Journal of Electron Spectroscopy and Related Phenomena最新文献

In this research, electronic and optical properties of armchair (7,7), zigzag (7,0), and chiral (4,2) configurations of Single-Walled Carbon Nanotubes (SWCNT) and the effect of spin-orbit coupling (SOC) on their electronic structures were studied with density functional theory (DFT) computing. The armchair, zigzag, and chiral SWCNT structures were built using the CASTEP software. Then, this code was used to calculate the band structures, density of states and optical properties of these systems. Electronic and optical properties of SWCNT material could be influenced by its configuration, such as the bandgap energy, total density of states (TDOS) and partial density of states (PDOS), absorption coefficient, dielectric function, optical conductivity, complex refractive index, and the loss function. In the absence or presence of SOC effect, armchair, zigzag and chiral nanotubes are semiconductors. SOC causes the bandgap energy to increase and the TDOS of "armchair, zigzag, and chiral SWCNTs" to alter. These results provide crucial physical information regarding the control of the electronic properties of SWCNTs using SOC.

We report a scanning transmission X-ray microscopy (STXM) study of hematite nanorods, prototypical photoanode used in solar water splitting. Hematite nanorods were obtained by hydrothermal growth from aqueous solutions using FeCl₃ as precursor. Potentials for onset of water splitting are smaller using this synthesis method, compared to values reported for hematite photoanodes obtained by epitaxial growth. STXM revealed the presence of a hexahydrate iron chloride phase at the surface of the nanorods, which is linked to the low onset potential values. We detail the quantification approach that revealed the specific microstructure of individual hematite nanorods.

We develop a software package SPADExp (simulator of photoemission angular distribution for experiments) to calculate the photoemission angular distribution (PAD), which is the momentum dependence of spectrum intensity in angle-resolved photoemission spectroscopy (ARPES). The software can directly load the output of the first-principles software package OpenMX, so users do not need to construct tight-binding models as previous studies did for PAD calculations. As a result, we can calculate the PADs of large systems such as quasicrystals and slab systems. We calculate the PADs of sublattice systems (graphene and graphite) to reproduce characteristic intensity distributions, which ARPES has experimentally observed. After that, we investigate twisted bilayer graphene, a quasicrystal showing 12-fold rotational symmetric spectra in ARPES, and the surface states of the topological insulator ${\mathrm{Bi}}_2{\mathrm{Se}}_3$. Our calculations show good agreement with previous ARPES measurements, showing the correctness of our calculation software and further potential to investigate the photoemission spectra of novel quantum materials.

This article reviews the application of near-edge X-ray absorption fine structure (NEXAFS) spectroscopy to characterization of self-assembled monolayers (SAMs) which are an important part of modern nanotechnology, being particular useful in context of surface and interface engineering. NEXAFS spectroscopy provides information about the electronic structure of the SAMs, which allows to recognize specific functional groups and building blocks of the SAM-forming molecules. Due to the linear dichroism effects in X-ray absorption, this technique is also capable to give insight into orientational order and molecular orientation in the SAMs, both overall and building-block-specific. To illustrate the above points, a variety of representative examples for different classes of SAMs is provided, accompanied by the information about the general aspects of the technique and the description of suitable data evaluation procedures. Finally, it is shown that the application of NEXAFS spectroscopy to SAMs is not only limited by their characterization but is also useful to monitor chemical and physical processes involving these systems.

With the advent of ambient pressure X-ray excited electron spectroscopy, near-edge X-ray absorption fine structure spectroscopy is widely used to investigate the hydrogen-bonding environment in aqueous solutions, ice, and adsorbed water. When Auger-Meitner electrons are detected, the method becomes inherently surface-sensitive because of the limited escape depth of electrons. In such X-ray absorption experiments with aqueous samples, gas-phase water is inevitably present. It impacts the acquired spectra in two ways: (1) Absorption along the X-ray path upstream of the sample reduces the photon flux reaching the condensed phase. (2) Spectra originating from gas-phase water in front of the analyzer contribute to the recorded spectra. Here, we develop and discuss a procedure to disentangle the gas-phase and condensed-phase contribution in the acquired spectra. A novel approach to quantify and remove the gas-phase contribution allows receiving condensed-phase near-edge X-ray absorption fine structure spectra at high water vapor pressure free of gas-phase artifacts.

The typical output of a STXM (Scanning Transmission X-ray (spectro)Microscopy) measurement is a data cube consisting of a set of images (measurements of X-ray transmission at a grid of pixels) taken at a sequence of incident energies. As with any experimental measurement, this raw data must be reduced to some standard form and interpreted. In this paper, I review the basics of how to go from raw data to information about the sample. I will discuss the fundamentals of X-ray spectromicroscopy, data reduction, descriptive and model-based analysis, and available software, with examples taken from the literature.

In this work, we discuss the possibility of improving charge neutralization in near ambient pressure X-ray photoelectron spectroscopy by co-irradiating the sample with He I photons of 21.2 eV. This UV-enhanced neutralization of charges is a variation of the so-called environmental charge compensation, which uses the electrons produced by the photoionization of the ambient gas to neutralize the positive charges built at the sample surface. Adding an additional ionization source generates more charges at the sample but also larger amounts of electrons available for neutralization. The final surface charge equilibrium depends on different aspects of the experiment, such as the sample composition and geometry, the total ionization cross sections of the gas compared to the surface materials, the gas used, the luminosity and spot size of the sources used for photoionization, and the energy of the electrons present in the gas phase. Here we illustrate the efficiency of the UV-enhanced neutralization using three different dielectric samples with different geometries (a porous SiO₂ monolith with an irregular surface, a flat mica sample, and a thin SiO₂ film deposited onto a Si substrate), different X-ray spot sizes, and two different gases (N₂ and Ar). The effect of biasing on the efficiency of the sample surface to attract electrons produced in the gas phase is also discussed.

The use of carbon nitride-based materials and light to drive catalytic water splitting has enormous potential for the production of hydrogen. Revealing the processes of molecular conjugation, nucleation, and crystallization in crystalline carbon nitride is expected to enhance the photocatalytic activity through the creation of isotype heterojunctions and active sites. In this work, the addition of cobalt salts in ionothermal synthesis was found to promote the phase transition of heptazine-based crystalline carbon nitride (CCN) to triazine-based poly (triazine imide) (PTI), resulting in the formation of a single-atom cobalt-doped coordinated isotype CCN/PTI heterojunction. The new hybrid orbital modulates the atomic/electronic structure and the band gap of the CCN/PTI heterojunction, and synergistically increases the absorption of visible light, accelerating the separation and transfer of photoexcited electrons and holes. Synchrotron-based X-ray spectroscopy and microscopy are used to identify the origin of the improved performance of the single-atom cobalt-doped CCN/PTI heterojunction in the photocatalytic hydrogen evolution reaction. This work demonstrates that synchrotron X-ray spectroscopy is a promising tool for designing materials aimed at enhancing photocatalytic activity in solar energy conversion applications.