Molecular mobility of amorphous N-acetyl-α-methylbenzylamine and Debye relaxation evidenced by dielectric relaxation spectroscopy and molecular dynamics simulations

Literature Information

Publication Date 2018-12-03
DOI 10.1039/C8CP04880K
Impact Factor 3.676
Authors

Natália T. Correia, Nicolas Couvrat, Frédéric Affouard, Gérard Coquerel, Eric Dargent, Allisson Saiter


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Abstract

The present work focusses on the molecular mobility characterization of amorphous N-acetyl-α-methylbenzylamine (Nac-MBA) by Broadband Dielectric Relaxation Spectroscopy (DRS) coupled with Fast Scanning Calorimetry (FSC) and Molecular Dynamics (MD) simulations covering over 12 decades in the frequency range. This study reveals another example of a secondary amide that shows a very intense Debye-like contribution (almost 90% of the global dielectric intensity) in addition to the structural α-relaxation and secondary Johari–Goldstein β-relaxation. The D- and α-relaxations are separated by about one decade (in frequency) and their relaxation times follow a near parallel temperature evolution (Vogel–Fulcher–Tammann–Hesse). The micro-structure of Nac-MBA has been investigated from MD simulations. It is shown that the intense Debye-like process emanates from the formation of linear intermolecular H-bonding aggregates (precursors of the crystalline structure) generating super-dipole moments.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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