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Journal of Experimental and Theoretical Physics Letters

Observation of high efficiency of Raman scattering in the process of the three-photon ionization of samarium atom

Aleksandr I. Gomonai

Published Sep 1, 2007• 0 citations
Publisher

Abstract

Very high efficiency of Raman scattering on samarium atoms in the process of three-photon ionization has been detected. An intense maximum attributed to the one-photon transition 4f 65d6s 9 H 2 → 4f 55d6s 2 7 D 3° between two excited states is observed in the dependence of the yield of Sm+ ions on the laser-radiation frequency. The 4f 65d6s 9 H 2 state is populated owing to the spontaneous Raman scattering 4f 66s 2 7 F 3 + ω − ν → 4f 65d6s 9 H 2.

DOI
10.1134/s0021364007140044

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Very high efficiency of Raman scattering on samarium atoms in the process of three-photon ionization has been detected. An intense maximum attributed to the one-photon transition 4f 65d6s 9 H 2 → 4f 55d6s 2 7 D 3° between two excited states is observed in the dependence of the yield of Sm+ ions on the laser-radiation frequency. The 4f 65d6s 9 H 2 state is populated owing to the spontaneous Raman scattering 4f 66s 2 7 F 3 + ω − ν → 4f 65d6s 9 H 2.
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.
The advent of the laser has brought about a revolution in the kinds of experimental phenomena that can be investigated. In particular, ultra-high power monochromatic, collimated sources have intensities of sufficient magnitude to enable studies to be carried out in the regime where 'non-linear' effects are important, even dominant. Important among these are processes which are characterised by the simultaneous absorption of two or more optical photons. While multiple photon processes are not completely new, those in the optical part of the spectrum, like Raman scattering, have, until the advent of the laser, been thought of as linear in the incident intensity, or, like the two-quantum decay of the metastable 2s states of hydrogen-like atoms and ions, been confined to theory. Of the multiple photon, non-linear optical processes, multiquantum ionization is one of the more fruitful for detailed, quantitative measurements, and for comparison with theory, since (1) one does not require precise coincidence between the laser light and an absorption line (2) the ionizations can be detected unambiguously with 100% efficiency (3) atomic wave functions are simple, and sufficiently accurate to enable one to make reasonable precise calculations.
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.