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Collective modes are responsible for the emergence of novel quantum phases in topological materials. In the quasi-one dimensional (1D) Weyl semimetal (TaSe4)2I, a charge density wave (CDW) opens band gaps at the Weyl points, thus turning the system into an axionic insulator. Melting the CDW would restore the Weyl phase, but 1D fluctuations extend the gapped regime far above the 3D transition temperature (T CDW = 263 K), thus preventing the investigation of this topological phase transition with conventional spectroscopic methods. Here we use a non-equilibrium approach: we perturb the CDW phase by photoexcitation, and we monitor the dynamical evolution of the band structure by time- and angle-resolved photoelectron spectroscopy. We find that, upon optical excitation, electrons populate the linearly dispersing states at the Fermi level (E F ), and fill the CDW gap. The dynamics of both the charge carrier population and the band gap renormalization (BGR) show a fast component with a characteristic time scale of a few hundreds femtoseconds. However, the BGR also exhibits a second slow component on the μs time scale. The combination of an ultrafast response and of persistent changes in the spectral weight at E F, and the resulting sensitivity of the linearly dispersing states to optical excitations, may explain the high performances of (TaSe4)2I as a material for broadband infrared photodetectors.

Trigonal tellurium, a small-gap semiconductor with pronounced magneto-electric and magneto-optical responses, is among the simplest realizations of a chiral crystal. We have studied by spin- and angle-resolved photoelectron spectroscopy its unconventional electronic structure and unique spin texture. We identify Kramers-Weyl, composite, and accordionlike Weyl fermions, so far only predicted by theory, and show that the spin polarization is parallel to the wave vector along the lines in k space connecting high-symmetry points. Our results clarify the symmetries that enforce such spin texture in a chiral crystal, thus bringing new insight in the formation of a spin vectorial field more complex than the previously proposed hedgehog configuration. Our findings thus pave the way to a classification scheme for these exotic spin textures and their search in chiral crystals.

In nodal-line semimetals, linearly dispersing states form Dirac loops in the reciprocal space with a high degree of electron-hole symmetry and a reduced density of states near the Fermi level. The result is reduced electronic screening and enhanced correlations between Dirac quasiparticles. Here we investigate the electronic structure of ZrSiSe, by combining time- and angle-resolved photoelectron spectroscopy with ab initio density functional theory (DFT) complemented by an extended Hubbard model (DFT+U+V) and by time-dependent DFT+U+V. We show that electronic correlations are reduced on an ultrashort timescale by optical excitation of high-energy electrons-hole pairs, which transiently screen the Coulomb interaction. Our findings demonstrate an all-optical method for engineering the band structure of a quantum material.

We present a new setup for resonant inelastic hard x-ray scattering at the Bernina beamline of SwissFEL with energy, momentum, and temporal resolution. The compact R  = 0.5 m Johann-type spectrometer can be equipped with up to three crystal analyzers and allows efficient collection of RIXS spectra. Optical pumping for time-resolved studies can be realized with a broad span of optical wavelengths. We demonstrate the performance of the setup at an overall ∼180 meV resolution in a study of ground-state and photoexcited (at 400 nm) honeycomb 5d iridate α-Li 2 IrO 3 . Steady-state RIXS spectra at the iridium L 3 -edge (11.214 keV) have been collected and are in very good agreement with data collected at synchrotrons. The time-resolved RIXS transients exhibit changes in the energy loss region <2 eV, whose features mostly result from the hopping nature of 5d electrons in the honeycomb lattice. These changes are ascribed to modulations of the Ir-to-Ir inter-site transition scattering efficiency, which we associate to a transient screening of the on-site Coulomb interaction., Competing Interests: The authors have no conflicts to disclose., (© 2024 Author(s).)

