Multi-electron processes in 4.15-11.08 keV/u(13)C(6+) on argon collisions

The relative partial cross sections for C-13(6+)-Ar collisions at 4.15-11.08 keV/u incident energy are measured. The cross-section ratios sigma(2E)/sigma(SC), sigma(3E)/sigma(SC), sigma(4E)/sigma(SC) and sigma(5E)/sigma(SC) are approximately the constants of 0.51 +/- 0.05, 0.20 +/- 0.03, 0.06 +/- 0.03 and 0.02 +/- 0.01 in this region. The significance of the multi-electron process in highly charged ions (HCIs) with argon collisions is demonstrated (sigma(ME)/sigma(SC) as high as 0.79 +/- 0.06). In multi-electron processes, it is shown that transfer ionization is dominant while pure electron capture is weak and negligible. For all reaction channels, the cross-sections are independent of the incident energy in the present energy region, which is in agreement with the static characteristic of classic models, i.e. the molecular Coulomb over-the-barrier model (MCBM), the extended classical over-the-barrier (ECBM) and the semiempirical scaling laws (SL). The result is compared with these classical models and with our previous work of C-13(6+)-Ne collisions

Multi-electron processes in C-13(6+) ions with neon collisions in energy region 4.15-11.08 keV/u

The cross-section ratios of double-, triple-, quadruple-, and the total multi-electron processes to the single electron capture process sigma(DE)/sigma(SC), sigma(TE)/sigma(SC), sigma(QE)/sigma(SC) and sigma(ME)/sigma(SC)) as well as the relative ratios among reaction channels in double-electron active, triple-electron active and quadruple- electron active are measured in C-13(6+) -Ne collision in the energy region of 4.15-11.08 keV/u by employing position-sensitive and time-of-flight coincident techniques. It is determined that the cross-section ratios sigma(DE)/sigma(SC), sigma(TE)/sigma(SC), sigma(QE)/sigma(SC) and sigma(ME)/sigma(SC) are approximately the constants of 0.20 +/- 0.03, 0.16 +/- 0.04, 0.06 +/- 0.02 and 0.42 +/- 0.05. These values are obviously smaller than the predictions of the molecular Coulomb over-the-barrier model (MCBM) [J. Phys. B 23 (1990) 4293], the extended classical over-the-barrier model (ECBM) [J. Phys. B 19 (1986) 2925] and the semiempirical scaling laws (SL) [Phys. Rev. A 54 (1996) 4127]. However, the relative ratios among partial processes of DE, TE and QE are found to depend on collision energy, which suggests that the collision dynamics depends on the collision velocity. The limitation of velocity-independent character of ECBM, MCBM and SL is undoubtedly shown.

Shell effect on stabilization processes following multi-electron transfer in slow Arq+-Ar (g=6-9, 11) collisions

We experimentally investigate the shell effect on the stabilization processes following the multi-electron transfer in slow collisions of Arq+-Ar (q = 6-9, It) The relative cross-section ratios of multi-electron transfer and of the subsequent stabilization with respect to single-electron capture are measured meanwhile compared with the theoretical results predicted by the classical over-barrier model. Our result indicates that the multi-electron transfer is dominant when the projectile charge is large and the subsequent stabilization shows a dramatic variation if the projectile L-shell configuration becomes open. It shows that the subsequent stabilization processes of multiply excited scattering ions have a strong dependence on the projectile shell. (C) 2010 Elsevier BV All rights reserved.

Influence of core property on multi-electron process in slow collisions of isocharged sequence ions with neon

Influence of core property on multi-electron process in the collisions of q = 6-9 and 11 isocharged sequence ions with Ne is investigated in the keV/u region The cross-section ratios of double-, triple-, quadruple- and total multi-electron processes to the single electron capture process as well as the partial ratios of different reaction channels to the relevant multi-electron process are measured by using position-sensitive and time-of-flight techniques The experimental data are compared with the theoretical predictions including the extended classical over-barrier model, the molecular Columbic barrier model and the semi-empirical scaling law Results show a core effect on multi-electron process of isocharge ions colliding with Neon, which is consistent with the results of Helium we obtained previously

Atomic excitation during recollision-free ultrafast multi-electron tunnel ionization

