Low energy positron interactions with uracil--total scattering, positronium formation, and differential elastic scattering cross sections.

Measurements of the grand total and total positronium formation cross sections for positron scattering from uracil have been performed for energies between 1 and 180 eV, using a trap-based beam apparatus. Angular, quasi-elastic differential cross section measurements at 1, 3, 5, 10, and 20 eV are also presented and discussed. These measurements are compared to existing experimental results and theoretical calculations, including our own calculations using a variant of the independent atom approach.

Observation of threshold effects in positron scattering from the noble gases.

Channel coupling is a phenomenon that has been investigated for many scattering processes, and is responsible for the formation of cusps or steps in the cross sections for open scattering channels at, or near, the onset of a new scattering channel. It has long been speculated that the opening of the positronium formation channel may lead to the formation of such cusp features in the elastic positron scattering cross section. In this work, elastic scattering of positrons has been measured in the region of the positronium formation threshold for the noble gases He-Xe. Cusplike behavior is observed and, while the features which are observed appear broad, they represent a magnitude of between 4 and 15% of the total elastic cross section. No evidence is found of any other features in this region, at least within the uncertainty of the present data, discounting the possibility of scattering resonances.

A positron trap and beam apparatus for atomic and molecular scattering experiments.

An instrument has been designed and constructed to provide new insights into fundamental, low energy positron scattering processes. The design is based on the Surko trap system and produces a pulsed positron beam with an energy resolution of as good as 54 meV. The design and operation of the apparatus is explained, while the first experimental results from this apparatus have been demonstrated in recent publications.

Electron and positron scattering from 1,1-C2H2F2.

1,1-difluoroethylene (1,1-C2H2F2) molecules have been studied for the first time experimentally and theoretically by electron and positron impact. 0.4-1000 eV electron and 0.2-1000 eV positron impact total cross sections (TCSs) were measured using a retarding potential time-of-flight apparatus. In order to probe the resonances observed in the electron TCSs, a crossed-beam method was used to investigate vibrational excitation cross sections over the energy range of 1.3-49 eV and scattering angles 90 degrees and 120 degrees for the two loss energies 0.115 and 0.381 eV corresponding to the dominant C-H (nu2 and nu9) stretching and the combined C-F (nu3) stretching and CH2 (nu11) rocking vibrations, respectively. Electron impact elastic integral cross sections are also reported for calculations carried out using the Schwinger multichannel method with pseudopotentials for the energy range from 0.5 to 50 eV in the static-exchange approximation and from 0.5 to 20 eV in the static-exchange plus polarization approximation. Resonance peaks observed centered at about 2.3, 6.5, and 16 eV in the TCSs have been shown to be mainly due to the vibrational and elastic channels, and assigned to the B2, B1, and A1 symmetries, respectively. The pi* resonance peak at 1.8 eV in C2H4 is observed shifted to 2.3 eV in 1,1-C2H2F2 and to 2.5 eV in C2F4; a phenomenon attributed to the decreasing C=C bond length from C2H4 to C2F4. For positron impact a conspicuous peak is observed below the positronium formation threshold at about 1 eV, and other less pronounced ones centered at about 5 and 20 eV.

Low energy electron energy-loss spectroscopy of CF3X (X=Cl,Br).

We report threshold electron energy-loss spectra for the fluorohalomethanes CF3X (X=Cl,Br). Measurements were made at incident electron energies of 30 and 100 eV in energy-loss range of 4-14 eV, and at scattering angles of 4 degrees and 15 degrees. Several new electronic transitions are observed which are ascribable to excitation of low-lying states as well as are intrinsically overlapped in the molecules themselves. Assignments of these electronic transitions are suggested. These assignments are based on present spectroscopic and cross-section measurements, high-energy scattering spectra, and ab initio molecular orbital calculations. The calculated potential curves along the C-X bond show repulsive nature, suggesting that these transitions may lead to dissociation of the C-X bond. The present results are also compared with the previous ones for CF3H, CF4, and CF3I.

Symmetry-dependent vibrational excitation in N 1s photoionization of N2: experiment and theory.

