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The Journal of Atomic and Molecular Sciences

Excitation and Ionization of Xenon Atoms in Strong UV Laser Fields

Tong Yang, Yi Lian, R. Wang, Song Zhang, Lanhai He, Hang Lv, Haifeng Xu

Published Aug 1, 2017• 0 citations
Publisher

Abstract

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 $O_2$ with similar ionization potentials have been performed, showing the suppressed excitation of molecules in strong UV laser fields.

DOI
10.4208/jams.051817.062017a

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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.
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Rather than being freed to the continuum, the strong-field tunneled electrons can make a trajectory driven by the remaining laser fields and have certain probability to be captured by the high lying Rydberg states of the parent atoms or molecules. To explore the effect of molecular orbital on Rydberg state excitation, the ellipticity dependence of Rydberg state yields of N2 and O2 molecules are experimentally investigated using cold target recoil ion momentum spectroscopy and are compared with their counterpart atoms Ar and Xe with comparable ionization potentials. We found the generation probability of the neutral Rydberg fragment O2* was orders of magnitude higher than that of Xe* due to the butterfly-shaped highest occupied molecular orbital of O2. Meanwhile, our experimental and simulation results reveal that it is the initial momentum distribution (determined by the detailed characteristics of orbitals) that finally leads to the tendency that the Rydberg state yield of O2 (Ar) decreased slower than that obtained for Xe (N2) when the ellipticity of the excitation laser field is increased.
Nonresonant ac Stark shifts of Rydberg states in Xe have been investigated by probing an atomic transition with a weak UV light in the presence of an intense YAG-laser pulse. Rydberg atoms produced through two-photon excitation, 5p → np (n = 15–48) and 5p → nf (n = 12–49), are subsequently ionized. IR-laser-induced shifts of the resonant ionization profiles are then measured. The measured shift, 3.9 ± 0.3 cm−1 at 1010 W cm−2, is more than a factor of 2 smaller than that expected from the basis of ponderomotive term, 8.5 cm−1 at 1010 W cm−2. In addition, the shift varies linearly as a function of the IR-laser intensity and does not depend on the principal quantum number of the np and nf series investigated here.
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.