Optical constants of Cu measured with reflection electron energy loss spectroscopy (REELS)

Two energy loss spectra of 1000 and 3000 eV electrons reflected from a Cu surface are analysed to give the normalized distribution of energy losses in a single surface and volume inelastic scattering process. These single scattering loss distributions are subsequently fitted to theoretical expressions for the differential inverse inelastic mean free path (DIIMFP) and differential surface excitation probability (DSEP) providing the real and imaginary part of the dielectric function in terms of a set of Drude-Lorentz oscillators. The optical constants obtained in this way are subjected to several sum rule checks and compared with other experimental data and with density-functional-theory (DFT) calculations. The present optical data agree excellently with the DFT-results, while the earlier optical data deviate significantly from these two data sets for energies below 30 eV. The mean free path for inelastic electron scattering for energies below 2000 eV is derived from the dielectric data and is found to agree satisfactorily with values reported earlier.     

Partial intensity approach for quantitative analysis of reflection-electron-energy-loss spectra

We have considered a formalism, known as partial intensity approach (PIA), previously developed to quantitatively analyze reflection electron energy loss (REEL) spectra [1,2]. The aim of the approach is, in particular, to recover the single scattering distribution of energy losses and to separate it into bulk and surface contributions, respectively referred to as the differential inverse inelastic mean free path (DIIMFP) and the differential surface excitation parameter (DSEP). As compared to [1] and [2], we have implemented a modified approach, and we have applied it to the specific geometry of the cylindrical mirror analyzer (CMA), used to acquire the REEL spectra shown here. Silicon, a material with well-defined surface and bulk plasmons, is taken as a case study to investigate the approach as a function of electron energy over the energy range typical of REELS, i.e. from 250 eV to 2 keV. Our goal is, on the one hand, to examine possible limits for the applicability of the approach and, on the other hand, to test a basic assumption of the PIA, namely that a unique DIIMFP and a unique DSEP account for REEL spectra, whatever the acquisition conditions (i.e. electron energy or angle of surface crossing) are. We find that a minimum energy exists below which the PIA cannot be applied and that the assumption of REEL spectra accounted for by unique DIIMFP and DSEP is indeed an approximation.     

Quantification of surface effects: Monte Carlo simulation of REELS spectra to obtain surface excitation parameter

The surface excitation effect is investigated by using the quantum mechanical frame work of complex self-energy of electrons which interact with a bounded semi-infinite medium. In the self-energy formalism, differential inverse inelastic mean free path (DIIMFP) has contributions from bulk and surface plasmons. Monte Carlo simulation of the interaction of electrons with a solid medium and surface has been performed. The surface excitation parameter (SEP) is then obtained from the simulated reflection electron energy loss spectroscopy (REELS) spectra. The calculated SEP results by Monte Carlo simulation are compared with the previous calculations of total surface excitation probability, which was estimated by a numerical integration of surface term of DIIMFP. The contribution merely due to surface excitations towards REELS spectra is extracted by subtracting the two Monte Carlo simulated REELS spectra that based on the two models of electron inelastic scattering, i.e. a full surface model (SM) and a pure bulk model (BM). The surface excitations found to be significant at low energy losses and diminish at higher energy losses whereas the bulk plasmon contributions show opposite behavior and are negligible at lower energy losses. The average number of surface excitations is then evaluated by the computation of ratio of the integrated surface contribution to the elastic peak. The calculated results for Ag are found to be reasonably in agreement with our previous results for total probability of surface excitations and other reported experimental data for SEP. Surface correction factor (SCF) is calculated using SEP for several metals and is compared with the reported ratio of SCF with Ni sample as reference.     

