Spectral moments and orientation correlation functions of asymmetric top molecules

A method for calculating the spectral moments of dipole absorption and Raman scattering by asymmetric top molecules is proposed. The method is based on the calculation of coefficients of expansion of the corresponding orientation correlation functions in a Taylor series using the formalism of the angular momentum theory.     

Optical properties of pigmented coatings taking into account particle interactions

A T-matrix approach is used to obtain the orientation-averaged scattering and absorption cross sections of randomly oriented particle clusters, and the average angular distribution of the radiation scattered by them. The coefficients involved in the expansion of the phase function are obtained from this T-matrix approach, and used in a multiple scattering formalism to characterize the angular distribution of the diffuse radiation propagating through a particulate coating perpendicularly illuminated with collimated visible radiation. Asymmetry between forward and backward propagating diffuse radiation intensities is taken into account by means of this multiple scattering approach, which is based on solving the radiative transfer equation for successive scattering order contributions. A four-flux model is applied to compute the reflectance in terms of wavelength of the incident radiation and particle concentration. An application of the formalism is carried out to predict the optical properties of titanium dioxide pigmented polymer coatings, in terms of the pigment volume fraction and the degree of aggregation.     

Extended X-Ray absorption fine structure from hydrogen atoms in water

We report the first quantitative measurement of extended x-ray absorption fine structure (EXAFS) from hydrogen atoms. A single oscillation is observed from gaseous water consistent with the location of the covalently bonded hydrogen in H 2O. The experimental phase and amplitude of the oscillation are in excellent agreement with curved wave multiple scattering calculations for isolated water molecules. With this determination of the O-H scattering phase shift we have quantified the covalent hydrogen bond distance (0.95+/-0.03 A) in liquid water, thus demonstrating that hydrogen EXAFS can become a valuable complement to existing structural methods in chemistry and biology.     

Scattering of CO and N(2) molecules by a graphite surface

Measurements of angular distributions for the scattering of well-defined incident beams of CO and N(2) molecules from a graphite surface are presented. The measurements were carried out over a range of graphite surface temperatures from 150 to 400?K and a range of incident translational energies from 275 to over 600?meV. The behavior of the widths, positions and relative intensities of the angular distributions for both CO and N(2) were found to be quite similar. The experimental measurements are discussed in comparison with calculations using a classical mechanical model that describes single collisions with a surface. Based on the behavior of the angular distributions as functions of temperature and incident translational energy, and the agreement between measured data and calculations of the single-collision model, it is concluded that the scattering process is predominantly a single collision with a collective surface for which the effective mass is significantly larger than that of a single carbon atom. This conclusion is consistent with that of earlier experiments for molecular beams of O(2) molecules and Xe atoms scattering from graphite. Further calculations are carried out with the theoretical molecular scattering model in order to predict translational and rotational energy transfers to and from the molecule during scattering events under similar initial conditions.     

High-resolution study of x-ray resonant Raman scattering at the K edge of silicon

We report on the first high-resolution measurements of the K x-ray resonant Raman scattering (RRS) in Si. The measured x-ray RRS spectra, interpreted using the Kramers-Heisenberg approach, revealed spectral features corresponding to electronic excitations to the conduction and valence bands in silicon. The total cross sections for the x-ray RRS at the 1s absorption edge and the 1s-3p excitation were derived. The Kramers-Heisenberg formalism was found to reproduce quite well the x-ray RRS spectra, which is of prime importance for applications of the total-reflection x-ray fluorescence technique.     

