Advertisement

Ab initio MRD-CI study of neutral and charged Ga2, Ga3 and Ga4 clusters and comparison with corresponding boron and aluminum clusters

  • U. Meier
  • S. D. Peyerimhoff
  • F. Grein
Original Contributions

Abstract

MRD-CI calculations were performed on Ga, Ga2, Ga3, Ga4 and on the corresponding positive and negative ions. In general, pseudopotentials were used, and 4s4p/2s2p basis sets withs andp diffuse functions and one or twod functions. For Ga2, all-electron calculations were also performed. For Ga 2 (±) , potential functions for ground and low-lying excited states are given. For Ga 3 (±) , geometries were optimized both inC2v andD∞h symmetry. The lowest state of Ga 3 + is found to be1Σ g + , of Ga34A2, and of Ga 3 1A1 (D3h). Ionization potentials and electron affinities of Ga3 were evaluated. Many low-lying excited states of Ga 3 (±) were found. Rhombic (D2h, including squareD4h), tetrahedral (T d ), T-shaped (C2v) and linear structures (D∞h) were investigated in the search for the lowest state of Ga4. A square-planar arrangement of the nuclei, withR e = 5.30 a0, was found to have the lowest energy. The other geometries lie about 0.5 eV higher. InD2h symmetry, low-lying excited states of Ga4, as well as ground and excited states of Ga 4 + and Ga 4 were studied.

Geometries, ionization potentials, electron affinities, atomization and fragmentation energies of Ga n are compared with corresponding data for B n and Al n . Typical changes in going from first-row to third-row atoms are observed.

PACS

31.20.D 

Preview

Unable to display preview. Download preview PDF.

Unable to display preview. Download preview PDF.