Modern intense ultrafast pulsed lasers generate an electric field of sufficient strength to permit tunnel ionization of the valence electrons in atoms(1). This process is usually treated as a rapid succession of isolated events, in which the states of the remaining electrons are neglected(2). Such electronic interactions are predicted to be weak, the exception being recollision excitation and ionization caused by linearly polarized radiation(3). In contrast, it has recently been suggested that intense field ionization may be accompanied by a two-stage 'shake-up' reaction(4). Here we report a unique combination of experimental techniques(5-8) that allows us to accurately measure the tunnel ionization probability for argon exposed to 50-fs laser pulses. Most significantly for the current study, this measurement is independent of the optical focal geometry(7,8), equivalent to a homogenous electric field. Furthermore, circularly polarized radiation negates recollision. The present measurements indicate that tunnel ionization results in simultaneous excitation of one or more remaining electrons through shake-up(9). From an atomic physics standpoint, it may be possible to induce ionization from specific states, and will influence the development of coherent attosecond extreme-ultraviolet-radiation sources(10). Such pulses have vital scientific and economic potential in areas such as high-resolution imaging of in vivo cells and nanoscale extreme-ultraviolet lithography.

On the recollision-free excitation of krypton during ultrafast multi-electron tunnel ionization

The probability of multiple ionization of krypton by 50 femtosecond circularly polarized laser pulses, independent of the optical focal geometry, has been obtained for the first time. The excellent agreement over the intensity range 100 TW cm-2 to 100 PW cm-2 with the recent predictions of Kornev et al (2003 Phys. Rev. A 68 043414) provides the first experimental confirmation that non-recollisional electronic excitation can occur in strong-field ionization. This is particularly true for higher stages of ionization, when the laser intensity exceeds 10 PW cm-2 as the energetic departure of the ionized electron(s) diabatically distorts the wavefunctions of the bound electrons. By scaling the probability of ionization by the focal volume, we discuss why this mechanism was not apparent in previous studies.

High-mass Drell-Yan cross-section and search for new phenomena in multi-electron/positron final states with the ATLAS detector

The Standard Model of particle physics is a very successful theory which describes nearly all known processes of particle physics very precisely. Nevertheless, there are several observations which cannot be explained within the existing theory. In this thesis, two analyses with high energy electrons and positrons using data of the ATLAS detector are presented. One, probing the Standard Model of particle physics and another searching for phenomena beyond the Standard Model.rnThe production of an electron-positron pair via the Drell-Yan process leads to a very clean signature in the detector with low background contributions. This allows for a very precise measurement of the cross-section and can be used as a precision test of perturbative quantum chromodynamics (pQCD) where this process has been calculated at next-to-next-to-leading order (NNLO). The invariant mass spectrum mee is sensitive to parton distribution functions (PFDs), in particular to the poorly known distribution of antiquarks at large momentum fraction (Bjoerken x). The measurementrnof the high-mass Drell-Yan cross-section in proton-proton collisions at a center-of-mass energy of sqrt(s) = 7 TeV is performed on a dataset collected with the ATLAS detector, corresponding to an integrated luminosity of 4.7 fb-1. The differential cross-section of pp -> Z/gamma + X -> e+e- + X is measured as a function of the invariant mass in the range 116 GeV < mee < 1500 GeV. The background is estimated using a data driven method and Monte Carlo simulations. The final cross-section is corrected for detector effects and different levels of final state radiation corrections. A comparison isrnmade to various event generators and to predictions of pQCD calculations at NNLO. A good agreement within the uncertainties between measured cross-sections and Standard Model predictions is observed.rnExamples of observed phenomena which can not be explained by the Standard Model are the amount of dark matter in the universe and neutrino oscillations. To explain these phenomena several extensions of the Standard Model are proposed, some of them leading to new processes with a high multiplicity of electrons and/or positrons in the final state. A model independent search in multi-object final states, with objects defined as electrons and positrons, is performed to search for these phenomenas. Therndataset collected at a center-of-mass energy of sqrt(s) = 8 TeV, corresponding to an integrated luminosity of 20.3 fb-1 is used. The events are separated in different categories using the object multiplicity. The data-driven background method, already used for the cross-section measurement was developed further for up to five objects to get an estimation of the number of events including fake contributions. Within the uncertainties the comparison between data and Standard Model predictions shows no significant deviations.

Double electron processes in collisions of partially stripped ions Cq+ (q=1-4) with helium

The multi-electron processes are investigated for 17.9-120keV/u C1+, 30-323 keV/u C2+, 120-438 keV/u C3+, 287-480keV/u C4+ incident on a helium target. The cross-section ratios of double electron (DE) process to the total of the single electron (SE) and the double electron process (i.e. SE+DE), the direct double electron (DDI) to the direct single ionization (DSI) as well as the contributions of DDI to DE and of TI to DE are measured using coincidence techniques. The energy and charge state dependences of the measured cross-section ratios are studied and discussed.

