Rank-dependent orientational relaxation in an ionic liquid: an all-atom simulation study

Regular Article
Part of the following topical collections:
  1. Foundations of Molecular Modeling and Simulation 2012 Collection

Abstract

We have employed all-atom molecular dynamics simulation to investigate the heterogeneity effects on reorientation correlation time in the ionic liquid (IL), 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim][PF6]), at 298 and 450 K. Our simulated density, radial distribution functions, viscosity, and self-diffusion coefficients compare well with the existing literature data. Even though the room temperature (298 K) simulations could not probe the entire decay of the reorientation correlation function (Cl(t)) due to the inherent slow diffusional timescale in this IL and limited computational resources available, the simulated Cl(t) at high temperature (450 K) captures the entire decay. The ratio between the simulated reorientation time constants, \( R = \frac{{\int_{0}^{\infty } {{\text{d}}tC_{1} (t )} }}{{\int_{0}^{\infty } {{\text{d}}tC_{2} (t )} }} = \frac{{\left\langle {\tau_{1} } \right\rangle }}{{\left\langle {\tau_{2} } \right\rangle }} \), differs considerably from 3 at 450 K, indicating the presence of significant heterogeneity effects even at this high temperature. This observation corroborates well with the simulated non-Gaussian parameter at this temperature.

Keywords

Ionic liquid Simulation Orientational relaxation Rank dependence 

Supplementary material

214_2013_1348_MOESM1_ESM.doc (232 kb)
Supplementary material 1 (DOC 232 kb)

