Advertisement

Theoretical study of femtosecond pump—probe signals of nonstoichiometric alkali halide clusters

  • M. Hartmann
  • J. Pittner
  • H. van Dam
  • V. Bonačić-Koutecký
Conference paper

Abstract

We present the outline of the ab-initio molecular dynamics method for adiabatic excited states which is suitable to treat the involved excited electronic states simultaneously with the motion of the nuclei. The method allows the simulation of time-resolved pump-probe signals and the analysis of the signals in terms of the underlying nuclear dynamics. Moreover, the timescales of the structural relaxation in excited electronic states vs. intramolecular vibrational relaxation processes can be estimated and the influence of the initial temperature of the cluster can be determined.

The method is applied to the analysis of the timescales as well as of the dynamics of localized/delocalized electronic excitations in the Na2F molecule which represents a test example for nonstoichiometric alkali-halides with one excess electron. The aim is to develop a method for the investigation of time-dependent laser induced processes in clusters which is capable to extract the leading physical effects responsible for the controlled excitation dynamics and for the evolution of the non-equilibrium states.

PACS

31.15.Ar Ab initio calculations 31.15.Qg Molecular dynamics and other numerical methods 31.50.+w Excited states 31.70.Hq Time-dependent phenomena: excitation and relaxation processes and reaction rates 

Preview

Unable to display preview. Download preview PDF.

Unable to display preview. Download preview PDF.

References

  1. 1.
    M. Hartmann, J. Pittner, V. Bonaei&-KouteckS-, A. Heidenreich, J. Jortner: J. Chem. Phys. 108, 3096 (1998)ADSCrossRefGoogle Scholar
  2. 2.
    M. Hartmann, A. Heidenreich, J. Pittner, V. Bona.C.ieKouteck3lr, Jortner: J. Phys. Chem. A. 102, 4069 (1998)CrossRefGoogle Scholar
  3. 3.
    V. BonaCi&-Kouteck)l-, J. Pittner: Chem. Phys. 225, 173 (19971Google Scholar
  4. 4.
    J. Pittner: “Ab Initio Study of Optical Properties of Neutral and Charged Pure and Mixed Alkali Metal Clusters”, Dissertation Humboldt–Universitat zu Berlin (Verlag für Wissenschaft und Forschung, Berlin 1997) ISBN 3–930324–96–2Google Scholar
  5. 5.
    Y. Yamaguchi, Y. Osamura, J.D. Goddard, H.F. Schaefer III: “A New Dimension to Quantum Chemistry: Analytic Derivative Methods”, in: Ab Initio Molecular Electronic Structure Theory (Oxford University Press, New York 199–1) ISBN 0–19–507028–3, p. 72, Eq, (5.26)Google Scholar
  6. 6.
    as [5], p, 148, Eq. (11.20)Google Scholar
  7. 7.
    as [5], p. 152, Eq. (11,39)Google Scholar
  8. 8.
    J.E. Rice, R.D. Amos, N.C. Handy, T.J. Lee, H.F. Schaefer: J. Chem, Phys. 85, 963 (1986)ADSCrossRefGoogle Scholar
  9. 9.
    T.J. Lee, N.C. Handy, J.E. Rice, A.C. Scheiner, B.F. Schaefer: J. Chem. Phys. 85, 3930 (1986)ADSCrossRefGoogle Scholar
  10. 10.
    V. BonaZie-KouteckY, J. Pittner, J. KouteckYr: Chem. Phys. 210, 313 (1996)ADSCrossRefGoogle Scholar
  11. 11.
    M. Hillary, RI“. O’Connell, M.O. Scully, E.P. Wigner: Phys. Rep. 106, 121 (1984)Google Scholar

Copyright information

© Springer-Verlag Italia 1999

Authors and Affiliations

  • M. Hartmann
    • 1
  • J. Pittner
    • 1
  • H. van Dam
    • 1
  • V. Bonačić-Koutecký
    • 1
  1. 1.Walther-Nernst-Institut für Physikalische und Theoretische ChemieHumboldt-Universität zu BerlinBerlinGermany

Personalised recommendations