Photoemission Angular Distribution Beyond the Single Wavevector Description of Photoelectron Final States

We develop a novel simulation procedure for angle-resolved photoemission spectroscopy (ARPES), where a photoelectron wave function is set to be an outgoing plane wave in a vacuum associated with the emitted photoelectron wave packet. ARPES measurements on the transition metal dichalcogenide $1T$-$\mathrm{Ti}\mathrm{S}_2$ are performed, and our simulations exhibit good agreement with experiments. Analysis of our calculated final state wave functions quantitatively visualizes that they include various waves due to the boundary condition and the uneven crystal potential. These results show that a more detailed investigation of the photoelectron final states is necessary to fully explain the photon-energy- and light-polarization-dependent ARPES spectra.Comment: 6+14 pages, 4+15 figure

Spin-polarized saddle points in the topological surface states of the elemental Bismuth revealed by a pump-probe spin-resolved ARPES

We use a pump-probe, spin-, and angle-resolved photoemission spectroscopy (ARPES) with a 10.7 eV laser accessible up to the Brillouin zone edge, and reveal for the first time the entire band structure, including the unoccupied side, for the elemental bismuth (Bi) with the spin-polarized surface states. Our data identify Bi as in a strong topological insulator phase ($Z_2$=1) against the prediction of most band calculations. We unveil that the unoccupied topological surface states possess spin-polarized saddle points yielding the van Hove singularity, providing an excellent platform for the future development of opto-spintronics.Comment: 6 pages, 4 figure

Time-, spin-, and angle-resolved photoemission spectroscopy with a 1-MHz 10.7-eV pulse laser

We describe a setup of time-, spin-, and angle-resolved photoemission spectroscopy (tr-SARPES) employing a 10.7-eV ($\lambda$=115.6 nm) pulse laser at 1-MHz repetition rate as a probe photon source. This equipment effectively combines technologies of a high-power Yb:fiber laser, ultraviolet-driven harmonic generation in Xe gas, and a SARPES apparatus equipped with very-low-energy-electron-diffraction (VLEED) spin detectors. A high repetition rate (1 MHz) of the probe laser allows experiments with the photoemission space-charge effects significantly reduced, despite a high flux of 10$^{13}$ photons/s on the sample. The relatively high photon energy (10.7 eV) also brings the capability of observing a wide momentum range that covers the entire Brillouin zone of many materials while ensuring high momentum resolution. The experimental setup overcomes a low efficiency of spin-resolved measurements, which gets even more severe for the pump-probed unoccupied states, and affords for investigating ultrafast electron and spin dynamics of modern quantum materials with energy and time resolutions of 25 meV and 360 fs, respectively.Comment: 11 pages, 7 figure