References

  1. 1.
    Hansen JP, McDonald IR (2006) Theory of simple liquids, 3rd edn. Academic, San DiegoGoogle Scholar
  2. 2.
    Rogers RD, Seddon KR (2002) Ionic liquids: industrial application for green chemistry. ACS symposium series 818. American Chemical society, WashingtonCrossRefGoogle Scholar
  3. 3.
    Wasserscheid P, Welton T (2003) Ionic liquids in synthesis. Wiley-VCH, New YorkGoogle Scholar
  4. 4.
    Kobrak MN, Sandalow N (2006) In: Mantz A, Trulove P (eds) Molten salts XIV. Electrochemical Society, New JerseyGoogle Scholar
  5. 5.
    Triolo A, Russina O, Fazio B, Triolo R, Cola ED (2008) Chem Phys Lett 467:362CrossRefGoogle Scholar
  6. 6.
    Wang Y, Voth GA (2005) J Am Chem Soc 127:12192CrossRefGoogle Scholar
  7. 7.
    Samanta A (2010) J Phys Chem Lett 1:1557CrossRefGoogle Scholar
  8. 8.
    Samanta A (2006) J Phys Chem B 110:13704CrossRefGoogle Scholar
  9. 9.
    Arzhantsev S, Jin H, Baker GA, Maroncelli M (2007) J Phys Chem B 111:4978CrossRefGoogle Scholar
  10. 10.
    Zhang X-X, Liang M, Ernsting NP, Maroncelli M (2012) J Phys Chem B. doi:10.1021/jp305430a
  11. 11.
    Turton DA, Hunger J, Stoppa A, Hefter G, Thoman A, Walther M, Buchner R, Wynne K (2009) J Am Chem Soc 131:11140CrossRefGoogle Scholar
  12. 12.
    Huang M-M, Bulut S, Crossing I, Weingertner H (2010) J Chem Phys 133:101101CrossRefGoogle Scholar
  13. 13.
    Muramatsu M, Nagasawa Y, Miyasaka H (2011) J Phys Chem A 115:3886CrossRefGoogle Scholar
  14. 14.
    Kashyap HK, Biswas R (2010) J Phys Chem B 114:16811CrossRefGoogle Scholar
  15. 15.
    Kashyap HK, Biswas R (2010) J Phys Chem B 114:254CrossRefGoogle Scholar
  16. 16.
    Daschakraborty S, Biswas R (2012) J Chem Phys 137:114501CrossRefGoogle Scholar
  17. 17.
    Daschakraborty S, Biswas R (2011) Chem Phys Lett 510:210CrossRefGoogle Scholar
  18. 18.
    Daschakraborty S, Biswas R (2011) J Phys Chem B 115:4011CrossRefGoogle Scholar
  19. 19.
    Triolo A, Russina O, Fazio B, Appetecchi GB, Carewska M, Passerini S (2009) J Chem Phys 130:164521CrossRefGoogle Scholar
  20. 20.
    Santos CS, Murthy NS, Baker GA, Castner EW Jr (2011) J Chem Phys 134:121101CrossRefGoogle Scholar
  21. 21.
    Kashyap HK, Santos CS, Annapureddy HVR, Murthy NS, Margulis CJ, Castner EW Jr (2012) Faraday Discuss 154:133CrossRefGoogle Scholar
  22. 22.
    Mandal PK, Sarkar M, Samanta A (2004) J Phys Chem A 108:9048CrossRefGoogle Scholar
  23. 23.
    Sasmal DK, Mandal AK, Mondal T, Bhattacharyya K (2011) J Phys Chem B 115:7781CrossRefGoogle Scholar
  24. 24.
    Shah JK, Brennecke JF, Maginn EJ (2001) Green Chem 4:112CrossRefGoogle Scholar
  25. 25.
    Lopes JNC, Deschamps J, Padua AAH (2004) J Phys Chem B 108:2038CrossRefGoogle Scholar
  26. 26.
    Liu Z, Huang S, Wang W (2004) J Phys Chem B 108:12978CrossRefGoogle Scholar
  27. 27.
    Liu Z, Wu X, Wang W (2006) Phys Chem Chem Phys 8:1096CrossRefGoogle Scholar
  28. 28.
    Bhargava BL, Balasubramanian S (2007) J Chem Phys 127:114510CrossRefGoogle Scholar
  29. 29.
    Morrow TI, Maginn EJ (2002) J Phys Chem B 106:12807CrossRefGoogle Scholar
  30. 30.
    Margulis CJ, Stern HA, Berne BJ (2002) J Phys Chem B 106:12017CrossRefGoogle Scholar
  31. 31.
    Sarangi SS, Zhao W, Muller-Plathe F, Balasubramanian S (2010) ChemPhysChem 11:2001Google Scholar
  32. 32.
    Hu Z, Margulis CJ (2006) Proc Natl Acad Sci USA 103:831CrossRefGoogle Scholar
  33. 33.
    Powles JG (1953) J Chem Phys 21:633CrossRefGoogle Scholar
  34. 34.
    Madden P, Kivelson D (1984) Adv Chem Phys 56:467CrossRefGoogle Scholar
  35. 35.
    Biswas R, Bagchi B (1996) J Phys Chem 100:1238CrossRefGoogle Scholar
  36. 36.
    Bagchi B (2012) Molecular relaxation in liquids. Oxford University Press, New YorkGoogle Scholar
  37. 37.
    Smith W, Forester TR (eds) (2010) DL_POLY_2.2. CCLRC Daresbury Laboratory, DaresburyGoogle Scholar
  38. 38.
    Lyubartsev AP, Laaksonen A (2000) Comput Phys Commun 128:565CrossRefGoogle Scholar
  39. 39.
    Cornell WD, Cieplak P, Bayly CI, Gould IR, Merz KM, Ferguson DM, Spellmeyer DC, Fox T, Caldwell JW, Kollman PA (1995) J Am Chem Soc 117:5179CrossRefGoogle Scholar
  40. 40.
    Allen MP, Tildesley DJ (1987) Computer simulations of liquids. Oxford University Press, New YorkGoogle Scholar
  41. 41.
    Kumar PV, Maroncelli M (1995) J Chem Phys 103:3038CrossRefGoogle Scholar
  42. 42.
    Martyna GJ, Tuckerman ME, Tobias DJ, Klein M (1996) Mol Phys 87:1117CrossRefGoogle Scholar
  43. 43.
    Martyna GJ, Klein M, Tuckerman ME (1992) J Chem Phys 97:2635CrossRefGoogle Scholar
  44. 44.
    Nose S (1984) J Chem Phys 81:511CrossRefGoogle Scholar
  45. 45.
