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Real-time study of chemical events by ultra-fast IR measurements: unimolecular conformational dynamics and solute solvent interactions


Tuneable femtosecond pulses in the mid-infrared spectral range provide an ultimate tool for real-time studies on chemical events of fundamental importance. In this proposal two conceptually different subjects are to be investigated: the conformational dyna mics of formic acid, and solute-solvent interactions in aqueous solutions. For the study of the conformational dynamics of formic acid, a one-colour infrared-infrared pump-probe population experiment will be designed to interrogate the dynamics of infrared induced isomerization reaction of formic acid in low temperature matrices. We expect to obtain real-time information on population decay of the ground conformational state of formic acid, phonon-assisted vibrational redistribution and relaxation, and form ation of the high energy conformer. For the study of solute-solvent interactions in aqueous solutions, a setup for technically very challenging ultra-fast three photon vibrational echo experiments will be developed in order to investigate in real-time the solute-solvent interactions in aqueous solutions, where steady-state spectra are strongly congested by inhomogenous broadening. Very promising systems for such studies are NH4+/H2O and ND4+/D2O solutions. Fitting the echo data according to the non-linear m aterial response of the given Liouville space path yields detailed picture of the fast structural fluctuations responsible for broad absorption of solvated species. This is perhaps the most fascinating chemical application of ultra-fast technology in the i nfrared.

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