The authors present an exact treatment of two- and multiquantum transitions in three-level systems driven by two intense linearly polarised monochromatic fields based on the semiclassical many-mode Floquet theory developed recently. Further they extend the almost degenerate perturbation theory of Salwen (1955-6) to the two-mode Floquet Hamiltonian and obtain approximate analytical formulae for multiphoton transition probabilities, resonance bichromatic shifts and widths, and absorption lineshapes beyond the conventional rotating-wave approximation (RWA). Detailed comparison of the analytical, the RWA, and the exact results is given. Several novel features of multiphoton lineshape characteristics are pointed out.
The authors present an exact treatment of two- and multiquantum transitions in three-level systems driven by two intense linearly polarised monochromatic fields based on the semiclassical many-mode Floquet theory developed recently. Further they extend the almost degenerate perturbation theory of Salwen (1955-6) to the two-mode Floquet Hamiltonian and obtain approximate analytical formulae for multiphoton transition probabilities, resonance bichromatic shifts and widths, and absorption lineshapes beyond the conventional rotating-wave approximation (RWA). Detailed comparison of the analytical, the RWA, and the exact results is given. Several novel features of multiphoton lineshape characteristics are pointed out.
For pt.I see Chem. Phys. Lett. vol.96, p.464 (1983). The non-linear multiphoton excitation dynamics of two-level systems under the influence of two strong linearly polarised monochromatic fields is studied exactly for the first time along the semiclassical many-mode Floquet theory. The present approach relaxes the restrictions of the conventional generalised rotating-wave approximation (GRWA) and allows correct treatment of various non-linear features such as power broadening, resonance shift, asymmetry in absorption lineshape, etc. By extending the nearly degenerate perturbative method of Salwen (1955), approximate analytical expressions for transition probabilities are obtained for multiphoton resonance processes for which (n+1) photons of one field are absorbed, whereas n photons of the other field are emitted, where n is an arbitrary integer. Detailed comparison of the analytical, the GRWA and the numerically exact results is given. Also presented is a case study of the time evolution of spin 1/2 systems in multi-quantum NMR transitions driven by pulsed bichromatic radiofrequency fields.
The SU(3) dynamical evolution of three-level systems at two-photon resonance induced by two strong linearly polarized monochromatic fields is studied exactly by means of the semiclassical many-mode Floquet theory (MMFT) recently developed by the authors. Within the rotating-wave approximation (RWA), Hioe and Eberly have recently shown that the eight-dimensional SU(3) coherent vector S\ensuremath{\rightarrow} characterizing the time evolution of three-level systems can be factored into three independent vectors of dimensions three, four, and one, at appropriate two-photon resonance conditions. In practice, however, if the laser-atom interactions occur away from the two-photon resonance, or if the RWA is not valid, etc., this Gell-Mann--type SU(3) dynamical symmetry will be broken. It is shown in this paper that instead of solving the time-dependent generalized Bloch equations, the SU(3) dynamical evolution of the coherent vector S\ensuremath{\rightarrow} as well as various symmetry-breaking effects can be expediently studied by the use of the MMFT and expressed in terms of a few time-independent quasienergy eigenvalues and eigenvectors. Furthermore, we have extended the generalized Van Vleck (GVV) nearly degenerate perturbation theory to an analytical treatment of the two-mode Floquet Hamiltonian. This reduces the infinite-dimensional time-independent Floquet Hamiltonian into a 3\ifmmode\times\else\texttimes\fi{}3 effective Hamiltonian, from which useful analytical properties of the SU(3) coherent vector can be easily obtained. The combination of the MMFT and the GVV method thus greatly facilitates the study of the dynamical evolution. Pictorial comparison of the exact and the RWA results of the time evolution of the eight-dimensional coherent vector under several different physical conditions is presented and discussed at length.
