Journal of Chemical Physics, Vol.106, No.17, 6839-6847, 1997
Photoabsorption Probability for a System Governed by a Time-Dependent Hamiltonian Through the (T,T’)-Formalism
Heller’s expression for the absorption cross-section in the weak field limit is extended to cases where the total Hamiltonian contains a strong time-dependent component, supplemented by a weak field. A very similar expression to the original case then results when the (t,t’) formalism is used; one only needs to construct a correlation function for the system without the weak field, and use it to extract the absorption probability for any value of the weak-field frequency (or pulse shape). In addition, a numerical approach for extracting Floquet states without full-matrix diagonalization is demonstrated, by filtering (or filter-diagonalization) a single wave function (or the correlation function) propagated under the (t,t’) Hamiltonian.
Keywords:ABSORBING BOUNDARY-CONDITIONS;SCHRODINGER-EQUATION;QUANTUM-DYNAMICS;COMPUTATIONAL ALGORITHM;FILTER-DIAGONALIZATION;POLYNOMIAL EXPANSION;REACTIVE SCATTERING;FREQUENCIES;PROPAGATORS;RESONANCES