We have measured the vibrational structures of the N 1s photoelectron mainline and satellites of the gaseous N2 molecule with the resolution better than 75 meV. The gerade and ungerade symmetries of the core-ionized (mainline) states are resolved energetically, and symmetry-dependent angular distributions for the satellite emission allow us to resolve the Sigma and Pi symmetries of the shake-up (satellite) states. Symmetry-adapted cluster-expansion configuration-interaction calculations of the potential energy curves for the mainline and satellite states along with a Franck-Condon analysis well reproduce the observed vibrational excitation of the bands, illustrating that the theoretical calculations well predict the symmetry-dependent geometry relaxation effects. The energies of both mainline states and satellite states, as well as the splitting between the mainline gerade and ungerade states, are also well reproduced by the calculation: the splitting between the satellite gerade and ungerade states is calculated to be smaller than the experimental detection limit.

Experimental and theoretical elastic cross sections for electron collisions with the C3H6 isomers.

In the present work we report cross sections for electron collisions with the isomers propene (C3H6) and cyclopropane (c-C3H6). Electron-scattering differential cross sections (DCS) are reported for measurements carried out for energies 1.5-100 eV and the angular range of 20 degrees-120 degrees. Elastic integral cross sections (ECS), DCS, and momentum-transfer cross sections (MTCS) are reported for calculations carried out using the Schwinger multichannel method with pseudopotentials for the energy range of 2.0-40 eV and angular range of 0 degrees-180 degrees. The resemblance of the pi* shape resonance in the cross sections, observed at 1.5-2.0 eV for propene, to those in C2H4 and C2F4 clearly points to the effect of the double bond in the molecular structures for these molecules. Below 60 eV, we observed clear differences in peak positions and magnitudes between the DCS, ECS, and MTCS for C3H6 and c-C3H6, which we view as the isomer effect.

Symmetry-resolved absorption spectra of vibrationally excited CO2 molecules.

Symmetry-resolved x-ray absorption spectroscopy has been first carried out on high-temperature molecules. From the angle-resolved ion yield spectra of CO2 both at room temperature and at 430 degrees C, symmetry-resolved absorption profiles of the C 1s(-1) 2pi(u) and O 1s(-1) 2pi(u) resonances have been extracted for the vibrational ground state molecules and bending-vibration excited ones. The profiles change dramatically between them, and the Renner-Teller effect becomes more evident for the vibrationally excited molecules. The effects of the multimode vibronic coupling are suggested for the O 1s(-1) 2pi(u) and O 1s(-1) 3s sigma(g) resonances.

Violation of the Franck-Condon principle due to recoil effects in high energy molecular core-level photoionization.

Carbon 1s photoelectron spectra of methane are measured over a photon energy range between 480 eV and 1200 eV. Additional components appear between the individual symmetric stretching vibrational components and are attributed to the excitations of asymmetric stretching and bending vibrations due to recoil of the high-energy photoelectron emission. This recoil effect is the evidence for the violation of the Franck-Condon principle which states that neither the positions nor the momenta of the nuclei change during the ionization event.

Individual fundamental mode dependence of H2O vibrational excitation in the 6-8 eV resonance region by electron impact.

Resonance phenomena in the bending (010), symmetric (100), and asymmetric (001) stretching vibrational modes in water (H(2)O) molecules have been investigated by measuring differential cross sections (DCSs) at fixed energy losses of 0.43, 0.46, 0.49, and 0.51 eV while sweeping the impact energies from 1.6 to 10 eV, at angles 60 degrees and 90 degrees, using a crossed-beam method. No resonancelike enhanced features have been observed in the study of the (010) mode. In the DCSs for the combined (100+001) mode, a single broad hump was observed at each angle, whose position shifts towards the higher energy side with increasing scattering angle, a feature typical of the interference profiles previously observed in a study of the (301) vibrational mode. DCSs for the (001) mode exhibited a rather isotropic angular distribution with no evidence of resonances. However, enhancement of DCSs were indeed observed for the (100) mode, at the energy loss of 0.46 eV, which is attributable to the A(1) symmetry resonance that was studied by Seng and Linder [J. Phys. B 9, 2539 (1976)], with a typical s-wave characteristic angular distribution. Theoretical analysis based on the continuum multiple-scattering approach has been carried out to provide rationale to the experimental results.