Structural properties of atactic polystyrene of different thermal history obtained from a multiscale simulation

T. Mulder; V.A. Harmandaris; A.V. Lyulin; N.F.A. Vegt,  van der; K. Kremer; M.A.J. Michels

doi:10.1021/ma800873z

Structural properties of atactic polystyrene of different thermal history obtained from a multiscale simulation

T. Mulder, V.A. Harmandaris, A.V. Lyulin, N.F.A. Vegt, van der, K. Kremer, M.A.J. Michels

Research output: Contribution to journal › Article › Academic › peer-review

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Abstract

A method is presented to obtain well-equilibrated atactic polystyrene (aPS) samples for molecular simulations. The method starts with equilibrating the polymer in the melt at length scales beyond the Kuhn length lK, using end-bridging Monte Carlo techniques; at this level a (2:1)-coarse-grained description of aPS is being employed. Subsequently atomistic detail is reintroduced, and the sample is equilibrated at the smallest length scales as well. At length scales beyond lK the simulated polymer chain conformations fulfill the random-coil hypothesis of Flory, and C8 = 8.7 ± 0.1 at 463 K. Eventually various glassy samples are created by subjecting the melt sample to different cooling rates. Pair correlations are in agreement with existing X-ray data, and the amount of dihedral angles in the trans (t) state agrees with NMR data. On the level of dyads, the conformations of racemic dyads agree well with existing NMR results. At the same time, meso dyads conformations do not agree: 65% of meso dyads is in the gt/tg state (NMR: 80%); 25% is in tt state (NMR:

Original language	English
Pages (from-to)	384-391
Number of pages	8
Journal	Macromolecules
Volume	42
Issue number	1
DOIs	https://doi.org/10.1021/ma800873z
Publication status	Published - 2009

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@article{1cd7813858cf4fff9b1c5ebe2dbebee0,

title = "Structural properties of atactic polystyrene of different thermal history obtained from a multiscale simulation",

abstract = "A method is presented to obtain well-equilibrated atactic polystyrene (aPS) samples for molecular simulations. The method starts with equilibrating the polymer in the melt at length scales beyond the Kuhn length lK, using end-bridging Monte Carlo techniques; at this level a (2:1)-coarse-grained description of aPS is being employed. Subsequently atomistic detail is reintroduced, and the sample is equilibrated at the smallest length scales as well. At length scales beyond lK the simulated polymer chain conformations fulfill the random-coil hypothesis of Flory, and C8 = 8.7 ± 0.1 at 463 K. Eventually various glassy samples are created by subjecting the melt sample to different cooling rates. Pair correlations are in agreement with existing X-ray data, and the amount of dihedral angles in the trans (t) state agrees with NMR data. On the level of dyads, the conformations of racemic dyads agree well with existing NMR results. At the same time, meso dyads conformations do not agree: 65% of meso dyads is in the gt/tg state (NMR: 80%); 25% is in tt state (NMR:",

author = "T. Mulder and V.A. Harmandaris and A.V. Lyulin and {Vegt, van der}, N.F.A. and K. Kremer and M.A.J. Michels",

year = "2009",

doi = "10.1021/ma800873z",

language = "English",

volume = "42",

pages = "384--391",

journal = "Macromolecules",

issn = "0024-9297",

publisher = "American Chemical Society",

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T1 - Structural properties of atactic polystyrene of different thermal history obtained from a multiscale simulation

AU - Mulder, T.

AU - Harmandaris, V.A.

AU - Lyulin, A.V.

AU - Vegt, van der, N.F.A.

AU - Kremer, K.

AU - Michels, M.A.J.

PY - 2009

Y1 - 2009

N2 - A method is presented to obtain well-equilibrated atactic polystyrene (aPS) samples for molecular simulations. The method starts with equilibrating the polymer in the melt at length scales beyond the Kuhn length lK, using end-bridging Monte Carlo techniques; at this level a (2:1)-coarse-grained description of aPS is being employed. Subsequently atomistic detail is reintroduced, and the sample is equilibrated at the smallest length scales as well. At length scales beyond lK the simulated polymer chain conformations fulfill the random-coil hypothesis of Flory, and C8 = 8.7 ± 0.1 at 463 K. Eventually various glassy samples are created by subjecting the melt sample to different cooling rates. Pair correlations are in agreement with existing X-ray data, and the amount of dihedral angles in the trans (t) state agrees with NMR data. On the level of dyads, the conformations of racemic dyads agree well with existing NMR results. At the same time, meso dyads conformations do not agree: 65% of meso dyads is in the gt/tg state (NMR: 80%); 25% is in tt state (NMR:

AB - A method is presented to obtain well-equilibrated atactic polystyrene (aPS) samples for molecular simulations. The method starts with equilibrating the polymer in the melt at length scales beyond the Kuhn length lK, using end-bridging Monte Carlo techniques; at this level a (2:1)-coarse-grained description of aPS is being employed. Subsequently atomistic detail is reintroduced, and the sample is equilibrated at the smallest length scales as well. At length scales beyond lK the simulated polymer chain conformations fulfill the random-coil hypothesis of Flory, and C8 = 8.7 ± 0.1 at 463 K. Eventually various glassy samples are created by subjecting the melt sample to different cooling rates. Pair correlations are in agreement with existing X-ray data, and the amount of dihedral angles in the trans (t) state agrees with NMR data. On the level of dyads, the conformations of racemic dyads agree well with existing NMR results. At the same time, meso dyads conformations do not agree: 65% of meso dyads is in the gt/tg state (NMR: 80%); 25% is in tt state (NMR:

U2 - 10.1021/ma800873z

DO - 10.1021/ma800873z

M3 - Article

SN - 0024-9297

VL - 42

SP - 384

EP - 391

JO - Macromolecules

JF - Macromolecules

IS - 1

ER -

Structural properties of atactic polystyrene of different thermal history obtained from a multiscale simulation

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