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.     

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.     

Comparative analysis of characteristic electron energy loss spectra and inelastic scattering cross-section spectra of Fe

The inelastic electron scattering cross section spectra of Fe have been calculated based on experimental spectra of characteristic reflection electron energy loss as dependences of the product of the inelastic mean free path by the differential inelastic electron scattering cross section on the electron energy loss. It has been shown that the inelastic electron scattering cross-section spectra have certain advantages over the electron energy loss spectra in the analysis of the interaction of electrons with substance. The peaks of energy loss in the spectra of characteristic electron energy loss and inelastic electron scattering cross sections have been determined from the integral and differential spectra. It has been shown that the energy of the bulk plasmon is practically independent of the energy of primary electrons in the characteristic electron energy loss spectra and monotonically increases with increasing energy of primary electrons in the inelastic electron scattering cross-section spectra. The variation in the maximum energy of the inelastic electron scattering cross-section spectra is caused by the redistribution of intensities over the peaks of losses due to various excitations. The inelastic electron scattering cross-section spectra have been analyzed using the decomposition of the spectra into peaks of the energy loss. This method has been used for the quantitative estimation of the contributions from different energy loss processes to the inelastic electron scattering cross-section spectra of Fe and for the determination of the nature of the energy loss peaks.     

Energy dependence of electron energy loss processes in Ge 2s photoemission

Deep core Ge 2s photoelectron spectra from polycrystalline Ge films induced by monochromatic synchrotron radiation, of 4, 6 and 8 keV were measured and analysed using two different methods, the partial intensity analysis and the extended Hüfner method to determine the spectral contributions from different electron energy loss processes due to bulk extrinsic, intrinsic and surface excitations. The obtained photon energy dependence of the ratio of these contributions was compared as a function of the photoelectron kinetic energy. It was found that the relative contribution of intrinsic excitations increase with the photon energy.     

On line shape analysis in X-ray photoelectron spectroscopy

Any solid state X-ray photoelectron spectrum (XPS) contains contributions due to multiple inelastic scattering in the bulk, surface excitations, energy losses originating from the screening of the final state hole (intrinsic losses), and, for non-monochromatized incident radiation, ghost lines originating from the X-ray satellites. In the present paper it is shown how all these contributions can be consecutively removed from an experimental spectrum employing a single general deconvolution procedure. Application of this method is possible whenever the contributions mentioned above are uncorrelated. It is shown that this is usually true in XPS to a good approximation. The method is illustrated on experimental non-monochromatized MgK spectra of Au acquired at different detection angles but for the same angle of incidence of the X-rays.     

Scattering of atomic beams by surface and bulk phonons

The general expressions obtained in a previous work are further developed to get general formulae for one-phonon scattering of atomic beams in closed form. The scattering by bulk and surface phonons are discussed separately and the respective scattered energy spectra and behaviour near the Bragg angles are carefully treated. Interesting differences are found, which may have experimental importance in separating events of scattering from different modes. The expressions for the inelastic scattering differential cross-sections obtained are applied to the experiment by Williams et al. on the He/NaF(001) system. Despite the use of estimated values for the unknown parameters, a good quantitative agreement with the experiment is obtained, and the structure observed by Williams near the specular peak is clearly explained. The contribution of transverse bulk modes is found to be about 30% of that of transverse surface modes. The contribution of longitudinal modes in smaller than the contribution of the respective transverse modes by a factor 0.01.     

Momentum‐resolved resonant inelastic X‐ray scattering on a single crystal under high pressure

A single‐crystal momentum‐resolved resonant inelastic X‐ray scattering (RIXS) experiment under high pressure using an originally designed diamond anvil cell (DAC) is reported. The diamond‐in/diamond‐out geometry was adopted with both the incident and scattered beams passing through a 1 mm‐thick diamond. This enabled us to cover wide momentum space keeping the scattering angle condition near 90°. Elastic and inelastic scattering from the diamond was drastically reduced using a pinhole placed after the DAC. Measurement of the momentum‐resolved RIXS spectra of Sr_2.5Ca_11.5Cu₂₄O₄₁ at the Cu K‐edge was thus successful. Though the inelastic intensity becomes weaker by two orders than the ambient pressure, RIXS spectra both at the center and the edge of the Brillouin zone were obtained at 3 GPa and low‐energy electronic excitations of the cuprate were found to change with pressure.     