The time- and angle-resolved photoemission spectroscopy (trARPES) allows for direct mapping of the electronic band structure and its dynamic response on femtosecond timescales. Here, we present a new ARPES system, powered by a new fiber-based femtosecond light source in the vacuum ultraviolet range, accessing the complete first Brillouin zone for most materials. We present trARPES data on Au(111), polycrystalline Au, Bi2Se3, and TaTe2, demonstrating an energy resolution of 21 meV with a time resolution of <360 fs, at a high repetition rate of 1 MHz. The system is integrated with an extreme ultraviolet high harmonic generation beamline, enabling an excellent tunability of the time-bandwidth resolution., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)

A comprehensive microscopic description of thermally induced distortions in lead halide perovskites is crucial for their realistic applications, yet still unclear. Here, we quantify the effects of thermal activation in CsPbBr 3 nanocrystals across length scales with atomic-level precision, and we provide a framework for the description of phase transitions therein, beyond the simplistic picture of unit-cell symmetry increase upon heating. The temperature increase significantly enhances the short-range structural distortions of the lead halide framework as a consequence of the phonon anharmonicity, which causes the excess free energy surface to change as a function of temperature. As a result, phase transitions can be rationalized via the soft-mode model, which also describes displacive thermal phase transitions in oxide perovskites. Our findings allow to reconcile temperature-dependent modifications of physical properties, such as changes in the optical band gap, that are incompatible with the perovskite time- and space-average structures.

Describing the nanoscale charge carrier transport at surfaces and interfaces is fundamental for designing high-performance optoelectronic devices. To achieve this, we employ time- and angle-resolved photoelectron spectroscopy with ultraviolet pump and extreme ultraviolet probe pulses. The resulting high surface sensitivity reveals an ultrafast carrier population decay associated with surface-to-bulk transport, which was tracked with a sub-nanometer spatial resolution normal to the surface, and on a femtosecond time scale, in the case of the inorganic CsPbBr 3 lead halide perovskite. The decay time exhibits a pronounced carrier density dependence, which is attributed via modeling to enhanced diffusive transport and concurrent recombination. The transport is found to approach an ordinary diffusive regime, limited by electron-hole scattering, at the highest excitation fluences. This approach constitutes an important milestone in our capability to probe hot-carrier transport at solid interfaces with sub-nanometer resolution in a theoretically and experimentally challenging, yet technologically relevant, high-carrier-density regime.

The development of next-generation perovskite-based optoelectronic devices relies critically on the understanding of the interaction between charge carriers and the polar lattice in out-of-equilibrium conditions. While it has become increasingly evident for CsPbBr 3 perovskites that the Pb-Br framework flexibility plays a key role in their light-activated functionality, the corresponding local structural rearrangement has not yet been unambiguously identified. In this work, we demonstrate that the photoinduced lattice changes in the system are due to a specific polaronic distortion, associated with the activation of a longitudinal optical phonon mode at 18 meV by electron-phonon coupling, and we quantify the associated structural changes with atomic-level precision. Key to this achievement is the combination of time-resolved and temperature-dependent studies at Br K and Pb L 3 X-ray absorption edges with refined ab initio simulations, which fully account for the screened core-hole final state effects on the X-ray absorption spectra. From the temporal kinetics, we show that carrier recombination reversibly unlocks the structural deformation at both Br and Pb sites. The comparison with the temperature-dependent XAS results rules out thermal effects as the primary source of distortion of the Pb-Br bonding motif during photoexcitation. Our work provides a comprehensive description of the CsPbBr 3 perovskites' photophysics, offering novel insights on the light-induced response of the system and its exceptional optoelectronic properties.

Charge transport properties of a vertically stacked organic heterojunction based on the amino-carboxylic (A-C) hydrogen bond coupling scheme are investigated by means of X-ray resonant photoemission and the core-hole clock method. We demonstrate that hydrogen bonding in molecular bilayers of benzoic acid/cysteamine (BA/CA) with an A-C coupling scheme opens a site selective pathway for ultrafast charge transport through the junction. Whereas charge transport from single BA layer directly coupled to the Au(111) is very fast and it is mediated by the phenyl group, the interposition of an anchoring layer of CA selectively hinders the delocalization of electrons from the BA phenyl group but opens a fast charge delocalization route through the BA orbitals close to the A-C bond. This evidences that hydrogen bonding established upon A-C recognition can be exploited to spatially/orbitally manipulate the charge transport properties of heteromolecular junctions.

