Why does the intermolecular dynamics of liquid biphenyl so closely resemble that of liquid benzene? molecular dynamics simulation of the optical-kerr-effect spectra

Journal of Physical Chemistry B

Volumn 110, Issue 2, 2006, Pages 976-987

  Tao, Guohua ^a   Stratt, Richard M ^a  

^a BROWN UNIVERSITY   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

COMPUTER SIMULATION; MOLECULAR DYNAMICS; OPTICAL KERR EFFECT; OSCILLATIONS; TORQUE; ULTRAFAST PHENOMENA;

INTERMOLECULAR DYNAMICS; LIBRATIONAL DYNAMICS; LIQUID BIPHENYL; MOMENTS OF INERTIA;

BENZENE;

EID: 31544483318     PISSN: 15206106     EISSN: None     Source Type: Journal    
DOI: 10.1021/jp0558932     Document Type: Article

References (73)

1. Fourkas, J. T. In Ultrafast Infrared and Raman Spectroscopy; Fayer, M. D., Ed.; Marcel Dekker: New York, 2001.
2. Andersen, H. C.; Chandler, D.; Weeks, J. D. Adv. Chem. Phys. 1976, 34, 105.
3. Chandler, D. Annu. Rev. Phys. Chem. 1978, 29, 441.
4. Lowden, L. J.; Chandler, D. J. Chem. Phys. 1974, 61, 5228.
5. Narten, A. H. J. Chem. Phys. 1977, 67, 2102.
6. McMorrow, D.; Lotshaw, W. T. Chem. Phys. Lett. 1993, 201, 369.
7. Cong, P.; Duel, H. P.; Simon, J. D. Chem. Phys. Lett. 1995, 240, 72.
8. Chang, Y. J.; Castner, E. W., Jr. J. Phys. Chem. 1996, 100, 3330.
9. Neelakandan, M.; Pant, D.; Quitevis, E. L. J. Phys. Chem. A 1997, 101, 2936.
10. Neelakandan, M.; Pant, D.; Quitevis, E. L. Chem. Phys. Lett. 1997, 265, 283.
11. Smith, N. A.; Lin, S.; Meech, S. R.; Yoshihara, K. J. Phys. Chem. A 1997, 101, 3641.
12. Smith, N. A.; Lin, S.; Meech, S. R.; Shirota, H.; Yoshihara, K. J. Phys. Chem. A 1997, 101, 9578.
13. Smith, N. A.; Meech, S. R. J. Phys. Chem. A 2000, 104, 4223.
14. Ricci, M.; Bartolini, P.; Chelli, R.; Cardini, G.; Califano, S.; Righini, R. Phys. Chem. Chem. Phys. 2001, 3, 2795.
15. Chelli, R.; Cardini, G.; Ricci, M.; Bartolini, P.; Righini, R.; Califano, S. Phys. Chem. Chem. Phys. 2001, 3, 2803.
16. Shirota, H. J. Chem. Phys. 2005, 122, 044514.
17. Ryu, S.; Stratt, R. M. J. Phys. Chem. B 2004, 108, 6782.
18. Ladanyi, B. M.; Liang, Y. Q. J. Chem. Phys. 1995, 103, 6325.
19. Ladanyi, B. M.; Klein, S. J. Chem. Phys. 1996, 105, 1552.
20. Paolantoni, M.; Ladanyi, B. M. J. Chem. Phys. 2002, 117, 3856.
21. Elola, M. D.; Ladanyi, B. M. J. Chem. Phys. 2005, 122, 224506.
22. Skaf, M. S.; Vechi, S. M. J. Chem. Phys. 2003, 119, 2181.
23. Kiyohara, K.; Kamada, K.; Ohta, K. J. Chem. Phys. 2000, 112, 6338.
24. Kiyohara, K.; Kimura, Y.; Takebayashi, Y.; Hirota, N.; Ohta, K. J. Chem. Phys. 2002, 117, 9867.
25. Murry, R. L.; Fourkas, J. T.; Keyes, T. J. Chem. Phys. 1998, 109, 2814.
26. Saito, S.; Ohmine, I. J. Chem. Phys. 1998, 108, 240.
27. Ma, A.; Stratt, R. J. Chem. Phys. 2002, 116, 4972.
28. Ji, X.; Ahlborn, H.; Space, B.; Moore, P. B.; Zhou, Y.; Constantine, S.; Ziegler, L. D. J. Chem. Phys. 2000, 112, 4186.
29. Ji, X.; Ahlborn, H.; Space, B.; Moore, P. B. J. Chem. Phys. 2000, 113, 8693.
30. Friedman, J. S.; She, C. Y. J. Chem. Phys. 1993, 99, 4960.
31. Cong, P.; Simon, J. D.; She, C. Y. J. Chem. Phys. 1996, 104, 962.
