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Physical Review Letters

Photon-Correlation Effects in Resonant Two-Photon Ionization

Lloyd Armstrong, P. Lambropoulos, N. K. Rahman

Published Apr 19, 1976• 29 citations
Publisher

Abstract

The effect of photon correlations (coherence) on the transition probability of resonant two-photon processes is discussed. It is shown that coherence influences not only the transition probability but also the linewidth of the resonance. The implications for higher-order multiphoton ionization are discussed.
DOI
10.1103/physrevlett.36.952

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Physical Review Letters•Jan 9, 1978•12 citations
The effect of photon correlations on two- and three-photon ionization via two near-resonant levels is discussed in terms of the resolvent-operator formalism. It is shown that under certain circumstances the ionization probability for a chaotic light can be enhanced by a factor larger than N!N!N! compared to the ionization probability for a coherent light. The dependence of this enhancement factor on the interaction time, the average intensity, the detunings of the photon frequency from the near-resonant levels, and the separation between the two near-resonant levels is discussed.
I present a perturbation theory of multiphoton ionization based on the resolvent operator. The theory is applied to a detailed study of two-photon ionization under near-resonance conditions. It is shown that a distinction must be made between linear level shifts and widths, and resonance shifts and widths which appear in the transition probability. The resonance shifts and widths exhibit saturation effects and their values tend to be much smaller than those of the linear level shifts and widths. Using numerical examples corresponding to tunable dye lasers and alkali-metal atoms, we show that the above shifts can have a dramatic effect on the ionization rate even when the laser is not in exact resonance with the intermediate level. The question of "one-step" vs "two-step" two-photon ionization is also discussed. It is shown that exact resonance does not necessarily imply a two-step process. In fact, in most cases it is quite the opposite. A quantitative criterion for this distinction is established. Finally, a distinction is made between instrumental saturation and saturation of the transition probability. The two are shown to be of different nature. Further extensions of the work are also discussed.
Time - dependent behaviors of molecular coherence in resonant multiphotoni onization spectra of molecules are theoretically investigated . An expression for the transition probability of time-resolved two-photon ionization processes via coherently excited resonant intermediate states is derived in the perturbative density matrix formalism. Model calculations of the probability of ionization are performed to predict appearance of quantum beats in pump-probe two-photon ionization experiments. The quantum beat signals in the time-resolved ionization spectra are compared with those in time-resolved total photon emission spectra.
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.
It is shown that in near-resonant NNN-photon ionization, chaotic light can be more efficient than purely coherent light by more than the usual factor of N!N!N! (NNN factorial). This occurs when the resonant intermediate state interferes with another nearby state. Specific results are presented for two-photon ionization.