The Turkish Soft X-ray Photoelectron Spectroscopy (TXPES) beamline project at the Synchrotron-light for Experimental Science and Applications in the Middle East (SESAME) synchrotron, led by Turkish Energy Nuclear and Mineral Research Agency (TENMAK) is an important development as it marks SESAME’s first beamline fully designed, manufactured, and installed by a member country, Turkiye in 2025. TXPES will be installed on the free branch of the Helmholtz-SESAME Soft X-Ray Beamline (HESEB) and will share the same photon source and monochromator. The beamline will provide tunable photon energies ranging from 90 eV to 1800 eV for detailed analysis of the electronic structure and chemical bonding of materials. The end station supports techniques such as X-ray Photoelectron Spectroscopy (XPS), Ultraviolet Photoelectron Spectroscopy (UPS) and Low-Energy Ion Scattering (LEIS), thanks to advanced tools like the PHOIBOS 150 Complementary Metal-Oxide-Semiconductor (CMOS) XPS/LEIS/UPS Analyzer. With its versatile design and High-Pressure Cell (HPC), the TXPES system offers exceptional surface sensitivity, spatial resolution, and energy resolution, making it ideal for interdisciplinary research in physics, chemistry, materials science, and engineering.
The ID11-L HESEB Soft X-ray beamline and end station significantly enhance soft X-ray research capabilities. Operating in an energy range of 90–1800 eV, extendable to 70–2000 eV, the beamline achieves high performance with an energy resolution of E/ΔE > 8000 and a photon flux of 10 10 to 3.4 × 10 12 photons/s. Its 500 × 250 µm 2 beam spot size allows for precise measurements, including studies on magnetic materials using variable circular polarization. This paper presents the end station’s design, including the receptacle, magnetic sample holder, and ambient pressure capabilities, along with experimental results that demonstrate the beamline’s potential for diverse scientific applications.
Photoemission from a solid surface provides a wealth of information about the electronic structure of the surface and its dynamic evolution. Ultrafast pump-probe experiments are particularly useful to study the dynamic interactions of photons with surfaces as well as the ensuing electron dynamics induced by these interactions. Time-resolved laser-assisted photoemission (tr-LAPE) from surfaces is a novel technique to gain deeper understanding of the fundamentals underlying the photoemission process. Here, we present the results of a femtosecond time-resolved soft X-ray photoelectron spectroscopy experiment on two different metal surfaces conducted at the X-ray Free-Electron Laser FLASH in Hamburg. We study photoemission from the W 4f and Pt 4f core levels using ultrashort soft X-ray pulses in combination with synchronized infrared (IR) laser pulses. When both pulses overlap in time and space, laser-assisted photoemission results in the formation of a series of sidebands that reflect the dynamics of the laser-surface interaction. We demonstrate a qualitatively new level of sideband generation up to the sixth order and a surprising material dependence of the number of sidebands that has so far not been predicted by theory. We provide a semi-quantitative explanation of this phenomenon based on the different dynamic dielectric responses of the two materials. Our results advance the understanding of the LAPE process and reveal new details of the IR field present in the surface region, which is determined by the dynamic interplay between the IR laser field and the dielectric response of the metal surfaces.
A surface photovoltage (SPV) is observed whenever a doped semiconductor with non-negligible band bending is illuminated by light and charge carriers are excited across the band gap. The sign of the SPV depends on the nature of the doping, the amplitude of the SPV increases with the fluence of the light illumination up to a saturation value, which is determined by the doping concentration. We have investigated Si(100) samples with well-characterized doping levels over a wide range of illumination fluences. Surprisingly, the sign of the SPV upon illumination with 532 nm photons reverses for some p-doping concentrations at high fluences. This is a new effect associated with a crossover between electronic excitations in the bulk and at the surface of the semiconductor.
A 790-nm-driven high-harmonic generation source with a repetition rate of 6 kHz is combined with a toroidal-grating monochromator and a high-detection-efficiency photoelectron time-of-flight momentum microscope to enable time- and momentum-resolved photoemission spectroscopy over a spectral range of 23.6-45.5 eV with sub-100 fs time resolution. Three-dimensional (3D) Fermi surface mapping is demonstrated on graphene-covered Ir(111) with energy and momentum resolutions of ≲100 meV and ≲0.1 Å-1, respectively. The tabletop experiment sets the stage for measuring the kz-dependent ultrafast dynamics of 3D electronic structure, including band structure, Fermi surface, and carrier dynamics in 3D materials as well as 3D orbital dynamics in molecular layers.
SESAME and a consortium of five Helmholtz Centers are designing and installing a state-of-the-art soft X-Ray undulator beamline at the SESAME light source in Amman, Jordan. Funding is provided by the Helmholtz Association over a four year project cycle that started in January 2019. This is an interim report covering the first 36 months of the project where the construction and installation has been almost completed and commissioning and characterization of the beamline is about to start. Additionally, seminars, workshops, and a training program are part of the project aimed at establishing a broad user community.
We report a high-resolution angle-resolved photoemission (ARPES) study of the prototypical nearly-free-electron metal sodium. The observed mass enhancement is slightly smaller than that derived in previous studies. The new results on the lifetime broadening increase the demand for theories beyond the random phase approximation. Our results do not support the proposed strong enhancement of the scattering rates of the charge carriers due to a coupling to spin fluctuations. Moreover, a comparison with earlier electron energy-loss data on sodium yields a strong reduction of the mass enhancement of dipolar electron-hole excitations compared to that of monopole hole excitations, measured by ARPES.
