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Physical Review Letters

Multiphoton Double Ionization via Field-Independent Resonant Excitation

J. Rudati, Jan L. Chaloupka, Pierre Agostini, K. C. Kulander, Louis F. DiMauro

Published May 19, 2004• 47 citations
Publisher

Abstract

The double ionization of xenon in the multiphoton regime has been studied at two wavelengths (0.77 and 0.79 microm) using an electron-ion coincidence technique and an intensity binned ion ratio method. Sharp resonant structures in the electron energy distribution correlated with the doubly charged ion, as well as a wavelength dependence of the Xe(2+)/Xe(+) ratio provides new insights. A mechanism involving the shelving of population in Rydberg states followed by excitation of a core electron is proposed.

DOI
10.1103/physrevlett.92.203001

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The double ionization of xenon in the multiphoton regime has been studied at two wavelengths (0.77 and 0.79 microm) using an electron-ion coincidence technique and an intensity binned ion ratio method. Sharp resonant structures in the electron energy distribution correlated with the doubly charged ion, as well as a wavelength dependence of the Xe(2+)/Xe(+) ratio provides new insights. A mechanism involving the shelving of population in Rydberg states followed by excitation of a core electron is proposed.
With quantum calculations, we have investigated the multiphoton nonsequential double ionization of helium atoms in intense laser fields at ultraviolet wavelengths. Very surprisingly, we found a so-far unobserved double-circle structure in the correlated electron momentum spectra. The double-circle structure essentially reveals multiphoton Rabi oscillations of two electrons, which are strongly supported by the oscillating population of a certain doubly excited state and by the oscillating double ionization signals. This two-electron multiphoton Rabi effect provides a profound understanding of electronic correlations and complicated multiphoton phenomena and is expected to be a new tool for broad applications, such as quantum coherent control.
Neutral Rydberg state excitation in strong UV laser fields of Xe atoms has been studied and compared with direct ionization. The yields of both strong-field excitation and ionization have been measured as a function of UV laser intensity and ellipticity. The underlying physical mechanism has been discussed based on the experimental results, indicating that the Rydberg states are populated via multi-photon resonance excitation in strong 400 nm laser fields. Finally, a comparative study of Xe and O2O_2O2​ with similar ionization potentials have been performed, showing the suppressed excitation of molecules in strong UV laser fields.
With quantum calculations, we have investigated the multiphoton nonsequential double ionization of helium atoms in intense laser fields at ultraviolet wavelengths. Very surprisingly, we find a so-far unobserved double-circle structure in the correlated electron momentum spectra. The double-circle structure essentially reveals multiphoton Rabi oscillations of two electrons, which are strongly supported by the oscillating population of a certain doubly excited state and by the oscillating double ionization signals. This two-electron multiphoton Rabi effect provides profound understandings of electronic correlations and complicated multiphoton phenomena and is expected to be a new tool for broad applications, such as quantum coherent control.
The authors have studied double ionization of Ba 6snl Rydberg states through resonant two-photon excitation of 8snl double-Rydberg states with n=13 and 14 and different l. The laser intensity dependence of Ba 2+ yield measured for l>or=8, when the electrons suffer long-range dipole interaction, shows a decrease from four-photon for l=8 to less than three for l=11. The four-photon dependence is due to autoionization decay populating the Ba + (7p) levels which gives an indirect signature to the Ba 2+ production. By increasing l this decay vanishes and the data show evidence of a direct double-ionization process via planetary-electron states for l>or=10. Additional intensity measurements performed for low l=6 states strongly mixed with 5fn'l' ones by short-range multipole interaction, reveal indirect Ba 2+ production and an individual case of partial stabilization due to destructive interference leading to direct double ionization.
Experimental investigations of resonant structure in doubly charged ion (A 2+ ) formation were carried out during Sr and Ba atom ionization by infrared laser radiation (ω = 8400-9100 cm -1 ). It has been shown that in this case the mechanism of ion formation is a two-electron process - the ions are produced immediately from the neutral atoms. It has been found for the first time that the resonant structure in A 2+ ion formation in such conditions is due to the excitation and ionization of neutral-atom mixed states. The atomic-state mixing in this case results from the Stark effect provided that the polarizability of these states is very high.
We report on the single and double multiphoton ionization of ground state Sr atoms observed in an atomic beam experiment with laser pulses of ∼5 ns duration, maximum intensity ∼4 × 10 11 W cm −2 and within the 710–740 nm wavelength range. The Sr + spectrum consists of two strong lines originating from three-photon resonant four-photon ionization of bound states, a number of weak autoionizing resonances and a broad line due to four-photon excitation of the doubly excited 5p 2 1 S 0 state. The latter, along with a strong, broad and structured spectral feature, is also evident in the wavelength dependence of the doubly charged Sr 2+ ion. A weakly evident but reproducible inflection point ('knee' structure) appears in the intensity dependence of the Sr 2+ yield at the location of the 5p 2 1 S 0 resonance. A complementary fluorescence experiment revealed the accumulation of population in the 5p 1/2 , 3/2 , 6s 1/2 and 5d 3/2 , 5/2 excited Sr + states during the laser pulse. All fluorescence signals depend on laser wavelength in a manner similar to the recorded Sr + spectrum. The population accumulation in the 5p 1/2 , 3/2 ionic states unambiguously proves the absorption of two photons above the first 5s 1/2 atomic threshold while that of the 5d 3/2 , 5/2 and 6s 1/2 ones suggest the absorption of at least two more. Since under our laser pulse duration and intensity the absorption of such a number of photons in an unstructured continuum is highly improbable, it may be concluded that the process is mediated by dense manifolds of near- resonant doubly excited states, their role in the dynamics of laser–atom interaction under our conditions being far more crucial than in studies conducted using intense ultrashort pulses.