the width of the three-pulse photon echo signal at long population times can be used to determine the strength of the system-bath interaction. Using simulation with finite pulses we show that a simple relation exist between the width of the echo signal, the coupling strength, and the pulse autocorrelation. The derived model is applied to Rhodamine 6G in alcoholic solution, a paradigm system for the study of solvation dynamics, and the results are compared to conventional methods. The independently determined coupling strength forms the basis for a computationally inexpensive route to determine the entire spectral density, the key parameter when considering system-bath interactions. Our method allows us to accurately estimate the relative amplitude of fast and slow components in the correlation function using only impulsive limit simulations. We show that the peak shift significantly overestimates the amplitude of the fastest decay component for our experimental data. Changing solvent from methanol to 1-hexanol we observe a narrowing of the width of the echo profile. The changes in the echo width allow us to estimate the changes of the coupling strength in various solvents.
The first observation is reported of the primary femtosecond photon echo at a liquid nitrogen temperature in a dye-doped polymer film at a wavelength of 780 nm. Echo signals were generated by pulses with the duration of 130 fs. The echo signal decay can not be described by a simple exponential function. There is a fast decay region below 250-300 fs and a slow decay region at longer time intervals. There were also detected signals of the self-diffraction of exciting pulses on a nonequilibrium population difference grating, induced in resonant medium by these pulses.