Force-field modeling through quantum mechanical calculations: Molecular dynamics simulations of a nematogenic molecule in its condensed phases (original) (raw)

Abstract

Interaction energy of the 4-n-pentyloxy-4 -cyanobiphenyl (5OCB) dimer is computed at MP2 level, for many geometrical arrangements using the Fragmentation Reconstruction Method (FRM). DFT calculations are performed for a number of geometries of the monomer. The resulting database is used to parameterize an atomistic intra-and intermolecular force-field suitable for classical bulk simulations. Several structural and dynamical properties in 5OCB isotropic and liquid crystalline phases are computed from molecular dynamics simulation mainly in the NPT ensemble. Lengthy runs (more than 70 ns) and large sample sizes (up to 806 molecules) were used to determine the nematic to isotropic transition temperature up to a precision of few K. Good agreement was found in most of the investigated properties, thus validating the accuracy of the proposed model potential, only derived by quantum mechanical calculations.

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References (76)

  1. Allen, M. P.; Tildesley, D. J. Computer Simulation of Liquids; Claren- don: Oxford, 1987. Journal of Computational Chemistry DOI 10.1002/jcc
  2. Frenkel, D.; Smith, B. Understanding Molecular Simulations, Academic Press: San Diego, 1996.
  3. Pasini, P.; Zannoni, C. Eds. Advances in the Computer Simulations of Liquid Crystals, NATO ASI series; Kluwer: Dordrecht, 2000.
  4. Kremer, K. Macromol Chem Phys 2003, 204, 257.
  5. Pasini, P.; Zannoni, C.; Zumer, S. Computer Simulations of Liquid Crystals and Polymers, NATO ASI series; Kluwer: Dordrecht, 2005.
  6. Hautpmann, S.; Mosell, T.; Reiling, S.; Brickmann, J. J Chem Phys 1996, 208, 57.
  7. Yakovenko, S. Y.; Muravski, A. A.; Eikelschulte, F.; Geiger, A. Liq Cryst 1998, 24, 657.
  8. Cacelli, I.; Campanile, S.; Prampolini, G.; Tani, A. J Chem Phys 2002, 117, 448.
  9. Cheung, D. L.; Clark, S. J.; Wilson, M. R. Chem Phys Lett 2002, 356, 140.
  10. Crain, J.; Komolkin, A. V. Adv Chem Phys 1999, 109, 39.
  11. Care, C. M.; Cleaver, D. J. Rep Prog Phys 2005, 68, 2665.
  12. Berardi, R.; Muccioli, L.; Zannoni, C. Chem Phys Chem 2004, 5, 104.
  13. Peláez, J.; Wilson, M. Phys Chem Chem Phys 2007, 9, 2968.
  14. Tiberio, G.; Muccioli, L.; Berardi, R., Zannoni, C. ChemPhysChem, submitted
  15. Chandrasekhar, S. Liquid Crystals; Cambridge University Press: Cam- bridge, 1977.
  16. Collings, P. J. Liquid Crystals-Nature's Delicate Phase of Matter; Adam Hilger: Bristol, 1990.
  17. Collings, P. J.; Hird, M. Introduction to Liquid Crystals; Adam Hilger: Bristol, 1997.
  18. deGennes, P. G.; Prost, J. The Physics of Liquid Crystals, second edition; Oxford University Press: Oxford, 1993.
  19. Cacelli, I.; Prampolini, G.; Tani, A. J Phys Chem B 2005, 109, 3531.
  20. Cacelli, I.; De Gaetani, L.; Prampolini, G.; Tani, A. J Phys Chem B 2007, 111, 2130.
  21. Amovilli, C.; Cacelli, I.; Campanile, S.; Prampolini, G. J Chem Phys 2002, 117, 3003.
  22. Amovilli, A.; Cacelli, I.; Cinacchi, G.; De Gaetani, L.; Prampolini, G.; Tani, A. Theor Chim Accounts 2007, 117, 885.