We present a novel technique to monitor dynamics in interfacial systems through temporal correlations in x-ray photoelectron spectroscopy (XPS) signals. To date, the vast majority of time-resolved x-ray spectroscopy techniques rely on pump–probe schemes, in which the sample is excited out of equilibrium by a pump pulse, and the subsequent dynamics are monitored by probe pulses arriving at a series of well-defined delays relative to the excitation. By definition, this approach is restricted to processes that can either directly or indirectly be initiated by light. It cannot access spontaneous dynamics or the microscopic fluctuations of ensembles in chemical or thermal equilibrium. Enabling this capability requires measurements to be performed in real (laboratory) time with high temporal resolution and, ultimately, without the need for a well-defined trigger event. The time-correlation XPS technique presented here is a first step toward this goal. The correlation-based technique is implemented by extending an existing optical-laser pump/multiple x-ray probe setup by the capability to record the kinetic energy and absolute time of arrival of every detected photoelectron. The method is benchmarked by monitoring energy-dependent, periodic signal modulations in a prototypical time-resolved XPS experiment on photoinduced surface-photovoltage dynamics in silicon, using both conventional pump–probe data acquisition, and the new technique based on laboratory time. The two measurements lead to the same result. The findings provide a critical milestone toward the overarching goal of studying equilibrium dynamics at surfaces and interfaces through time correlation-based XPS measurements.
The ultrafast dynamics of photon-to-charge conversion in an organic light-harvesting system is studied by femtosecond time-resolved X-ray photoemission spectroscopy (TR-XPS) at the free-electron laser FLASH. This novel experimental technique provides site-specific information about charge separation and enables the monitoring of free charge carrier generation dynamics on their natural timescale, here applied to the model donor-acceptor system CuPc:C60. A previously unobserved channel for exciton dissociation into mobile charge carriers is identified, providing the first direct, real-time characterization of the timescale and efficiency of charge generation from low-energy charge-transfer states in an organic heterojunction. The findings give strong support to the emerging realization that charge separation even from energetically disfavored excitonic states is contributing significantly, indicating new options for light harvesting in organic heterojunctions.
Electronic and lattice contributions to transient X-ray absorption spectra of CuO are analyzed using picosecond time-resolved and temperature-dependent measurements. Super-bandgap excitation with 355 nm and 532 nm laser pulses leads to significantly different trends.
The success of many emerging molecular electronics concepts hinges on an atomistic understanding of the underlying electronic dynamics. We employ picosecond time-resolved x-ray photoemission spectroscopy (tr-XPS) to elucidate the roles of singlet and triplet excitons for photoinduced charge generation at a copperphthalocyanine-C-60 heterojunction. Contrary to common belief, fast intersystem crossing to triplet excitons after photoexcitation is not a loss channel but contributes to a significantly larger extent to the time-integrated interfacial charge generation than the initially excited singlet excitons. The tr-XPS data provide direct access to the diffusivity of the triplet excitons D-CuPc= (1.8 +/- 1.2) x 10(-5) cm(2)/s (where CuPc is copper-phthalocyanine) and their diffusion length Lin(diff) = (8 +/- 3) nm.
Electronic and lattice contributions to picosecond time-resolved X-ray absorption spectra (trXAS) of CuO at the oxygen K-edge are analyzed by comparing trXAS spectra, recorded using excitation wavelengths of 355 nm and 532 nm, to steady-state, temperature-dependent XAS measurements. The trXAS spectra at pump-probe time-delays ≥150 ps are dominated by lattice heating effects. Insight into the temporal evolution of lattice temperature profiles on timescales up to 100s of nanoseconds after laser excitation are reported, on an absolute temperature scale, with a temporal sensitivity and a spatial selectivity on the order of 10s of picoseconds and 10s of nanometers, respectively, effectively establishing an "ultrafast thermometer". In particular, for the 532 nm experiment at ∼5 mJ cm-2 fluence, both the initial sample temperature and its dynamic evolution are well captured by a one-dimensional thermal energy deposition and diffusion model. The thermal conductivity k = (1.3 ± 0.4) W m-1 K-1 derived from this model is in good agreement with the literature value for CuO powder, kpowder = 1.013 W m-1 K-1. For 355 nm excitation, a quantitative analysis of the experiments is hampered by the large temperature gradients within the probed sample volume owing to the small UV penetration depth. The impact of the findings on mitigating or utilizing photoinduced lattice temperature changes in future X-ray free electron laser (XFEL) experiments is discussed.
Photo-induced charge carrier dynamics and transient interfacial fields at the interface between N3 polypyridine complexes and films of nanocrystalline ZnO are probed by picosecond time-resolved X-ray photoelectron spectroscopy.
At the Metrology Light Source (MLS), the compact electron storage ring of the Physikalisch-Technische Bundesanstalt (PTB) with a circumference of 48 m, a specific operation mode with two stable closed orbits for stored electrons was realized by transverse resonance island buckets. One of these orbits is closing only after three turns. In combination with single-bunch operation, the new mode was applied for electron time-of-flight spectroscopy with an interval of the synchrotron radiation pulses which is three times the revolution period at the MLS of 160 ns. The achievement is of significant importance for PTB's future programs of angular-resolved electron spectroscopy with synchrotron radiation and similar projects at other compact electron storage rings. The scheme applied here for selecting the photons originating from a particular orbit by optical imaging has been used before in fs slicing applications and may be relevant for the BESSY VSR project of the Helmholtz-Zentrum Berlin.