Structure and low-frequency vibrational properties of (H₂O)₁₀ composed of a ring form of (H₂O)₄ and a cage form of (H₂O)₆

Abstract

One minimum energy structure of the water decamer composed of a ring form of the water tetramer and a cage form of the water hexamer is calculated at the Hartree–Fock, MP2, and density functional theory levels using the 6-31++G(d,p) and/or aug-cc-pVDZ basis sets. It has been shown that the basic structure of the isolated water tetramer and hexamer is retained in the decamer structure irrespective of the levels of theory. As a result of the intercluster hydrogen bonds between the water tetramer and hexamer, two types of four-coordinated water molecules are formed in the decamer. We have further carried out frequency calculations for the water decamer as well as the water tetramer and hexamer to investigate how the intermolecular dynamics of the water clusters are affected by their size and the coordination environments of the constituent water molecules. It has been found that a two-band feature around 60 and 170 cm^-1 can be seen in the vibrational density of states of the water decamer and that a similar feature can also be seen in those of the water tetramer and hexamer. These intermolecular modes around 60 and 170 cm^-1 are described as the O···O···O bending and the O···O···O stretching vibrations of hydrogen bonds, respectively. On the basis of these calculated results, we then discuss the low-frequency Raman spectra of liquid water, which is also characterized by two bands in this frequency range.