  23. Bizzarri, M.; Cacelli, I.; Prampolini, G.; Tani, A. J Phys Chem A 2004, 108, 10336.
  24. Cacelli, I.; De Gaetani, L.; Prampolini, G.; Tani, A. Mol Cryst Liq Cryst 2007, 465, 175.
  25. De Gaetani L., Prampolini, G., Tani A. J Phys Chem B, accepted.
  26. Gray, G. W.; Herrison, K. J.; Constant, J.; Hulme, D. S.; Kirton, J.; Raynes, E. P. In Liquid Crystals and Ordered Fluids; Johnson, J. F.; Porter, R. S.; Plenum Press: New York, 1974.
  27. Hobza, P.; Selzle, H. L.; Schlag, E. W. J Phys Chem 1996, 100, 18790.
  28. Tsuzuki, S.; Honda, K.; Uchimaru, T.; Mikami, M.; Tanabe, K. J Am Chem Soc 2002, 124, 104.
  29. Hobza, P.; Sponer, J. J Am Chem Soc 2002, 124, 11802.
  30. Reyes, A.; Tlenkopatchev, M. A.; Fomina, L.; Guadarrama, P.; Fomine, S. J Phys Chem A 2003, 107, 7027.
  31. Sinnokrot, M. O.; Sherrill, C. D. J Phys Chem A 2006, 110, 10656.
  32. Cacelli, I.; Cinacchi, G.; Prampolini, G.; Tani, A. J Am Chem Soc 2004, 126, 14278.
  33. Hobza, P.; Zahradník, R.; Müller-Dethlefs, K. Collect Czech Chem. Commun 2006, 71, 443.
  34. De Gaetani, L.; Prampolini, G.; Tani, A. J Phys Chem B 2006, 110, 2847.
  35. Cacelli, I.; Prampolini, G. J Chem Theory Comput 2007, 3, 1803.
  36. Tsuzuki, S.; Uchimaru, T.; Mikami, M.; Urata, S. J Chem Phys 2004, 121, 9917.
  37. Hernandes, M. Z.; Longo, R. L. J Mol Model 2005, 11, 61.
  38. Rowley, R.; Tracy, C.; Pakkanen, T. J Chem Phys 2006, 125, 154302.
  39. Sushmita Sen, M.; Brahma, P.; Roy, S. K.; Mukherjee, D. K.; Roy, S. B. Mol Cryst Liq. Cryst 1983, 100, 327.
  40. Becke, A. D. J Chem Phys 1993, 98, 5648.
  41. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Gill, P. M. W.; Johnson, B. G.; Robb, M. A.; Cheeseman, J. R.; Keith, T. A.; Petersson, G. A.; Montgomery, J. A.; Raghavachari, K.; Al-Laham, M. A.; Zakrzewski, V. G.; Ortiz, J. V.; Foresman, J. B.; Cioslowski, J.; Stefanov, B. B.; Nanayakkara, A.; Challacombe, M.; Peng, C. Y.; Ayala, P. Y.; Chen, W.; Wong, M. W.; Andres, J. L.; Replogle, E. S.; Gomperts, R.; Martin, R. L.; Fox, D. J.; Binkley, J. S.; Defrees, D. J.; Baker, J.; Stewart, J. P.; Head-Gordon, M.; Gonzalez, C.; Pople, J. A. Gaussian 03 (Revision A.1), Gaussian, Inc., Pittsburgh PA, 2003.
