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Register a new userA quantitative comparison of time-of-flight momentum microscopes and hemispherical analyzers for time- and angle-resolved photoemission spectroscopy experiments
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Time-of-flight-based momentum microscopy has a growing presence in photoemission studies, as it enables parallel energy- and momentum-resolved acquisition of the full photoelectron distribution. Here, we report table-top extreme ultraviolet (XUV) time- and angle-resolved photoemission spectroscopy (trARPES) featuring both a hemispherical analyzer and a momentum microscope within the same setup. We present a systematic comparison of the two detection schemes and quantify experimentally relevant parameters, including pump- and probe-induced space-charge effects, detection efficiency, photoelectron count rates, and depth of focus. We highlight the advantages and limitations of both instruments based on exemplary trARPES measurements of bulk WSe2. Our analysis demonstrates the complementary nature of the two spectrometers for time-resolved ARPES experiments. Their combination in a single experimental apparatus allows us to address a broad range of scientific questions with trARPES.
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In photoelectron spectroscopy, the measured electron momentum range is intrinsically related to the excitation photon energy. Low photon energies $<10$ eV are commonly encountered in laser-based photoemission and lead to a momentum range that is smaller than the Brillouin zones of most materials. This can become a limiting factor when studying condensed matter with laser-based photoemission. An additional restriction is introduced by widely used hemispherical analyzers that record only electrons photoemitted in a solid angle set by the aperture size at the analyzer entrance. Here, we present an upgrade to increase the effective solid angle that is measured with a hemispherical analyzer. We achieve this by accelerating the photoelectrons towards the analyzer with an electric field that is generated by a bias voltage on the sample. Our experimental geometry is comparable to a parallel plate capacitor and, therefore, we approximate the electric field to be uniform along the photoelectron trajectory. With this assumption, we developed an analytic, parameter-free model that relates the measured angles to the electron momenta in the solid and verify its validity by comparing with experimental results on the charge density wave material TbTe$_3$. By providing a larger field of view in momentum space, our approach using a bias potential considerably expands the flexibility of laser-based photoemission setups.
Quantum gas microscopes are a promising tool to study interacting quantum many-body systems and bridge the gap between theoretical models and real materials. So far they were limited to measurements of instantaneous correlation functions of the form $langle hat{O}(t) rangle$, even though extensions to frequency-resolved response functions $langle hat{O}(t) hat{O}(0) rangle$ would provide important information about the elementary excitations in a many-body system. For example, single particle spectral functions, which are usually measured using photoemission experiments in electron systems, contain direct information about fractionalization and the quasiparticle excitation spectrum. Here, we propose a measurement scheme to experimentally access the momentum and energy resolved spectral function in a quantum gas microscope with currently available techniques. As an example for possible applications, we numerically calculate the spectrum of a single hole excitation in one-dimensional $t-J$ models with isotropic and anisotropic antiferromagnetic couplings. A sharp asymmetry in the distribution of spectral weight appears when a hole is created in an isotropic Heisenberg spin chain. This effect slowly vanishes for anisotropic spin interactions and disappears completely in the case of pure Ising interactions. The asymmetry strongly depends on the total magnetization of the spin chain, which can be tuned in experiments with quantum gas microscopes. An intuitive picture for the observed behavior is provided by a slave-fermion mean field theory. The key properties of the spectra are visible at currently accessible temperatures.
Time- and angle-resolved photoelectron spectroscopy (trARPES) employing a 500 kHz extreme-ultravioled (XUV) light source operating at 21.7 eV probe photon energy is reported. Based on a high-power ytterbium laser, optical parametric chirped pulse amplification (OPCPA), and ultraviolet-driven high-harmonic generation, the light source produces an isolated high-harmonic with 110 meV bandwidth and a flux of more than $10^{11}$ photons/second on the sample. Combined with a state-of-the-art ARPES chamber, this table-top experiment allows high-repetition rate pump-probe experiments of electron dynamics in occupied and normally unoccupied (excited) states in the entire Brillouin zone and with a temporal system response function below 40 fs.
Time-resolved photoemission with ultrafast pump and probe pulses is an emerging technique with wide application potential. Real-time recording of non-equilibrium electronic processes, transient states in chemical reactions or the interplay of electronic and structural dynamics offers fascinating opportunities for future research. Combining valence-band and core-level spectroscopy with photoelectron diffraction for electronic, chemical and structural analysis requires few 10 fs soft X-ray pulses with some 10 meV spectral resolution, which are currently available at high repetition rate free-electron lasers. The PG2 beamline at FLASH (DESY, Hamburg) provides a high pulse rate of 5000 pulses/s, 60 fs pulse duration and 40 meV bandwidth in an energy range of 25-830 eV with a photon beam size down to 50 microns in diameter. We have constructed and optimized a versatile setup commissioned at FLASH/PG2 that combines FEL capabilities together with a multidimensional recording scheme for photoemission studies. We use a full-field imaging momentum microscope with time-of-flight energy recording as the detector for mapping of 3D band structures in ($k_x$, $k_y$, $E$) parameter space with unprecedented efficiency. Our instrument can image full surface Brillouin zones with up to 7 {AA} $^{-1}$ diameter in a binding-energy range of several eV, resolving about $2.5times10^5$ data voxels. As an example, we present results for the ultrafast excited state dynamics in the model van der Waals semiconductor WSe$_2$.
We present an experimental setup for laser-based angle-resolved time-of-flight (LARTOF) photoemission. Using a picosecond pulsed laser, photons of energy 10.5 eV are generated through higher harmonic generation in xenon. The high repetition rate of the light source, variable between 0.2-8 MHz, enables high photoelectron count rates and short acquisition times. By using a Time-of-Flight (ToF) analyzer with angle-resolving capabilities electrons emitted from the sample within a circular cone of up to pm15 degrees can be collected. Hence, simultaneous acquisition of photoemission data for a complete area of the Brillouin zone is possible. The current photon energy enables bulk sensitive measurements, high angular resolution and the resulting covered momentum space is large enough to enclose the entire Brillouin zone in cuprate high-Tc superconductors. Fermi edge measurements on polycrystalline Au shows an energy resolution better than 5 meV. Data from a test measurement of the Au(111) surface state is presented along with measurements of the Fermi surface of the high-Tc superconductor Bi2212.
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