References

  1. 1.
    Koutecký, J., Fantucci, P.: Chem. Rev.86, 539 (1986) and references thereinGoogle Scholar
  2. 2.
    See for instance Surf. Sci156 (1985) and Z. Phys. D — Atoms, Molecules and Clusters3 (1986) devoted entirely to this subjectGoogle Scholar
  3. 3.
    Hanley, L., Whitten, J.L., Anderson, S.L.: J. Phys. Chem.92, 5803 (1988)Google Scholar
  4. 4.
    Ginter, D.S., Ginter, M.L., Innes, K.K.: Astrophys. J.139, 365 (1963)Google Scholar
  5. 5.
    Douglas, M.A., Hauge, R.H., Margrave, J.L.: J. Phys. Chem.87, 2945 (1983)Google Scholar
  6. 6.
    Bauschlicher, C.W., Partridge, H., Langhoff, S.R., Taylor, P.R., Walch, S.P.: J. Chem. Phys.86, 7007 (1987)Google Scholar
  7. 7.
    Cai, M.F., Dzugan, T.P., Boudybey, V.E.: Chem. Phys. Lett.155, 430 (1989)Google Scholar
  8. 8.
    Bruna, P.J., Peyerimhoff, S.D.: In: Advances in Chemical Physics, Vol. 67, K.P. Lawley (ed.), p. 1, New York: Wiley 1987Google Scholar
  9. 9.
    Balasubramanian, K.: J. Phys. Chem.90, 6786 (1986)Google Scholar
  10. 10.
    Balasubramanian, K.: J. Phys. Chem.93, 8388 (1989)Google Scholar
  11. 11.
    Meier, U., Peyerimhoff, S.D., Bruna, P.J., Grein, F.: J. Mol. Spectr.134, 259 (1989)Google Scholar
  12. 12.
    Balasubramanian, K.: J. Chem. Phys.86, 3410 (1987)Google Scholar
  13. 13.
    Balasubramanian, K., Feng, P.Y.: Chem. Phys. Lett.146, 155 (1988)Google Scholar
  14. 14.
    O'Brien, S.C., Liu, Y., Zhang, Q., Heath, J.R., Tittel, F.K., Curl, R.F., Smalley, R.E.: J. Chem. Phys.84, 4074 (1986)Google Scholar
  15. 15.
    Liu, Y., Zhang, Q.-L., Tittel, F.K., Curl, R.F., Smalley, R.E.: J. Chem. Phys.85, 7434 (1986)Google Scholar
  16. 16.
    Zhang, Q.L., Liu, Y., Curl, R.F., Tittel, F.K., Smalley, R.E.: J. Chem. Phys.88, 1670 (1988)Google Scholar
  17. 17.
    Buenker, R.J., Peyerimhoff, S.D.: Theor. Chim. Acta35, 33 (1974); ibid39, 217 (1975)Google Scholar
  18. 18.
    Buenker, R.J., Peyerimhoff, S.D., Butscher, W.: Mol. Phys.35, 771 (1978)Google Scholar
  19. 19.
    Buenker, R.J., Peyerimhoff, S.D.: In: New horizons of quantum chemistry, P.P. Löwdin, B. Pullman (eds.), p. 183, Dordrecht: Reidel 1983Google Scholar
  20. 20. (a)
    Barthelat, J.C., Durand, Ph., Serafini, A.: Mol. Phys.33, 159 (1977);Google Scholar
  21. 20. (b)
    Durand, Ph., Barthelat, J.C.: Mol. Phys.33, 283 (1977)Google Scholar
  22. 21.
    Meier, U., Peyerimhoff, S.D., Grein, F.: Chem. Phys. (in press)Google Scholar
  23. 22.
    Pacchioni, G.F., Fantucci, P., Giunchi, G., Barthelat, J.C.: Gazz. Chim. Ital.110, 183 (1980)Google Scholar
  24. 23.
    Pacchioni, G., Fantucci, P.: Gazz. Chim. Ital.111, 233 (1981)Google Scholar
  25. 24.
    Pacchioni, G., Fantucci, P., Koutecký, J.: Chem. Phys. Lett.142, 85 (1987)Google Scholar
  26. 25.
    Dunning, T.H.: J. Chem. Phys.66, 1382 (1977)Google Scholar
  27. 26.
    Huzinaga, S.: J. Chem. Phys.42, 1293 (1965)Google Scholar
  28. 27.
    Dunning, T.H.: J. Chem. Phys.55, 716 (1971)Google Scholar
  29. 28.
    Dunning, T.H., Hay, P.J.: Modern theoretical chemistry, Vol. 3, Methods of electronic structure theory. Schaefer, H.F. (ed.), p. 1, New York: Plenum 1978Google Scholar
  30. 29.
    Langhoff, S.R., Davidson, E.R.: Int. J. Quantum. Chem.8, 61 (1974)Google Scholar
  31. 30. (a)
    Bruna, P.J., Peyerimhoff, S.D.: Chem. Phys. Lett.72, 278 (1980);Google Scholar
  32. 30. (b)
    Buenker, R.J., Peyerimhoff, S.D., Bruna, P.J.: Computational organic chemistry. Csizmadia, I.G., Daudel, R. (eds.), p. 55, Dordrecht: Reidel 1981Google Scholar
  33. 31.
    Moore, C.E.: Atomic Energy Levels, National Bureau on Standards, Washington, D.C. (1971)Google Scholar
  34. 32.
    Hotop, H., Lineberger, W.C.: Phys. Chem. Ref. Data14, 731 (1985)Google Scholar
