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Journal of Physics A Mathematical and General

Atoms in multi-mode radiation fields

Harm Geert Muller, A. Tip

Published Apr 21, 1986• 6 citations
Publisher

Abstract

The Floquet formalism for atoms in semiclassical monochromatic radiation fields has recently been extended to the multi-mode case by Chu and co-workers (1983). The authors generalise a version of the Floquet formalism for the single-mode case originated by Howland to the multi-mode situation and give expressions for multi-photon ionisation amplitudes in the spirit of time-independent scattering theory. A comparison is made with the corresponding second quantised formalism.

DOI
10.1088/0305-4470/19/6/020

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The Floquet formalism for atoms in semiclassical monochromatic radiation fields has recently been extended to the multi-mode case by Chu and co-workers (1983). The authors generalise a version of the Floquet formalism for the single-mode case originated by Howland to the multi-mode situation and give expressions for multi-photon ionisation amplitudes in the spirit of time-independent scattering theory. A comparison is made with the corresponding second quantised formalism.
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 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.
Formal time-independent scattering theory is applied to multiphoton ionization of atoms in intense electromagnetic fields. The quantized-field version of the Volkov solution makes this approach possible. With the electron-photon interaction in a monochromatic photon field, it is found that, in the nonrelativistic and large-photon-number limits, the final scattering state exists only in the special case in which the ponderomotive potential per unit photon energy is an integer; otherwise the final state vanishes. In the integer case the corresponding wave function reduces to a single Volkov function, multiplied by an overlap factor. A simple interpretation of this result is given, and some other consequences of this work are discussed.
We present a formalism that enables the analytic calculation of the interaction of a spin-half particle with a polychromatic electromagnetic field. This powerful new approach provides a clear physical picture even for cases with highly degenerate energy levels, which are complicated to interpret in the standard dressed-atom picture. Typically semi-classical methods are used for such problems (leading to equations that are solved by Floquet theory). Our formalism is derived from quantum electrodynamics and thus is more widely applicable. In particular it makes accessible the intermediate regime between quantum and semi-classical dynamics. We give examples of the application to multi-frequency multi-photon processes in strong fields by deriving the Hamiltonians of such systems, and also to the dynamics of weak fields at long times for which semi-classical methods are insufficient.
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.
We formulate a computationally feasible method for calculating multiphoton ionization rates for atoms exposed to intense fields in the intensity regime where perturbation theory ceases to apply. The method is based on the time-independent picture of ionization, which starts with the Floquet ansatz. The question of the gauge of the radiation field is discussed in some detail. Various expressions for the ionization amplitude are derived from a variational principle, with the radiation field expressed in the velocity gauge. We consider in particular an approximation in which the wave vector developing from the initial state is replaced by a trial vector that is the Floquet expansion truncated just below the threshold for ionization, and in which the wave vector developing into the final state is replaced by a trial vector that is just the wave vector appearing in the Kroll-Watson low-frequency approximation in scattering theory. We have applied this approximation to hydrogen and we present some results for both nonresonant and resonant multiphoton ionization. We argue that the experimentally observed resonance structure in the above-threshold peaks of the ionization signal occurs through the electron jumping from one dressed-state energy-eigenvalue curve to another.