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Physical Review A

Absorption spectroscopy of strongly perturbed bound-continuum transitions

Seenipandian Ravi, G. S. Agarwal

Published Apr 1, 1987• 14 citations
Publisher

Abstract

Absorption properties of a system consisting of two autoionizing states coupled strongly either by internal interactions or by external fields are investigated. The autoionizing states may themselves correspond to those induced by laser fields as in resonant multiphoton ionization. The analysis is based on the density matrices and incoherent processes like spontaneous emission and radiative recombination are included. Optical susceptibilities exist in a number of special cases for autoionizing transitions. Exact results for such optical susceptibilities are obtained. Explicit numerical results for susceptibilities, corresponding traditionally to strong-field inverse Raman effect, are given with a view to recent work on dc-field-coupled autoionizing states and on laser-induced autoionization. The behavior of both absorptive and dispersive parts is discussed for a range of parameters.

DOI
10.1103/physreva.35.3354

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Absorption properties of a system consisting of two autoionizing states coupled strongly either by internal interactions or by external fields are investigated. The autoionizing states may themselves correspond to those induced by laser fields as in resonant multiphoton ionization. The analysis is based on the density matrices and incoherent processes like spontaneous emission and radiative recombination are included. Optical susceptibilities exist in a number of special cases for autoionizing transitions. Exact results for such optical susceptibilities are obtained. Explicit numerical results for susceptibilities, corresponding traditionally to strong-field inverse Raman effect, are given with a view to recent work on dc-field-coupled autoionizing states and on laser-induced autoionization. The behavior of both absorptive and dispersive parts is discussed for a range of parameters.
A theory describing the radiative decay of an autoionizing state under strong pumping by a coherent field is developed. The theory systematically takes into account the radiative decay of the unperturbed continuum. The problem at hand corresponds to the case of strongly coupled bound states decaying to electron and photon continua with the two continua also weakly coupled to each other. A master equation describing the time evolution of the atomic system is derived, and its exact solution under arbitrary initial conditions is given. The effect of radiative decay on the Fano profiles and photoelectron spectra is analyzed in detail. The time development of the system is also examined. The radiative decay of the autoionizing state and the unperturbed continuum changes the spectra in a significant way. The characteristics of the spectra are correlated with the dressed states (with complex energies) of the system. The changes in the structure of the dressed states as a function of the system parameters such as the spontaneous-emission rate and laser intensity are discussed in detail.
This paper investigates nonlinear processes in transitions to the continuum, and their manifestations in the photoabsorption, polarization, and angular distribution of the electrons, as well as in the nonlinear susceptibility in the case of frequency gases. Change of photoabsorption line shape by strong laser radiation upon transition to the continuum is examined. Conditions for the appearance of an induced autoionizing-like resonance in absorption are described, and allowance for the energy dependence of the matrix elements of the transitions to the continuum are examined. A discussion of narrow nonlinear resonances in ionization and recombination is presented. Induction of nonlinear resonances in a continuum when strong/radiation interacts with several close-lying discrete states is described. A presentation is given on the use of laser to induce nonlinear autoionizinglike resonances in a continuum to generate coherent radiation on the basis of frequency mixing in gases. Doppler broadening of nonlinear resonance is discussed. Phase modulation, frequency modulation and amplitude-phase modulation are outlined.
Efficient harmonic generation at laser-induced autoionizing state in continuum, were observed for the first time by our laboratory [1,2,3]. In this paper, nonlinear frequency mixing in alkali metal vapors at induced continuum structure in Na, are studied in detail. Besides, measurement of nonlinear optical susceptibility at induced autoionizing resonance, is performed. Tunable ultraviolet radiations by four-photon processes near induced resonances are obtained. Estimations of the real and imaginary parts of the nonlinearities, are estimated. We will specially note, that the resonant photoabsorption of ions is experimentally investigated since it gives information about the autoionizing states, which is impossible to obtain on the base only of the emission spectra. We use also laser inducing for obtaining of powerful radiation source in VUV. Thus, many actual problems as the selective impact on matter, laser photochemistry and laser isotope separation are connected directly with the induced autoionizing nonlinear resonances. The main interest is to control the spectral characteristics of continuum. The discrete level from the continuum structure leads to appearance of asymmetrical autoionizing resonance onto the background of the broad-band absorption line.
We have performed an experimental study of the atomic system ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$, for which the ground state 5s2{\mathit{s}}^{2}s2 is coupled to the autoionizing state 5${\mathit{p}}_{1/2}$6s by means of a strong resonant laser field. The investigations are based on irradiation of ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$ with intense (I\ensuremath{\le}1.5\ifmmode\times\else\texttimes\fi{}1010{10}^{10}1010 W/cm2{\mathrm{cm}}^{2}cm2) laser pulses of duration \ensuremath{\sim}1 ns. Single-photon detachment of ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$ is suppressed due to the Fano interference between transitions directly to the continuum and transitions via the autoionizing state. In contrast, two-photon absorption is at the same time resonantly enhanced since no such destructive interference is present in this process. These observations constitute experimental evidence of general features predicted from theoretical considerations of autoionizing states in strong laser fields. Furthermore, we discuss the role of autoionizing states in multiphoton double-ionization processes. Electron spectroscopy has been used to show that double ionization of ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$ primarily is the result of a sequential removal of the two electrons via an excited Rb state. The perspectives for direct two-electron ionization in negative ions are briefly discussed.
We present the experimental and theoretical investigation of the effects of the strong electromagnetic coupling of two autoionizing states (AIS's) on the photoionization properties of an atomic system. These effects are observed by probing the ladder system from the ground state of the atom through a weak two-photon transition to the region of the lower AIS. The experimental observation of the modification of the total ionization and partial photoelectron spectra at different wavelengths of the coupling and probe lasers are accurately reproduced by a theoretical analysis which uses a density-matrix approach. Both theory and experiment indicate a strong inhibition of the ionization of the system in the case when both lasers are resonant with the two atomic transitions, while displaying a rapidly varying asymmetry induced as the detuning between the two states and the fields increases. In the extreme case of a large detuning, two separate structures appear as distinct total ionization and photoelectron peaks. The above findings combined with the full theoretical treatment indicate that the phenomena observed are an experimental demonstration of ac Stark splitting between two AIS's. \textcopyright{} 1996 The American Physical Society.
The dc-field-induced interference effects in recombination in a model system consisting of two close-lying autoionizing states are studied. The two states are strongly coupled by a dc field and can decay via both autoionization and spontaneous emission. All possible channels of radiative decay are included for the model system. In special cases the isomorphism of the recombination and photoionization studies is established. The total integrated recombination probability is calculated and its behavior as a function of dc field is presented. Our density-matrix calculations lead to the known results in the limiting case of no dc field.