Floquet-Liouville supermatrix approach: Time development of density-matrix operator and multiphoton resonance fluorescence spectra in intense laser fields

Abstract

A Floquet-Liouville supermatrix (FLSM) approach is presented for nonperturbative treatment of the time development of the density-matrix operator of atoms and molecules exposed to intense polychromatic fields. By extending the many-mode Floquet theory (MMFT) recently developed, the time-dependent Liouville equation for the density matrix of quantum systems undergoing relaxations (due to radiative decays and collisional dampings, etc.) can be transformed into an equivalent time-independent non-Hermitian FLSM eigenvalue problem. This yields a numerically stable and computationally efficient approach for the unified treatment of nonresonant and resonant, one- and multiple-photon, steady-state and transient phenomena in nonlinear optical processes, much beyond the conventional rotating-wave-approximation (RWA) method. Connections of the FLSM approach to the MMFT in the limit of zero relaxations are also made, providing the understanding of the physical significance of FLSM supereigenvalues and eigenvectors. In addition to the exact FLSM formalism, we have also presented higher-order perturbative results, based on the extension of the generalized Van Vleck (GVV) nearly degenerate perturbation theory, appropriate for somewhat weaker fields and near-resonant processes, but beyond the RWA limit. The implementation of the GVV method in the time-independent Floquet-Liouvillian allows the reduction of the infinite-dimensional FLSM into a finite-dimensional GVV-Liouville matrix, from which essential analytical results are readily obtained. As an illustration of the usefulness of the new formalism, we extend both the FLSM and the GVV methods to a formal study of the multiphoton-induced resonance fluorescence spectra of two-level systems subject to purely radiation relaxations. Both the time-averaged power spectrum and the time-dependent physical spectrum are exploited in details, and novel new features in intense fields are pointed out.