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In the present work, we analyze the influence of the polarization effectstaking place during the course of a 2DIR spectroscopy experiment performed on amolecular system undergoing an intermolecular vibrational energy transferprocess. When both donor and acceptor molecules participating in thevibrational energy transfer are embedded in a host solvent, they facerotational diffusion that strongly distorts the resulting 2DIR spectra. Itcould be expected that the difference between rotational diffusion constantswill be of particular interest. For this purpose, the polarization effects arediscussed according to the different orderings of the laser-moleculeinteractions. Next, we study the distortions of the spectra as a function ofthe rotational diffusion constants of the individual molecules. The knowledgeof these polarization effects are relevant to the interpretation of thespectra. Finally, the conclusions reached in this work for a vibrational energytransfer are valid for any other type of third-order optical process performedon the same molecular system.

Polarization effects on intermolecular vibrational energy transfer analyzed by 2DIR spectroscopy