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Multiscale modeling of polymers closely coupled to Broad Q neutron scattering from NIMROD

Published online by Cambridge University Press:  25 January 2013

Thomas Gkourmpis
Affiliation:
Innovation & Technology, Borealis AB, Stenungsund SE-444 86, Sweden
Daniel Lopez
Affiliation:
Instituto de Ciencia y Tecnología de Polímeros, CSIC, 28006 Madrid, Spain
Geoffrey R. Mitchell
Affiliation:
Centre for Rapid and Sustainable Product Development, Institute Polytechnic Leiria, Marinha Grande, Portugal
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Abstract

We use data over an extended Q range from 0.01 to 100Å-1 from the recently commissioned NIMROD instrument at the ISIS pulsed neutron source to develop a multi-scale inverse modeling procedure which will provide insight in to the phase transformations of polymer systems. The first level of our procedure is atomistic and we use internal coordinates (bond length, bond angles and torsion angles) to define the polymer chain in full atomistic detail. Values were assigned to each internal coordinate within the chain using a stochastic Monte Carlo method in which the probabilities were drawn from distributions representing the possible range of values. Using this approach, random chain configurations could be rapidly built and the intrachain structure factor calculated utilizing a small set of parameters and compared with the experimental function. Parameters representing the probability distribution functions were systematically varied using a grid search to find the values which gave the best fit to the structure factor for Q > 3Å-1 in order to determine the details of the chain conformation in the molten phase. This process was repeated for data over the same extended Q range obtained at lower temperatures where the polymer was expected to crystallize. Polymers crystallize via chainfolded thin lamellae crystals. Such crystals give rise to an intense peak at Q ∼ 0.03Å-1. This scattering can be calculated using a lamellar stack model, coarse-grained from the single chain structure. We describe this approach using data obtained on the crystallization from the melt phase of perdeuterated polymers. The objective here is to follow the three key length scales; the chain folded lamellar thickness of ∼ 10nm, the crystal unit cell ∼ 1nm and the detail of the chain conformation is ∼ 0.1nm.

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Articles
Copyright
Copyright © Materials Research Society 2013

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References

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