  42. Boys, S. F.; Bernardi, F. Mol Phys 1970, 19, 553.
  43. Paschen, D.; Geiger, A. MOSCITO 3.9; Department of Physical Chemistry: University of Dortmund, 2000.
  44. Ryckaert, J. P.; Ciccotti, G.; Berendsen, H. J. C. J Comput Phys 1977, 55, 3336.
  45. Darden, T. A.; York, D.; Pedersen, L. J Chem Phys 1993, 98, 10089.
  46. Essmann, U.; Perera, L.; Berkowitz, M. L.; Darden, A.; Lee, H.; Pedersen, L. J Chem Phys 1995, 103, 8577.
  47. Berendsen, H. J. C.; Postma, J. P. M.; van Gusteren, W. F.; Di Nola, A.; Haak, J. R. J Chem Phys 1984, 81, 3684.
  48. Bates, M. A.; Luckhurst, G. R. J Chem Phys 1999, 110, 7087.
  49. Steele, W. A. J Chem Phys 1963, 38, 2404.
  50. Zakharov, A. Phys Lett A 1994, 193, 471.
  51. Nemstov, V. B. Theor Math Phys 1975, 25, 118.
  52. Zakharov, A. Phys Solid State 1998, 40, 1765.
  53. Fialkowski, M. Phys Rev E 1998, 58, 1955.
  54. Emsley, J. W.; De Luca, G.; Lesage, A.; Merlet, D.; Pileio, G. Liq Cryst 2007, 34, 1071.
  55. Tsuzuki, S.; Honda, K.; Uchimaru, T.; Mikami, M.; Tanabe, K. J Am Chem Soc 2000, 122, 3746.
  56. Emsley, J. W.; DeLuca, G.; Celebre, G.; Longeri, M. Liq Cryst 1996, 20, 569.
  57. Adam, C. J.; Clark, S. J.; Wilson, M. R.; Ackland, G. J.; Crain, J. Mol Phys 1998, 93, 947.
  58. Clark, S. J.; Adam, C. J.; Cleaver, D. J.; Crain, J. Liq Cryst 1997, 22, 477.
  59. Cacelli, I.; Prampolini, G. J Phys Chem A 2003, 107, 8665.
  60. Cinacchi, G.; Prampolini, G. J Phys Chem A 2003, 107, 5228.
  61. Oweimreen, G. A.; Morsy, M. A. Thermochimica Acta 2000, 346, 37.
  62. Wilson, M. R. Int Rev Phys Chem 2005, 24, 421.
  63. Bhattacharjee, B.; Paul, S.; Paul, R. Mol Cry Liq Cry 1982, 89, 181.
  64. Heeks, S. K.; Luckhurst, G. R. J Chem Soc Faraday Trans 1993, 89, 3783.
  65. Guo, W.; Fung, B. M. J Chem Phys 1991, 95, 3917.
  66. Urban, S.; Gestblom, B.; Kuczyński, W.; Pawlus, S.; Würflinger, A. Phys Chem Chem Phys 2003, 5, 924.
  67. Counsell, C. J. R.; Emsley, J. W.; Luckhurst, G. R.; Sachdev, H. S. Mol Phys 1988, 63, 33.
  68. Adam, C. J.; Ferrarini, A.; Wilson, M. R.; Ackland, G. J., and Crain, J. Mol Phys 1999, 97, 541.
  69. Noack, F.; Becker, S.; Struppe, J. Annu Rep NMR Spectrosc 1997, 33, 1.
  70. Hansen, J. P.; McDonald, I. R. Theory of Simple Liquids, Academic Press: New York, 1986.
  71. Dvinskikh, S. V.; Furò, I.; Zimmermann, H.; Maliniak, A. Phys Rev E 2002, 65, 061701.
  72. Kim, M. J.; Cardwell, K.; Khitrin, A. K. J Chem Phys 2004, 120, 11327.
  73. Dong, R. Y. Phys Rev E 1998, 57, 4316.
  74. Dong, R. Y. J Chem Phys 1988, 88, 3962.
  75. Dong, R. Y.; Richards, G. M. Chem Phys Lett 1992, 200, 541.
  76. Siedler, L. T. S.; Hyde, A. J.; Petrick, R. A.; Leslie, F. M. Mol Cryst Liq Cryst 1983, 90, 255.