32. Farrer, R. A.; Loughnane, B. J.; Deschenes, L. A.; Fourkas, J. T. J. Chem. Phys. 1997, 106, 6901.
33. McMorrow, D.; Thantu, N.; Melinger, J. S.; Kim, S. K.; Lotshaw, W. T. J. Phys. Chem. 1996, 100, 10389.
34. Steffen, T.; Meinders, N. A. C. M.; Duppen, K. J. Phys. Chem. A 1998, 102, 4213.
35. Scodinu, A.; Fourkas, J. T. J. Phys. Chem. B 2003, 107, 44.
36. McMorrow, D.; Lotshaw, W. T. J. Phys. Chem. 1991, 95, 10395.
37. Foggi, P.; Bartolini, P.; Bellini, M.; Giorgini, M. G.; Morresi, A.; Sassi, P.; Cataliotti, R. S. Eur. Phys. J. D 2002, 21, 143.
38. Rajian, J. R.; Hyun, B.-R.; Quitevis, E. L. J. Phys. Chem. A 2004, 108, 10107.
39. Eaton, V. J.; Steele, D. J. Chem. Soc., Fraday Trans. 2 1973, 69, 1601.
40. Chakrabarti, A.; Yashonath, S.; Rao, C. N. R. Mol. Phys. 1995, 84, 49.
41. Buchner, M.; Ladanyi, B. M.; Stratt, R. M. J. Chem. Phys. 1992, 97, 8522.
42. Ladanyi, B. M.; Stratt, R. M. J. Phys. Chem. 1996, 100, 1266.
43. Ladanyi, B. M.; Stratt, R. M. J. Phys. Chem. 1995, 99, 2502.
44. Williams, D. E.; Cox, S. R. Acta Crystallogr. 1984, B40, 404.
45. The molecular structure of biphenyl and the numerical values for the biphenyl potential parameters are taken from Baranyai, A.; Welberry, T. R. Mol. Phys. 1991, 73, 1317. Both this paper and ref 37 use the Williams potential in their simulations of condensed-phase biphenyl.
46. Elola, M. D.; Ladanyi, B. M. J. Chem. Phys. 2005, 122, 224508.
47. MOLDY uses a quaternion representation for the molecular Euler angles and propagates all the molecular coordinates via a modified Beeman predictor-corrector algorithm. Refson, K. MOLDY, release 2.16; 2001; (http://www.earth.ox.ac.uk/~keithr/moldy-manual/moldy.html).
48. Refson, K. Comput. Phys. Commun. 2000, 126, 310.
49. Refson, K. Physica 1985, 131B, 256.
50. -1 for benzene's angular momentum correlation functions.
51. Thermodynamic data for biphenyl were taken from (or derived from the information given in) Daubert, T. E.; Danner, R. P.; Sibul, H. M.; Stebbins, C. C.; Rowley, R. L.; Wilding, W. V.; Oscarson, J. L.; Adams, M. E.; Marshall, T. L. Physical and Thermodynamic Properties of Pure Chemicals: Evaluated Process Design Data; Taylor and Francis: Philadelphia, 1999. The density used in simulating 348 K biphenyl was taken from ref 35.
52. Tensor invariants provide a higher level of configurational averaging than do the individual tensor elements.
53. When we use a single-site model for the polarizability in liquid biphenyl, we also find poor convergence of the dipole-induced-dipole series.
54. Barron, L. D.; Buckingham, A. D. J. Am. Chem. Soc. 1974, 96, 4769.
55. Okruss, M.; Müller, R.; Hese, A. J. Chem. Phys. 1999, 110, 10393.
56. Note that, unlike the approach adopted in ref 18, eq 2.8 does not include any intramolecular renormalization of the two biphenyl site polarizabilities.
57. LeFevre, R. J. W.; Murthy, D. S. N. Aust. J. Chem. 1968, 21, 1903.
58. Some of the amplitude of this peak may also come from direct low-frequency contributions from biphenyl z-axis rotation, a possibility that is symmetry forbidden in benzene. Such low-frequency contributions may also occur in other planar, or near-planar, molecules lacking the special symmetry of benzene.
