Tracking a glassy polymer on its energy landscape in the course of elastic deformation

N. Lempesis, G.G. Vogiatzis, G.C. Boulougouris, L.C.A. Breemen, van, M. Hutter, D.N. Theodorou

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

10 Citaties (Scopus)

Uittreksel

The response to deformation of a detailed computer model of glassy atactic polystyrene, represented as a collection of basins on its potential energy landscape, has been investigated. The volumetric behaviour of the polymer is calculated via ‘brute force’ molecular dynamics quenching simulations. Results are compared with corresponding estimates obtained by invoking the quasi-harmonic approximation (QHA) for a variety of temperatures below the glass temperature and with experimental data. The stress-controlled uniaxial deformations fall in the linear elastic regime and the resulting strains are calculated as ensemble averages of QHA estimates over 200 uncorrelated inherent structures of the potential energy landscape. The elastic constants (Young’s modulus and Poisson ratio) and their temperature dependence are in very good agreement with experiments for glassy atactic polystyrene. Additionally, a classification of the deformed inherent structures in respect to the geometry and general shape of their energy minima is undertaken. A distortion of the potential energy basins upon mechanical deformation in the elastic regime is observed in all cases.
TaalEngels
Pagina's3430–3441
Aantal pagina's12
TijdschriftMolecular Physics
Volume111
Nummer van het tijdschrift22-23
DOI's
StatusGepubliceerd - 2013

Vingerafdruk

elastic deformation
Elastic deformation
Potential energy
Polymers
potential energy
Polystyrenes
Temperature
polystyrene
polymers
harmonics
Elastic Modulus
Poisson ratio
Elastic constants
Molecular Dynamics Simulation
estimates
approximation
Computer Simulation
Glass
Molecular dynamics
energy

Citeer dit

Lempesis, N. ; Vogiatzis, G.G. ; Boulougouris, G.C. ; Breemen, van, L.C.A. ; Hutter, M. ; Theodorou, D.N./ Tracking a glassy polymer on its energy landscape in the course of elastic deformation. In: Molecular Physics. 2013 ; Vol. 111, Nr. 22-23. blz. 3430–3441
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abstract = "The response to deformation of a detailed computer model of glassy atactic polystyrene, represented as a collection of basins on its potential energy landscape, has been investigated. The volumetric behaviour of the polymer is calculated via ‘brute force’ molecular dynamics quenching simulations. Results are compared with corresponding estimates obtained by invoking the quasi-harmonic approximation (QHA) for a variety of temperatures below the glass temperature and with experimental data. The stress-controlled uniaxial deformations fall in the linear elastic regime and the resulting strains are calculated as ensemble averages of QHA estimates over 200 uncorrelated inherent structures of the potential energy landscape. The elastic constants (Young’s modulus and Poisson ratio) and their temperature dependence are in very good agreement with experiments for glassy atactic polystyrene. Additionally, a classification of the deformed inherent structures in respect to the geometry and general shape of their energy minima is undertaken. A distortion of the potential energy basins upon mechanical deformation in the elastic regime is observed in all cases.",
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Tracking a glassy polymer on its energy landscape in the course of elastic deformation. / Lempesis, N.; Vogiatzis, G.G.; Boulougouris, G.C.; Breemen, van, L.C.A.; Hutter, M.; Theodorou, D.N.

In: Molecular Physics, Vol. 111, Nr. 22-23, 2013, blz. 3430–3441.

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

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AB - The response to deformation of a detailed computer model of glassy atactic polystyrene, represented as a collection of basins on its potential energy landscape, has been investigated. The volumetric behaviour of the polymer is calculated via ‘brute force’ molecular dynamics quenching simulations. Results are compared with corresponding estimates obtained by invoking the quasi-harmonic approximation (QHA) for a variety of temperatures below the glass temperature and with experimental data. The stress-controlled uniaxial deformations fall in the linear elastic regime and the resulting strains are calculated as ensemble averages of QHA estimates over 200 uncorrelated inherent structures of the potential energy landscape. The elastic constants (Young’s modulus and Poisson ratio) and their temperature dependence are in very good agreement with experiments for glassy atactic polystyrene. Additionally, a classification of the deformed inherent structures in respect to the geometry and general shape of their energy minima is undertaken. A distortion of the potential energy basins upon mechanical deformation in the elastic regime is observed in all cases.

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