Search Results (16)

Angle-resolved photoemission spectroscopy (ARPES) clearly resolves surface-localized (SL) states, yet conventional density functional theory (DFT) band structures from slab calculations do not readily distinguish weakly confined SL states on surfaces such as Al(001), as traditional layer-threshold criteria fail for surfaces with long surface-state decay lengths. We establish a dual-criterion scheme using the surface ratio R and the localization integral L weighted by the inelastic mean free path (IMFP) to quantitatively distinguish SL states: R quantifies the surface-projected charge fraction, while L incorporates the photoelectron IMFP to mimic ARPES surface sensitivity, both evaluated within a fully converged 81-layer Al(001) slab that eliminates artificial inter-surface coupling. Band structures color-coded by R and L intuitively highlight SL states as bright yellow-white bands against red bulk backgrounds. Our calculations show that continuum SL features arise from multi-band hybridization (sharp surface resonances). Notably, R and L alone cannot separate absolute surface states from resonances. All DFT calculations were performed using the PBEsol exchange-correlation functional within the GGA framework, the PAW formalism, and an 81-layer Al(001) slab model. This work reveals the electronic nature of surface features on Al(001) and provides a quantitative SL-state identification tool that is conceptually transferable to other crystalline surfaces. Full article

The family of BiS₂-based superconductors has attracted considerable attention since their discovery in 2012 due to the unique structural and electronic properties of these materials. Several experimental and theoretical studies have been performed to explore the basic properties and the underlying mechanism for superconductivity. In this review, we discuss the current understanding of pairing symmetry in BiS₂-based superconductors and particularly the role of point-contact spectroscopy in unravelling the mechanism underlying the superconducting state. We also review experimental results obtained with different techniques including angle-resolved photoemission spectroscopy, scanning tunnelling spectroscopy, specific heat measurements, and nuclear magnetic resonance spectroscopy. The integration of experimental results and theoretical predictions sheds light on the complex interplay between electronic correlations, spin fluctuations, and Fermi surface topology in determining the coupling mechanism. Finally, we highlight recent advances and future directions in the field of BiS₂-based superconductors, underlining the potential technological applications. Full article

VO₂ is one of the most studied vanadium oxides because it undergoes a reversible metal-insulator transition (MIT) upon heating with a critical temperature of around 340 K. One of the most overlooked aspects of VO₂ is the band’s anisotropy in the metallic phase when the Fermi level is crossed by two bands: π* and d_||. They are oriented perpendicularly in one respect to the other, hence generating anisotropy. One of the parameters tuning MIT properties is the unbalance of the electron population of π* and d_|| bands that arise from their different energy position with respect to the Fermi level. In systems with reduced dimensionality, the electron population disproportion is different with respect to the bulk leading to a different anisotropy. Investigating such a system with a band-selective spectroscopic tool is mandatory. In this manuscript, we show the results of the investigation of a single crystalline 8 nm VO₂/TiO₂(101) film. We report on the effectiveness of linearly polarized resonant photoemission (ResPES) as a band-selective technique probing the intrinsic anisotropy of VO₂. Full article

The discovery of high-$T_c$ superconductivity in cuprates in 1986 moved strongly correlated systems from exotic worlds interesting only for pure theorists to the focus of solid-state research. In recent decades, the majority of hot topics in condensed matter physics (high-$T_c$ superconductivity, colossal magnetoresistance, multiferroicity, ferromagnetism in diluted magnetic semiconductors, etc.) have been related to strongly correlated transition metal compounds. The highly successful electronic structure calculations based on density functional theory lose their predictive power when applied to such compounds. It is necessary to go beyond the mean field approximation and use the many-body theory. The methods and models that were developed for the description of strongly correlated systems are reviewed together with the examples of response function calculations that are needed for the interpretation of experimental information (inelastic neutron scattering, optical conductivity, resonant inelastic X-ray scattering, electron energy loss spectroscopy, angle-resolved photoemission, electron spin resonance, and magnetic and magnetoelectric properties). The peculiarities of (quasi-) 0-, 1-, 2-, and 3- dimensional systems are discussed. Full article