  35. 33.
    Böhmer, H.-U., Peyerimhoff, S.D.: Z. Phys. D — Atoms, Molecules and Clusters3, 195 (1986)Google Scholar
  36. 34.
    v. Arnim, M., Nestmann, B., Peyerimhoff, S.D.: to be publishedGoogle Scholar
  37. 35.
    Bauschlicher, C.W., Pettersson, L.G.M.: J. Chem. Phys.87, 2198 (1987)Google Scholar
  38. 36.
    Froben, F.W., Schulze, W., Kloss, U.: Chem. Phys. Lett.99, 500 (1983)Google Scholar
  39. 37.
    Huber, K.P., Herzberg, G.: Molecular Spectra and Molecular Structure. IV. Constants of Diatomic Molecules; New York: Van Nostrand 1979Google Scholar
  40. 38.
    Buenker, R.J., Peyerimhoff, S.D.: Chem. Rev.74, 127 (1974) and references thereinGoogle Scholar
  41. 39.
    Pettersson, L.G.M., Bauschlicher, C.W., Halicioglu, T.: J. Chem. Phys.87, 2205 (1987)Google Scholar
  42. 40.
    Basch, H.: Chem. Phys. Lett.136, 289 (1987)Google Scholar
  43. 41.
    Upton, T.H.: J. Chem. Phys.86, 7054 (1987)Google Scholar
  44. 42.
    Tse, J.S.: J. Mol. Spectr. (THEOCHEM)165, 21 (1988)Google Scholar
  45. 43.
    Abe, H., Kolb, D.: Ber. Bunsenges. Phys. Chem.87, 523 (1983)Google Scholar
  46. 44.
    Leleyter, M., Joyes, P.J.: J. Phys. B13, 2165 (1980)Google Scholar
  47. 45.
    Pacchioni, G.: Theor. Chim. Acta (Berl.)62, 461 (1983)Google Scholar
  48. 46.
    Lamson, S.H., Messmer, R.P.: Chem. Phys. Lett.98 (1983)Google Scholar
  49. 47.
    Fox, D.J., Schaefer, F.F.: J. Chem. Phys.78, 328 (1983)Google Scholar
  50. 48.
    Basch, H., Stevens, W.J., Krauss, M.: Chem. Phys. Lett.109, 212 (1984)Google Scholar
  51. 49.
    McLean, A.D., Liu, B., Chandler, G.S.: J. Chem. Phys.80, 5130 (1984)Google Scholar
  52. 50.
    Upton, T.H.: J. Phys. Chem.90, 754 (1986)Google Scholar
  53. 51.
    Sunil, K.K., Jordan, K.D.: J. Phys. Chem.92, 2774 (1988)Google Scholar
  54. 52.
    Howard, J.A., Sutcliffe, R., Tse, J.S., Dahmane, H., Mile, B.: J. Phys. Chem.89, 3595 (1985)Google Scholar
  55. 53.
    Cox, D.M., Trevor, D.J., Whetten, R.L., Rohlfing, E.A., Kaldor, A.: J. Chem. Phys.84, 4651 (1986)Google Scholar
  56. 54.
    Pacchioni, G., Plavsić, D., Koutecký, J.: Ber. Bunsenges. Phys. Chem.87, 503 (1983)Google Scholar
  57. 55.
    Pacchioni, G., Koutecký, J.: Ber. Bunsenges. Phys. Chem.88, 242 (1984)Google Scholar
  58. 56.
    Koutecký, J., Pacchioni, G., Jeung, G.H., Hass, E.C.: Surf. Sci.156, 650 (1985)Google Scholar
  59. 57.
    Bauschlicher, C.W., Pettersson, L.G.M.: J. Chem. Phys.84, 2226 (1986)Google Scholar
  60. 58.
    Kutzelnigg, W.: Angew. Chem.96, 262 (1984)Google Scholar
  61. 59.
    Martin, J.M.L., Francois, J.P., Gijbels, R.: J. Chem. Phys.90, 6469 (1989)Google Scholar
  62. 60.
    Marinelli, F., Pellegatti, A.: Chem. Phys. Lett.158, 545 (1989)Google Scholar
  63. 61.
    Hanley, L., Anderson, S.L.: J. Phys. Chem.91, 5161 (1987)Google Scholar
  64. 62.
    Upton, T.H., Cox, D.M., Kaldor, A.: In: The physics and chemistry of small clusters. Jena P. (ed.), New York: Plenum 1987Google Scholar
  65. 63.
    Jarrold, M.F., Bower, J.E., Kraus, J.S.: J. Chem. Phys.86, 3876 (1987)Google Scholar
  66. 64.
    Hanley, L., Ruatta, S.A., Anderson, S.L.: J. Chem. Phys.87, 260 (1987)Google Scholar
  67. 65.
    Ganteför, G., Gausa, M., Meiwes-Broer, K.H., Lutz, H.O.: Z. Phys. D — Atoms, Molecules and Clusters9, 253 (1988)Google Scholar
  68. 66.
    Mulliken, R.S.: J. Chem. Phys.23, 1833 (1955)Google Scholar

Copyright information

© Springer-Verlag 1990

Authors and Affiliations

  • U. Meier
    • 1
  • S. D. Peyerimhoff
    • 1
  • F. Grein
    • 2
  1. 1.Lehrstuhl für Theoretische ChemieUniversität BonnBonn 1Federal Republic of Germany
  2. 2.Department of ChemistryUniversity of New BrunswickFrederictonCanada

Personalised recommendations