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arXiv:physics/0311032 · Applied Physics B

Harmonic generation by atoms in circularly polarized laser fields: far-off and near resonance regimes

F. Ceccherini, N. Davini, D. Bauer, F. Cornolti

Published Mar 29, 2004• 2 citations
arXivHTMLPDF
DOI
10.1007/s00340-004-1458-x

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We theoretically study multiphoton ionization of the Ca atom irradiated by the second (photon energy 3.13.13.1 eV) and third (photon energy 4.65 eV) harmonics of Ti:sapphire laser pulses (photon energy 1.551.551.55 eV). Because of the dense energy level structure the second and third harmonics of a Ti:sapphire laser are nearly single-photon resonant with the 4s4p4s4p4s4p 1Po{}^{1}{P}^{o}1Po and 4s5p4s5p4s5p 1Po{}^{1}{P}^{o}1Po states, respectively. Although two-photon ionization takes place through the near-resonant intermediate states with the same symmetry in both cases, it turns out that there are significant differences between them. The photoelectron energy spectra exhibit the absence or presence of substructures. More interestingly, the photoelectron angular distributions clearly show that the main contribution to the ionization processes by the third harmonic arises from the far-off-resonant 4s4p4s4p4s4p 1Po{}^{1}{P}^{o}1Po state rather than the near-resonant 4s5p4s5p4s5p 1Po{}^{1}{P}^{o}1Po state. These findings can be attributed to the fact that the dipole moment for the 4s24{s}^{2}4s2 ${}^{1}{S}^{e}\ensuremath{-}4s5p$ 1Po{}^{1}{P}^{o}1Po transition is much smaller than that for the 4s24{s}^{2}4s2 ${}^{1}{S}^{e}\ensuremath{-}4s4p$ 1Po{}^{1}{P}^{o}1Po transition.
Magnetic-field-induced resonant third-harmonic generation in I2{\mathrm{I}}_{2}I2​ with circularly polarized light is studied. With a magnetic field perpendicular to the propagating direction of the light, the axial symmetry is broken and the angular momentum is no longer conserved in such a system, and the third harmonic may be generated under such conditions. Quantum beats in photon-echo-like third-harmonic generation with nonsynchronous laser pulses are also studied. The intensity of the harmonic generated may be interpreted in terms of the interference between a molecule and itself as well as the interference between different molecules. The gyromagnetic ratio of the resonant states is measured.