Energy dependence of the Penning ionization electron spectrum of Ne* (3P2,0)+Kr

A crossed beam experiment is carried out to measure the energy of electrons emitted in Penning ionization processes by Ne^*(³P_2,0)–Kr collisions. The electron energy spectra have been measured at four different collision energies: 0.050, 0.140, 0.190, 0.460 eV. The analysis of the results allows the separation of spin orbit contributions both in the entrance and in the exit channels providing the related cross-section ratios. Some theoretical considerations have been made to clarify nature and role of interatomic potentials driving the collisions and some general features about the role of atomic fine structure in the Penning ionization processes.     

Vibrational excitation by positron collisions with molecular gases: a study of O and NO targets

The scattering of slow positrons from and NO molecules is treated using exact static interactions and a model potential for correlation-polarisation forces. The quantum coupled equations for the elastic scattering are extended to vibrationally inelastic processes and the different excitation probabilities are evaluated. Comparison with existing experiments for the NO target indicates that the present calculations provide a realistic treatment of positron scattering below Ps formation and give computational estimates on the efficiency of such projectiles in producing vibrationally excited molecules in the ambient gas. Received: 23 April 1999 / Received in final form: 3 June 1999     

Kinetic energy release for the collision-induced dissociation of CO<Superscript>+</Superscript>

The kinetic energy release distributions (KERDs) of C⁺ and O⁺ fragments arising from 5 keV collision-induced dissociation (CID) of CO⁺ ions with helium have been measured. The KERDs of C⁺ and O⁺ exhibit different features corresponding to the states that participate in CID processes. We have identified groups of dissociative and predissociative states, and compare them with theoretical and experimental values.     

Steric effect in O+/H2 and H+/H2O collisions

The positive water and hydronium ions are of interest in a variety of chemical and biological applications. Here we study the steric effect in charge transfer collisions, i.e. the spatial dependence of single electron capture, in collisions mediated by these ions. In particular, the steric effect is demonstrated in the O⁺(²D)/H₂ and H⁺/H₂O charge transfer collisions in the energy range of 100 eV/amu to 10 keV/amu.     

Resonance enhanced multiphoton ionization (REMPI) and REMPI-photoelectron spectroscopy of ammonia

Resonance enhanced multiphoton ionization (REMPI) spectroscopy, preferably linked with kinetic energy analysis of the resulting photoelectrons (REMPI-photoelectron spectroscopy (PES)), continues to make enormous contributions to our understanding of the spectroscopy and, in many cases, the decay dynamics of small molecules in excited (normally Rydberg) electronic states. Here we present results of recent REMPI and REMPI-PES studies involving the ammonia molecule which provide further illustration of some of the many opportunities offered by these techniques. Received: 28 January 1998 / Revised: 3 April 1998 / Accepted: 15 April 1998     

Collision-energy-resolved Penning ionization electron spectroscopy of styrene, 2-vinylpyridine, and 4-vinylpyridine with He*(23S) metastable atoms

Collisional ionization of styrene (phenylethylene), 2-vinylpyridine, and 4-vinylpyridine with metastable He*(2³S) atoms were studied by means of collision-energy/electron-energy resolved two-dimensional Penning ionization electron spectroscopy. Collision energy dependence of partial ionization cross-sections, which reflects the anisotropic interactions between a He*(2³S) atom and the target molecules, indicates that attractive interaction for the out-of-plane access of a He*(2³S) atom to phenyl group is stronger than that for the out-of-plane access to vinyl group. Moreover, it was found for vinylpyridines that the attractive interaction around π electrons became weaker than that for styrene, and that the attractive interaction for the in-plane access to the nitrogen atom is stronger than that for out-of-plane π-directions. However, in 2-vinylpyridine, the hydrogen atom of vinyl group prevents a He*(2³S) atom from approaching to the nitrogen atom along in-plane directions, and thus the attractive interactions around the nitrogen atom were shielded by the vinyl group. The experimentally observed anisotropic interactions were qualitatively supported with ab initio model interaction potential calculations between a Li (He*(2³S)) atom and the target molecule. Concerning with electronic structures of investigated molecules, the assignment of Penning ionization electron spectrum for 4-vinylpyridine was discussed on the basis of different behavior of collision-energy dependence of partial ionization cross-sections, and the satellite ionization band in Penning ionization electron spectra was also reported for styrene.     

