Experimentally driven atomistic model of 1,2 Polybutadiene

Lists

Download

[thumbnail of Experimentally_driven_atomistic_model_of_1,2_polybutadiene.pdf]

Preview

Experimentally_driven_atomistic_model_of_1,2_polybutadiene.pdf - Accepted Version (1MB) | Preview

Available under license: Creative Commons Attribution

Tools

Gkourmpis, T. and Mitchell, G. R. (2014) Experimentally driven atomistic model of 1,2 Polybutadiene. Journal of Applied Physics, 115 (5). 053505. ISSN 0021-8979 doi: 10.1063/1.4863950

Abstract/Summary

We present an efficient method of combining wide angle neutron scattering data with detailed atomistic models, allowing us to perform a quantitative and qualitative mapping of the organisation of the chain conformation in both glass and liquid phases. The structural refinement method presented in this work is based on the exploitation of the intrachain features of the diffraction pattern and its intimate linkage with atomistic models by the use of internal coordinates for bond lengths, valence angles and torsion rotations. Atomic connectivity is defined through these coordinates that are in turn assigned by pre-defined probability distributions, thus allowing for the models in question to be built stochastically. Incremental variation of these coordinates allows for the construction of models that minimise the differences between the observed and calculated structure factors. We present a series of neutron scattering data of 1,2 polybutadiene at the region 120-400K. Analysis of the experimental data yield bond lengths for C-C and C=C of 1.54Å and 1.35Å respectively. Valence angles of the backbone were found to be at 112° and the torsion distributions are characterised by five rotational states, a three-fold trans-skew± for the backbone and gauche± for the vinyl group. Rotational states of the vinyl group were found to be equally populated, indicating a largely atactic chan. The two backbone torsion angles exhibit different behaviour with respect to temperature of their trans population, with one of them adopting an almost all trans sequence. Consequently the resulting configuration leads to a rather persistent chain, something indicated by the value of the characteristic ratio extrapolated from the model. We compare our results with theoretical predictions, computer simulations, RIS models and previously reported experimental results.

Altmetric Badge

Additional Information	STFC
Item Type	Article
URI	https://reading-clone.eprints-hosting.org/id/eprint/35727
Item Type	Article
Refereed	Yes
Divisions	Interdisciplinary centres and themes > Chemical Analysis Facility (CAF) > Electron Microscopy Laboratory (CAF)
Additional Information	STFC
Publisher	American Institue of Physics
Publisher Statement	The following article has been accepted by Journal of Applied Physics. After it is published, it will be found at http://scitation.aip.org/content/aip/journal/jap Copyright (year) Author(s). This article is distributed under a Creative Commons Attribution 3.0 Unported License.
Download/View statistics	View download statistics for this item

Download Statistics

Downloads

Downloads per month over past year

Deposit Details

Date Deposited:	22 Jan 2014 11:18	Date item deposited into CentAUR
Last Modified:	23 Jun 2024 04:43	Date item last modified

