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Physical Review Letters

Atomic Transitions in Intense Fields and the Breakdown of Perturbation Calculations

Howard R. Reiss

Published Oct 26, 1970• 65 citations
Publisher

Abstract

Results valid for arbitrarily high intensity of electromagnetic field are presented for induced emission from an excited state of an atom. Comparison with perturbation theory shows that perturbative calculations fail quantitatively and qualitatively at lower intensity than had been expected. Distinctive intense-field features are discussed such as vanishing of the transition probability for certain intensities and photon multiplicities, and appearance of two extrema of the transition amplitude for multiphoton processes at very high intensities.

DOI
10.1103/physrevlett.25.1149

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Results valid for arbitrarily high intensity of electromagnetic field are presented for induced emission from an excited state of an atom. Comparison with perturbation theory shows that perturbative calculations fail quantitatively and qualitatively at lower intensity than had been expected. Distinctive intense-field features are discussed such as vanishing of the transition probability for certain intensities and photon multiplicities, and appearance of two extrema of the transition amplitude for multiphoton processes at very high intensities.
Transition amplitudes corresponding to bound-bound multiphoton transitions with the emission or absorption of one and two Raman photons in the hydrogen atom have been evaluated following a recent method of Reiss. Results show that the transition probability varies smoothly for low values of NNN, where NNN is the number of intense photons absorbed or emitted during the transition. For larger values of NNN the amplitude, however, has oscillatory behavior. A particular feature of the present method of calculation is that we find the "reduced" transition amplitude for induced emission of two Raman photons is enhanced compared with single-Raman-photon emission. Another distinctive feature is the appearance of many more extrema in the transition amplitude for higher transitions for multiphoton processes at high intensity.
A previous theory of atomic transitions in ultrastrong electromagnetic fields is applied to the problem of the ionization of highly excited hydrogen atoms. The magnitude of the fields necessary for the validity of the theory is greatly reduced by using excited hydrogen in the initial state, and the requirement of only multiphoton ionization limits the application to lowfrequency (microwave) fields. The requirement can probably be satisfied with currently available equipment. A result of the calculation is that the average number of photons absorbed is twice the minimum number.
Multiphoton spectroscopy The subject of multiphoton excitation spectroscopy began in 1931 when Göppert-Mayer [450] wrote a theoretical paper in which she calculated the transition rate for an atom in the presence of two photons rather than just one. At the time, the process seemed rather exotic, and it was reassuring that the calculated rate was so low as to guarantee that it could not readily be observed in the laboratory with conventional sources. This conclusion was reassuring because it implies that a simple perturbative theory (one photon per transition is the weak-field limit) is adequate for most purposes. The subject came to life with the advent of lasers, when it became easy to create intense beams of light. Since the probability of excitation by two photons grows as the square of the photon density, whereas the probability of single-photon excitation grows only linearly with photon density, two-photon transitions gain in relative strength with increasing intensity despite the small value of the rate coefficient. The development of multiphoton spectroscopy has followed that of lasers: as the available power has increased, so has the number of photons involved in individual transitions. More significantly, it has become apparent that the physics of the interaction between radiation and matter is not the same at high laser powers as under weak illumination, i.e. that there is a qualitative change which sets in at strong laser fields. This is normally expressed by saying that perturbative approximations break down.
A new approach to the study of the spontaneous emission of the quantum system driven by a high-intensity laser field is developed. This approach is based on the accurate consideration of quantum system interaction with vacuum quantized field modes in the first order of perturbation theory, while the intense laser field is considered classically beyond the perturbation theory which allows to observe any-order stimulated processes governed by classical field. The proposed approach is applied to the study of a number of quantum systems in intense laser field. The obtained data are compared with those obtained in the frames of semiclassical approximation typically used for analyzing of the strong-field dynamic. It is found that the applicability of the semiclassical approach is strictly limited. It is valid for calculation of transitions to the initially populated state only if the population of this state is close to unity during the pulse and in the after-pulse regime. If its population is depleted, the semiclassical approach fails.
An approximation method is developed which yields very simple and general analytical results for electromagnetic bound-bound or bound-free transitions for any arbitrarily high order of interaction with the electromagnetic field. The approximation is perturbative in the sense that transition probabilities are proportional to the field intensity raised to the power NNN, where NNN is the order of the interaction. Limiting values of electromagnetic field strength are given within which the approximation is valid. These limits depend upon the binding potential which produces the bound states. A feature of the results is that they show the onset of high-order dominance effects which can occur at high-field intensities.