Diffraction of photoelectrons emitted from the core 1s and valence band of monolayer and bilayer graphene is studied within the one-step theory of photoemission. The energy-dependent angular distribution of the photoelectrons is compared to the simulated electron reflection pattern of a low-energy electron diffraction experiment in the kinetic energy range up to about 55 eV, and the implications for the structure determination are discussed. Constant energy contours due to scattering resonances are well visible in photoelectron diffraction, and their experimental shape is well reproduced. The example of the bilayer graphene is used to reveal the effect of the scattering by the subsurface layer. The photoemission and LEED patterns are shown to contain essentially the same information about the long-range order. The diffraction patterns of C $1s$ and valence band photoelectrons bear similar anisotropy and are equally suitable for diffraction analysis. Full article

The effect of localized plasmon on the photoemission and absorption in hybrid molybdenum disulfide-Gallium nitride (MoS₂-GaN) heterostructure has been studied. Localized plasmon induced by platinum nanoparticles was resonantly coupled to the bandedge states of GaN to enhance the UV emission from the hybrid semiconductor system. The presence of the platinum nanoparticles also increases the effective absorption and the transient gain of the excitonic absorption in MoS₂. Localized plasmons were also resonantly coupled to the defect states of GaN and the exciton states using gold nanoparticles. The transfer of hot carriers from Au plasmons to the conduction band of MoS₂ and the trapping of excited carriers in MoS₂ within GaN defects results in transient plasmon-induced transparency at ~1.28 ps. Selective optical excitation of the specific resonances in the presence of the localized plasmons can be used to tune the absorption or emission properties of this layered 2D-3D semiconductor material system. Full article

The valence band photoemission (VB PE) spectra of the [Ni(Salen)] molecular complex were measured by ultraviolet, soft X-ray and resonant photoemission (ResPE) using photons with energies ranging from 21.2 eV to 860 eV. It was found that the Ni 3d atomic orbitals’ (AOs) contributions are most significant for molecular orbitals (MOs), which are responsible for the low-energy PE band at a binding energy of 3.8 eV in the VB PE spectra. In turn, the PE bands in the binding energies range of 8–16 eV are due to the photoionization of the MOs of the [Ni(Salen)] complex with dominant contributions from C 2p AOs. A detailed consideration was made for the ResPE spectra obtained using photons with absorption resonance energies in the Ni 2p_3/2, N 1s, and O 1s Near-Edge X-ray Absorption Fine Structure (NEXAFS) spectra. A strong increase in the intensity of the PE band ab was found when using photons with an energy 854.4 eV in the Ni 2p_3/2 NEXAFS spectrum. This finding is due to the high probability of the participator-Auger decay of the Ni 2p_3/2⁻¹3d⁹ excitation and confirms the relationship between the PE band ab with the Ni 3d-derived MOs. Full article

Bismuth compounds are of growing interest with regard to potential applications in catalysis, medicine, and electronics, for which their environmentally benign nature is one of the key factors. One thing that currently hampers the further development of bismuth oxido-based materials, however, is the often low solubility of the precursors, which makes targeted immobilisation on substrates challenging. We present an approach towards the solubilisation of bismuth oxido clusters by introducing an amino carboxylate as a functional group. For this purpose, the bismuth oxido cluster [Bi₃₈O₄₅(NO₃)₂₀(dmso)₂₈](NO₃)₄·4dmso (dmso = dimethyl sulfoxide) was reacted with the sodium salt of tert-butyloxycabonyl (Boc)-protected phenylalanine (L-Phe) to obtain the soluble and chiral nanocluster [Bi₃₈O₄₅(Boc–Phe–O)₂₄(dmso)₉]. The exchange of the nitrates by the amino carboxylates was proven by nuclear magnetic resonance, Fourier-transform infrared spectroscopy, as well as elemental analysis and X-ray photoemission spectroscopy. The solubility of the bismuth oxido cluster in a protic as well as an aprotic polar organic solvent and the growth mode of the clusters upon spin, dip, and drop coating on gold surfaces were studied by a variety of microscopy, as well as spectroscopic techniques. In all cases, the bismuth oxido clusters form crystalline agglomerations with size, height, and distribution on the substrate that can be controlled by the choice of the solvent and of the deposition method. Full article