References

1. Volkenstein M. V. Configurational Statistics of Polymer Chains, New York, Wiley-Interscience, 1963. 2. Flory P. J. Statistical Mechanics of Chain Molecules, New York, Wiley-Interscience, 1969. 3. Lovell R., Mitchell, G. R. and Windle, A. H., Faraday Discuss. Chem. Soc. 68, 46 (1979) 4. Frick, B. and Richter, D. Science 267, 1939 (1995) 5. Richter, D. Physica B 276-278, 22 (2000) 6. Mitchell, G. R. in Order in the Amorphous State of Polymers Eds. Keinath S. E. Miller R. L. Rieke J. K. Plenum, New York, 1987. 7. Mitchell, G. R. in Comprehensive Polymer Science Eds. Allen G. Bevington J. C. Booth C. Price C. Pergamon, Oxford, 1989. 8. Mitchell G. R. and Rosi-Schwartz B. Physica B 180, 558 (1992) 9. Rosi-Schwartz B. and Mitchell G. R., Polymer, 35, 3139 (1994) 10. Mitchell G. R., Rosi-Schwartz B. and Ward D. J., Phil. Trans. R. Soc. Lond. A, 348, 97 (1994) 11. Rosi-Schwartz B. and Mitchell G. R., Nucl. Instr. And Meth. In Phys. A, 354, 17 (1995) 12. Rosi-Schwartz B. and Mitchell G. R., Physica Scripta, T57, 161 (1995) 13. Gkourmpis T. and Mitchell G. R., Macromolecules, 44, 3140 (2011) 14. McGreevy R. L. and Pusztai L., Mol. Sim., 1, 359 (1988) 15. Chanda, M. and Roy, S. K. Plastics Technology Handbook, CRC Press, New York 2007. 16. Solomon, G. Discuss. Faraday Soc. 2, 361 (1947) 17. Natta, G. and Corradini, P. Angew. Chem. 68, 615 (1956) 18. Mark, J. E. J. Am. Chem. Soc. 88, 4354 (1966) 19. Deegan, R. D. and Nagel, S. R. Phys Rev B, 52, 5653 (1995) 20. Arbe, A. Richter, D. Colmenero, J. and Farago, B. Rhys Rev E, 54, 3853 (1996) 21. Ma, H. and Zhang, L. Polym. J. 26, 121 (1994) 22. Kim, E. Misra, S. and Mattice, W. L. Macromolecules 26, 3424 (1993) 23. Getoso, P. Nicol, E. Doxastakis, M. and Theodorou, D. N. Macromolecules 36, 6925 (2003) 24. Smith, G. D. Paul, W. Monkenbush, M. Willner, L. Richter, D. Qiu, X. H. and Ediger, M. D. Macromolecules 32, 8857 (1999) 25. Birshtein, T. M. and Pitisyn, O. B. Conformations of Macromolecules, Interscience, New York 1966 26. Mitchell G. R. MESA, A Molecular Editor for Structural Analysis, Reading UK 1996 27. Flory P. J. J. Chem. Phys. 17, 303 (1949) 28. Warren B. E. X-Ray Diffraction, Addison-Wesley, Reading, MA 1969 29. Mitchell, G. R. Lovell, R. and Windle A. H. Polymer 23, 1273 (1982) 30. Squires, G. L. Introduction to the Theory of Thermal Neutron Scattering, Dover, London, 1996 31. Windsor, C. G. Pulsed Neutron Scattering, Taylor & Francis, London, 1981 32. Turner, J. Z. Soper, A. K. Howells, W. S. Hannon, A. C. and Ansell, S. SANDALS Survival Guide version 2.5, Rutherford-Appleton Laboratory, ISIS Facility, Chilton, 1995. 33. Bevington P. R. Data Reduction and Error Analysis for the Physical Sciences, McGraw-Hill, New York, 1969 34. Mitchell G. R. in Essentials of Neutron Techniques in Soft Matter, Eds. Imae T., Kanaya T., Furusaka T., Willey 2010 35. Gkourmpis T., Lopez D. and Mitchell G. R., 2012 Mater. Res. Soc. Symp. Proc., 1524, (2013) 36. Benmore, C. J. and Soper, A. K. RAL Technical Report RAL-TR-1998-006, Rutherford-Appleton Laboratory, ISIS Facility, Chilton, 1998 37. McLain S. E., Bowron D. T., Hannon A. C. and Soper A. K. Gudrun A Computer Program Developed for Analysis of Neutron Diffraction Data, ISIS Facility, Rutherford-Appleton Laboratory, UK 2012 38. Frick B. Richter B. and Ritter C. Europhys. Lett. 9, 557 (1989) 39. Mitchell G. R. in Concise Encyclopaedia of the Structure of Materials Ed. Martin J. W.; Elsevier, London 2007 40. Mitchell G. R. and Chiou Y-S. Advances in X-Ray Analysis 41, 640 (1997) 41. Carpenter R. L. Kramer O. and Ferry J. D. Macromolecules, 10, 117 (1977) 42. He T. Li B. and Ren S. J. Appl. Polym. Sci., 31, 873 (1986) 43. Ni S. Yu F. Shen L. and Qian B. Chin. J. Polym. Sci., 5, 120 (1987) 44. De Rosa C. Zhi G. Napolitano R. and Pirozzi B. Macromolecules, 18, 2328 (1985) 45. Corradini P. Napolitano R. Petraccone V. Pirozzi B. and Tuzi A. Macromolecules, 15, 1207 (1982) 46. Corradini P. De Rosa C. Zhi G. Napolitano R. and Pirozzi B. Eur. Polym. J., 21, 635 (1985) 47. Hattam P., Gauntlett S., Mays J. W., Hadjichristidis N., Young R. N. and Fetters L. J. Macromolecules 24, 6199 (1991) 48. Jang J. H. Halioglu T. von Meerwall E. D. and Mattice W. L. Macromolecules 33, 4271 (2000) 49. Smith G. D. and Paul W. J. Phys. Chem. A, 102, 1200 (1998) 50. Mitchell G. R. and Windle A. H. Polymer, 25, 906 (1984)

University Staff: Request a correction | Centaur Editors: Update this record

Search Google Scholar