Abstract
Femtosecond two-dimensional infrared (2DIR) spectroscopy was carried out on stereo-selectively synthesized poly-alcohols featuring a quasi-linear array of hydrogen-bonds. From the 2DIR spectra pump-frequency-dependent vibrational lifetimes are extracted, which in turn reflect the strength of the coupling between the hydroxyls constituting the H-bonded chain. The line-broadening dynamics reflect uniquely the conformational control of the scaffold supporting the H-bond wire and the resulting structural flexibility of the hydrogen-bond network.
Highlights
We recently introduced stereoselectively synthesized poly-alcohols as superb low-dimensional model systems for the structural dynamics and the vibrational spectroscopy of random hydrogenbond (H-bond) networks typically encountered in nature [1,2]
We discuss the interrelation between vibrational line broadening dynamics and vibrational relaxation dynamics as exposed by femtosecond two-dimensional infrared spectroscopy (2DIR) in the hydroxyl stretching spectral region of the networks
We focus on the vibrational relaxation dynamics following an initial excitation of the OHstretching fundamental
Summary
We recently introduced stereoselectively synthesized poly-alcohols as superb low-dimensional model systems for the structural dynamics and the vibrational spectroscopy of random hydrogenbond (H-bond) networks typically encountered in nature [1,2]. From the 2DIR spectra pump-frequency-dependent vibrational lifetimes are extracted, which in turn reflect the strength of the coupling between the hydroxyls constituting the H-bonded chain. The line-broadening dynamics reflect uniquely the conformational control of the scaffold supporting the H-bond wire and the resulting structural flexibility of the hydrogen-bond network.
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