Molecular dynamics and the translational–rotational coupling of an ionically conducting glass-former: amlodipine besylate?

RSC Advances Pub Date: 2018-06-06 DOI: 10.1039/C8RA01544A

Abstract

We studied the conductivity relaxation originating from a glass-former composed of cations and anions, and the relation to the structural α-relaxation at temperatures above and below the glass transition temperature. The material chosen was amorphous amlodipine besylate (AMB), which is also a pharmaceutical with a complex chemical structure. Measurements were made using differential scanning calorimetry (DSC), broadband dielectric spectroscopy (BDS) and X-ray diffraction, and the characterization was assisted using density functional theory (DFT). The X-ray diffraction pattern confirms the amorphous nature of vitrified AMB. Both the ionic and dipolar aspects of the dynamics of AMB were examined using these measurements and were used to probe the nature of the secondary conductivity and dipolar relaxations and their relation to the conductivity α-relaxation and the structural α-relaxation. The coupling model predictions and quantum mechanical simulations were used side by side to reveal the properties and nature of the secondary conductivity relaxation and the secondary dipolar relaxation. Remarkably, the two secondary relaxations have the same relaxation times, and are one and the same process performing dual roles in conductivity and dipolar relaxations. This is caused by the translation–rotation coupling of the AMB molecule. Thus, AMB has both conductivity α- and β-relaxations, and application of the coupling model shows that these two relaxations are related in the same way as the structural α-relaxation and the Johari–Goldstein β-relaxation are. This important result has an impact on the fundamental understanding of the dynamics of ionic conductivity.

Graphical abstract: Molecular dynamics and the translational–rotational coupling of an ionically conducting glass-former: amlodipine besylate
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