Nonlocal complex potential theory of dissociative electron attachment: Inclusion of two vibrational modes

The process of dissociative electron attachment (DEA) to molecules with several vibrational degrees of freedom is usually treated in the approximation of the local potential for the description of the nuclear motion. We develop the nonlocal complex potential theory to treat the dissociation dynamics when there is more than one vibrational mode in the neutral molecule. We demonstrate the application of the multimode nonlocal theory to a generic molecule of the type CY3X, where Y denotes the H or F atom and X denotes the halogen atom, with the inclusion of symmetric C–X stretch and CY3 deform (“umbrella”) vibrational modes. We present results for the dependence of DEA cross sections on the electron energy and vibrational energy for the CF3Cl molecule in the two-mode approximation. The 1.5 eV peak in the DEA cross section is well described in the one-mode approximation. However, inclusion of additional modes is required to explain the experimentally observed low-energy peak in the DEA cross section at the vibrational temperature Tv = 800 K

Classical theory of laser-assisted spontaneous bremsstrahlung

We study the process of laser-assisted spontaneous electron bremsstrahlung by running classical trajectories in a combined Coulomb and laser (ac) fields. Due to chaotic scattering in the combined Coulomb and ac fields, the radiation probability as a function of the impact parameter and the constant phase of the laser field exhibits fractal structures. However, these structures are smeared out when the cross section is integrated over the impact parameter and averaged over the phase. We analyze the role of different types of orbits, including the trapped orbits, and the dependence of the radiation probability on the impact parameter and the initial phase of the ac field.We show that, at low incident electron kinetic energy, the Coulomb focusing leads to a substantial extension of the range of impact parameters contributing to the bremsstrahlung cross section and results in a substantial increase (by one to two orders of magnitude) of the cross section as compared with the pure Coulomb case. As examples, we discuss the case of relatively high ponderomotive energy Ep when we obtain an efficient production of photons with frequencies up to 2Ep, and the case of low Ep when only infrared photons are produced. Overall accuracy of the classical approach is estimated to be very good, although it does not describe resonant processes studied previously by quantum-mechanical methods

Semiclassical theory of laser-assisted radiative recombination

We study the process of laser-assisted radiative recombination of an electron with a proton by using a semiclassical approach involving calculation of classical trajectories in combined laser and Coulomb fields. Due to chaotic scattering in the combined fields, the radiation probability as a function of the impact parameter and the constant phase of the laser field exhibits chaotic behavior and fractal structures. We obtain a strong enhancement of the recombination cross section as compared to the laser-free case due to the Coulomb focusing effect. For sufficiently low incident electron velocities the cross section becomes infinite, and we limit it by assuming a finite laser pulse duration. With the pulse duration tp = 5 ps we obtain the gain factor for capture into the ground state of the hydrogen atom of about 220 for infrared fields in the intensity range 109–1012 W/cm2. The gain factor grows with tp but slower than linearly

Positronium collisions with rare-gas atoms: Free-electron gas plus orthogonalizing pseudopotential model

Positronium collisions with rare-gas atoms are treated using the free-electron-gas approximation for exchange and correlation potential. The results confirm the absence of the Ramsauer-Townsend minimum in elastic scattering cross sections, but show lower cross sections in the lower-energy region when compared to previous pseudopotential calculations. This is explained by a more attractive ab initio correlation potential as compared to the previously used empirical potential. The results in the thermal-energy region agree very well with most swarm measurements for all rare-gas atoms. At higher energies, the results are compared with beam experiments and agreement for heavier rare-gas atoms Ar, Kr, and Xe is found to be very good. For He and Ne, some discrepancies with beam measurements are observed. This is explained by a poorer performance of the free-electron-gas potentials, based on the statistical Thomas-Fermi model, for systems with fewer electrons

Elastic scattering, vibrational excitation, and attachment in low-energy electron-SF₆ scattering: Experiment and effective range theory

