Theoretical calculations for electron impact ionization of atoms and molecules

In the last twenty years, significant progress has been made for the theoretical treatment of electron impact ionization (e,2e) of atoms and molecules and, for some cases, very nice agreement between experiment and theory has been achieved. In particular, excellent agreement between theory and experiment and theory has been achieved for ionization of hydrogen and helium. However, agreement between experiment and theory is not nearly as good for ionization of larger atoms and molecules. In the first part of this dissertation, different theoretical approaches will be employed to study the triply differential cross section (TDCS) for low and intermediate energy electron-impact ionization of Neon and Argon for different orbital states. There is a very recent interest in studying ionization of Laser aligned atoms in order to get a better understanding about electron impact ionization of molecules. In the next part of this dissertation, results will be presented for electron-impact ionization of three laser aligned atoms, Mg, Ca, and Na. The comparison between the theory and experiment showed that our three body distorted wave (3DW) model gave excellent agreement with experiment in the scattering plane but very poor agreement perpendicular to the scattering plane. An explanation for this poor agreement out of the scattering plane has been provided by comparing our theoretical results with those of the time depended close coupling (TDCC) model and this explanation is also provided in this dissertation. Recently, significant attention has been directed towards obtaining a better understanding of electron-impact ionization of molecules which are significantly more challenging than atoms. In the last part of this dissertation, results will be presented for electron-impact ionization of three different molecules (N₂, H₂O, and CH₄ ) which have been studied comprehensively using different theoretical approximations for different types of geometries. The published papers in section two contain a detailed analysis and discussion for each of these topics --Abstract, page iv

(e,2e) Ionization Studies of N₂ at Low to Intermediate Energies from a Coplanar Geometry to the Perpendicular Plane

Synopsis. The progress of experimental and theoretical measurements for (e,2e) ionization cross sections from Nitrogen molecules is presented. Results are given for energies from ~10 eV above the ionization potential (IP) through to ~100 eV above the IP for the 3σg, 1πu and 2σg states

Comparison of Experiment and Theory for Electron Impact Ionization of Isoelectronic Atoms and Molecules

Experimental and Theoretical Triply Differential Cross sections will be presented for low energy electron impact ionization of Ne, CH4, and NH3. The collision mechanisms responsible for the various structures found in the cross sections will be discussed

Coplanar Asymmetric Angles and Symmetric Energy Sharing Triple Differential Cross Sections for 200 EV Electron-Impact Ionization of Ar (3p)

We have measured triple differential cross sections (TDCSs) for electron-impact ionization of the 3p shell of Ar at 200 eV incident electron energy. The experiments have been performed in coplanar asymmetric energy sharing geometry. The experimental results are compared with the theoretical models of three body distorted wave (3DW) and distorted wave Born approximation (DWBA)

Low Energy (e,2e) Measurements of Ch⁴ and Neon in the Perpendicular Plane

Low energy experimental and theoretical triple differential cross sections for the highest occupied molecular orbital of methane (1t2) and for the 2p atomic orbital of neon are presented and compared. These targets are iso-electronic, each containing 10 electrons and the chosen orbital within each target has p-electron character. Observation of the differences and similarities of the cross sections for these two species hence gives insight into the different scattering mechanisms occurring for atomic and molecular targets. The experiments used perpendicular, symmetric kinematics with outgoing electron energies between 1.5 eV and 30 eV for CH4 and 2.5 eV and 25 eV for neon. The experimental data from these targets are compared with theoretical predictions using a distorted-wave Born approximation. Reasonably good agreement is seen between the experiment and theory for neon while mixed results are observed for CH4. This is most likely due to approximations of the target orientation made within the model

Kinematically Complete Study of Low-Energy Electron-Impact Ionization of Argon: Internormalized Cross Sections in Three-Dimensional Kinematics

As a further test of advanced theoretical methods to describe electron-impact single-ionization processes in complex atomic targets, we extended our recent work on Ne(2p) ionization [X. Ren, S. Amami, O. Zatsarinny, T. Pflüger, M. Weyland, W. Y. Baek, H. Rabus, K. Bartschat, D. Madison, and A. Dorn, Phys. Rev. A 91, 032707 (2015)PLRAAN1050-294710.1103/PhysRevA.91.032707] to Ar(3p) ionization at the relatively low incident energy of E0 = 66 eV. The experimental data were obtained with a reaction microscope, which can cover nearly the entire 4π solid angle for the secondary electron emission. We present experimental data for detection angles of 10, 15, and 20⁰ for the faster of the two outgoing electrons as a function of the detection angle of the secondary electron with energies of 3, 5, and 10 eV, respectively. Comparison with theoretical predictions from a B-spline R-matrix (BSR) with pseudostates approach and a three-body distorted-wave (3DW) approach, for detection of the secondary electron in three orthogonal planes as well as the entire solid angle, shows overall satisfactory agreement between experiment and the BSR results, whereas the 3DW approach faces difficulties in predicting some of the details of the angular distributions. These findings are different from our earlier work on Ne(2p), where both the BSR and 3DW approaches yielded comparable levels of agreement with the experimental data