The many-mode Floquet theory (MMFT) recently developed by authors is extended to incorporate the irreversible damping mechanisms for the nonperturbative treatment of the dynamical evolution of dissipative three-level systems at two-photon or multiphoton coherent resonance trapping conditions induced by two strong linearly polarized monochromatic fields. It has been recently shown by several workers that under the rotating-wave approximation (RWA), population may be permanently trapped in the three-level system if the coherent monochromatic fields are exactly two-photon resonant with the initial and final states, decoupled from the intermediate decaying level. In practice, the inclusion of the non-RWA terms necessarily modifies the resonant trapping conditions and behavior. In this paper we extend the generalized Van Vleck (GVV) nearly degenerate perturbation theory to an analytical treatment of the non-Hermitian two-mode Floquet Hamiltonian. This reduces the infinite-dimensional time-independent non-Hermitian Floquet Hamiltonian to a 3\ifmmode\times\else\texttimes\fi{}3 effective Hamiltonian, from which essential properties of the coherent population-trapping behavior as well as the dynamical evolution of the dissipative SU(3) coherence vector S\ensuremath{\rightarrow}(t) can be readily obtained and expressed in terms of only three complex quasienergy eigenvalues and eigenvectors. The MMFT-GVV studies show that the RWA two-photon resonant trapping condition is substantially modified by the effects of non-RWA terms, and that the system can be ``quasitrapped'' for only a finite amount of time characterized by a small imaginary energy (width) associated with a coherent superposition state of the initial and final levels. Furthermore, it is found that the initially eight-dimensional coherence vector S\ensuremath{\rightarrow}(t) evolves predominantly to a one-dimensional scalar at the two-photon or multiphoton resonant quasitrapping conditions. Detailed results and pictorial representations of the population trapping and SU(3) dissipative dynamical evolution are presented.
We study the fluorescence spectrum of a strongly driven two-level system (TLS) with modulated transition frequency, which is a bichromatically driven TLS and has multiple resonance frequencies. We are aiming to provide a reliable description of the fluorescence in a regime that is difficult to tackle with perturbation theory and the rotating-wave approximation (RWA), and illustrate the spectral features of the fluorescence under off- and multiphoton-resonance conditions. To go beyond the RWA, we use a semianalytical counter-rotating-hybridized rotating-wave method that combines a unitary transformation and Floquet theory to calculate the two-mode Floquet states and quasienergies for the bichromatically driven TLS. We then solve the master equation accounting for the spontaneous decay in the bases of the two-mode Floquet states, and derive a physically transparent fluorescence spectrum. In comparison with the numerically exact spectrum from the generalized Floquet-Liouville approach, the present spectrum is found to be applicable in a wide range of the parameters where the RWA and the secular approximation may break down. We find that the counter-rotating (CR) terms of the transverse field omitted in the RWA have non-negligible contributions to the spectrum under certain conditions. Particularly, at the multiphoton resonance the width of which is comparable with the Bloch-Siegert shift, the RWA and non-RWA spectra markedly differ from each other because of the CR-induced shift. We also analyze the symmetry of the spectrum in terms of the transition matrix elements between the two-mode Floquet states. We show that the strict symmetry of the spectrum cannot be expected without the RWA but the almost symmetric spectrum can be obtained at the single-photon resonance that takes the Bloch-Siegert shift into account if the driving is moderately strong and at the multiphoton resonance with a sufficiently weak transverse field.
We present a practical nonperturbative method for exact treatment of intensity-dependent generalized nonlinear optical susceptibilities χ(ω) in intense polychromatic fields, valid for arbitrary laser intensities, detunings, and relaxation. By means of the many-mode Floquet theory, the time-dependent Liouville equation can be transformed into an equivalent time-independent infinite-dimensional Floquet–Liouville supermatrix (FLSM) eigenvalue problem. It is then shown that the nonlinear optical susceptibilities χ(ω) can be completely determined simply from the supereigenvalues and eigenfunctions of the Floquet–Liouvillian L̂F. In addition to this exact FLSM approach, we have also presented higher-order perturbative results, based on the extension of the Salwen’s nearly degenerate perturbation theory, appropriate for somewhat weaker fields and near-resonant multiphoton processes, but beyond the conventional perturbative or rotating wave approximation (RWA). In the case of two-level systems, for example, the implementation of Salwen’s method in the time-independent L̂F allows the reduction of the infinite-dimensional FLSM into a 4×4 dimensional effective Hamiltonian, from which essential analytical formulas for intensity-dependent χ(ω) can be obtained. These methods are applied to a detailed study of intensity-dependent spectral line shapes (such as hole burning and extra resonance peaks at the line center, and the effects of saturation, detuning, and radiative and collisional damping, etc.) and subharmonic structures in nonlinear multiple wave mixings χ[(m+1)ω1−mω2] for two-level systems in intense linearly polarized bichromatic fields.
A previously developed exact semiclassical method is used to evaluate multi-photon spectra and Floquet characteristic exponents (dressed-atom energies) for several multi-level systems interacting with both strong oscillating and static fields under varying degrees of saturation. The usefulness of characteristic exponent plots in extracting the physically significant features of the spectrum, without the necessity of evaluating portions of the complete spectrum, is demonstrated for a number of model three-level systems which are not directly amenable to study by the often used rotating-wave approximation. The effect of neighbouring non-resonant states on two-photon resonance profiles is also discussed using three to six level systems (H and Na atoms) as models.