Skip to main content
SpringerLink
Log in

New Methods in Quantum Molecular Dynamics of Large Polyatomic Systems

  • Conference paper
Computational Molecular Dynamics: Challenges, Methods, Ideas

Part of the book series: Lecture Notes in Computational Science and Engineering ((LNCSE,volume 4))

  • 1916 Accesses

Abstract

We present new methods for time-dependent quantum mechanical simulations of large polyatomic systems and their applications to photochemical processes in clusters. Two related approaches are discussed: The Classical Separable Potential (CSP) approach, and its extension towards Configuration Interaction (CICSP). The former scheme assumes separability of the vibrational modes of the system, and describes each mode as moving in a mean field due to the other modes. The basic idea, which allows for quantum simulations of hitherto unaccesibly large systems, is that the effective single-mode potentials are obtained from a classical MD simulation that precedes the quantum calculation. The second approach represents an improvement that corrects for correlations between different modes, resulting in a scheme of good accuracy. Applications of the methods are presented for dynamics following photodetachment in a small I−(Ar) 2 cluster (where comparison with numerically exact calculation is possible) and for photoexcitation dynamics and spectroscopy of atomic and molecular impurities in large clusters, such as I 2(Ar) 17 and I 2(Ar) 47 Future directions of method development are suggested in the light of the algorithmic aspects and the applications.

This is a preview of subscription content, log in via an institution to check access.

Access this chapter

Log in via an institution
Chapter
USD 29.95
Price excludes VAT (USA)
  • Available as PDF
  • Read on any device
  • Instant download
  • Own it forever
eBook
USD 84.99
Price excludes VAT (USA)
  • Available as PDF
  • Read on any device
  • Instant download
  • Own it forever
Softcover Book
USD 109.99
Price excludes VAT (USA)
  • Compact, lightweight edition
  • Dispatched in 3 to 5 business days
  • Free shipping worldwide - see info

Tax calculation will be finalised at checkout

Purchases are for personal use only

Institutional subscriptions

Preview

Unable to display preview. Download preview PDF.

Unable to display preview. Download preview PDF.

