Journal of Chemical Physics, Vol.112, No.3, 1229-1239, 2000
Molecular dichotomy within an intense high-frequency laser field
It is shown that, under an intense high-frequency laser field, electronic distributions in molecules exhibit a dichotomy effect just as previously found in atoms. The generalization of the formal demonstration of the dichotomy effect as given in M. Gavrila and J. Shertzer, Phys. Rev. A 41, 477 (1990) to many-electron, polyatomic molecules is considered and the validity of the alpha(0)(-2/3) scaling law of the Floquet eigenvalues, with respect to the field intensity parameter alpha(0) of the HFFT, is discussed. To test the molecular dichotomy effect, numerical calculations are performed using a quantum chemical package (Gaussian 94), modified appropriately to incorporate the cycle-averaged displacements of the nuclear-electron Coulomb potential as found in the HFFT hamiltonian. Results of calculations on the two-electron H-2 molecule are presented with an emphasis placed on the character of the total and orbital charge distributions and on trends to be observed in the electronic correlation at high intensities.