Cross sections at low energies for vibrationally elastic and inelastic scattering, as well as electron attachment to SF₆, have been calculated using a multichannel effective range theory (ERT) with complex boundary conditions. The most active vibrational modes, the totally symmetric mode ν1 and the infrared active mode ν3, have been included in the calculation. The ERT parameters were fitted to reproduce the experimental total and attachment cross sections. Differential elastic and vibrational excitation cross sections have been measured at 30° and 135° using a spectrometer with hemispherical analyzers. The calculation reproduces correctly the magnitudes and shapes of the differential elastic and ν1, ν3, and 2ν1 excitation cross sections, in particular the sharp structures at vibrational thresholds. The s- and p-wave phase shifts obtained in the present analysis differ from those recently derived by Field et al. [Phys. Rev. A, 69, 052716 (2004)]

Dissociative electron attachment and vibrational excitation of CF3Cl\mathbf{CF_3Cl}: Effect of two vibrational modes revisited

We present a study of dissociative electron attachment and vibrational excitation processes in electron collisions with the CF$_3$Cl molecule. The calculations are based on the two-dimensional nuclear dynamics including the C-Cl symmetric stretch coordinate and the CF$_3$ symmetric deformation (umbrella) coordinate. The complex potential energy surfaces are calculated using the ab initio R-matrix method. The results for dissociative attachment and vibrational excitation of the umbrella mode agree quite well with experiment while the cross section for excitation of the C-Cl symmetric stretch vibrations is about a factor of three low as compared to experimental data.Comment: 24 pages, 7 figures, submitted to Physical Review

Threshold effects in strong-field ionization: Energy shifts and Rydberg structures

The behavior of strong-field ionization rates of neutral atoms in the vicinity ofmultiphoton ionization thresholds is analyzed using formal collision theory.Our approach,which accounts nonperturbatively for effects of an intense laser field, shows that the ionization rates have a nearly constant behavior below and above each multiphoton threshold and that between such thresholds there are an apparently finite number of rapid oscillations due to resonances with laser-field-modified Rydberg states. This pattern is typical for any atomic target, as we illustrate specifically for hydrogen and neon atoms. The flat behavior of the ionization yield near multiphoton thresholds gives the appearance of an energy shift of the ionization thresholds, which have been postulated in a number of recent studies concerning diverse aspects of above-threshold ionization and high-harmonic generation of atoms. The flat behaviors of the rates near threshold exhibit only a rather weak dependence on the laser-field intensity. Other aspects of the near-threshold behavior of ionization rates and their dependence on the laser-field parameters are also discussed

Threshold effects in strong-field ionization: Energy shifts and Rydberg structures

The behavior of strong-field ionization rates of neutral atoms in the vicinity ofmultiphoton ionization thresholds is analyzed using formal collision theory.Our approach,which accounts nonperturbatively for effects of an intense laser field, shows that the ionization rates have a nearly constant behavior below and above each multiphoton threshold and that between such thresholds there are an apparently finite number of rapid oscillations due to resonances with laser-field-modified Rydberg states. This pattern is typical for any atomic target, as we illustrate specifically for hydrogen and neon atoms. The flat behavior of the ionization yield near multiphoton thresholds gives the appearance of an energy shift of the ionization thresholds, which have been postulated in a number of recent studies concerning diverse aspects of above-threshold ionization and high-harmonic generation of atoms. The flat behaviors of the rates near threshold exhibit only a rather weak dependence on the laser-field intensity. Other aspects of the near-threshold behavior of ionization rates and their dependence on the laser-field parameters are also discussed

Reply to “Comment on ‘Electron-induced bond breaking at low energies in HCOOH and glycine: The role of very short-lived σ anion states’ ”

Rescigno et al. [Phys. Rev. A 80, 046701 (2009)] criticized our theoretical treatment of dissociative electron attachment in formic acid in which we show that this process can be explained by electron attachment into the temporary negative ion state formed by occupation of the σ*(OH) orbital. We argue that their objections do not hold up to scrutiny

Reply to “Comment on ‘Electron-induced bond breaking at low energies in HCOOH and glycine: The role of very short-lived σ anion states’ ”

Rescigno et al. [Phys. Rev. A 80, 046701 (2009)] criticized our theoretical treatment of dissociative electron attachment in formic acid in which we show that this process can be explained by electron attachment into the temporary negative ion state formed by occupation of the σ*(OH) orbital. We argue that their objections do not hold up to scrutiny