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Register a new userTime- and momentum-resolved photoemission studies using time-of-flight momentum microscopy at a free-electron laser
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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$_2$.
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The Fe pnictide parent compound EuFe2As2 exhibits a strongly momentum dependent carrier dynamics around the hole pocket at the center of the Brillouin zone. The very different dynamics of electrons and holes cannot be explained solely by intraband scattering and interband contributions have to be considered. In addition, three coherently excited modes at frequencies of 5.6, 3.1 and 2.4 THz are observed. An estimate of the electron-phonon coupling parameter reveals lambda < 0.5, suggesting a limited importance of e-ph coupling to superconductivity in Fe pnictides.
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.
We demonstrate the structural sensitivity and accuracy of the standing wave technique at a high repetition rate free-electron laser, FLASH at DESY in Hamburg, by measuring the photoelectron yield from the surface SiO2 of Mo/Si multilayers. These experiments open up the possibility to obtain unprecedented structural information of adsorbate and surface atoms with picometer spatial accuracy and femtosecond temporal resolution. This technique will substantially contribute to a fundamental understanding of chemical reactions at catalytic surfaces and the structural dynamics of superconductors.
With rapidly growing photoconversion efficiencies, hybrid perovskite solar cells have emerged as promising contenders for next generation, low-cost photovoltaic technologies. Yet, the presence of nanoscale defect clusters, that form during the fabrication process, remains critical to overall device operation, including efficiency and long-term stability. To successfully deploy hybrid perovskites, we must understand the nature of the different types of defects, assess their potentially varied roles in device performance, and understand how they respond to passivation strategies. Here, by correlating photoemission and synchrotron-based scanning probe X-ray microscopies, we unveil three different types of defect clusters in state-of-the-art triple cation mixed halide perovskite thin films. Incorporating ultrafast time-resolution into our photoemission measurements, we show that defect clusters originating at grain boundaries are the most detrimental for photocarrier trapping, while lead iodide defect clusters are relatively benign. Hexagonal polytype defect clusters are only mildly detrimental individually, but can have a significant impact overall if abundant in occurrence. We also show that passivating defects with oxygen in the presence of light, a previously used approach to improve efficiency, has a varied impact on the different types of defects. Even with just mild oxygen treatment, the grain boundary defects are completely healed, while the lead iodide defects begin to show signs of chemical alteration. Our findings highlight the need for multi-pronged strategies tailored to selectively address the detrimental impact of the different defect types in hybrid perovskite solar cells.
In a recent paper [Phys. Rev. Lett. 125, 043201 (2020)] (Ref.1) Liao et al. propose a theory of the interferometric photoemission delay based on the concepts of the photoelectron phase and photoelectron effective mass. The present comment discusses the applicability and limitations of the proposed approach based on an ab initio analysis supported by vast literature. Two central assumptions of the paper are questioned, namely that the photoelectron can be characterized by a phase (have a well-defined phase velocity), and that it can always be ascribed an effective mass Theories based on these concepts are concluded to be inapplicable to real solids, which is illustrated by the example of the system addressed in Ref. 1. That the basic assumptions of the theory are never fulfilled in nature discredits the underlying idea of the time-domain interferometric solid-state energy-momentum-dispersion imaging method suggested in Ref. 1. Apart from providing a necessary caution to experimentalists, the present comment also gives an insight into the photoelectron wave function and points out problems and pitfalls inherent in modeling real crystals.
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