Physica Scripta. T92, 227^229, 2001 Mechanisms for Plasmon Production by Highly Charged Neon Ions Interacting with an Al Surface N. Stolterfoht1, J. H. Bremer1, V. Ho¡mann1, D. Niemann1, M. RÎsler1 and R. Baragiola2 1 2 Hahn-Meitner-Institut Berlin GmbH, Glienickerstr. 100, D-14109 Berlin, Germany Laboratory for Atomic and Surface Physics, University of Virginia, Engineering Physics, Charlottesville, VA 22901, USA Received July 31, 2000; accepted September 20, 2000 pacs ref: 71.45.GM, 73.20.Mf, 34.50.Dy Abstract 4 Low-energy electrons ejected by 1^4 keV Ne ion impact on an Al surface were measured. Spectral structures found near 11 eV were attributed to the decay of plasmons induced by potential energy of the projectile. The data were used to determine absolute values for electron yields from the plasmon decay, which were primarily studied as a function of the incidence angle of the Ne4 projectile. Strong variations of the plasmon yield are observed when the angle of incidence reaches that of specular re£ection indicating signi¢cant changes in the contributions to plasmon production from below and above surface. 1. Introduction Valence electrons in metals can take part in quantized collective oscillations known as plasmons whose formation by charged particle impact can be described within the framework of the free-electron gas approximation [1,2]. The decay of plasmons occurs predominantly by energy transfer into a single valence electron in an interband transition [3]. Hence, electrons of characteristic energies are ejected from the metal providing a signature for plasmons, which can experimentally be studied by means of electron spectroscopy. Early experiments with ion impact have been performed using fast projectiles that create plasmons via direct Coulomb excitation [4]. Only recently, an increasing attention has been devoted to plasmon production by slow projectiles. For ions with energies below a few keV, various groups have considered the process of plasmon-assisted capture where the transfer of potential energy from the projectile produces a plasmon [5^11]. Particular attention has been focused on slow heavy ions incident on a surface with a high charge state [7,12^14]. The characteristic feature of a highly charged ion is its large potential energy which has prompted much interest in the ¢eld of ion-solid interactions [15]. Above the surface, highly charged ions strongly attract several electrons, which are resonantly captured into high Rydberg states whereas inner shells remain empty. Thus, the projectiles evolve into hollow atoms whose formation and decay imply various novel processes. The mechanisms for plasmon production resulting in spectral structures at low electron energies are still under debate. In particular, controversial ideas have been raised in view of structures observed near 11 eV for Al surfaces. Apart from Auger capture processes [16], the decay of both bulk plasmons [6,7,13] and surface plasmons [8,10,11] have been considered to be responsible for the structure near 11 eV. The production of bulk and surface plasmons was found to be dependent on the incident energy and angle [10]. # Physica Scripta 2001 In the present work, to gain more information about highly charged ions, we study structures in the electron spectra near 11 eV by impact of 1^4 keV Ne4 on Al as a function of the incidence angle of the projectile. It is shown that the use of highly charged projectiles, give rise to characteristic properties in the scenario of plasmon production. 2. Experimental method and results The measurements were carried out at the 14.5 GHz electron cyclotron resonance (ECR) source at the Ionenstrahl-Labor (ISL) in Berlin using an ultra-high vacuum chamber equipped with a rotatable electron spectrometer [17]. Details of the experimental method have been presented before [12,13,18]. A beam of Ne4 ions was collimated to a diameter of about 1 mm and directed onto a clean Al(111) target. The pressure in the chamber was a few 10^10 mbar. The emission of electrons from the target was measured using an electrostatic parallel-plate spectrometer. The spectrometer e¤ciency and the ion current were determined [18] so that absolute values for electron emission yield could be measured. The experimental set-up was optimized to reliably measure these electron yields at energies as low as 2^4 eV. Examples for results of absolute electron yields N e; O dY =dedO measured in our group are given in Ref. [7,12,13]. The electron spectra exhibit various structures which can be attributed to emission of Auger electrons as well as the decay of plasmons produced within the surface and the bulk. Structures due to the decay of surface and bulk plasmons can be observed in the low-energy range from about 5 to 14 eV [2,4]. To enhance the visibility of the plasmon structures, which are superimposed on an intense background from other processes, it is common practice to di¡erentiate the measured electron intensities N e; O. Results for the derivative dN=de are given in Fig. 1 for 2 keV Ne4 impact on Al. The graphs labeled (a), (b), and (c) on the left-hand