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arXiv:1204.4812 · Journal of Physics B Atomic Molecular and Optical Physics

Photoelectron angular distributions for the two-photon ionization of helium by ultrashort extreme ultraviolet free-electron laser pulses

Ruilin Ma, Koji Motomura, Kenichi L. Ishikawa, Subhendu Mondal, H. Fukuzawa, A Yamada, Kiyoshi Ueda, Kiyonobu Nagaya, S Yase, Y Mizoguchi, Mengyu Yao, Arnaud Rouze, A. Hundermark, Marc J. J. Vrakking, P. Johnsson, Mitsuru Nagasono, Kensuke Tono, Tadashi Togashi, Yasunori Senba, Haruhiko Ohashi, Makina Yabashi, Tetsuya Ishikawa

Published Aug 13, 2013• 21 citations
arXivHTMLPDF

Abstract

Phase-shift differences and amplitude ratios of the outgoing $s$ and $d$ continuum wave packets generated by two-photon ionization of helium atoms are determined from the photoelectron angular distributions obtained using velocity map imaging. Helium atoms are ionized with ultrashort extreme-ultraviolet free-electron laser pulses with a photon energy of 20.3, 21.3, 23.0, and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The measured values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to an excited level or Rydberg manifold. The difference stems from the competition between resonant and non-resonant paths in two-photon ionization by ultrashort pulses. Since the competition can be controlled in principle by the pulse shape, the present results illustrate a new way to tailor the continuum wave packet.

DOI
10.1088/0953-4075/46/16/164018

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Phase-shift differences and amplitude ratios of the outgoing sss and ddd continuum wave packets generated by two-photon ionization of helium atoms are determined from the photoelectron angular distributions obtained using velocity map imaging. Helium atoms are ionized with ultrashort extreme-ultraviolet free-electron laser pulses with a photon energy of 20.3, 21.3, 23.0, and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The measured values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to an excited level or Rydberg manifold. The difference stems from the competition between resonant and non-resonant paths in two-photon ionization by ultrashort pulses. Since the competition can be controlled in principle by the pulse shape, the present results illustrate a new way to tailor the continuum wave packet.
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Two-photon ionization of atomic helium has been measured by combining femtosecond extreme-ultraviolet pulses from the free-electron laser in Hamburg (FLASH at DESY) with intense light pulses from a synchronized neodymium-doped yttrium lithium fluoride laser. Sidebands appear in the photoelectron spectra when the two laser pulses overlap in both space and time. Their intensity exhibits a characteristic dependence on the relative time delay between the ionizing and the dressing pulses and provides an inherent time marker for time-resolved pump-probe experiments. The measurements of the sidebands are in good agreement with theoretical predictions and allow for a direct analysis of two-photon ionization, free from processes related to interference between multiple quantum paths.
We present our study on complete measurements of two-photon ionization in atomic rubidium. In this study we developed an effective technique to measure the angular distributions of photoelectrons. Through the measurements with this technique and using elliptically-polarized light we have successfully determined the atomic parameters—the relative cross sections for various ionization channels as well as the phase difference between s- and d-continuum waves. The measured phase differences are in excellent agreement with expected values over the entire range of photoelectron kinetic energy from 0 to 0.5 eV. The measured relative cross sections for ionization into S and D channels are also in good agreement with theoretical data. Both the relative cross sections and phase differences show a slow variation as a function of photoelectron energy. The ratios of cross sections of the two D channels are not in agreement with the expected value, suggesting fine structure effects. We also studied a quantum mechanical interference using two-color laser fields and observed the extremely asymmetric photoelectron angular distribution produced by interfering even- and odd-order photoionization processes in atomic rubidium as the optical phase was varied. We observed these effects with both perpendicularly and parallel-polarized fields components. It is worthy to note that the quantum interference observed with perpendicularly-polarized two-color fields is unique. Based on the analysis of measured angular distributions we derived the phase difference between even and odd continuum waves for the first time. The measured value of the phase difference is in good agreement with the calculated value from quantum defect theory.