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arXiv:1803.02761 · Physical Review A

Revisiting photon-statistics effects on multiphoton ionization

G. Mouloudakis, P. Lambropoulos

Published May 25, 2018• 6 citations
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Abstract

We present a detailed analysis of the effects of photon statistics on multiphoton ionization. Through a detailed study of the role of intermediate states, we evaluate the conditions under which the premise of nonresonant processes is valid. The limitations of its validity are manifested in the dependence of the process on the stochastic properties of the radiation and found to be quite sensitive to the intensity. The results are quantified through detailed calculations for coherent, chaotic, and squeezed vacuum radiation. Their significance in the context of recent developments in radiation sources such as the short-wavelength free-electron laser and squeezed vacuum radiation is also discussed.

DOI
10.1103/physreva.97.053413

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We present a detailed analysis of the effects of photon statistics on multiphoton ionization. Through a detailed study of the role of intermediate states, we evaluate the conditions under which the premise of nonresonant processes is valid. The limitations of its validity are manifested in the dependence of the process on the stochastic properties of the radiation and found to be quite sensitive to the intensity. The results are quantified through detailed calculations for coherent, chaotic, and squeezed vacuum radiation. Their significance in the context of recent developments in radiation sources such as the short-wavelength free-electron laser and squeezed vacuum radiation is also discussed.
In this paper, we extend the results of an earlier paper [G. Mouloudakis and P. Lambropoulos, Phys. Rev. A 97, 053413 (2018)] in which we had demonstrated the limitations of the notion of nonresonant multiphoton ionization, in the exploration of photon statistics effects in nonlinear processes. Through the quantitative analysis of specific realistic processes, we provide the connection to conditions of intensity and pulse duration necessary in relevant experiments, including a recent seminal experiment demonstrating the effect of superbunching found in squeezed radiation. The outlook for a future era of studies on the interplay between stochasticity and nonlinearity in transitions driven by electromagnetic radiation is also discussed.
The non linear interaction between an intense laser radiation and atoms leads to ionization through the absorption of N photons from the laser radiation via laser-induced virtual states. The multiphoton ionization rate varies as a function of the laser intensity I as IN. We discuss the two most important effects which govern multiphoton ionization processes : resonance effects and laser-coherence effects. In a moderate laser intensity range (107 - 109 W cm-2) corresponding to the two, three or four-photon ionization of atoms, resonance effects play a dominant role while the photon statistics of the laser radiation are relatively unimportant. On the contrary, in the very high intensity range (1012 - 1013 W cm-2) required to observe large Nth - order ionization processes, coherence effects play a dominant role through N! enhancement in the N-photon ionization rate, while resonance effects are completely damped due to the high laser intensity. We conclude by reviewing the possible applications of multiphoton absorption processes in other fields.
Resonant multiphoton ionization by finite bandwidth multimode radiation is investigated without the restriction of either a "long" or a "short" correlation time of the field. By approximating the multimode radiation by a stochastic model of a chaotic field, the stochastic atomic-density-matrix equation is reduced to a tractable infinite set of differential equations. For a given bandwidth this set can be suitably truncated and numerically integrated. For large-bandwidth fields it turns out that these truncated equations constitute a systematic improvement of the method usually employed of decorrelating the atom-field variables. For zero-bandwidth fields the well-known result is recovered in that the statistical averaging of the ionization probability reduces to an average with respect to the Glauber PPP-distribution function of the chaotic field. Detailed results of numerical calculations for two-photon ionization are presented which reveal a number of new interesting features.
The review is devoted to new effects discovered recently in the course of studying the process of nonlinear ionization of atoms in the field of laser radiation—above-threshold ionization, manifestation of multielectron structure of complex atoms, formation of multiply charged ions, tunneling ionization, and emission of short-wavelength radiation. The main experimental data and their theoretical interpretation are presented. A discussion is given of the criteria for the applicability of the lowest non-vanishing order of non-steady-state perturbation theory to the description of the interaction of an atom with the electromagnetic field.
We present a quantitative theory with detailed calculations pertaining to multiphoton ionization of helium under moderately strong uv radiation of photon energy 13eV13\phantom{\rule{0.3em}{0ex}}\mathrm{eV}13eV. Employing both, the nonperturbative solution of the time-dependent Schr\"odinger equation, as well as perturbation theory, we obtain detailed results for all processes expected to be of quantitative relevance within the range of intensities and pulse durations in this work, which have been chosen so as to match the conditions of a recent experiment on exactly this problem [T. Laarman et al., Phys. Rev. A 72, 023409 (2005)]. The conclusion, in connection with the experimental data, which our results lead to is that, without the presence of the second harmonic of the fundamental in the radiation, it is impossible to reconcile the reported observations with fundamental features of the processes involved. A more general conclusion seems to be that the presence of these harmonics, even at intensities less than 1% of that of the fundamental, are apt to produce profound side effects that will mask multiphoton processes by the fundamental.