References

1. K. Liu, J. D. Cruzan and R. J. Saykally, Science, 1996, 271, 929.
2. K. Liu, M. G. Brown and R. J. Saykally, J. Phys. Chem., 1997, 101, 8995.
3. J. K. Gregory and D. C. Clary, J. Phys. Chem., 1996, 100, 18014.
4. S. S. Xantheas and T. H. Dunning, Jr., J. Chem. Phys., 1993, 98, 8037; S. S. Xantheas and T. H. Dunning, Jr., J. Chem. Phys., 1993, 99, 8774; S. S. Xantheas, J. Chem. Phys., 1995, 102, 4505; S. S. Xantheas, J. Chem. Phys., 1996, 104, 8821.
5. M. W. Feyereisen, D. Feller and D. A. Dixon, J. Phys. Chem., 1996, 100, 2993.
6. C. J. Tsai and K. D. Jordan, Chem. Phys. Lett., 1993, 213, 181; C. J. Tsai and K. D. Jordan, J. Phys. Chem., 1993, 97, 5208.
7. K. Kim, K. D. Jordan and T. Z. Zwier, J. Am. Chem. Soc., 1994, 116, 11568.
8. C. Lee, H. Chen and G. Fitzgerald, J. Chem. Phys., 1994, 101, 4472; C. Lee, H. Chen and G. Fitzgerald, J. Chem. Phys., 1995, 102, 1266.
9. B. J. Mhin, J. Kim, S. Lee, J. Y. Lee and K. S. Kim, J. Chem. Phys., 1994, 100, 4484.
10. K. Laasonen, F. Csajka and M. Parinello, Chem. Phys. Lett., 1992, 194, 172; K. Laasonen, M. Parinello, R. Car, C. Lee and D. Vanderbilt, Chem. Phys. Lett., 1993, 207, 208; K. Laasonen and M. L. Klein, J. Phys. Chem., 1994, 98, 10079.
11. J. M. Pedulla, F. Vila and K. D. Jordan, J. Chem. Phys., 1996, 105, 11091.
12. L. S. Sremaniak, L. Perera and M. L. Berkowitz, J. Chem. Phys., 1996, 105, 3715.
13. E. Honegger and S. Leutwyler, J. Chem. Phys., 1998, 88, 2582; R. Knochenmuss and S. Leutwyler, J. Chem. Phys., 1992, 96, 5233.
14. M. Schütz, W. Klopper, H.-P. Lüthi and S. Leutwyler, J. Chem. Phys., 1995, 103, 6114.
15. D. J. Wales and T. R. Walsh, J. Chem. Phys., 1997, 106, 7193.
16. O. Mó, M. Yánez and J. Elguero, J. Chem. Phys., 1992, 97, 6628.
17. J. K. Gregory and D. C. Clary, J. Chem. Phys., 1995, 102, 7817; J. K. Gregory and D. C. Clary, J. Chem. Phys., 1995, 103, 8924.
18. K. Liu, M. G. Brown, C. Carter, R. J. Saykally, J. K. Gregory and D. C. Clary, Nature, 1996, 381, 501.
19. D. Eisenberg and W. Kauzmann, in The Structure and Properties of Water, Oxford University Press, London, 1969.
20. C. Møller and M. S. Plesset, Phys. Rev., 1934, 46, 618.
21. A. D. Becke, J. Chem. Phys., 1993, 98, 5648; P. J. Stephens, F. J. Devlin, M. J. Frisch and C. F. Chabalowski, J. Phys. Chem., 1994, 98, 11623.
22. R. Ditchfield, W. J. Hehre and J. A. Pople, J. Chem. Phys., 1971, 54, 724; W. J. Hehre, R. Ditchfield and J. A. Pople, J. Chem. Phys., 1972, 56, 2257; P. C. Hariharan and J. A. Pople, Mol. Phys., 1974, 27, 209; M. S. Gordon, Chem. Phys. Lett., 1980, 76, 163; P. C. Hariharan and J. A. Pople, Theor. Chim. Acta, 1973, 28, 213.
23. D. E. Woon and T. H. Dunning, Jr., J. Chem. Phys., 1993, 98, 1358; R. A. Kendall, T. H. Dunning, Jr. and R. J. Harrison, J. Chem. Phys., 1992, 96, 6796; T. H. Dunning, Jr., J. Chem. Phys., 1989, 90, 1007.
24. U. Buck, I. Ettischer, M. Melzer, V. Buck and J. Sadlej, Phys. Rev. Lett., 1998, 80, 2578.
25. M. Masella and J. P. Flament, J. Chem. Phys., 1997, 107, 9105.
26. M. J. Frisch, G. W. Trucks, H. B. Schlegel, P. M. W. Gill, B. G. Johnson, M. A. Robb, J. R. Cheeseman, T. Keith, G. A. Petersson, J. A. Montgomery, K. Raghavachari, M. A. Al-Laham, V. G. Zakrzewski, J. V. Ortiz, J. B. Foresman, C. Y. Peng, P. Y. Ayala, W. Chen, M. W. Wong, J. L. Andres, E. S. Replogle, R. Gomperts, R. L. Martin, D. J. Fox, J. S. Binkley, D. J. Defrees, J. Baker, J. P. Stewart, M. Head-Gordon, C. Gonzalez and J. A. Pople, Gaussian 94, Revision D3, Gaussian Inc., Pittsburgh, 1995.
27. J. E. H. Koehler, W. Saenger and B. Lesyng, J. Comput. Chem., 1987, 8, 1090.
28. J. K. Gregory, D. C. Clary, K. Liu, M. G. Brown and R. J. Saykally, Science, 1997, 275, 814.
29. A. H. Narten, W. E. Thiessen and L. Blum, Science, 1982, 217, 1033.
30. J. O. Jung and R. B. Gerber, J. Chem. Phys., 1996, 105, 10332.
31. G. E. Walrafen, J. Chem. Phys., 1964, 40, 3249.
32. A. K. Soper, J. Chem. Phys., 1994, 101, 6888.
33. S. Krishnamurthy, R. Bansil and J. Waife-Akenten, J. Chem. Phys., 1983, 79, 5863.
34. F. Aliotta, C. Vasi, G. Maisano, D. Majolino, F. Mallamace and P. Migliardo, J. Chem. Phys., 1986, 84, 4731.
35. G. E. Walrafen, M. R. Fisher, M. S. Hokmabadi and W.-H. Yang, J. Chem. Phys., 1986, 85, 6970.
36. G. E. Walrafen, M. S. Hokmabadi, W.-H. Yang, Y. C. Chu and B. Monosmith, J. Phys. Chem., 1989, 93, 2909.
37. J. L. Rousset, E. Duval and A. Boukenter, J. Chem. Phys., 1990, 92, 2150.
38. G. E. Walrafen, J. Phys. Chem., 1990, 94, 2237.
39. K. Mizoguchi, A. Hori and Y. Tominaga, J. Chem. Phys., 1992, 97, 1961.
40. M. H. Brooker, G. Hancock, B. C. Rice and J. Shapter, J. Raman Spectrosc., 1989, 20, 683.
41. E. W. Castner, Jr., Y. J. Chang, Y. C. Chu and G. E. Walrafen, J. Chem. Phys., 1995, 102, 653.
42. M. Sampoli, G. Ruocco and F. Sette, Phys. Rev. Lett., 1997, 79, 1678.
43. M. A. Ricci, R. Ruocco and M. Sampoli, Mol. Phys., 1989, 67, 19.
44. W. B. Bosma, L. E. Fried and S. Mukamel, J. Chem. Phys., 1993, 98, 4413.
45. S. Sastry, H. E. Stanley and F. Sciortino, J. Chem. Phys., 1994, 100, 5361.
46. S. Saito and I. Ohmine, J. Chem. Phys., 1995, 102, 3566.
47. F. Sciortino and P. Tartaglia, Phys. Rev. Lett., 1997, 78, 2385.
48. I. Ohmine and H. Tanaka, J. Chem. Phys., 1990, 93, 8138.
49. T. Nakamura, Phys. Rev. Lett., 1998, 80, 1244.
50. Y. Wang and Y. Tominaga, J. Chem. Phys., 1994, 101, 3453.
51. M. Frisch, Y. Yamaguchi, H. F. Schaefer, III and J. S. Binkley, J. Chem. Phys., 1986, 84, 531.
52. D. J. DeFrees and A. D. McLean, J. Chem. Phys., 1985, 82, 333.
53. J. Jäckle, in Topics in Current Physics, ed. W. A. Phillips, Springer, Berlin, 1981, vol. 24, p. 135.
54. T. Pang, Phys. Rev. B: Condens. Matter, 1992, 45, 2490.
55. M. Krüger, M. Soltwisch, I. Petscherizin and D. Quitmann, J. Chem. Phys., 1992, 96, 7352.
56. T. Achibat, A. Boukenter, E. Duval, G. Lorentz and S. Etienne, J. Chem. Phys., 1991, 95, 2949.
57. T. Uchino and T. Yoko, J. Chem. Phys., 1998, 108, 8130.
58. T. Uchino and T. Yoko, J. Chem. Phys., 1996, 105, 4140.
59. T. Uchino and T. Yoko, Science, 1996, 273, 480.