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Communication: Slow supramolecular mode in amine and thiol derivatives of 2-ethyl-1-hexanol revealed by combined dielectric and shear-mechanical studies
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44. The geometries of 2-ethylohexanol, 2-ethylhexylamine, and 2-ethylhexanethiol molecules, as well as the 5-molecular systems in the ring and the chain configurations, were optimized using Becke’s hybrid exchange and correlated three-parameter with the Lee-Yang-Parr correlation functional (B3LYP) at standard Gaussian basis sets 6-31G(d,p). These calculations were carried out in the gas phase using density functional theory (DFT) approach and the Gaussian09 software package.
See supplementary material at http://dx.doi.org/10.1063/1.4935510
for information about experimental methods and additional results (comparison of the dielectric and shear mechanical dynamics and theoretical calculations of the dipole moment for the chain and ring like structures).[Supplementary Material]
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54. We obtain the following values: G∞ = 0.7 GPa for 2-ethyl-1-hexylamine at 160 K, G∞ = 0.79 GPa for 2-ethyl-1-hexanethiol at 137 K, G∞ = 0.97 GPa for 5PPE at 260 K. Dielectric and shear mechanical data for amine and thiol derivatives of 2-ethyl-1-hexanol can be found in “Glass and Time” data repository.
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In this paper, we present results of dielectric and shear-mechanical studies for amine (2-ethyl-1-hexylamine) and thiol (2-ethyl-1-hexanethiol) derivatives of the monohydroxy alcohol, 2-ethyl-1-hexanol. The amine and thiol can form hydrogen bonds weaker in strength than those of the alcohol. The combination of dielectric and shear-mechanical data enables us to reveal the presence of a relaxation mode slower than the α-relaxation. This mode is analogous to the Debye mode seen in monohydroxy alcohols and demonstrates that supramolecular structures are present for systems with lower hydrogen bonding strength. We report some key features accompanying the decrease in the strength of the hydrogen bonding interactions on the relaxationdynamics close to the glass-transition. This includes changes (i) in the amplitude of the Debye and α-relaxations and (ii) the separation between primary and secondary modes.
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