Weigold, Erich. Electron momentum spectroscopy / Erich Weigold and lan E. McCarthy. p. cm. --(Physics of atoms and molecules) Includes bibliographical references and index.
We present orientation-dependent stereo Wigner time delays of CO molecules, which reveal the electron localization at the ionization moment. Together with theoretical calculations this constitutes a spatially-and temporally-resolved reconstruction of the molecular photoelectric effect.
Nature 431, 437--440 (2004) In Figs 2 and 3 of this Letter, we calculated the angle between the molecular axis and the in-plane electron as Q e,mol 5 Q mol -Q e , where Q e and Q mol are the angles of the electron and the molecular axis with respect to the polarization vector e. This distribution was then rotated by the angle of the molecular axis to picture the electron emission in the polar plots. Here a sign error occurred: instead of calculating and plotting Q mol -Q e,mol 5 Q e , we presented Q mol 1 Q e,mol 5 2Q mol -Q e . Figure 1 illustrates the corrected results (compare with Figs 2, 3 in our Letter). The data now show an even stronger dependence of the angular distribution of the electrons on the molecular orientation, emphasizing the importance of the new internal reference axis. Thus, the angular distribution in Fig. 1a does not resemble a helium-like dipole pattern any more (as we stated originally), which would be aligned mainly along the polarization axis, but shows a preferred emission of electrons rectangular to the molecular axis.
Attosecond photoionization delays have mostly been interpreted within the single-particle approximation of multi-electron systems. The strong electron correlation between the photoionization channels associated with the 3p and 3s orbitals of argon presents an interesting arena where this single-particle approximation breaks down. Around photon energies of 42 eV, the 3s photoionization channel of argon experiences a "Cooper-like" minimum, which is exclusively the result of inter-electronic correlations with the 3p shell. Photoionization delays around this "Cooper-like" minimum have been predicted theoretically, but experimental verification has remained a challenge since the associated photoionization cross section is inherently very low. Here, we report the measurement of photoionization delays around the Cooper-like minimum that were acquired with the 100 kHz High-Repetition 1 laser system at the ELI-ALPS facility. We report relative photoionization delays reaching up to unprecedented values of 430±20 as, as a result of electron correlation. Our experimental results are in partial agreement with state-of-the-art theoretical results, but also demonstrate the need for additional theoretical developments.
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