The RMT method for many-electron atomic systems in intense short-pulse laser light

We describe a new ab initio method for solving the time-dependent Schrödinger equation for multi-electron atomic systems exposed to intense short-pulse laser light. We call the method the R-matrix with time-dependence (RMT) method. Our starting point is a finite-difference numerical integrator (HELIUM), which has proved successful at describing few-electron atoms and atomic ions in strong laser fields with high accuracy. By exploiting the R-matrix division-of-space concept, we bring together a numerical method most appropriate to the multi-electron finite inner region (R-matrix basis set) and a different numerical method most appropriate to the one-electron outer region (finite difference). In order to exploit massively parallel supercomputers efficiently, we time-propagate the wavefunction in both regions by employing Arnoldi methods, originally developed for HELIUM.

Chelation-enforced metal-arene interactions : insights into substrate binding and catalysis by late transition metal complexes

Understanding and catalyzing chemical reactions requiring multiple electron transfers is an endeavor relevant to many outstanding challenges in the field of chemistry. To study multi-electron reactions, a terphenyl diphosphine framework was designed to support one or more metals in multiple redox states via stabilizing interactions with the central arene of the terphenyl backbone. A variety of unusual compounds and reactions and their relevance toward prominent research efforts in chemistry are the subject of this dissertation.

Chapter 2 introduces the para-terphenyl diphosphine framework and its coordination chemistry with group 10 transition metal centers. Both mononuclear and dinuclear compounds are characterized. In many cases, the metal center(s) are stabilized by the terphenyl central arene. These metal–arene interactions are characterized both statically, in the solid state, and fluxionally, in solution. As a proof-of-principle, a dinickel framework is shown to span multiple redox states, showing that multielectron chemistry can be supported by the coordinatively flexible terphenyl diphosphine.

Chapter 3 presents reactivity of the terphenyl diphosphine when bound to a metal center. Because of the dearomatizing effect of the metal center, the central arene of the ligand is susceptible to reactions that do not normally affect arenes. In particular, Ni-to-arene H-transfer and arene dihydrogenation reactions are presented. Additionally, evidence for reversibility of the Ni-to-arene H-transfer is discussed.

Chapter 4 expands beyond the chelated metal-arene interactions of the previous chapters. A dipalladium(I) terphenyl diphosphine framework is used to bind a variety of exogenous organic ligands including arenes, dienes, heteroarenes, thioethers, and anionic ligands. The compounds are structurally characterized, and many ligands exhibit unprecedented bindng modes across two metal centers. The relative binding affinities are evaluated spectroscopically, and equilibrium binding constants for the examined ligands are determined to span over 13 orders of magnitude. As an application of this framework, mild hydrogenation conditions of bound thiophene are presented.

Chapter 5 studies nickel-mediated C–O bond cleavage of aryl alkyl ethers, a transformation with emerging applications in fields such as lignin biofuels and organic methodology. Other group members have shown the mechanism of C–O bond cleavage of an aryl methyl ether incorporated into a meta-terphenyl diphosphine framework to proceed through β-H elimination of an alkoxide. First, the electronic selectivity of the model system is examined computationally and compared with catalytic systems. The lessons learned from the model system are then applied to isotopic labeling studies for catalytic aryl alkyl ether cleavage under dihydrogen. Results from selective deuteration experiments and mass spectrometry draw a clear analogy between the mechanisms of the model and catalytic systems that does not require dihydrogen for C–O bond cleavage, although dihydrogen is proposed to play a role in catalyst activation and catalytic turnover.

Appendix A presents initial efforts toward heterodinuclear complexes as models for CO dehydrogenase and Fischer Tropsch chemistry. A catechol-incorporating terphenyl diphosphine is reported, and metal complexes thereof are discussed.

Appendix B highlights some structurally characterized terphenyl diphosphine complexes that either do not thematically belong in the research chapters or proved to be difficult to reproduce. These compounds show unusual coordination modes of the terphenyl diphosphine from which other researchers may glean insights.

X-ray spectra induced by slow highly charged Arq+ ions in collision with Nb surface

The X-ray spectra of Nb surface induced by Arq+ (q = 16,17) ions with the energy range from 10 to 20 keV/q were studied by the optical spectrum technology. The experimental results indicate that the multi-electron excitation occurred as a highly charged Ar16+ ion was neutralized below the metal surface. The K shell electron of Ar16+ was excited and then de-excited cascadly to emit K X-ray. The intensity of the X-ray emitted from K shell of the hollow Ar atom decreased with the increase of projectile kinetic energy. The intensity of the X-ray emitted from L shell of the target atom Nb increased with the increase of projectile kinetic energy. The X-ray yield of Ar17+ is three magnitude orders larger than that of Ar16+.

