The triply differential cross section has been measured for electron-impact ionization of the outer valence 1t2 and the inner valence 2a1 orbitals of methane using the (e,2e) technique with coplanar asymmetric kinematics. The measurements are performed at scattered electron energy of 500 eV, ejected electron energy of 12, 37 and 74 eV and for scattering angle of the fast outgoing electron of 6°. This kinematics is characterized by a target ion recoil momentum ranging from moderate (0.25 au) to very large (3.2 au) values. The results are compared with theoretical cross sections calculated using the 1CW and the BBK models recently extended to molecules. The experimental cross sections exhibit a very large recoil scattering, especially for the inner 2a1 molecular orbital, which is not predicted by the theory. The differences between experiment and theory are attributed to the very strong scattering from the ion, not properly accounted for by theory. This indicates the need for further theoretical developments as well as experimental investigations in order to correctly model the process of molecular ionization.

Relative (e,2e) triply differential cross sections (TDCS) are measured for the ionization of the helium atom and the hydrogen molecule in coplanar asymmetric geometry at a scattered electron energy of 500 eV and ejected electron energies of 205, 74 and 37 eV. The He experimental results are found to be in very good agreement with convergent close-coupling calculations (CCC). The H2 experimental results are compared with two state-of-the-art available theoretical models for treating differential electron impact ionization of molecules. Both models yield an overall good agreement with experiments, except for some intensity deviations in the recoil region. Similar (e,2e) works were recently published on H2 with contrasted conclusions to the hypothesis that the two H nuclei could give rise to an interference pattern in the TDCS structure. Murray (2005 J. Phys. B: At. Mol. Opt. Phys. 38 1999) found no evidence for such an effect, whereas Milne-Brownlie et al (2006 Phys. Rev. Lett. 96 233201) reported its indirect observation. In this work, based on a direct comparison between experimental results for He and H2, we observe an oscillatory pattern due to these interference effects, and for the first time the destructive or constructive character of the interference is observed, depending on the de Broglie wavelength of the ejected electron wave. The experimental finding is in good agreement with the theoretical prediction by Stia et al (2003 J. Phys. B: At. Mol. Opt. Phys. 36 L257).

We perform calculations of electron impact ionization of noble gas atoms within the distorted wave Born approximation (DWBA) corrected by the Gamow factor (G) to account for the post-collision interaction. We make an extensive comparison with experimental data on He 1s2, Ne 2s2, 2p6 and Ar 3p6 under kinematics characterized by large energy transfer and close to minimum momentum transfer from the projectile to the target. For all atoms, good agreement between theory and experiment is achieved. In the case of Ar, the disagreement of experimental data with theory reported earlier by Catoire et al (2006 J. Phys. B: At. Mol. Opt. Phys. 39 2827) is reconciled.

The (e,2e) triple differential cross sections (TDCS) are measured for the ionization of nitrogen and carbon dioxide molecules in a coplanar asymmetric geometry for a wide range of ejected electron energies and at an incident energy about 500–700 eV. This kinematics corresponds to a large momentum imparted to the ion, and is meant to enhance the recoil scattering. The experimental binary and recoil angular distributions of the TDCS are characterized both by a shift towards larger angles with respect to the momentum transfer direction and by a large intensity in the recoil region, in particular for the ionization of the ‘inner’ N2(2σg) molecular orbital. The data are compared with the results of calculations using the first Born approximation–two centre continuum (FBA–TCC) theoretical model for treating differential electron impact ionization. The experimentally observed shifts and recoil intensity enhancement are not predicted by the model calculations, which rather yield a TDCS symmetrically distributed around the momentum transfer direction, and completely fail in describing the recoil distribution. It is hoped that these new results will stimulate the development of more refined theories for correctly modelling single ionization of molecules.

The (e,3-1e) four-fold differential cross sections (4DCS) are measured for the double ionization of helium in coplanar asymmetric geometry for a wide range of ejected electron energies and at an incident energy of about 600 eV. The experimental angular distributions of the 4DCS are characterized by large angular shifts of the forward and backward lobes with respect to the momentum transfer direction or its opposite, respectively. This validates our previously published results [

Measurements of the (e,2e) triply differential cross sections (TDCS) are presented for the ionization of the nitrogen molecule in coplanar asymmetric geometry at an incident energy of about 600 eV and a large energy transfer to the target. The experimental results are compared with state-of-the-art available theoretical models for treating differential electron impact ionization of molecules. The experimental TDCS are characterized by a shift towards larger angles of the angular distribution with respect to the momentum transfer direction, and by a large intensity in the recoil region, especially for ionization of the 'inner' 2σ g molecular orbital. Such shifts and intensity enhancement are not predicted by the model calculations which rather yield a TDCS symmetrically distributed around the momentum transfer direction.

We describe new developments aimed to extend the capabilities and the sensitivity of the (e,2e)(e,3e) multicoincidence spectrometer at Orsay University [Duguet et al., Rev. Sci. Instrum. 69, 3524 (1998)]. The spectrometer has been improved by the addition of a third multiangle detection channel for the fast "scattered" electron. The present system is unique in that it is the only system which combines three toroidal analyzers all equipped with position sensitive detectors, thus allowing the triple coincidence detection of the three electrons present in the final state of an electron impact double ionization process. The setup allows measurement of the angular and energy distributions of the ejected electrons over almost the totality of the collision plane as well as that of the scattered electron over a large range of scattering angles in the forward direction. The resulting gain in sensitivity ( approximately 25) has rendered feasible a whole class of experiments which could not be otherwise envisaged. The setup is described with a special emphasis on the new toroidal analyzer, data acquisition hardware, and data analysis procedures. The performances are illustrated by selected results of (e,2e) and (e,3e) experiments on the rare gases.

We analyse the recoil-to-binary (RB) peak intensity ratio in an energetic (e,2e) reaction performed on the valence ns sub-shell of noble gas atoms away from the Bethe ridge condition. A qualitative change in the RB ratio dependence on the ejected electron energy from He to Ar can be explained by the variation of reflectivity of the short-range Hartree-Fock potential. The reflectivity increases profoundly from lighter (He) to heavier (Ne and Ar) noble gas atoms because of modification of the scattering phases due to occupation of the target p orbitals (Levinson-Seaton theorem). This effect is further modified due to strong inter-shell correlations in Ar. These theoretical predictions are confirmed experimentally.