References

  1. G.C. Schatz, J. Phys. Chem. 100, 12839 (1996).

    Google Scholar 

  2. R. Kosloff, Ann. Rev. Phys. Chem. 45, 145 (1994).

    Google Scholar 

  3. J.Z.H. Zang and W.H. Miller, J. Chem. Phys. 92, 1811 (1990).

    Google Scholar 

  4. U. Manthe, T. Seideman and W.H. Miller, J. Chem. Phys. 92, 10078 (1990).

    Google Scholar 

  5. D. Neuhauser, J. Chem. Phys. 9272 (1994).

    Google Scholar 

  6. U. Peskin and N. Moiseyev, J. Chem. Phys. 99, 4590 (1993).

    Google Scholar 

  7. D.J. Kouri, Y. Houng, W. Zhu and D.K. Hoffman, J. Chem. Phys. 100, 3362 (1994).

    Google Scholar 

  8. D.H. Zang and J.Z.K. Zang, J. Chem. Phys. 100, 2679 (1994).

    Google Scholar 

  9. R. Schinke, Photodissociation Dynamics (Cambridge University Press, Cambridge, 1993).

    Book  Google Scholar 

  10. W.H. Miller, Adv. Chem. Phys. 30, 77 (1975).

    Google Scholar 

  11. E.J. Heller, J. Chem. Phys. 94, 2723 (1994).

    Google Scholar 

  12. B.W. Spath and W.H. Miller, J. Chem. Phys. 104, 95 (1996).

    Google Scholar 

  13. J.G. Kay and W.H. Miller, J. Chem. Phys. 104, 95 (1996).

    Google Scholar 

  14. G.C. Schatz and M.A. Ratner, Quantum Mechanics in Chemistry (Prentice Hall, New Jersey, 1993).

    Google Scholar 

  15. J.B. Anderson, J. Chem. Phys. 63, 1499 (1975).

    Google Scholar 

  16. M.A. Suhm and R.O. Watts, Phys. Rep. 204, 293 (1991).

    Google Scholar 

  17. M.A. McMahan, R.N. Barnet and K.B. Whaley, J. Chem. Phys. 99, 8816 (1993).

    Google Scholar 

  18. S. Broude and R.B. Gerber, Chem. Phys. Lett. 258, 416 (1996).

    Google Scholar 

  19. D. Scharf, G.J. Martyna and M.L. Klein, J. Chem. Phys. 99, 8997 (1993).

    Google Scholar 

  20. V. Buch, J. Chem. Phys. 100, 7610 (1994).

    Google Scholar 

  21. D. Scharf, G.J. Martyna, D. Li, G.A. Voth and M.L. Klein, J. Chem. Phys. 99, 9013 (1993).

    Google Scholar 

  22. J.M. Bowman, Acc. Chem. Res. 19, 202 (1986).

    Google Scholar 

  23. R.B. Gerber and M.A. Ratner, Adv. Chem. Phys. 70, 97 (1988).

    Google Scholar 

  24. A.E. Roitberg, R.B. Gerber, R. Elber and M.A. Ratner, Science 268, 1319 (1995).

    Google Scholar 

  25. N. Makri, Chem. Phys. Lett. 193, 435 (1992).25. N. Makri, Chem. Phys. Lett. 193, 435 (1992).

    Google Scholar 

  26. M. Topaler and N. Makri, Chem. Phys. Lett. 210, 285 (1993).

    Google Scholar 

  27. J. Cao and G.A. Voth, J. Chem. Phys. 100, 5106 (1994).

    Google Scholar 

