PROJECTILE CHARGE EFFECTS IN MULTIPLE IONIZATION OF ARGON BY POSITRON AND ELECTRON IMPACT A. C. F. Santos, A. Hasan and R. D. DuBois Department of Physics, University of Missouri - Rolla MO 65409, USA. Abstract. Differential single- and multiple-ionization cross section ratios have been measured for 750 eV positron and electron impact on argon as a function of the projectile energy-loss from threshold up to 85% of the initial projectile energy. In addition, differential multiple ionization cross section ratios have been obtained for 500 eV electron impact as a function of both the scattering angle and projectile energy loss. The differential singleionization cross sections obtained with positrons and electrons are found to have the same shape, i.e., the same energy loss dependence, in agreement with distorted wave Born predictions. The differential double- and tripleionization cross sections obtained by electron impact, however, are systematically larger than those obtained with positron impact. This charge effect has been attributed to the quantal interference between the mechanisms leading to double ionization. ejection the cross sections for positron impact exceed those for electron impact by an order of magnitude. INTRODUCTION Single and multiple ionization of atoms and molecules has been a subject of interest for decades1-5. At sufficiently high projectile velocities, single ionization is well described by first order theories such as the first Born Approximation. At lower velocities, however, deviations from perturbative theories arise. Also the mass and charge of the projectile can influence which channels participate and what theoretical approximation can be applied. On the other hand, the study of multiple ionization is a tougher task; theoretically due to the presence of many bodies in the continuum, all interacting by the long range Coulomb field, and experimentally due to the inherent experimental difficulties. However, such information is important since comparisons of electron and positron impact data can be used to elucidate these complex many-body interactions and provide information about electron correlation, for example, e+ projectiles are distinguishable from the ejected electron. Another important difference is that the repulsive/attractive Coulomb field switches when the projectile charge is changed. Several important studies have also been performed by the University of London group4-6. For instance, they measured the energy distributions of positrons and electrons scattered at angles around 0o in coincidence with Ar+ ions at 100, 150 and 250 eV. Very similar distributions for both projectiles were found except in the region when the outgoing velocities of the scattered projectile and the ionized electron were equal. This paper compares single and multiple differential ionization fractions resulting from electron and positron impact on argon, as a function of projectile energy loss and scattering angle. The processes studied can be represented as e ± ( E ) + Ar → e ± ( E − ∆E , ∆θ ) + Ar q + + qe − . (1) In the case of electron impact, the projectile and the ejected electron are indistinguishable, however, the fastest of the electrons in the continuum is attributed to be the scattered projectile. For 750 eV electron and positron impact the horizontal and vertical acceptance angles were approximately ± 22o; for 500 eV electron impact, an improved angular resolution was used where horizontal and vertical angles were ± 6.5o and ± 22o, respectively. To date, few differential studies for positron impact have been performed. Notable work includes the studies of Schmitt et al.3 who determined doubly differential ionization cross sections for 100 eV positron and electron impact on argon atoms by energy- and angle- resolved measurements. They found that at small angles of electron CP680, Application of Accelerators in Research and Industry: 17th Int'l. Conference, edited by J. L. Duggan and I. L. Morgan © 2003 American Institute of Physics 0-7354-0149-7/03/$20.00 195 projectile charge on multiple ionization. Differential single and double ionization cross section fractions for 750 eV e+ and e- impact as a function of the projectile energy loss are presented in Fig. 2. The data are for projectiles scattered into forward vertical angles between ± 22o. The relative percent yields were obtained from EXPERIMENTAL Collimated e+ and e- beams are delivered by a 22Na source coupled to a tungsten-mesh moderator. After crossing a gas jet at right angles, the beams are energy and angle analyzed by a modified cylindrical spectrometer and recorded by a position sensitive microchannel plate detector housed at the focal plane of the spectrometer. N q+ f Projectiles having different energies are focused to different horizontal positions of the detector. One can investigate different projectile energy-loss ranges by setting the inner and outer spectrometer voltages, VIN and VOUT , respectively (see Fig. 1). In addition, angular information about the scattered projectiles is contained on the vertical positions. The argon gas flow is kept constant by a flow controller and monitored by a thermocouple. Typical operating conditions gave a chamber pressure of 1-2 × 10-5 Torr. The singly and multiply charged recoil ions are extracted from interaction region by a weak (10 V/cm) electric field and separated according to their mass-tocharge ratio by a time-of-flight spectrometer. Finally, the recoil ions created by projectiles in the interaction region impinge onto another position sensitive microchannel plate detector. The recoil signals provide time marks for the start of a time-to-digital converter (TDC). Fig.1 shows schematically the experimental apparatus. = 3 ∑N i =1 ε q+ (2) i+ ε i+ where f q+ is the charge-state fraction of q times ionized argon, ε q+ is the microchannel plate detection efficiency for the ion Arq+, and N q+ is the number of scattered positrons or electrons in coincidence with the Arq+ recoil ions. The target gas pressure was kept low enough to guarantee single collision conditions. The same projectile detection efficiencies were assumed for positron and electron impact. The single ionization cross sections for both positron and electron impact (not shown) were found to have the same energy loss dependence, as expected, and to be in good agreement with theoretical calculations using distorted wave Born calculations9, since the cross section for positronium formation is expected to be negligible at this energy. As seen in Fig. 2, the contributions of single ionization of argon by electron and positron impact decrease slowly and monotonically as a function of the PS M C P TD C q+ 0 10 PS M C P gas needle -1 V IN Fraction TO F V+ Incidentbeam V- 10 -2 10 VO UT Figure 1. Schematic of the experimental set-up showing beam trajectories. The modified cylindrical spectrometer is used to collect and focus a wide range of horizontal scattering energies onto the projectile detector, a 50 mm diameter microchannel plate mounted in chevron configuration. By changing the spectrometer voltages, VIN and VOUT, different projectile energy loss ranges are accessed. -3 10 0 100 200 300 400 500 600 700 Energy-Loss (eV) projectile energy-loss. Figure 2. Fractions of single and double ionization of argon as a function of the projectile energy loss for 750 eV positron and electron impact on argon. Data are for projectiles scattered into horizontal and vertical angles between ± 22o. The solid lines show double photoionization fractions from Holland et al. [10]. Closed circles: single ionization by electron impact; open circles: single ionization by positron impact; closed triangles: double ionization EXPERIMENTAL METHOD The main scope of the present article is to study multiple ionization processes and, particularly the role played by the 196 by electron impact; open triangles: double ionization by positron impact. eV, the amount of double photoionization is slightly larger than the corresponding amount for 500 eV electron impact. The fraction of triple ionization presents an even faster rise and stays constant at about 7% at higher energy losses. The fractions of double ionization increase rapidly for the first 100 eV and continue increasing more slowly up to 250 eV (Fig. 2). For large energy-loss, they are approximately constant for both projectiles. The relative amount of double ionization is systematically larger for electrons than for positron impact. At higher projectile energy-losses, the amount of double ionization is roughly 30% for electrons and 20% for positrons. Fig. 2 also presents the double ionization fraction by photoionization from ref. [10]. The sharp increase in the photon data above 248 eV is due to the opening of the L shell. 0 10 Fraction -1 In the case of argon triple ionization, a huge difference is observed in Fig. 3 between positron and electron impact in both shape and magnitude. The threshold for removing three electrons from the M-shell in argon is 84.1 eV. For positron impact, triple ionization was not observed below 200 eV, only a steep rise after the L shell is opened. For electron impact, triple ionization is clearly observable below the L-shell threshold. This can perhaps be attributed to the detection of ionized electrons, which did not occur in our positron study since scattered projectiles are detected. 