Angle-resolved photoemission from monolayer and bilayer graphene is studied based on an ab initio one-step theory. The outgoing photoelectron is represented by the time-reversed low energy electron diffraction (LEED) state ${\mathsf{\Phi }}_{\mathrm{LEED}}^{*}$, which is calculated using a scattering theory formulated in terms of augmented plane waves. A strong enhancement of the emission intensity is found to occur around the scattering resonances. The effect of the photoelectron scattering by the underlying substrate on the polarization dependence of the photocurrent is discussed. The constant initial state spectra $I({\mathbf{k}}_{\left|\right|},\hslash \omega )$ are compared to electron transmission spectra $T\left(E\right)$ of graphene, and the spatial structure of the outgoing waves is analyzed. It turns out that the emission intensity variations do not correlate with the structure of the $T\left(E\right)$ spectra and are caused by rather subtle interference effects. Earlier experimental observations of the photon energy and polarization dependence of the emission intensity $I({\mathbf{k}}_{\left|\right|},\hslash \omega )$ are well reproduced within the dipole approximation, and the Kohn–Sham eigenstates are found to provide a quite reasonable description of the photoemission final states. Full article

The VO₂ is a 3d¹ electron system that undergoes a reversible metal–insulator transition (MIT) triggered by temperature and characterized by an interplay between orbital, charge and lattice degrees of freedom. The characterization of the MIT features are therefore extremely challenging and powerful investigation tools are required. In this work, we demonstrate how a combination of resonant photoemission and constant initial state (CIS) spectroscopy can be used as an orbital selective probe of the MIT studying three different VO₂/TiO₂(001) strained films. The CIS spectra of the V 3d and V 3p photo-electrons shows sensitivity to different orbital contribution and the presence of a spin polarized band close to the Fermi level. Full article

In this work a new concept of silicon resonant cavity enhanced photodetector working at 1550 nm has been theoretically investigated. The absorption mechanism is based on the internal photoemission effect through a graphene/silicon Schottky junction incorporated into a silicon-based Fabry–Pérot optical microcavity whose input mirror is constituted by a double silicon-on-insulator substrate. As output mirror we have investigated two options: a distributed Bragg reflector constituted by some periods of silicon nitride/hydrogenated amorphous silicon and a metallic gold reflector. In addition, we have investigated and compared two configurations: one where the current is collected in the transverse direction with respect to the direction of the incident light, the other where it is collected in the longitudinal direction. We show that while the former configuration is characterized by a better responsivity, spectral selectivity and noise equivalent power, the latter configuration is superior in terms of bandwidth and responsivity × bandwidth product. Our results show responsivity of 0.24 A/W, bandwidth in GHz regime, noise equivalent power of 0.6 nW/cm√Hz and full with at half maximum of 8.5 nm. The whole structure has been designed to be compatible with silicon technology. Full article

The purpose of this work is the structural analysis of graphene oxide (GO) and by means of a new structural model to answer the questions arising from the Lerf–Klinowski and the Lee structural models. Surface functional groups of GO layers and the oxidative debris (OD) stacked on them were investigated after OD was extracted. Analysis was performed successfully using Fourier transform infrared spectroscopy (FTIR), ultraviolet-visible spectroscopy (UV-Vis), X-ray photoemission spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDX), Raman spectroscopy, solid-state nuclear magnetic resonance spectroscopy (SSNMR), standardized Boehm potentiometric titration analysis, elemental analysis, X-ray diffraction (XRD), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The analysis showed that graphene oxide layers, as well as oxidative debris contain different functional groups such as phenolic –OH, ketone, lactone, carboxyl, quinone and epoxy. Based on these results, a new structural model for GO layers is proposed, which covers all spectroscopic data and explains the presence of the other oxygen functionalities besides carboxyl, phenolic –OH and epoxy groups. Full article

