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Dynamics in condensed molecular systems studied by incoherent light

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Abstract

Applications of incoherent light techniques to time-resolved studies in condensed matter are reviewed. Vibrational dephasing ofβ-carotene and a heptamethine dye was studied by interferometric coherent anti-Stokes Raman scattering in solution revealing dephasing times between 300 fs and 1.1 ps. This technique gives results that are analogos to spectral methods, but vibrational frequencies can be determined more precisely. Electronic dephasing was studied for a variety of dyes. Forced light scattering is used to measure the initial evolution of the lineshape functiong(t) up to about 50 fs. In the lowest order approximation,g(t) =Δ 2 t 2/2,, the dephasing is characterized by a modulation strengthΔ = 25 to 150 THz depending on the dye, the solvent and its temperature, and the pump laser wavelength. Interestingly, the modulation decreases for heptamethine in the long-wavelength tail of the absorption band. Brillouin scattering gives rise to finite dephasing times of neat solvents in forced light scattering.

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Kummrow, A., Lau, A. Dynamics in condensed molecular systems studied by incoherent light. Appl. Phys. B 63, 209–223 (1996). https://doi.org/10.1007/BF01833789

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