0 -3 10 50 100 150 200 250 300 Figure 4. Fractions of single and double ionization of argon as a function of the projectile energy loss for 500 eV electron impact on argon. Data are for projectiles scattered into horizontal and vertical angles between ± 6 and 8o, respectively. The solid lines show double photoionization fractions from Holland et al. [10]. Closed squares: single ionization; open circles: double ionization; closed triangles: triple ionization. Ar -1 Fraction 0 Energy-Loss (eV) 10 DISCUSSION Figures 3 and 4 show that double and triple ionization cross sections fractions for electron impact are systematically higher than the corresponding fraction for positron impact, while the photoionization fractions are intermediate between the positron and electron fractions. McGuire11 suggested that the difference between the double ionization cross sections for electron and proton impact to be a charge effect due to the interference between the so called two-step and shake-off processes resulting in an interference term proportional to the third power of the projectile charge. -2 10 3+ Ar L II, III LI -3 10 -2 10 3+ 10 10 0 100 200 300 400 500 600 700 Energy-Loss (eV) Figure 3. Fractions of triple ionization of argon as a function of the projectile energy loss for 750 eV positrons and electrons scattered into vertical angles between ± 22o. The dotted line represents the fraction of triple photoionization of argon from ref. [10]. The vertical lines indicate thresholds for single, double and triple ionization as well as the thresholds for removing electrons from the L shell. Andersen et al.12 showed that the double ionization total cross sections of helium for proton and antiproton impact also depended upon the sign of the projectile charge. Another explanation for the dependence of the double ionization on the projectile charge was given by Olson13 using the classical trajectory Monte Carlo calculations as an effect of the transient destabilization of the target due to the difference in screening by the projectiles. Figure 4 shows the results for single, double and triple ionization of argon by 500 eV electron impact as a function of the projectile energy-loss. Included is the fraction of double photoionization of argon10. Generally speaking, the amount of multiple ionization is smaller at 500 eV when compared with 750 eV, as expected. The amount of double ionization increases rapidly up to 130 eV and reaches a plateau at about roughly 15%. Between 130 eV and 230 The contributions of the inner-shell ionization cross sections cannot be neglected in the analysis of the multiple ionization cross sections. Negative particles may be 197 expected to have larger inner-shell ionization cross sections due to the static interaction with the nucleus9,11. electron impact systematically exceed those for positron impact. This effect has been attributed to the quantal interference of the processes leading to multiple ionization. 0 10 ACKNOWLEDGMENTS DDCS (arb. units) This work is supported by National Science Foundation, grant No. PHY0097902 and CNPq (Brazil). REFERENCES 1. M.Charlton and G. Laricchia, J. Phys. B 23, 1045 (1990). -2 10 2. G. Laricchia, The Physics of Electronic and Atomic Collisions ed. L. J. Dube, J. B. A. Mitchell, J. W. McConkey, and C. E. Brion (New York: AIP) 385 (1995). 3. A. Schmitt, U. Cerny, H. Möller, W. Raith, and M. Weber, Phys. Rev. A 49, R5 (1994). -8 -6 -4 -2 0 2 4 6 4. Á. K`vJr, G. Laricchia, and M. Carlton, J. Phys. B 26, L575 (1993). 8 Angle (deg) 5. Á. K`vJr, G. Laricchia, and M. Carlton, J. Phys. B 27, 2409 (1994). Figure 5. Doubly differential cross sections (in arbitrary units) for 500 eV electron impact on argon, in the final electron energy range from 470-460 eV as a function of the electron scattering angle. Single ionization: closed circles; double ionization (open circles). The data were corrected by the recoil detection efficiency. 6. Á. K`vJr, R. M. Finch, M. Charlton, and G. Laricchia, J. Phys. 30, L507 (1997). 7. R. A. Sparrow and R. E. Olson, J. Phys. B 27, 2647-2655 (1994). 8. Á. K`vJr, G. Laricchia, and M. Carlton, J. Phys. B 26, L575 (1993). Figure 5 presents DDCS for 500 eV electron impact on argon in the scattered electron energy range from 460 to 470 eV as a function of the scattering angle. The present angular resolution is approximately 2o. Both the single and double ionization cross sections decrease as a function of the scattering angle. The ratio of double-to-single ionization cross sections presented in Fig. 5 ranges from roughly 1% at the larger angles (± 8o) to 1.6% near zero degrees. 9. R. D. DuBois, C. Doudna, C. Lloyd, M. Khaveci, Kh. Khayyat, Y. Zhou, and D. H. Madison, J. Phys. B 34, L783 (2001). 10. D. M. P. Holland, K. Codling, J. B. West, and G. V. Marr, J. Phys. B 12, 2465 (1979). 11. J. H. McGuire, Phys. Rev. Lett 49, 1153 (1982). 12. L. H. Andersen, P. Hvelplund, H.Knudsen, S. P. Møller, and A. H. Sørensen, Phys. Rev. A 36, 3612 (1987). CONCLUSIONS 13. R. E. Olson, Phys. Rev. A 36, 1519 (1987). In conclusion, we have compared the multiple ionization differential cross sections fractions for 750 eV e+ and e- impact on Ar as a function of projectile energy-loss. Angular distributions of the projectiles have also been measured for 500 eV electrons. The relative contribution of multiple ionization increases with increasing projectile energy loss. The double and triple ionization fractions for 198
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