Electron-Impact Ionization of H₂O at Low Projectile Energy: Internormalized Triple-Differential Cross Sections in Three-Dimensional Kinematics

We report a combined experimental and theoretical study of the electron-impact ionization of water (H2O) at the relatively low incident energy of E0=81eV in which either the 1b1 or 3a1 orbitals are ionized leading to the stable H2O cation. The experimental data were measured by using a reaction microscope, which can cover nearly the entire 4π solid angle for the secondary electron emission over a range of ejection energies. We present experimental data for the scattering angles of 6⁰ and 10⁰ for the faster of the two outgoing electrons as a function of the detection angle of the secondary electron with energies of 5 and 10 eV. The experimental triple-differential cross sections are internormalized across the measured scattering angles and ejected energies. The experimental data are compared with predictions from two molecular three-body distorted-wave approaches: one applying the orientation-averaged molecular orbital (OAMO) approximation and one using a proper average (PA) over orientation-dependent cross sections. The PA calculations are in better agreement with the experimental data than the OAMO calculations for both the angular dependence and the relative magnitude of the observed cross-section structures

Theoretical and Experimental Investigation of (e, 2e) Ionization of Argon 3p in Asymmetric Kinematics at Intermediate Energy

The field of electron-impact ionization of atoms, or (e, 2e), has provided significant detailed information about the physics of collisions. For ionization of hydrogen and helium, essentially exact numerical methods have been developed which can correctly predict what will happen. For larger atoms, we do not have theories of comparable accuracy. Considerable attention has been given to ionization of inert gases and, of the inert gases, argon seems to be the most difficult target for theory. There have been several studies comparing experiment and perturbative theoretical approaches over the last few decades, and generally qualitative but not quantitative agreement is found for intermediate energy incident electrons. Recently a nonperturbative method, the B-spline R-matrix (BSR) method, was introduced which appears to be very promising for ionization of heavier atoms. We have recently performed an experimental and theoretical investigation for ionization of argon, and we found that, although the BSR gave reasonably good agreement with experiment, there were also some cases of significant disagreement. The previous study was performed for 200-eV incident electrons and ejected electron energies of 15 and 20 eV. The purpose of the present work is to extend this study to a much larger range of ejected electron energies (15-50 eV) to see if theory gets better with increasing energy as would be expected for a perturbative calculation. The experimental results are compared with both the BSR and two different perturbative calculations

Theoretical and experimental(e,2e)study of electron-impact ionization of laser-aligned Mg atoms

We have performed calculations of the fully differential cross sections for electron impact ionization of magnesium atoms. Three theoretical approximations, the time dependent close coupling (TDCC), the three body distorted wave (3DW), and the Distorted Wave Born Approximation (DWBA), are compared with experiment in this article. Results will be shown for ionization of the 3s ground state of Mg for both asymmetric and symmetric coplanar geometries. Results will also be shown for ionization of the 3p state which has been excited by a linearly-polarized laser which produces a charge cloud aligned perpendicular to the laser beam direction and parallel to the linear polarization. Theoretical and experimental results will be compared for several different alignment angles, both in the scattering plane as well as in the plane perpendicular to the incident beam direction

Theoretical and Experimental Investigation of (e, 2e) Ionization of Argon 3p in Asymmetric Kinematics at Intermediate Energy

The field of electron-impact ionization of atoms, or (e, 2e), has provided significant detailed information about the physics of collisions. For ionization of hydrogen and helium, essentially exact numerical methods have been developed which can correctly predict what will happen. For larger atoms, we do not have theories of comparable accuracy. Considerable attention has been given to ionization of inert gases and, of the inert gases, argon seems to be the most difficult target for theory. There have been several studies comparing experiment and perturbative theoretical approaches over the last few decades, and generally qualitative but not quantitative agreement is found for intermediate energy incident electrons. Recently a nonperturbative method, the B-spline R-matrix (BSR) method, was introduced which appears to be very promising for ionization of heavier atoms. We have recently performed an experimental and theoretical investigation for ionization of argon, and we found that, although the BSR gave reasonably good agreement with experiment, there were also some cases of significant disagreement. The previous study was performed for 200-eV incident electrons and ejected electron energies of 15 and 20 eV. The purpose of the present work is to extend this study to a much larger range of ejected electron energies (15-50 eV) to see if theory gets better with increasing energy as would be expected for a perturbative calculation. The experimental results are compared with both the BSR and two different perturbative calculations