Title :

Impact of chirality on the amorphous state of conglomerate forming systems: a case study of N-acetyl-α-methylbenzylamine

Author(s) :

Atawa, Bienvenu [Auteur]
Groupe de physique des matériaux [GPM]
Couvrat, Nicolas [Auteur]
Sciences et Méthodes Séparatives [SMS]
Affouard, Frédéric [Auteur]
Unité Matériaux et Transformations (UMET) - UMR 8207
T. Correia, Natália [Auteur]
Unité Matériaux et Transformations (UMET) - UMR 8207
Coquerel, Gérard [Auteur]
Sciences et Méthodes Séparatives [SMS]
Saiter-Fourcin, Allisson [Auteur]
Groupe de physique des matériaux [GPM]

Journal title :

Physical Chemistry Chemical Physics

Abbreviated title :

Phys. Chem. Chem. Phys.

Volume number :

23

Pages :

24282-24293

Publisher :

Royal Society of Chemistry (RSC)

Publication date :

2021

ISSN :

1463-9076

HAL domain(s) :

Physique [physics]/Matière Condensée [cond-mat]/Science des matériaux [cond-mat.mtrl-sci]
Physique [physics]/Matière Condensée [cond-mat]/Matière Molle [cond-mat.soft]
Physique [physics]/Matière Condensée [cond-mat]/Systèmes désordonnés et réseaux de neurones [cond-mat.dis-nn]

English abstract : [en]

The present work aims at addressing the issue of molecular handedness in glassy and liquid states and its impact on heterogeneous equilibrium. For this purpose, we evaluated the glass forming ability (GFA), crystallization ...
Show more >The present work aims at addressing the issue of molecular handedness in glassy and liquid states and its impact on heterogeneous equilibrium. For this purpose, we evaluated the glass forming ability (GFA), crystallization propensity, molecular mobility and hydrogen bonding structure of a chiral conglomerate forming system, N-acetyl-α-methylbenzylamine (Nac-MBA), at various enantiomeric excesses (ees) using experimental and computational techniques. We revealed that the rich relaxational landscape (Debye (D), α, βJG and ϒ) and the temperature dependence of the time scale of each process were insensitive to chirality. The most remarkable impact of chirality was expressed on the GFA and the recrystallization of heterochiral arrangements. In fact the GFA increases with decreasing ee, while the crystallization propensity increases with increasing ee. The counter enantiomer acted as a disruptor of crystallization and favored the glass formation upon cooling. The molecular dynamics simulation (MDS) results on the architecture of chiral sequences showed that homochiral sequences were more favorable when compared to heterochiral ones in the liquid state. However, this predisposition to form homochiral sequences in the liquid state was not the precursor of the future crystalline structure, since the liquid or the glassy system recrystallizes as heterochiral sequences. As per our understanding the crystallization was mostly controlled by the mean free migration path of an enantiomer to build homochiral or heterochiral sequences. In the present case, it seems that the mean free migration path achieved by an enantiomer for heterochiral sequences is shorter compared to homochiral arrangements in such a way that the crystallization of the metastable racemic compound is kinetically more favorable.Show less >

Language :

Anglais

Peer reviewed article :

Oui

Audience :

Internationale

Popular science :

Non

Administrative institution(s) :

Université de Lille
CNRS
INRA
ENSCL

Collections :

• Unité Matériaux et Transformations (UMET) - UMR 8207

Research team(s) :

Matériaux Moléculaires et Thérapeutiques

Submission date :

2021-11-16T16:06:09Z
2021-11-16T16:15:24Z
2021-11-19T07:43:13Z