  28. J. Cao and G.A. Voth, J. Chem. Phys. 101, 6168 (1994).

    Google Scholar 

  29. P.A.M. Dirac, Proc. Camb. Phil. Soc. 26, 376 (1930).

    Google Scholar 

  30. E.J. Heller, J. Chem. Phys. 64, 63 (1976).

    Google Scholar 

  31. R.B. Gerber, V. Buch and M.A. Ratner, J. Chem. Phys. 77, 3022 (1982).

    Google Scholar 

  32. Z. Li and R.B. Gerber, J. Chem. Phys. 99, 8637 (1993).

    Google Scholar 

  33. E. Predj, R.B. Gerber and M.A. Ratner, J. Chem. Phys. 105, 1121 (1996).

    Google Scholar 

  34. N. Makri and W.H. Miller, J. Chem. Phys. 87, 5781 (1987).

    Google Scholar 

  35. H.-D. Meyer, U. Manthe and L.S. Cederbaum, Chem. Phys. Lett. 165, 73 (1990).

    Google Scholar 

  36. U. Manthe, H.-D. Mayer and L.S. Cederbaum, J. Chem. Phys. 97, 3199 (1992).

    Google Scholar 

  37. G.A. Worth, H.-D. Mayer and L.S. Cederbaum, J. Chem. Phys. (in press).

    Google Scholar 

  38. J.-Y. Fang and H. Guo, J. Chem. Phys. 101, 5831 (1994).

    Google Scholar 

  39. J.-Y. Fang and H. Guo, J. Chem. Phys. 102, 2404 (1995).

    Google Scholar 

  40. Z. Kotler, E. Neria and A. Nitzan, Cornput. Phys. Commun. 63, 243 (1991).

    Google Scholar 

  41. J. Campos-Martinez and R.D. Coalson, J. Chem. Phys. 93, 4740 (1990).

    Google Scholar 

  42. A.D. Hammerich, R. Kosloff and M.A. Ranter, Chem. Phys. Lett. 171, 97 (1990).

    Google Scholar 

  43. P. Jungwirth and R.B. Gerber, J. Chem. Phys. 102, 6046 (1995).

    Google Scholar 

  44. P. Jungwirth and R.B. Gerber, J. Chem. Phys. 102, 8855 (1995).

    Google Scholar 

  45. P. Jungwirth and R.B. Gerber, J. Chem. Phys. 104, 5803 (1996).

    Google Scholar 

  46. P. Jungwirth, E. Fredj and R.B. Gerber, J. Chem. Phys. 104, 9932 (1996).

    Google Scholar 

  47. P. Jungwirth, E. Fredj, P. Zdanska and R.B. Gerber, Computers&Chemistry 21, 419 (1997).

    Google Scholar 

  48. P. Jungwirth, E. Fredj and R.B. Gerber, J. Chem. Phys. 107, 8963 (1997).

    Google Scholar 

  49. D.J. Thouless, The Quantum Mechanics of Many-Body Systems (Academic Press, New York, 1961) pp. 88–93.

    MATH  Google Scholar 

  50. P. Bonche, S.E. Koonin and J.W. Negele, Phys. Rev. C13, 1226 (1976).

    Google Scholar 

  51. S. Lent, Phys. Rev. C21, 1594 (1980).

    Google Scholar 

  52. J.W. Negele, Physics Today 38, 24 (1985).

    Google Scholar 

  53. K. Goeke and P.-G. Reinhard, Time-Dependent Hartree-Fock and Beyond, Lecture Notes in Physics, Vol. 171 (Springer-Verlag, Berlin, 1982).