This paper investigates the reliability of blue-emitting phosphors for Near-UV (NUV) laser excitation. By means of a series of thermal stress experiments, and of stress under high levels of optical excitation, we have been able to identify the physical process responsible for the degradation of Eu²⁺-activated alkaline-earth halophosphate phosphors under typical and extreme operating conditions. In particular, for temperatures equal to or greater than 450 °C the material exhibited a time-dependent drop in the Photo-Luminescence (PL), which was attributed to the thermally induced ionization of the Eu²⁺ optically active centers. Several analytical techniques, including spatially and spectrally resolved PL, Electron Paramagnetic Resonance (EPR) and X-ray Photo-emission Spectroscopy (XPS) were used to support this hypothesis and to gain insight on the degradation process. By means of further tests, evidence of this degradation process was also found on samples stressed under a relatively low power density of 3 W/mm² at 405 nm. This indicated that the optically (and thermally) induced ionization of the optically active species is the most critical degradation process for this family of phosphorescent material. The operating limits of a second-generation Eu-doped halophosphate phosphor were also investigated by means of short-term stress under optical excitation. The experimental data showed that a threshold excitation intensity for continuous pumping exists. Above this threshold, decay of the steady-state PL performance and non-recoverable degradation of the material were found to take place. This behavior is a consequence of the extremely harsh excitation regime, mainly due to the thermal management capabilities of the substrate material employed for our experimental purposes rather than from intrinsic properties of the phosphors. Full article

A variety of processes originating from the interaction of atomic or molecular N-electron states with strong and/or hypershort radiation pulses can be understood quantitatively only by first determining with good accuracy the solutions of the many-electron time-dependent Schrödinger equation (METDSE) that describe the corresponding physics. The METDSE is solvable nonperturbatively via the state-specific expansion approach (SSEA). SSEA solutions have been used, or can be used, for quantitative explanation and numerically reliable predictions of quantities that have been measured or are measurable in modern laser-driven experiments that can track, with hypershort (attosecond) time resolution, the effects of electron rearrangements in atoms and molecules. The calculations take into account in a transparent way the interplay between the phenomena and the electronic structures of the physically significant states in discrete and multichannel continuous spectra, including multiply- and inner-hole–excited resonance states. The discussion focuses on novel topics of time-resolved many-electron physics and includes a comparison of our predictions to recent quantitative measurements of attosecond-resolved generation of the profile of the ${(2s2p)}^1{P}^o$ doubly excited resonance state of helium during photoionization and of the relative time delay in photoemission of the (2s,2p) electrons of neon. Full article

Among transition metal oxides, VO₂ is a particularly interesting and challenging correlated electron material where an insulator to metal transition (MIT) occurs near room temperature. Here we investigate a 16 nm thick strained vanadium dioxide film, trying to clarify the dynamic behavior of the insulator/metal transition. We measured (resonant) photoemission below and above the MIT transition temperature, focusing on heating and cooling effects at the vanadium L₂₃-edge using X-ray Absorption Near-Edge Structure (XANES). The vanadium L₂₃-edges probe the transitions from the 2p core level to final unoccupied states with 3d orbital symmetry above the Fermi level. The dynamics of the 3d unoccupied states both at the L₃- and at the L₂-edge are in agreement with the hysteretic behavior of this thin film. In the first stage of the cooling, the 3d unoccupied states do not change while the transition in the insulating phase appears below 60 °C. Finally, Resonant Photoemission Spectra (ResPES) point out a shift of the Fermi level of ~0.75 eV, which can be correlated to the dynamics of the 3d_// orbitals, the electron–electron correlation, and the stability of the metallic state. Full article