Calculation of absolute electron-impact ionization cross-sections of dimers and trimers

We report calculations of the electron-impact ionization cross-sections of selected dimers (homonuclear diatomic molecules) and trimers (homonuclear triatomic molecules) using a method which relies only on macroscopic quantities in conjunction with a “defect concept”. The empirically determined defect describes the deviation of the cluster (dimer, trimer) cross-sections from a simple linear dependence on the cluster size. We compare the calculated cross-sections to experimental data for the dimers S₂ and F₂ and the trimer O₃ and we present predictions for the ionization cross-sections of Br₂, I₂, C₂ and C₃ for which no experimental data are available. Lastly, we extend the method to the calculation of ionization cross-sections for the fullerenes C₆₀ and C₇₀. Received 6 December 1999 and Received in final form 10 April 2000     

Electron-impact dissociation and transient properties of a stored LiH2 - beam

The fragmentation of LiH₂ ^- anions after electron impact was investigated at the heavy-ion storage ring TSR. The main reaction channel was found to be electron detachment followed by a breakup into LiH + H. In the first ms after production of the molecular ions in a cesium sputtering ion source, additional contributions were observed in the Li + H₂ and Li^- + H₂ channels, hinting at an initial population of a short-lived state of the anion. To gain a better understanding of the mechanisms underlying the observed behavior of the system, ab initio calculations of relevant potential energy surfaces were performed at selected geometries. The experimental findings are discussed in the light of these calculations.     

Multiple ionization and fragmentation of the DNA base thymine by interaction with C q+ ions

Ionization and fragmentation of the DNA base thymine upon interaction with keV C^q+ ions (q = 1 - 6) has been studied. By means of time-of-flight spectrometry of two or more thymine fragments in coincidence with an ejected electron we could investigate particular dissociation channels by means of their associated kinetic-energy-release. The fragmentation dynamics are strongly influenced by the C^q+ charge state: for low q values mainly fragmentation due to direct collisions is observed. With increasing q, electron capture becomes more important. For larger q we could identify several Coulomb explosion channels, leading to very energetic fragments.     

Inelastic interactions of protons and electrons with biologically relevant molecules

Ionization and fragmentation of water and uracil molecules was studied both by electron and proton impact. A special coincidence technique allows on an event by event basis the investigation of product ions formed upon the collision of protons with neutral molecules including the identification of the charge state of the projectile. This enables the characterization of the ionization processes occurring, i.e. direct ionization, single electron capture or double electron capture for 0, 1 or 2 electrons that are transferred from the target to the projectile, respectively. For uracil the fragmentation patterns obtained by electron and proton impact ionization reveal close similarities and indicate a comparable amount of excitation for the two different ionization mechanisms at high enough projectile energies. Received 25 February 2002 Published online 13 September 2002     

Femtosecond to nanosecond relaxation time scales in electronically excited tetrakis(dimethylamino)ethylene: identification of the intermediates

In the TDMAE molecule (title molecule), the time evolution has been analyzed from the very initial excitation step down to a fluorescent state, over widely different time scales. Pump probe measurements have been performed at 3 different excitation wavelengths 400, 266 and 200 nm. The decay has been followed over the femtosecond and subnanosecond ranges with this method and the decay of the final charge transfer state has been detected by its fluorescence emission. This allows an overview of the complete decay mechanism. The initial relaxation pathway is interpreted in a similar way to ethylenic molecules, where the initial wavepacket is quickly trapped in a doubly excited state Z with charge transfer character. Then the Z state decays slowly (10-100 picoseconds) into the final state. In difference to monoalkenes the final stage of this evolution is a charge transfer state. The decay of transient Z state to the charge transfer state is a further assessment of the partial ionic character of the Z state. This type of molecule with low ionization potential can be viewed as a demonstrative example of the interrelation between the charge induced forces and the deformations in excited state reaction dynamics. Received 17 January 2001 and Received in final form 23 February 2001     

Inelastic cross-sections and natural lifetimes for the 62D3/2, 5/2 and 82S1/2 states of Rb

The results of an experimental study of population dynamics following excitation of [0pt] and [0pt] states of rubidium are reported. Excitation transfer and quenching cross-sections in collisions with ground state rubidium atoms, and natural lifetimes have been measured. The experiment was performed in a vapour cell, using pulsed two-photon excitation and photon counting detection. The analysis of time dependent signals was based on a rate equation model in which transitions induced by thermal radiation have been accounted for. The measurements yielded following results: (1) [0pt] state J-mixing cross-section: [0pt] ; (2) cross-sections for [0pt] excitation transfer process: [0pt] ; (3) quenching cross-sections: [0pt] , [0pt] , [0pt] ; [0pt](4) radiative lifetimes: [0pt] ns, [0pt] ns, [0pt] ns. Received 1st December 1998 and Received in final form 17 May 1999     

Dynamics of ionization mechanisms in relativistic collisions involving heavy and highly-charged ions

The dynamics of mechanisms associated with the ionization of inner-shell electrons in relativistic collisions involving heavy and highly-charged ions is investigated within a nonperturbative approach formulated explicitly in the time domain. The theoretical treatment is based on the exact numerical solution of the time dependent Dirac equation for two Coulomb centers on a lattice in momentum space. We present results for ionization in encounters between 100 MeV/u Au⁷⁹⁺ projectile ions impinging on a hydrogen-like uranium target. By directly visualizing the collision dynamics we identify a new ionization mechanism in which electrons are emitted from the internuclear region preferentially in the transverse direction with respect to the projectile trajectory. A striking characteristic of this ionization mechanism is that the velocity of the electron is higher than the projectile velocity. Received 26 June 2001 and Received in final form 27 November 2001     

