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Optics and Spectroscopy

Spontaneous Raman scattering upon resonant three-photon ionization of a samarium atom

Aleksandr I. Gomonai, Eugene Yu. Remeta

Published Mar 1, 2009• 0 citations
Publisher

Abstract

The manifestation of spontaneous Raman scattering upon the three-photon ionization of a samarium atom has been investigated. The dependence of the Sm+ yield on the laser frequency, along with the peaks due to the two-photon excitation of bound states from different levels of the 4f 66s 2 7 F ground term, exhibits a strong peak due to single-photon excitation of the 4f 55d6s 2 7 D°3 state from the 4f 65d6s 9 H 2 excited state. The 4f 65d6s 9 H 2 state was populated as a result of spontaneous Raman scattering. The large amplitude of the observed peak indicates a high efficiency of this process. The estimations performed indicate that the probability of resonant ionization through an excited state populated due to spontaneous Raman scattering can be comparable with the probability of three-photon ionization through the two-photon intermediate resonance. The necessary conditions for implementing this channel of resonant three-photon ionization are formulated.

DOI
10.1134/s0030400x09030023

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The manifestation of spontaneous Raman scattering upon the three-photon ionization of a samarium atom has been investigated. The dependence of the Sm+ yield on the laser frequency, along with the peaks due to the two-photon excitation of bound states from different levels of the 4f 66s 2 7 F ground term, exhibits a strong peak due to single-photon excitation of the 4f 55d6s 2 7 D°3 state from the 4f 65d6s 9 H 2 excited state. The 4f 65d6s 9 H 2 state was populated as a result of spontaneous Raman scattering. The large amplitude of the observed peak indicates a high efficiency of this process. The estimations performed indicate that the probability of resonant ionization through an excited state populated due to spontaneous Raman scattering can be comparable with the probability of three-photon ionization through the two-photon intermediate resonance. The necessary conditions for implementing this channel of resonant three-photon ionization are formulated.
The manifestation of double resonances upon the three-photon ionization of the samarium atom has been studied in a frequency range of 17200–18400 cm −1 . Thirty peaks caused by double resonances have been found in the dependence of the yield of Sm + ions on the laser radiation frequency. The majority of these peaks greatly exceed in amplitude the peaks associated with ordinary two-photon resonances. The influence of double resonances on the three-photon ionization has been theoretically analyzed using the density matrix approximation. The calculations show that the probability of the three-photon resonance ionization can increase by more than two orders of magnitude due to the additional one-photon population of an intermediate level. The double resonance slows down the rate of increase in the probability of ionization with an increase in the laser radiation intensity compared to ordinary two-photon resonance.
Amplitude ratios of resonance maxima caused by two-photon transitions from different levels of the ground term of the samarium atom are studied experimentally and theoretically as functions of the laser-radiation field strength. The results of these studies are shown to be promising for identifying the resonance structure of three-photon ionization spectra of the samarium atom. A not yet observed excited even-parity state with energy E ≈ 36789.1 cm −1 and hypothetical values of total angular momentum J = 5, 6 has been discovered.
A semiclassical theory of hyper-Raman scattering and three-photon resonant ionization via the coupled density-matrix and Maxwell equations is presented. A simplified three-level atom model is obtained, which includes two-photon resonant pumping and time-dependent photoionization rates. We consider conditions typically encountered in atomic vapors to simulate numerically the pulse propagation. A strong depletion of the photoionization probability in the hyper-Raman field-saturation regime is predicted.