Quantized ATDHF and angular momentum projection: Three-dimensional applications to heavy ion scattering

The quantized adiabatic time-dependent Hartree-Fock (qATDHF) theory is extended to the calculation of observables in nuclear phenomena using general many-body techniques including angular momentum projection. All calculations are performed using three-dimensional coordinate and momentum-grid techniques. The Bonche-Koonin-Negele interaction as well as several Skyrme-type forces has been used in the simple Hartree-Fock (HF) calculations of ¹²C and ²⁰Ne nuclei. Further, the maximally decoupled collective path is evaluated within qaTDHF, and the angular momentum projected kernels are inserted into the GCM formalism. As a test case, this formalism is applied to the phase shifts of elastic α-α scattering because they can be compared to experimental values. The same techniques are applied to the α-¹⁶O system and the results are compared with those obtained by solving the collective Schrödinger equation in a Gaussian Overlap Approximation, as in a previous publication. The GCM, extended to complex energies, is used to extract the widths of the resonance levels of the 0₁⁺, 0₄⁺, 0 bands in α-¹⁶O scattering. A model calculation, in which the structure of the nuclei is kept fixed to their HF ground state, is performed for the same α-¹⁶O system. We get quite different results with this “sudden” approximation than with the adiabatic calculation. The present calculations show that it is indeed possible to connect general and symmetry conserving many-body techniques to the qATDHF theory and to obtain in this way a purely microscopic framework which can be handled numerically, thus allowing evaluation of observables which are accessible to experiments.     

Resonance behavior of electron scattering from nitrogen molecules adsorbed on metallic surfaces

We use the coupled angular modes theory of electron scattering from molecules to identify the important role played by substrate multiple scattering in determining the lifetime of transient negative ions in adsorbed molecules. For the ²Π_g negative ion resonance in N₂, we demonstrate the phenomenon of complete resonance quenchingwhich occurs when the resonance energy is such that the probe electron is strongly reflected from the substrate. This situation may occur when the resonance energy lies in a band-gap of the unoccupied states of a metallic substrate. It is proposed that the simple resonance energy shift and lifetime reduction observed in previous experimental and theoretical studies of resonance electron scattering from adsorbates is by no means a universal phenomenon. The importance of the unoccupied metallic band structure of the substrate in determining the properties of negative ions in adsorbed molecules is discussed.     

Direct reactions involving exotic nuclei 8He and 5H

The angular distribution of 26 MeV/n ⁸He ions elastically scattered from a gaseous helium target was measured in a wide CM angular range. Results are discussed in terms of the potential scattering and neutron transfer. The angular distributions of elastic scattering as well as 1n and 2n transfer reactions of these ions on protons are presented. Finite-range DWBA calculations made for the 2n transfer reaction leading to the ground (0⁺) and excited (2⁺) states of ⁶He underestimate the cross section for 2n transfer to ⁶He(0⁺). Analysis of data for this reaction channel suggests the importance of a direct ⁵H-cluster exchange process. A resonance state of ⁵H with an energy of 2 MeV above the decay threshold n+n+ ³H was obtained for the first time by making use of the reaction p(⁶He,²He)⁵H.     

Effect of hydrogen adsorption on the x-ray absorption spectra of small Pt clusters

Hydrogen adsorption on Pt(6)H(n) clusters leads to striking changes in the Pt L(2,3) x-ray absorption spectra. These effects are interpreted using a self-consistent real space Green's function approach. Calculations show that they are due largely to changes in the atomic background contribution to x-ray absorption (i.e., atomic x-ray absorption fine structure) and to reduced Pt-Pt scattering at the edge, while Pt-H multiple scattering is relatively weak. The origin of both effects is traced to the change in the local Pt potential due to Pt-H bonding.     

