Revisiting Dynamic Processes and Relaxation Mechanisms in a Heterocyclic Glass-Former: Direct Observation of a Transient State Article Swipe
Andrzej Nowok
,
Hubert Hellwig
,
Mateusz Dulski
,
Maria Książek
,
Joachim Kusz
,
P. Kuś
,
Sebastian Pawlus
·
YOU?
·
· 2024
· Open Access
·
· DOI: https://doi.org/10.1021/acs.jpcb.3c06727
YOU?
·
· 2024
· Open Access
·
· DOI: https://doi.org/10.1021/acs.jpcb.3c06727
Despite decades of studies, a clear understanding of near-Tg phenomena remains challenging for glass-forming systems. This review delves into the intricate molecular dynamics of the small, heterocyclic thioether, 6-methyl-2,3-dihydro-1,4-benzodithiine (MeBzS2), with a particular focus on its near-Tg cold crystallization and relaxation mechanisms. Investigating isothermal crystallization kinetics at various temperatures reveals a significant interplay between its molecular dynamics and recrystallization from a supercooled liquid. We also identify two independent interconversion paths between energetically privileged conformers, characterized by strained transition states. We demonstrate that these spatial transformations induce substantial alterations in the dipole moment orientation and magnitude. Our investigation also extends to the complex salt PdCl2(MeBzS2), where we observe the transient conformers directly, revealing a direct relationship between their abundance and the local or macroscopic electric field. The initially energetically privileged isomers in an undisturbed system become less favored in the presence of an external electric field or ions, resulting even in an unexpected inversion of states. Consequently, we confirm the intramolecular character of secondary relaxation in MeBzS2 and its mechanism related to conformational changes within the heterocyclic ring. The research is based on the combination of broadband dielectric spectroscopy, X-ray diffraction, and quantum density functional theory calculations.
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- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1021/acs.jpcb.3c06727
- OA Status
- hybrid
- Cited By
- 2
- References
- 57
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4392013583
All OpenAlex metadata
Raw OpenAlex JSON
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https://openalex.org/W4392013583Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.1021/acs.jpcb.3c06727Digital Object Identifier
- Title
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Revisiting Dynamic Processes and Relaxation Mechanisms in a Heterocyclic Glass-Former: Direct Observation of a Transient StateWork title
- Type
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articleOpenAlex work type
- Language
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enPrimary language
- Publication year
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2024Year of publication
- Publication date
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2024-02-21Full publication date if available
- Authors
-
Andrzej Nowok, Hubert Hellwig, Mateusz Dulski, Maria Książek, Joachim Kusz, P. Kuś, Sebastian PawlusList of authors in order
- Landing page
-
https://doi.org/10.1021/acs.jpcb.3c06727Publisher landing page
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YesWhether a free full text is available
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hybridOpen access status per OpenAlex
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https://doi.org/10.1021/acs.jpcb.3c06727Direct OA link when available
- Concepts
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Chemical physics, Relaxation (psychology), Dipole, Intramolecular force, Supercooling, Conformational isomerism, Molecular dynamics, Chemistry, Materials science, Computational chemistry, Crystallography, Thermodynamics, Stereochemistry, Molecule, Physics, Organic chemistry, Social psychology, PsychologyTop concepts (fields/topics) attached by OpenAlex
- Cited by
-
2Total citation count in OpenAlex
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2025: 2Per-year citation counts (last 5 years)
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57Number of works referenced by this work
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10Other works algorithmically related by OpenAlex
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