X-ray spectra produced by interaction of Ar16+ and Ar17+ with Zr

The 10-20 qkeV Ar16+ and Ar17+ ions produced by SECRAL enter on metallic surface of Zr. In this interaction, the multi-electron excitation possibly occurred in the neutralization of the highly charged Ar16+ ions, which produced vacancy in the K shell. Electron of the high n state de-excited to K vacancy gives off X-ray. The experimental results show that X-ray intensities for the Ar hollow atom decrease with increase of incidence energy, and L beta X-ray intensities of target atom Zr increase with increasing incidence energy. K alpha X-ray yield per ion for Ar17+ was five orders of magnitude greater than that for Ar16+

X-ray spectra induced in highly charged Ar-40(q+) interacting with Au surface

By use of optical spectrum technology, the spectra of X-ray induced by highly charged Ar-40(q+) ions interacting with Au surface have been studied. The results show that the argon K alpha X-ray were emitted from the hollow atoms formed below the surface. There is a process of multi-electron exciting in neutralization of the Ar16+ ion, with electronic configuration 1s(2) in its ground state below the solid surface. The yield of the projectile K alpha X-ray is related to its initial electronic configuration, and the yield of the target X-ray is related to the projectile kinetic energy.

X-ray emission produced by interaction of highly ionized Arq+ ions with metallic targets

This paper studies the X-ray spectra produced by the interaction of highly charged ions of Arq+ (q = 16, 17, 18) with metallic surface of Be, Al, Ni, Mo and Au respectively. The experimental results show that the K alpha X-ray emerges from under the surface of solid in the interaction of ions with targets. The multi-electron excitation occurred in the process neutralization of the Ar16+ in electronic configuration of 1s(2) in metallic surfaces, which produces vacancy in the K shell. Electron from high n state transition to K vacancy gives off X-ray. We find that there is no obvious relation between the shape of X-ray spectra and the different targets. The X-ray yield of incident ions are associated with initial electronic configuration. The X-ray yield of target is related to the kinetic energy of the incident ions.

基于ECRIS的等电荷态序列离子与氦、氖、氩碰撞反应中的多电子过程研究

本工作设计并建立了一个离子-原子碰撞实验终端。该终端具有一定的通用性，可用于我所EcRIS、ECRIS一300kV高压平台和兰州大学Zxl．7MV串列加速器。终端的设计特别考虑了气体靶实验中系统的动态真空和对高品质弱束流流强的控制。2004年7月-10月，利用我所ECRIS提供的束流，在该终端上进行了首轮实验。本工作指出，除了入射离子的电荷态和速度外，其空能级结构是碰撞反应的另一个主导因素，并在此基础上提出了等电荷态序列离子的概念。为了确定离子空能级结构对碰撞反应的影响，本工作系统研究了等速度的q＝6序列离子（C6＋、N6＋、。6＋、F6＋、Ne6＋、Ar6＋、co6＋）、q＝7序列离子（07＋、F7＋、Ne7＋、57＋、Ar7＋）、q＝8序列离子（FS＋、Nes＋、Ars＋、cos＋）、q：9序列离子（Fg＋、Neg＋、519＋、59＋、Arg＋、cag＋）和叮：11序列离子（Si1、Aill＋、Call＋）与氦、氖、氢的碰撞反应。实验证实，对于等速度、等电荷态序列离子，碰撞反应与离子种类强烈相关。利用同位素纯的13coZ作为EcRIs的工作气体，获得了纯净的全裸离子13C6＋束流，研究了13C6＋离子与氦、氖、氢碰撞反应与碰撞速度的关系。实验发现，在C6十一He的碰撞反应中，纯双电子俘获（DC）与双电子转移（DE）截面比JDcDIZ随碰撞速度的增加而明显下降，这暗示准分子俄歇机制在本能区C6＋一He碰撞反应中的贡献不可忽略。用MCBM描述离子-原子相互作用阶段，用电子蒸发模型统一处理碰撞后多电了激发态散射离子和反冲离子的衰变，作者编写了计算程序COBEEM。经典过垒模型（如ECBM和MCBM）仅用电荷态q一个参数描述入射离子，本工作实验证实了这种描述是不完备的。COBEEM程序对此问题进行了初步修正。该程序还包含了ECBM和Selberg等人提出了经验公式的计算。