Photoelectron momentum microscopy is an emerging powerful method for angle-resolved photoelectron spectroscopy (ARPES), especially in combination with imaging spin filters. These instruments record k-k images, typically exceeding a full Brillouin zone. As energy filters, double-hemispherical or time-of-flight (ToF) devices are in use. Here, we present a new approach for momentum mapping of the full half-space, based on a large single hemispherical analyzer (path radius of 225 mm). Excitation by an unfocused He lamp yielded an energy resolution of 7.7 meV. The performance is demonstrated by k-imaging of quantum-well states in Au and Xe multilayers. The α-aberration term (α, entrance angle in the dispersive plane) and the transit-time spread of the electrons in the spherical field are studied in a large pass-energy (6 eV-660 eV) and angular range (α up to ±7°). It is discussed how the method circumvents the preconditions of previous theoretical work on the resolution limitation due to the α-term and the transit-time spread, being detrimental for time-resolved experiments. Thanks to k-resolved detection, both effects can be corrected numerically. We introduce a dispersive-plus-ToF hybrid mode of operation, with an imaging ToF analyzer behind the exit slit of the hemisphere. This instrument captures 3D data arrays I (E, k, k), yielding a gain up to N in recording efficiency (N being the number of resolved time slices). A key application will be ARPES at sources with high pulse rates such as synchrotrons with 500 MHz time structure.
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Sci Rep
January 2025
Department of Physics, TU Dortmund University, Otto-Hahn-Straße 4, 44227, Dortmund, Germany.
Time-resolved momentum microscopy is an emerging technique based on photoelectron spectroscopy for characterizing ultrafast electron dynamics and the out-of-equilibrium electronic structure of materials in the entire Brillouin zone with high efficiency. In this article, we introduce a setup for time-resolved momentum microscopy based on an energy-filtered momentum microscope coupled to a custom-made high-harmonic generation photon source driven by a multi-100 kHz commercial Yb-ultrafast laser that delivers fs pulses in the extreme ultraviolet range. The laser setup includes a nonlinear pulse compression stage employing spectral broadening in a Herriott-type bulk-based multi-pass cell.
View Article and Find Full Text PDFJ Phys Condens Matter
January 2025
School of Materials Sciences, Indian Association for the Cultivation of Science, 2A & 2B Raja S. C. Mullick Road, Jadavpur, Kolkata, West Bengal 700032, India.
An exotic quantum mechanical ground state, i.e. the non-magnetic= 0 state, has been predicted for higher transition metalt2g4systems, due to the influence of strong spin-orbit coupling (SOC) or in other words, due to unquenched orbital moment contribution.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
Institute of Molecular Physical Sciences, ETH Zurich, CH-8093 Zurich, Switzerland.
The rovibrational energy-level structures of BaH and BaD in their XΣ electronic ground state have been characterised by pulsed-field-ionisation zero-kinetic-energy photoelectron spectroscopy following resonance-enhanced (1 + 1') two-photon excitation from the BaH/BaD X Σ ground state the E Π (' = 0, 1) intermediate levels. A full set of rovibrational molecular constants for the BaH and BaD ground states has been derived for the first time and the adiabatic ionisation energies of BaH and BaD were determined to be 38 679.96(20) and 38 652.
View Article and Find Full Text PDFThe emerging field of orbitronics aims to generate and control orbital angular momentum for information processing. Chiral crystals are promising orbitronic materials because they have been predicted to host monopole-like orbital textures, where the orbital angular momentum aligns isotropically with the electron's crystal momentum. However, such monopoles have not yet been directly observed in chiral crystals.
View Article and Find Full Text PDFBeilstein J Nanotechnol
November 2024
Department of Chemistry, Johns Hopkins University, Baltimore, MD, 21218, USA.
Ion beam-induced deposition (IBID) using Pt(CO)Cl and Pt(CO)Br as precursors has been studied with ultrahigh-vacuum (UHV) surface science techniques to provide insights into the elementary reaction steps involved in deposition, complemented by analysis of deposits formed under steady-state conditions. X-ray photoelectron spectroscopy (XPS) and mass spectrometry data from monolayer thick films of Pt(CO)Cl and Pt(CO)Br exposed to 3 keV Ar, He, and H ions indicate that deposition is initiated by the desorption of both CO ligands, a process ascribed to momentum transfer from the incident ion to adsorbed precursor molecules. This precursor decomposition step is accompanied by a decrease in the oxidation state of the Pt(II) atoms and, in IBID, represents the elementary reaction step that converts the molecular precursor into an involatile PtX species.
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