59. Berne, B. J.; Harp, G. D. Adv. Chem. Phys. 1970, 27, 63.
60. St. Pierre, A. G.; Steele, W. A. Mol. Phys. 1981, 43, 123.
61. Allen, M. P.; Tildesley, D. J. Computer Simulation of Liquids; Clarendon Press: Oxford, 1987; Section 3.3.
62. -4.
63. Stratt, R. M. Acc. Chem. Res. 1995, 28, 201.
64. Cho, M.; Fleming, G. R.; Saito, S.; Ohmine, I.; Stratt, R. M. J. Chem. Phys. 1994, 100, 6672.
65. The expression for the Einstein frequency, eq 4.12, is exact only if the liquid's imaginary frequencies are included in the density of state. However, including the imaginary, frequencies would severely limit the time span over which eq 4.11 remains accurate. In most applications, it is useful, and often quite accurate, to approximate the INM density of states by the normalized density of purely real modes. For liquid benzene under the conditions studied in ref 15, imaginary modes make up only 4.4% of the INM tumbling density of states.
66. "Cylindrical" here to refers to a situation in which all the atoms either lie at a common distance from a rotational axis or on the axis itself. The reader may also note that many of the same arguments could be used to establish the invariance of the translational Einstein frequencies to molecular geometry. Here, though, the similarities with libration end. Translational dynamics is not nearly as well characterized by any single frequency, at least until one reaches the upper band edge.
67. The diffusive behavior of biphenyl has itself been the subject of a detailed OKE study: Deeg, F. W.; Payer, M. D. J. Chem. Phys. 1989, 90, 6893.
68. Lotshaw, W. T.; McMorrow, D. J. Chem. Phys. 1990, 93, 2160.
69. Deeg, F. W.; Fayer, M. D. J. Chem. Phys. 1990, 93, 2162.
70. Our predictions for the near constancy of Einstein frequencies are predicated on the assumption that most of the molecule-to-molecule changes we are interested in involve changes in molecular geometry without significant changes in atomic mass. This assumption is, of course, not valid for simple isotopic substitutions. In such cases, our basic eq 4.16 model would predict that the Einstein frequencies should scale directly with the (inverse square roots of the) moments of inertia.
71. Although there was only a schematic microscopic interpretation proposed at the time, the suggestion that there could be a Gaussian distribution of librational oscillators (analogous to our eqs 4.13 and 4.14) was put forth by Lynden-Bell, R. M.; Steele, W. A. J. Phys. Chem. 1984, 88, 6514. (See also references therein).
72. Some of the quantitative implications of phenomenological librational oscillator pictures have been explored more recently by refs 5, 7, 13, 30, 31, and 35, and by Kamada, K.; Ueda, M.; Ohta, K.; Wang, Y.; Ushida, K.; Tominaga, Y. J. Chem. Phys. 1998, 109, 10948.
73. In much the same way, one could say that the basic energy scale for molecular orbitals is set by atomic orbital energies.