    Book  Google Scholar 

  54. V. Buch, M.A. Ratner and R.B. Gerber, Chem. Phys. Lett. 101, 44 (1983).

    Google Scholar 

  55. R.B. Gerber, R. Kosloff and M. Berman, Comput. Phys. Reports 5, 59 (1986).

    Google Scholar 

  56. M.D. Feit, J.A. Fleck and A. Steiger, J. Comp. Phys. 47, 412 (1982).

    Google Scholar 

  57. U. Peskin, R. Kosloff and N. Moiseyev, J. Chem. Phys. 99, 4590 (1993).

    Google Scholar 

  58. T.R. Horn, R.B. Gerber and M.A. Ratner, J. Chem. Phys. 91, 1813 (1989).

    Google Scholar 

  59. T.R. Horn, R.B. Gerber, J.J. Valentini and M.A. Ratner, J. Chem. Phys. 94, 6728 (1991).

    Google Scholar 

  60. R.H. Bisseling, R. Kosloff, R.B. Gerber, M.A. Ratner, L. Gibson and C. Cerjan, J. Chem. Phys. 87, 2760 (1987).

    Google Scholar 

  61. A. Garcia-Vela, J. Chem. Phys. 104, 1047 (1996).

    Google Scholar 

  62. R. Alimi, R.B. Gerber, A.D. Hammerich, R. Kosloff and M.A. Ratner, J. Chem. Phys. 93, 6484 (1990).

    Google Scholar 

  63. A. Garcia-Vela and R.B. Gerber, J. Chem. Phys. 103, 3463 (1995).

    Google Scholar 

  64. A.B. McCoy, R.B. Gerber and M.A. Ratner, J. Chem. Phys. 101, 1975 (1994).

    Google Scholar 

  65. A.B. McCoy, Mol. Phys. 85, 965 (1995).

    Google Scholar 

  66. Z. Li and R.B. Gerber, Chem. Phys. Lett. 104, 5803 (1996).

    Google Scholar 

  67. J.O. Jung and R.B. Gerber, J. Chem. Phys. (in press).

    Google Scholar 

  68. A.Y. Rom and R.B. Gerber, J. Chem. Phys. (submitted).

    Google Scholar 

  69. A. Jäckie and H.-D. Meyer, J. Chem. Phys. 104, 7974 (1996).

    Google Scholar 

  70. A. Jäckie and H.-D. Meyer, J. Chem. Phys. 102, 5605 (1995).

    Google Scholar 

  71. G.D. Billing and G. Jolicard, Chem. Phys. Lett. 221, 75 (1994).

    Google Scholar 

  72. J.R. Waldeck, J. Campos-Martinez and R.D. Coalson, J. Chem. Phys. 94, 2773 (1991).

    Google Scholar 

  73. N.P. Blake and H. Metiu, in Femtosecond Chemistry, ed. J. Manz and L. Wöste (VCH, Weinheim, 1995) p. 532.

    Google Scholar 

  74. J. Kucar, H.-D. Meyer and L.S. Cederbaum, Chem. Phys. Lett. 140, 525 (1987).

    Google Scholar 

  75. R.B. Gerber and A. Alimi, Chem. Phys. Lett. 184, 69 (1991).

    Google Scholar 

  76. J. Campos-Martinez and R.D. Coalson, J. Chem. Phys. 99, 9629 (1993).

    Google Scholar 

  77. E. Predj, R.B. Gerber and M.A. Ratner (to be published).

    Google Scholar 

  78. E.J. Heller, J. Chem. Phys. 62, 1544 (1975).

    Google Scholar 

  79. M.P. Allen and D. J. Tildesley, Computer Simulation of Liquids, (Clarendon, Oxford, 1987).

    MATH  Google Scholar 

  80. R. McWeeny, Methods of Molecular Quantum Mechanics, 2nd edition (Academic Press, San Diego, 1992).

    Google Scholar 

  81. A.I. Krylov, R.B. Gerber, M.A. Gaveau, J.M. Mestdagh, B. Schilling and J.P. Visticot, J. Chem. Phys. 104, 3651 (1996).

    Google Scholar 

  82. J.F. Grzykowski and L. Andrews, J. Raman Spectros. 4, 99 (1975).

    Google Scholar 

  83. P. Jungwirth and B. Schmidt, Chem. Phys. Lett, 275 (1997) 127.

    Google Scholar 

  84. R. B. Gerber, P. Jungwirth, E. Predj, and A. Y. Rom Modern methods for multidimensional dynamics computations in chemistry, ed. D. L. Thompson (World Scientific, River Edge, NJ, 1998).

    Google Scholar 

Download references

Author information

Authors and Affiliations

  1. J. Heyrovsky Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, Dolejskova 3, 18223, Prague 8, Czech Republic

    Pavel Jungwirth

  2. Department of Physical Chemistry and The Fritz Haber Research Center, The Hebrew University, Jerusalem, 91904, Israel

    R. Benny Gerber

  3. Department of Chemistry, University of California, Irvine, CA, 92697-2025, USA

    R. Benny Gerber

Authors
  1. Pavel Jungwirth
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. R. Benny Gerber
    View author publications

    You can also search for this author in PubMed Google Scholar

Editor information

Editors and Affiliations

  1. Konrad-Zuse-Zentrum Berlin (ZIB), Takustrasse 7, D-14195, Berlin-Dahlem, Germany

    Peter Deuflhard

  2. Department of Biochemistry and Biophysics, University of North Carolina, Chapel Hill, NC, 27599-7260, USA

    Jan Hermans

  3. Department of Mathematics, University of Kansas, 405 Snow Hall, Lawrence, KS, 66045, USA

    Benedict Leimkuhler

  4. Laboratorium für Physikalische Chemie ETH Zentrum, CH-8092, Zürich, Switzerland

    Alan E. Mark

  5. Department of Mathematics and Statistics, University of Surrey, Guildford, Surrey, GU2 5XH, UK

    Sebastian Reich

  6. Department of Computer Science, University of Illinois, 1304 West Springfield Avenue, Urbana, IL, 61801-6631, USA

    Robert D. Skeel

Rights and permissions

Reprints and permissions

Copyright information

© 1999 Springer-Verlag Berlin Heidelberg

About this paper

Cite this paper

Jungwirth, P., Gerber, R.B. (1999). New Methods in Quantum Molecular Dynamics of Large Polyatomic Systems. In: Deuflhard, P., Hermans, J., Leimkuhler, B., Mark, A.E., Reich, S., Skeel, R.D. (eds) Computational Molecular Dynamics: Challenges, Methods, Ideas. Lecture Notes in Computational Science and Engineering, vol 4. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-58360-5_20

Download citation

  • DOI: https://doi.org/10.1007/978-3-642-58360-5_20

  • Publisher Name: Springer, Berlin, Heidelberg

  • Print ISBN: 978-3-540-63242-9

  • Online ISBN: 978-3-642-58360-5

  • eBook Packages: Springer Book Archive

Publish with us

Policies and ethics

Search

Navigation