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We theoretically investigate the photoelectron momentum distributions (PMDs) of the argon atom by using an inhomogeneous polarization-gated pulse. The numerical results show that the symmetry of the PMDs is disrupted and a vertical interference stripe appears as the inhomogeneity parameters increase. We illustrate that the interference mechanisms of these vertical interference stripes are different from traditional interference mechanisms, which are interference between direct electrons ionized in the same quarter-cycle. In addition, by analyzing the electron trajectories, we find that the breakdown of symmetry is due to the strong suppression of the positive deviation of electrons along the x-axis by the inhomogeneous PG pulse.
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http://dx.doi.org/10.1364/OE.557584 | DOI Listing |
Nature
September 2025
Laboratorium für Physikalische Chemie, ETH Zürich, Zürich, Switzerland.
Many chirality-sensitive light-matter interactions are governed by chiral electron dynamics. Therefore, the development of advanced technologies making use of chiral phenomena would critically benefit from measuring and controlling chiral electron dynamics on their natural attosecond timescales. Such endeavours have so far been hampered by the lack of characterized circularly polarized attosecond pulses, an obstacle that has recently been overcome.
View Article and Find Full Text PDFJ Chem Theory Comput
September 2025
Kenneth S. Pitzer Center for Theoretical Chemistry, Department of Chemistry, University of California, Berkeley, California 94720, United States.
Quantum mechanical calculations of core electron binding energies (CEBEs) are relevant to interpreting X-ray photoelectron spectroscopy (XPS). Orbital-optimized density functional theory (OO-DFT) accurately predicts K-edge CEBEs but is challenged by the presence of significant spin-orbit coupling (SOC) at L- and higher edges involving inner-shell orbitals with nonzero angular momentum. To extend OO-DFT to L-edges and higher, our method utilizes scalar-relativistic, spin-restricted open-shell OO-DFT to construct a minimal, quasi-degenerate basis of core-hole states corresponding to a chosen inner-shell (e.
View Article and Find Full Text PDFOpt Express
March 2025
We theoretically investigate the photoelectron momentum distributions (PMDs) of the argon atom by using an inhomogeneous polarization-gated pulse. The numerical results show that the symmetry of the PMDs is disrupted and a vertical interference stripe appears as the inhomogeneity parameters increase. We illustrate that the interference mechanisms of these vertical interference stripes are different from traditional interference mechanisms, which are interference between direct electrons ionized in the same quarter-cycle.
View Article and Find Full Text PDFWe use the semi-classical two-step (SCTS) model to investigate the fan-structure in the photoelectron momentum distribution produced by hydrogen atoms irradiated by linearly polarized near-infrared femtosecond laser pulses. It is shown that the initial tunneling moment and momentum of the fan-structure can be classified into four separated regions corresponding to four trajectory types as direct, forward-deflected, forward-scattering, and backward-scattering. We find a one-to-one mapping between the initial tunneling coordinates and the final momentum for the first three types of trajectories.
View Article and Find Full Text PDFPhys Rev Lett
July 2025
Universität Kassel, Institut für Physik und CINSaT, Heinrich-Plett-Straße 40, 34132 Kassel, Germany.
We report theoretical momentum distributions of electrons ejected from the C and O K shells of fixed-in-space CO molecules by Compton scattering of 20 keV photons for different magnitudes and orientations of the photon momentum transfer with respect to the molecular axis. We observe distinct diffraction patterns in our computed momentum distributions, which are governed by the interference of the direct Compton electrons and those which are scattered on the parent and neighboring nuclei. The observed phenomenon is similar to that employed in diffraction imaging using high-energy photoelectrons.
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