Inelastic mean free path, surface excitation parameter, and differential surface excitation parameter in Au for 300-3000 eV electrons

An analytical approach for simultaneously determining an inelastic mean free path (IMFP), a surface excitation parameter (SEP) and a differential SEP (DSEP) with absolute units was applied for the analysis of absolutely measured reflection electron energy loss spectra for Au. The IMFP, SEP and DSEP in Au for 300-3000 eV electrons are successfully obtained. The obtained DSEPs show a reasonable agreement with those theoretically calculated. The present SEPs were compared with those calculated by several empirical equations, revealing that the present SEPs are close to those calculated using the Oswald's equation. The IMFPs for Au determined by the present analysis were compared with those calculated by the TPP-2M predictive equation, revealing that the present IMFPs are in fairly good agreement with those calculated by the TPP-2M equation. The results confirmed that the present approach is effective for experimentally determining the SEP, DSEP, and IMFP for electrons in solids.     

Validity of the semi-classical approach for calculation of the surface excitation parameter

The problem of surface plasmon excitation by moving charges has been elaborated by several different approaches, mainly based on dielectric response theory within either semi-classical or quantum mechanical frameworks. In this work, a comparison of the surface excitation effect between two different frameworks is made by calculation of the differential inverse inelastic mean free path (DIIMFP) and a Monte Carlo simulation of reflection electron energy loss spectroscopy (REELS) spectra. A semi-classical modeling of the interaction between electrons and a solid surface is based on analyzing the work done by moving electrons; the stopping power and inelastic cross section are derived with the induced potential. On the other hand, a quantum mechanical approach is based on derivation of the complex inhomogeneous self-energy of the electrons. The numerical calculation shows that the semi-classical model presents almost the same values of DIIMFP as by the quantum model except at the glancing condition. The simulation of REELS spectra for Ag and SiO(2) as well as a comparison with experimental spectra also confirms that a good agreement with the spectral shape is found among the two simulation results and the experimental data.     

Reflected electron-energy-loss spectra,differential inverse inelastic mean free paths,and angular resolved X-ray photoelectron spectra of a niobium sample

A technique for recovering the differential inverse inelastic mean free paths (DIIMFP) of electrons in Nb from the reflected electron energy loss spectra (REELS) at initial energies of 5 to 40 keV using a threelayer model of the sample surface is presented. The recovered DIIMFP are used for analyzing X-ray photoelectron spectra measured at different viewing angles. Comparison with experimental data is carried out.     

Inelastic interactions of electrons with cylindrical interfaces

A theory was developed to deal with inelastic interactions for an electron moving parallel to the axis of a cylindrical structure. Formulas for the differential inverse inelastic mean free path (DIIMFP) and the total inverse inelastic mean free path (IIMFP) were derived using dielectric response theory. A sum-rule-constrained extended Drude dielectric function with spatial dispersion was applied to calculate DIIMFPs and IIMFPs for a solid wire and a cavity in solid. The calculated results showed that surface excitations occurred as the electron moved near the boundary either inside or outside the solid, whereas volume excitations arose only for electron moving inside the solid. It was found that the probability for surface excitations increases and that for volume excitations decreases for an electron moving close to the surface. Near the surface, the decrease in volume excitations is compensated by the increase in surface excitations. For a cavity in solid, the IIMFP inside the solid can be approximated by a constant value equal to the IIMFP for the infinite solid, except in the immediate vicinity of the cavity boundary.     

Surface excitation probabilities in surface electron spectroscopies

The phenomenon of surface excitation is competitive in nature for elastic and other inelastic scattering processes in surface electron spectroscopies; the knowledge of influence of surface excitations in electron energy loss spectra is then essential for quantitative surface analysis with these spectroscopies. The inelastic scattering of an electron moving in the vicinity of a surface is considered in a self-energy formalism to estimate the contribution of surface excitation in electron-solid interactions via the total surface excitation probability. The formulation uses the optical bulk dielectric function and provides the spatial and angular dependence of the differential and total inelastic cross-sections. The kinetic energy range of probing electrons considered is 100-5000 eV and the numerical evaluation of total surface excitation probabilities are performed for several metals, Au, Ag, Cu, Ni, Fe and Ti; empirical formulae for the surface excitation probability are given for each of these materials and compared with experimental results for the surface excitation parameter. The total surface excitation probability is higher in Ag as compared to other metals under consideration, for identical conditions of electron-solid interactions.     