Theoretical study of energy transfer in Rb(7S) + Rb(5S) and Rb(5D) + Rb(5S) collisions

We present results of theoretical studies of the non-resonant excitation transfer in Rb(7S) + Rb(5S) and Rb(5D) + Rb(5S) collisions at thermal collision energies. Rb₂ adiabatic molecular terms correlating with the 5S+7S, 5S+5D and 5P+5P states of separated atoms were calculated for internuclear distances R > 20 a.u. using asymptotic approximation. Mechanisms of collisional population and quenching of the 5D state were treated on the basis of the computed molecular terms, and the respective cross-sections were calculated. Theoretical cross-sections are in good agreement with the experimental values at thermal collision energies ( K). Received 13 November 1998 and Received in final form 22 November 1999     

Classical impact parameter approximation: Application to atomic collisions with n independent electrons and to recoil analysis

We show that a classical Impact Parameter Method may be derived when taking fully into account the smallness of the ratio between the electron and nuclear masses. It allows to calculate, exactly as in the quantum version, projectile scattering and therefore recoil momenta required for the interpretation of recent measurements. We prove an additivity theorem which allows, in particular, to reduce the n-non-interacting electron problem to a set of n one-electron problems. Consequences for the interpretation of target recoil measurements are discussed. Received 25 June 1999     

Classical study of and collisions in intense laser fields

In this paper, ion-atom and ion-ion collisions in the presence of intense laser fields are qualitatively studied by Classical Trajectory Monte Carlo (CTMC) simulations. It is found that in contrast to the field-free collisions, the colliding ion and the target nucleus could absorb energy from the applied laser fields when the electrons escape from the collision system. This result is explained in terms of Coulomb explosion induced by the enhanced ionization at the so-called critical internuclear distance. Also, the corresponding energy gain cross-sections are evaluated. Received: 7 October 1998 / Received in final form: 28 January 1999     

Radiative lifetime and oscillator strength determination in Mg-like potassium (K VIII)

Theoretical transition probabilities have been obtained for 54 n = 3 transitions depopulating the 3s3p ¹P^o, 3p^{2 3}P, ¹D, ¹S, 3s3d ¹D, ³D and 3p3d ³P^o, ³D^o, ³F^o, ¹F^o, ¹D^o, ¹P^o levels, including 14 transitions not yet observed. Some of these predictions have been compared with experimental lifetimes obtained by beam-foil spectroscopy for four n = 3 levels of K⁷⁺. An excellent agreement is observed between theory and experiment for all the levels. Received 23 January 2002 / Received in final form 23 April 2002 Published online 19 July 2002     

Forward and backward electron emission cross-sections for 23 MeVu<Superscript>-1</Superscript> C,Ni and Au projectiles traversing C,Al , Ni,Ag , Au and Bi foils

A rather complete experimental study of forward and backward electron velocity spectra from thin foils bombarded with ions at constant velocity of 30 atomic units (23MeV u^-1) was performed. Three different beams ( ¹²C³⁺ , ⁵⁸Ni¹⁴⁺ and ¹⁹⁷Au³⁶⁺ and six different targets ( ¹²C , ²⁷Al , ^natNi , ^natAg , ¹⁹⁷Au and ²⁰⁹Bi of approximately 90μg cm^-2 thickness were used. This procedure allowed to study the evolution of electron emission (velocity and angular distributions) for the [projectile; target] matrix [ C , Ni , Au ; C , Al , Ni , Ag , Au , Bi ] in a wide angular range. The projectile and target dependence of absolute cross-sections for binary encounter-, Auger- and backward-emitted electrons are analyzed.     

Singlet-triplet excitation ratios in Ne III, Ar III and N II under ion impact

Peculiar properties of ion-atom collision systems, in particular deviations from statistical populations of singlet and triplet levels, can be studied by optical spectroscopy. We have extended earlier studies by VUV spectroscopy of a number of collision systems at various collision energies in the 0.01-MeV/nucleon to 1-MeV/nucleon range, involving H₂ ⁺, H⁺, He⁺, He²⁺, Ne⁺, Ar⁺, and N₂ ⁺ as projectiles and Ne, Ar, and N₂ as target gases. Statistically significant deviations of the relative intensities of singlet and triplet lines from simple ratios are observed in the displaced terms of the valence shell of Ne III, corroborating and extending earlier work. For Ar III, the energy dependences of singlet-to-triplet excitation ratios are very different for different projectiles. For N II, in contrast, all observed line ratios are practically independent of the projectile energy. Received 17 November 2000 and Received in final form 31 January 2001