Dispersive crystal field excitations and quadrupolar interactions in UPd3

We report inelastic neutron scattering measurements and random phase approximation calculations of the dispersive crystal field excitations of UPd(3). The measured spectra at lower energies agree with those calculated using quadrupolar interaction parameters deduced from bulk and x-ray scattering measurements. The more intense excitations arising from the hexagonal sites were used to obtain exchange parameters which proved to be anisotropic.     

Low energy electronic excitations in the layered cuprates studied by copper L3 resonant inelastic x-ray scattering

We have measured the resonant inelastic x-ray scattering (RIXS) spectra at the Cu L3 edge in a variety of cuprates. Exploiting a considerably improved energy resolution (0.8 eV) we recorded significant dependencies on the sample composition and orientation, on the scattering geometry, and on the incident photon polarization. The RIXS final states correspond to two families of electronic excitations, having local (dd excitations) and nonlocal (charge-transfer) character. The dd energy splitting can be estimated with a simple crystal field model. The RIXS at the L3 edge demonstrates here a great potential, thanks to the resonance strength and to the large 2p spin-orbit splitting.     

Dependence of the intrinsic line width of surface states on the wave vector: The Cu(111) and Ag(111) surfaces

The dependence of the intrinsic line width Γ of electron and hole states due to inelastic scattering on the wave vector k _∥ in the occupied surface state and the first image potential state on the Cu(111) and Ag(111) surfaces has been calculated using the GW approximation, which simulates the self-energy of the quasiparticles by the product of the Greens’s function and the dynamically screened Coulomb potential. Different contributions to the relaxation of electron and hole excitations have been analyzed. It has been demonstrated that, for both surfaces, the main channel of relaxation of holes in the occupied surface states is intraband scattering and that, for electrons in the image potential states, the interband transitions play a decisive role. A sharp decrease in the intrinsic line width of the hole state with an increase in k _∥ is caused by a decrease in the number of final states, whereas an increase in Γ of the image potential state is predominantly determined by an increase of its overlap with bulk states.     

Crystal field and low energy excitations measured by high resolution RIXS at the L3 edge of Cu, Ni and Mn

Resonant inelastic x-ray scattering in the soft x-ray regime has been profiting much from technical advances that have lowered considerably the instru- mental linewidth. At the ADRESS beam line of the Swiss Light Source the SAXES spectrometer can be used to measure RIXS spectra at the L edges of the 3d transition metals with unprecedented energy resolution, of the order of 100 meV for Mn, Ni and Cu. We present here some preliminary spectra on CuO, malachite, NiO, NiCl₂, MnO and LaMnO₃. The dd excitations are very well resolved allowing accurate experimental evaluation of 3d state energy splitting. The low energy scale becomes accessible opening the way to the study of collective excitations in strongly correlated electron systems, like magnons and orbitons.     

Determination of the inelastic mean free paths (IMFPs) in Ti by elastic peak electron spectroscopy (EPES): Effect of impurities and surface excitations

Surface excitations are important in surface sensitive electron spectroscopes, especially in elastic peak electron spectroscopy (EPES) since they may distort quantitative information. This phenomenon is more pronounced at low electron energy and glancing emission angles and should be appropriately corrected.In the present work we investigate quantitatively the role of contaminations, density and surface excitations on electron inelastic mean free paths (IMFPs) in Ti determined by elastic peak electron spectroscopy (EPES) using Cu standard. In the Monte Carlo algorithm the new NIST 3.1 database of electron elastic scattering cross sections was applied. It has been also shown that accounting for surface excitations, as well as for appropriate input parameters (surface composition, density, hydrogen) in the EPES method, is important for accuracy of evaluated IMFPs. Due to high reactivity of Ti, the IMFPs for contaminated Ti may be of interest. The authors indicate the magnitude of various corrections on the IMFPs derived by EPES.     

Spatial quantum beats in vibrational resonant inelastic soft x-ray scattering at dissociating states in oxygen

Resonant inelastic soft x-ray scattering (RIXS) spectra excited at the 1σ(g) → 3σ(u) resonance in gas-phase O2 show excitations due to the nuclear degrees of freedom with up to 35 well-resolved discrete vibronic states and a continuum due to the kinetic energy distribution of the separated atoms. The RIXS profile demonstrates spatial quantum beats caused by two interfering wave packets with different momenta as the atoms separate. Thomson scattering strongly affects both the spectral profile and the scattering anisotropy.     