Direct Monte Carlo simulation of scattering processes of kV electrons in aluminum; comparison of theoretical N(E) spectra with experiment

A Monte Carlo simulation of the scattering processes of kV electrons penetrating into aluminum was performed. The simulation is based on the use of different types of differential cross-sections for individual elastic and inelastic scattering: (i) Elastic scattering; the differential cross-sections derived by partial wave expansion method. (ii) Inelastic scattering; Gryzinski's excitation function for inner-shell electron excitation, Streitwolfs excitation function for conduction electron excitation, and Quinn's mean free path for plasmon excitation. For verification the energy loss spectra obtained from the Monte Carlo calculations were then compared with experiment done with commercial type Auger microprobes, JAMP-3, for angle of incidence 45° and JAMP-10 for normal incidence at primary electron energies of 1.5 and 3.0 keV, respectively. The results show satisfactory agreement between theory and experiment.     

A microscopic model analysis of the 90Zr(p,n) IAS transition

Direct reaction (p, n) data to the isobaric analogue of the ground state of ⁹⁰Zr is analysed within a DWA using a complex effective two-nucleon transition interaction, the real part of which has been used in many previous inelastic scattering analyses. Using collective model form factors in the ansatz for the imaginary part of the transition interaction and allowing for virtual resonance excitation, the differential cross sections from the scattering of 18.5–45 MeV protons are well reproduced. The parameters of the required complex interaction have a smooth energy variation similar to that required by a microscopic model analysis of proton inelastic scattering to collective states in nuclei.     

Escape probability of signal photoelectrons from non-crystalline solids: influence of anisotropy of photoemission

The escape probability of photoelectrons as a function of depth of orgin haa been studied experimentally, analytically and by the Monte Carlo (MS) technique. The depth distribution function (DDF) describing the probability for an electron emitted at a certain depth to leave a surface without being scattered inelastically has been obtained by solving a kinetic equation in the transport approximation. The analytically derived DDF is a universal function of the ratio of the inealstic to the transport mean free paths and the asymmetry parameter. In the directions of minima of the angular distribution, this function is no longer exponential, but it may be essentially nonmonotonic, reaching its maximum value at the depth comparable with the inelastic mean free path. The maximum value of the DDF exceeds its surface value by about 50% for the asymmetry parameter being equal to 2 in the emission directions close to that of X-ray propagation. Under the same conditions, the mean escape depth of electrons may be several times larger than the value predicted by the usual XPS formalism. Such behaviour of the escape probability is explained by elastic scattering of photoelectrons.The solution to the kinetic equation for a uniform target is generalized for a sample with an arbitrary depth profile and depth-dependent elastic and inelastic scattering cross-sections under the condition of the ratio of the inelastic to the transport mean free paths being independent of depth. Analytical formulas for the photoelectron yield from overlayer/substrate structure have been derived and studied in detail. The analytical predictions are compared with the experimental and Monte Carlo simulation data obtained for aluminium oxide/aluminium specimen. A satisfactory agreement is observed between the experimental and theoretical results.     

Surface excitation effects in elastic peak electron spectroscopy

Surface electron inelastic excitations, a consequence of electron-surface interaction, effect the measured intensities in surface-sensitive electron spectroscopic methods and distort the quantitative information. This phenomenon is more pronounced at low electron energy and glancing emission angles. In this work we investigate quantitatively the influence of the surface excitation effects on the measured electron elastic backscattering probability. As a model system we used Si, Cu and Al, i.e. materials with different surface excitation properties. Results obtained show that properly corrected measured elastic electron backscattering probabilities lead to inelastic mean free path values which compare well with the theory.     

