ISSN:
0020-7608
Keywords:
quantum fluid dynamics
;
atom-laser interaction
;
femtosecond dynamics
;
density functional theory
;
high harmonic generation
;
Chemistry
;
Theoretical, Physical and Computational Chemistry
Source:
Wiley InterScience Backfile Collection 1832-2000
Topics:
Chemistry and Pharmacology
Notes:
A comprehensive, nonperturbative, time-dependent quantum mechanical (TDQM) approach is proposed for studying the dynamics of a helium atom under an intense, ultrashort (femtoseconds) laser pulse. The method combines quantum fluid dynamics (QFD) and density functional theory. It solves a single generalized nonlinear Schrödinger equation of motion (EOM), involving time and three space variables, which is obtained from two QFD equations, namely, a continuity equation and an Euler-type equation. A highly accurate finite difference scheme along with a stability analysis is presented for numerically solving the EOM. Starting from the ground-state Hartree-Fock density for He at t=0, the EOM yields the time-dependent (TD) electron density, effective potential surface, difference density, difference effective potential, ground-state probability, 〈r〉, magnetic susceptibility, polarizability, flux, etc. By a Fourier transformation of the TD dipole moment along the linearly polarized-field direction, the power and rate spectra for photoemission are calculated. Eleven mechanistic routes for photoemission are identified, which include high harmonic generation as well as many other spectral transitions involving ionized, singly excited, doubly excited (autoionizing), and continuum He states, based on the evolution of the system up to a particular time. Intimate connections between photoionization and photoemission are clearly observed through computer visualizations. Apart from being consistent with current experimental and theoretical results, the present results offer certain predictions on spectral transitions which are open to experimental verification. © 1998 John Wiley & Sons, Inc. Int J Quant Chem 70: 441-474, 1998
Additional Material:
14 Ill.
Type of Medium:
Electronic Resource