Localized electronic excitations in NiO studied with resonant inelastic X-Ray scattering at the Ni M threshold: evidence of spin flip

We studied the neutral electronic excitations of NiO localized at the Ni sites by measuring the resonant inelastic x-ray scattering (RIXS) spectra at the Ni M2,3 edges. The good energy resolution allows an unambiguous identification of several spectral features due to excitations. The dependence of the RIXS spectra on the excitation energy gives evidence of local spin flip and yields a value of 125 +/- 15 meV for the antiferromagnetic exchange interaction. Accurate crystal field parameters are also obtained.     

Electron spectroscopy of iron disilicide

We have reported on the results of a complex investigation of iron disilicide FeSi₂ using characteristic electron energy loss spectroscopy, inelastic electron scattering cross section spectroscopy, and X-ray photoelectron spectroscopy. It has been shown that the main peak in the spectra of inelastic electron scattering for FeSi₂ is a superposition of two unresolved peaks, viz., surface and bulk plasmons. An analysis of the fine structure of the spectra of inelastic electron scattering cross section by their decomposition into Lorentzlike Tougaard peaks has made it possible to quantitatively estimate the contributions of individual energy loss processes to the resulting spectrum and determine their origin and energy.     

Lifetimes of electronic excitations in unoccupied surface states and the image potential states on Pd(110)

The contribution of inelastic electron-electron scattering to the decay rate of excitations in the surface states and first two image potential states at the ? point on the surface is calculated in the GW approximation, and the quasi-momentum dependence of the corresponding contribution for the surface states is analyzed. The mechanisms of electron scattering in these states are studied, and the temperature dependence of the excitation lifetime is analyzed with allowance for the contribution of the electron-phonon interaction calculated earlier.     

Anomalous enhancement of the coupling to the magnetic resonance mode in underdoped Pb-Bi2212

High-resolution angle-resolved photoemission with variable excitation energies is used to disentangle bilayer splitting effects and intrinsic (self-energy) effects in the electronic spectral function near the (pi,0) point of differently doped (Pb,Bi)(2)Sr(2)CaCu(2)O(8+delta). In contrast to overdoped samples, where intrinsic effects at the (pi,0) point are virtually absent, we find in underdoped samples intrinsic effects in the superconducting-state (pi,0) spectra of the antibonding band. This intrinsic effect is present only below the critical temperature and weakens considerably with doping. Our results give strong support for models which involve a strong coupling of electronic excitations with the resonance mode seen in inelastic neutron scattering experiments.     

库仑程函近似下非弹性散射振幅角分布的广义函数分析

在库仑程函近似框架下,引进实参量(时间扫描参数)积分,将能壳上跃迁矩阵元分为靶的结构因子和弹的扭曲因子,导出了非分波扭曲因子的主项表达式和结构因子的解析表达式,利用广义函数方法分析了电子与类氢离子的非弹性散射角分布.     

Long-wavelength magnetic excitations in the Zn0.55Mn0.45Fe2O4 ferrite

The small-angle neutron scattering energy spectra of the Zn_0.55Mn_0.45Fe₂O₄ ferrite are analyzed at different temperatures (both below and above T _C ? 390 K) and scattering angles. The thermal expansion coefficient α(T) is measured in the temperature range 80–600 K. It is revealed that inelastic neutron scattering is governed not only by spin waves of the Holstein-Primakoff type but also by the substantial contribution of additional long-wavelength magnetic excitations. The physical nature of these low-energy magnetic excitations is discussed.     

Resonant mechanisms of inelastic light scattering by low-dimensional electron gases

The contribution of elementary excitations in low-dimensional electron gases to resonant inelastic light scattering is found to be determined by interband transitions involving states at specific wave vectors. In modulation-doped GaAs/GaAlAs quantum wells, we detect only the single-particle excitations (SPE) at resonances with electron-hole transitions at the Fermi wave vector, and only plasmons at resonances with zone-center excitons. The plasmon cross section is comparable to the SPE when double electronic resonance is achieved by tuning the plasmon energy to a valence subband separation.