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. This element allows flexible tuning of the driving pulse duration, providing a versatile time-resolved momentum microscopy setup featuring two operational modes designed to enhance either the energy or time resolution. We show the capabilities of the system by tracing ultrafast electron dynamics in the conduction band valleys of a bulk crystal of the 2D semiconductor WS2. Using uncompressed driving laser pulses, we demonstrate an energy resolution better than (107 ± 2) meV, while compressed pulses lead to a time resolution better than (48.8 ± 17) fs. [ABSTRACT FROM AUTHOR]

An optical parametric chirped pulse amplifier fully based on Yb lasers at 500 kHz is described. Passive optical-synchronization is achieved between a fiber laser-pumped white-light and a 515 nm pump produced with a 200 W picosecond Yb:YAG InnoSlab amplifier. An output power up to 19.7 W with long-term stability of 0.3% is demonstrated for wavelength tunable pulses between 680 nm and 900 nm and spectral stability of 0.2%; 16.5 W can be achieved with a bandwidth supporting 5.4 fs pulses. We demonstrate compression of 30 µJ pulses to sub-20 fs duration with a prism compressor, suitable for high harmonic generation.

We investigate the spin- and valley-dependent transport properties of electrons in silicene modulated by metallic gates, which can produce a potential barrier to affect the electron transport. The numerical results show that in such a silicene nanostructure the large spin polarization and valley polarization can be obtained, and they are strongly dependent on the height and width of the potential barrier. Therefore, the required degree of spin polarization and valley polarization can be realized through changing the height and/or width of the potential barrier. This valuable discovery well reveals the spin- and valley-dependent electron transport mechanism in such a silicene and is helpful for designing new kinds of spintronic and valleytronic devices modulated by metallic gates. [ABSTRACT FROM AUTHOR]

The Chinese Academy of Engineering Physics Terahertz Free Electron Laser Facility (CAEP THz FEL, CTFEL) is the only high-average power free electron laser terahertz source based on superconducting accelerators in China. The update of the CTFEL is now undergoing and will expand the frequency range from 0.1–4.2 THz to 0.1–125 THz. Two experimental stations for material spectroscopy and biomedicine will be built. A high harmonic generation (HHG) lightsource based beamline at the material spectroscopy experimental station for time-resolved angle-resolved photoemission spectroscopy (ARPES) research will be constructed and the optical design is presented. The HHG lightsource covers the extreme ultraviolet (XUV) photon energy range of 20–50 eV. A Czerny–Turner monochromator with two plane gratings worked in conical diffraction configuration is employed to maintain the transmission efficiency and preserve the pulse time duration. The calculated beamline transmission efficiency is better than 5% in the whole photon energy range. To our knowledge, this is the first time in China to combine THz-infrared FEL with HHG light source, and this experimental station will be a powerful and effective instrument that will give new research opportunities in the future for users doing research on the dynamic evolution of the excited electron band structure of a material's surface. [ABSTRACT FROM AUTHOR]

The carbon dioxide (CO2) conversion to useable compounds remains a great contest to scientists, engineers, and environmentalists with regard to the reverse of the oxidative degradation of organics. This conversion is essential for the development of complementary fuels and raw materials for various industries, which in turn will help in avoiding the drastic increase in tropospheric temperature due to greenhouse effect leading to global warming. The solar energy is the earth's essential power source along with the other various forms of energy for example fossil fuels, hydropower, wind, and biomaterials, etc. The final goal is to establish the artificial photosynthesis, which can be replicated thru various chemical reduction techniques of CO2 by employing appropriate photo-, thermal- and electro-catalysts in order to produce different one carbon atom (C1) and higher carbon atoms containing products. Besides, the utilization of clean and sustainable CO2 towards high-value products is of great interest today due to the recognized environmental worries and subsequent lessening of the fossil fuels utilization load to meet the energy demand of mankind. This way, solar energy can directly and/or indirectly be altered and stored in chemical energy form for industrial as well as societal applications. In this article our endeavor is to summarize the advances in CO2 chemical reduction research area till date especially in free radical-based methods such as electrochemical, photochemical and plasma chemical for the development of carbon species up to two carbon (C2) atoms containing products perceived in the chemical reduction of CO2. The author hopes that this piece of work will be helpful to researchers and readers who are focused on the field of CO2. [ABSTRACT FROM AUTHOR]