The deuteron breakup reaction induced by protons of 65, 85 and 100 MeV

Coplanar energy sharing spectra for p + d breakup at 65, 85 and 100 MeV proton bombarding energies were measured using the University of Maryland sectored isochronous cyclotron, by measuring the energies of either two protons or one proton and one neutron in coincidence. The detector angles were chosen to enhance either the p-p or p-n quasifree scattering, or the p-n final state interaction. The energy dependence of the peak cross section at equal symmetric quasifree scattering angle pairs was extracted for the ²H(p, 2p)n and ²H(p, pn)p reactions. Quasifree angular distributions were obtained for the reaction ²H(p, 2p)n at 65 MeV and for the reaction ²H(p, pn)p at 65, 85 and 100 MeV. The plane wave impulse approximation theory can only qualitatively reproduce the shape of the quasifree scattering peak in the energy sharing spectra and the shape of the p-p quasifree angular distribution. The discrepancies observed between the plane wave impulse approximation theory and the experimental data imply that the presence of the spectator particle (i.e., the multiple scattering effects) has a strong influence on the magnitude and the shape of the experimental results. Multiple scattering calculations were carried out in the three-body model of Aaron, Amado and Yam except that the S-wave separable two-body amplitudes were modified to fit two-nucleon elastic scattering data at higher energies. Comparisons of the results of these multiple scattering calculations to the experimental data show excellent quantitative agreement throughout the energy range and the angular region of this experiment, except for a few cases in which this model is inherently insufficient; namely, regions in which the Coulomb interaction is important, or regions for which a Hulthén wave function is inaccurate and the off-shell effects are not properly taken into account.     

On high-energy elastic scattering of protons by nuclei

The two coupled channel formalism for high energy elastic scattering [1] is extended to include spin and isospin effects. For a spin and isospin zero nucleus these manifest themselves by additional spin-orbit terms in the potentials. Explicit formulas for these potentials are obtained in terms of the fully spin and isospin dependent nucleon-nucleon scattering amplitude, the ground state nuclear form factor and the state dependent correlation functions. The coupling potential except for a small term arising from double spin and isospin flip process involving nuclear excitation depends only upon the pair correlations.Numerical calculations are performed for the elastic scattering of 1 GeV protons incident on ⁴He. Various phenomenological dynamical two-body correlations as well as correlations generated from the Reid soft-core and Tabakin potentials in an approximate Brueckner-Hartree-Fock calculation are considered. The angular distribution beyond its first diffraction minimum as well as the polarization in the same angular range are shown to be sensitive to these correlations. However, the present accuracy of the experimental data and the lack of knowledge of the nucleon-nucleon scattering amplitude prevent any definitive conclusion about their nature.     

Raman effect in the x-ray region

This paper presents a brief review of x-ray Raman scattering and some of our calculations on Raman scattered line shapes from light elements. We summarise the history of the Raman process in the x-ray region and present a detailed theory of the Raman scattering from an atomic many-electron system. Actual calculations of the Raman cross-section using this theory in single-particle approximation are given. The process of internal resonance Raman scattering is also discussed in the same formulation. The Raman cross-section is compared with the cross-sections of other x-ray scattering processes.     

Study of the angular and polarization structures of radiation scattered by monolayers of metal-containing nanostructures during their oxidation

The angular and polarization scattering characteristics of copper, nickel, and palladium monolayers composed of quasi-monodisperse nanograins 2–5 nm in size, as well as aggregates and chains of these nanograins, have been investigated during oxidation of monolayers with different packing densities of particles in a monolayer. On the basis of the experimental data, a number of integral scattering characteristics of monolayers of different metals and the angular dependences of the scattering matrix elements for laser wavelengths in the visible range have been calculated and analyzed. It is demonstrated that the polarization properties of the angular structure and the scattering matrix elements depend strongly on the degree of order of the structures and the presence of chains in monolayers of metal-containing nanostructures. Oxidation of nanostructures leads to the chaotic distribution of metal cores in a nanostructure. It is shown that scattering from nanostructures is more sensitive to oxidation in comparison with absorption. A nonlinear concentration dependence of scattering intensity was observed for copper nanostructures on a quartz substrate near the plasma resonance (at 633 nm) of all structures under study and at 440 nm for nanostructures on a silicon substrate (i.e., at the wavelength corresponding to strong absorption in silicon).     