蒙特卡洛方法计算材料表面激发参数

电子非弹性散射平均自由程（IMFP）是用表面电子能谱进行表面化学定量分析时极为重要的一个参数,它可以用测量的弹性峰电子能谱分析以及蒙特卡洛模拟来确定.为了更加精确地确定电子非弹性散射平均自由程,必须对弹性峰电子能谱中的表面激发效应进行修正,通常使用介电响应理论方法计算得到的表面激发参数.然而,通过理论计算得到的表面激发参数不能包含电子在材料内部输运过程中弹性散射的影响,进而影响所测的电子非弹性散射平均自由程的准确度.在这个工作中,我们采用蒙特卡洛方法来确定包含弹性散射效应时的表面激发参数.所得到的表面激发参数在不同能量、角度情况下,尤其是在弹性散射效应显著的60°以上的大角度入射、出射情况下,都与实验测量值符合得非常好.基于这些新确定的表面激发参数,可以在弹性峰电子能谱测量中获得更为准确的电子非弹性散射平均自由程数据.     

Quantitative chemical analysis by ESCA

Electron spectroscopy for chemical analysis (ESCA) can be used as a quantitative tool for the determination of the chemical composition of the surface region of a solid if certain parameters are known. The least well known is the electron mean free path. We present values of the electron mean free path for inelastic scattering as a function of energy for all elemental solids (with the exception of the rare earths and the actinides) and we give formulae for the calculation of the mean free paths for compounds. It is shown that this information makes it possible to deduce from ESCA measurements the relative concentration of atoms or molecules distributed homogeneously in the surface region of a material.     

中子与90,91,92,94Zr反应的理论计算和分析

根据中子与天然Zr及其同位素反应的总截面,去弹截面和弹性散射角分布的实验数据,得到一组普适的光学模型势参数;应用得到的光学模型势参数,光学模型,Hauser-Feshbach理论,预平衡反应的激子模型和扭曲波玻恩近似理论,系统计算和分析了中子与^90,91,92,94Zr反应的非弹散射角分布和双微分截面,理论结果与实验很好的一致.     

Deconvolution of inelastic background signal from XPS spectra of homogeneous solids

For noble and transition metals, the product of the inelastic electron mean free path and the differential inelastic scattering cross section is a weak function of both the particular metal and the electron energy. It is demonstrated that this property can be useful in the removal of inelastically scattered electrons from XPS spectra of homogeneous solids.     

Resonant inelastic contact scattering of X-ray photons on atoms and ions

The existence of an extended resonance structure outside the X-ray emission regions is theoretically predicted in the total double differential cross section for the scattering of linearly polarized photons on free atoms (ions). This structure is almost entirely determined by inelastic photon scattering of the contact type. The amplitude of the inelastic contact scattering probability is described using an analytical expression for a non-relativistic transition operator, which was previously obtained by the author outside the dipole and momentum approximations. The resonant inelastic contact scattering of X-ray photons on a neon atom and neonlike ions of argon, titanium, and iron has been studied. Calculations were performed in a nonrelativistic approximation for the wave functions of the scattering states, with allowance for many-body effects of the radial relaxation of one-electron orbitals in the Hartree-Fock field of a deep 1s vacancy and (for neon atom) the double excitation/ionization of the ground atomic state.     

Excitation of nuclear collective states by heavy ions within the model of semimicroscopic optical potential

The (semi)microscopic double-folding nucleus-nucleus optical potentials are suggested for consideration of inelastic scattering with excitation of collective nuclear states by using the adiabatic approach and the elastic scattering amplitude in the high-energy approximation. The analytical expression for inelastic scattering amplitude is obtained keeping the first-order terms in the deformation parameter of a potential. Calculations of inelastic cross sections for the ¹⁷O heavy ions scattered on different nuclei at about hundred MeV/nucleon are made, and the acceptable qualitative agreement with the experimental data is obtained without introducing free parameters. The prospect of the method for further applications is discussed. The text was submitted by the authors in English.