    Hoover WG (1985) Phys Rev A 31:1695CrossRefGoogle Scholar
  46. 46.
    Tokuda H, Hayamizu K, Ishii K, Susan ABH, Watanabe M (2004) J Phys Chem B 108:16593CrossRefGoogle Scholar
  47. 47.
    Gu ZY, Brennecke JF (2002) J Chem Eng Data 47:339CrossRefGoogle Scholar
  48. 48.
    Amyes TL, Diver ST, Richard JP, Rivas FM, Toth K (2004) J Am Chem Soc 126:4366CrossRefGoogle Scholar
  49. 49.
    Fernandes AM, Rocha MAA, Freire MG, Marrucho IM, Coutinho JAP, Santos LMNBF (2011) J Phys Chem B 115:4033CrossRefGoogle Scholar
  50. 50.
    Daschakraborty S, Biswas R (2012) J Chem Sci 124:763CrossRefGoogle Scholar
  51. 51.
    Fumino K, Wulf A, Ludwig R (2008) Angew Chem Int Ed 47:3830CrossRefGoogle Scholar
  52. 52.
    Men S, Lovelock KRJ, Licence P (2011) Phys Chem Chem Phys 13:15244CrossRefGoogle Scholar
  53. 53.
    Thar J, Brehm M, Seitsonen AP, Kirchner B (2009) J Phys Chem B 113:15129CrossRefGoogle Scholar
  54. 54.
    Brehm M, Weber H, Pensado AS, Stark A, Kirchner B (2012) Phys Chem Chem Phys 14:5030CrossRefGoogle Scholar
  55. 55.
    Pal T, Biswas R (2011) Chem Phys Lett 517:180CrossRefGoogle Scholar
  56. 56.
    Faupel F, Frank W, Macht M-P, Mehrer H, Naundorf V, Ratzke K, Schober HR et al (2003) Rev Mod Phys 75:237CrossRefGoogle Scholar
  57. 57.
    Habasaki J, Ngai KL (2006) J Non-Cryst Solids 352:5170CrossRefGoogle Scholar
  58. 58.
    Roy D, Patel N, Conte S, Maroncelli M (2010) J Phys Chem B 114:8410CrossRefGoogle Scholar
  59. 59.
    Del Popolo MG, Voth GA (2004) J Phys Chem B 108:1744CrossRefGoogle Scholar
  60. 60.
    Hunger J, Stoppa A, Schrodle S, Hefter G, Buchner R (2009) Chem Phys Chem 10:723CrossRefGoogle Scholar
  61. 61.
    Tokuda H, Hayamizu K, Ishii K, Susan MABH, Watanabe M (2005) J Phys Chem B 109:6103CrossRefGoogle Scholar
  62. 62.
    Matyushov DV (2005) J Chem Phys 122:044502CrossRefGoogle Scholar
  63. 63.
    Kometani N, Arzhantsev S, Maroncelli M (2006) J Phys Chem A 110:3405CrossRefGoogle Scholar
  64. 64.
    Fredlake CP, Crosthwaite JM, Hert DG, Aki SNVK, Brennecke JF (2004) J Chem Eng Data 49:954CrossRefGoogle Scholar
  65. 65.
    Huddleston JG, Visser AE, Reichert WM, Willauer HD, Broker GA, Rogers RD (2001) Green Chem 3:156CrossRefGoogle Scholar
  66. 66.
    Roy D, Maroncelli M (2010) J Phys Chem B 114:12629CrossRefGoogle Scholar
  67. 67.
    Gabl S, Schroder C, Steinhauser O (2012) J Chem Phys 137:094501CrossRefGoogle Scholar
  68. 68.
    Koddermann T, Ludwig R, Paschek D (2008) ChemPhysChem 9:1851CrossRefGoogle Scholar
  69. 69.
    Bhargava BL, Balasubramanian S (2005) J Chem Phys 123:144505CrossRefGoogle Scholar
  70. 70.
    Picalek J, Kolafa J (2009) Mol Simul 35:685CrossRefGoogle Scholar
  71. 71.
    Awad WH, Gilman JW, Nyden M, Harris RH, Sutto TE, Callahan J, Truelove PC, Delong HC, Fox DM (2004) Thermochim Acta 409:3CrossRefGoogle Scholar
  72. 72.
    Rahman A (1964) Phys Rev 136:405CrossRefGoogle Scholar
  73. 73.
    Faupel F, Frank W, Macht M-P, Mehrer H, Naundorf V, Ratzke K, Schober HR et al (2003) Rev Mod Phys 75:237CrossRefGoogle Scholar
  74. 74.
    Habasaki J, Ngai K (2008) J Chem Phys 129:194501CrossRefGoogle Scholar
  75. 75.
    Bagchi B (1989) Annu Rev Phys Chem 40:115CrossRefGoogle Scholar
  76. 76.
    Guchhait B, Daschakraborty S, Biswas R (2012) J Chem Phys 136:174503CrossRefGoogle Scholar
  77. 77.
    Funston AM, Fadeeva TA, Wishart JF, Castner EW Jr (2007) J Phys Chem B 111:4963CrossRefGoogle Scholar
  78. 78.
    Turton DA, Sonnleitner T, Ortner A, Walther M, Hefter G, Buchner R, Wynne K (2012) Faraday Discuss 154:145CrossRefGoogle Scholar
  79. 79.
    Patel N, Biswas R, Maroncelli M (2002) J Phys Chem B 106:7096CrossRefGoogle Scholar
  80. 80.
    Zhang Y, Maginn EJ (2012) J Phys Chem B 116:10036CrossRefGoogle Scholar
  81. 81.
    Dommert F, Wendler K, Berger R, Delle Site L, Holm C (2012) ChemPhysChem 13:1625CrossRefGoogle Scholar
  82. 82.
    Schmidt J, Krekeler C, Dommert F, Zhao Y, Berger R, Delle Site L, Holm C (2010) J Phys Chem B 114:6150CrossRefGoogle Scholar
  83. 83.
    Wendler K, Zahn S, Dommert F, Berger R, Holm C, Kirchner B, Delle Site L (2011) J Chem Theory Comput 7:3040CrossRefGoogle Scholar
  84. 84.
    Wendler K, Dommert F, Zhao Y, Berger R, Holm C, Delle Site L (2012) Faraday Discuss 154:111CrossRefGoogle Scholar
  85. 85.
    Dommert F, Schmidt J, Krekeler C, Zhao YY, Berger R, Delle Site L, Holm C (2010) J Mol Liq 152:2CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2013

Authors and Affiliations

  1. 1.Department of Chemical, Biological and Macromolecular SciencesS. N. Bose National Centre for Basic SciencesKolkataIndia

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