10－5000 伏下电子被多原子分子CF4, CF3H, C2F4, C2F6, 及 C2H3F3散射总结面的计算

利用可加性规则和光学势方法计算了能量在10-5000 eV范围内电子被多原子分子CF4, CF3H, C2F4, C2F6, 及 C2H3F3的总结面，并与已有的实验结果和理论计算进行了比较，与这些结果符合得很好。对于CF4, CF3H, C2F4, C2F6, 及 C2H3F3在1000eV以上没有实验数据，本文对实验研究提供了对比和预测的数据。     

Nucleon channel coupling in electrodisintegration of nuclei

The process of nuclear excitation above threshold for nucleon decay in high energy electron scattering is considered. On the basis of the particle-hole shell model a formalism is proposed which allows one to describe electroexcitation of nuclei in a unified manner both in the resonance and quasielastic scattering regions. Numerical calculations were made for the ¹²C nucleus taking into account the mixing of proton and neutron configurations (channels) of the particle-hole type in the continuum.     

Circular dichroism in K-shell ionization from fixed-in-space CO and N2 molecules

We have measured the angular distributions of 1s photoelectrons excited by circularly and linearly polarized light from fixed-in-space CO and N2 molecules, in the vicinity of their shape resonances. A strong circular dichroism, i.e., a strong dependence on the sense of rotation of the polarization vector of the photons, is found for both molecules. State-of-the-art one-electron multiple scattering and partially correlated random phase approximation calculations are in good agreement with many, but not all, aspects of the experimental data.     

Theory of resonant inelastic x-ray scattering by collective magnetic excitations

I present a tractable theory for the resonant inelastic x-ray scattering (RIXS) of magnons. The low-energy transition operator is written as a product of local spin operators and fundamental x-ray absorption spectral functions. This leads to simple selection rules. The scattering cross section linear (quadratic) in spin operators is proportional to the fundamental magnetic circular (linear) dichroic spectral function. RIXS is a novel tool to measure magnetic quasiparticles (magnons) and the incoherent spectral weight, as well as multiple magnons up to very high energy losses, in small samples, thin films, and multilayers, complementary to neutron scattering.     

Coupled channel description of O+Nd scattering around the Coulomb barrier using a complex microscopic potential

Angular distributions of elastic scattering and inelastic scattering from 2⁺₁ state are measured for ¹⁶O+^142,144,146Nd systems at several energies in the vicinity of the Coulomb barrier. The angular distributions are systematically analyzed in coupled channel framework. Renormalized double folded real optical and coupling potentials with DDM3Y interaction have been used in the calculation. Relevant nuclear densities needed to generate the potentials are derived from shell model wavefunctions. A truncated shell model calculation has been performed and the calculated energy levels are compared with the experimental ones. To simulate the absorption, a ‘hybrid’ approach is adopted. The contribution to the imaginary potential of couplings to the inelastic channels, other than the 2⁺₁ target excitation channel, is calculated in the Feshbach formalism. This calculated imaginary potential along with a short ranged volume Woods–Saxon potential to simulate the absorption in fusion channel reproduces the angular distributions for ¹⁶O+¹⁴⁶Nd quite well. But for ¹⁶O+^142,144Nd systems additional surface absorption is found to be necessary to fit the angular distribution data. The variations of this additional absorption term with incident energy and the mass of the target are explored.     

f-State occupancy at the gamma-alpha phase transition of Ce-Th and Ce-Sc alloys

Resonant inelastic x-ray scattering spectra were measured for a series of Ce solid solutions (Ce-Th and Ce-Sc) across the gamma-alpha phase transition. They reveal a well-defined feature associated with the 4f2 configuration when the incident energy is tuned to the Ce L3 preedge region. This component is normally hidden in x-ray absorption spectra because of lifetime broadening. The f1/f2 ratio estimated by resonant inelastic x-ray scattering presents a sharp drop across the gamma-alpha transition and hysteresis as a function of temperature that closely resemble the magnetization loop. These measurements confirm recent dynamical mean-field theory calculations that unexpectedly predict significant double occupancy of f orbitals in the ground state.