University of Silesia in Katowice

The dataset contains raw dielectric, calorimetric, FTIR, Raman measurement data, and MD and DFT calculation data, presented in the article entitled “Specific interactions and mechanism of association in highly viscous aldehyde 3-phenylpropanal”. In this work, we investigated thermal, dynamical, and structural properties as well as association patterns in 3-phenyl-1-propanol (3P1Pol) and 3-phenyl-1-propanal (3P1Pal) with special attention paid to the latter compound. Both systems turned out to be good glass formers, differing by 17 K in the glass transition temperature, which indicated a strong change in the self-assembly pattern. This supposition was further confirmed by the analysis of dielectric spectra, where, apart from the α-relaxation, a unique Debye (D)-mode, characteristic of self-association, was detected in both samples, marked by different dynamical properties (dielectric strength and timescale separation from the α-process). Further diffraction and infrared investigations, supported by DFT computations and MD simulations, revealed that hydrogen (H)-bonds play a crucial role in the association within 3P1Pol. In contrast, 3P1Pal exhibits at least five distinct intermolecular interactions, including dipole-dipole forces and π-stacking, as well as remarkable H-bonds formed between methylene groups adjacent to the formyl unit and carbonyl moiety. This data not only systematizes the previous understanding of association but also paves the way for new explorations of this phenomenon in aldehydes.