side show dN=de for incidence angles of c 1 ; 8 , and 18 , respectively, relative to the surface plane. The observation angle of the electrons is equal to b 70 relative to the surface normal. For the de¢nitions of the angles see also the inset in Fig. 1(a). Each dN=de curve clearly shows a structure near 11 eV which is attributed to plasmon decay [7,13]. As discussed in detail previously [13], the plasmon structure appears as a negative peak (dip) when performing the derivative of the electron intensity. This dip was separated from the electron background by ¢tting the intensities above and below Physica Scripta T92 228 N. Stolterfoht et al. Fig. 1. Derivative of electron yields measured for 2 keV Ne4 impact on Al as a function of the electron energy. In (a), (b), and (c) data are given for the incidence angles c 1 , 8 and 18, respectively, as shown in the left hand side graphs. On the right hand side the plasmon structures are shown after subtraction of the background. the plasmon structure by a second-order polynomial (given in Fig. 1(a^c) as dashed lines). On the right hand side, the corresponding plasmon dip structures are shown as obtained after subtraction of the background intensity. It is seen that the centroid energy of the dip is slightly shifted as the incidence angle increases. Furthermore, it is found that the dip intensity for the intermediate angle of c 8 is smaller than those for c 1 and 18 . For further analysis of the data we integrated the peak structures after background subtraction. As shown in detail previously, the electron yields from plasmon decay can be obtained by multiplying the integrated results by 6.3 eV [19]. In Fig. 2(a^c) absolute values of the electron yield dY =dO are plotted for projectile energies of 1, 2, and 4 keV, respectively. The dY =dO curves show strong variations with the incidence angle c. After a region of nearly constant values, the yield decreases to a minimum and rises again at small angles, whereby the location of the minimum changes with the projectile energy. To interpret the present observations we performed model calculations described in the following. 3. Interpretation and discussion As in previous work [5^7] we consider excitation by potential energy transfer as a primary mechanism for plasmon production by slow heavy ions. This mechanism involves the capture of a valence electron into the L shell of the Ne projectile, which provides the energy for plasmon creation. However, other mechanisms for plasmon creation may be Physica Scripta T92 Fig. 2. Plasmon yield from Al for Ne4 impact as a function of the incidence angle c. In (a), (b), and (c) data are given for impact energies of 1, 2, and 4 keV, respectively. The curves are due to model calculations indicating the contributions from above and below the surface. considered. Note ¢rst that Ne orbitals higher than the 2p shell cannot participate in the bulk plasmon creation, since those orbitals are not bound inside the solid [20]. However, energetic electrons produced directly in collisions as well as Auger electrons may excite plasmons when traveling through the solid [13,21]. For a better understanding of the data in Fig. 2, we consider two regions relevant for plasmon production: above the surface near the jellium edge and below the surface de¢ned by the ¢rst atomic layer. These contributions are likely to be associated with surface and bulk plasmons, respectively. One may argue that the consideration of surface plasmons is inconsistent with the present observations. In Fig. 1 the 11 eV structure observed for c 1 is signi¢cantly larger in energy than Al surface plasmons observed at 6.4 eV [4]. However, as emphasized previously [8,10], the latter energy refers to zero momentum plasmons, whereas surface plasmons with larger momentum may produce electrons of energies as high as 11 eV. An increase of the momentum transfer with increasing energy would be consistent with the shift of the plasmon dip observed in Fig. 1. Moreover, high momentum transfer may result in the production of surface plasmons of higher multipoles [10]. In addition, similar to He*[16] one should consider the Auger capture into Ne*, which also gives rise to electrons with energies near 11 eV for Al. # Physica Scripta 2001 Mechanisms for Plasmon Production by Highly Charged Neon Ions Interacting with an Al Surface In the following, the electron yields due to above- and below-surface processes are denoted dYA =dO and dYB = dO, respectively. These yields are governed by the re£ection probability pR of the projectile at the surface, which strongly depends on the incidence angle c. In a simple model we set dYB B 1 dO pR 1 where B is a constant assuming that the ions penetrating into the solid produce bulk plasmons. Similarly, we set dYA ApR 1 dO pD 2 where A is a constant and pD is the survival probability for the hollow neon atom moving through the jellium region of thickness d that is relevant for plasmon assisted capture (i.e. emerging into the vacuum with at least one vacancy in the L shell). By de¢nition these ions are lost for plasmon production. In the analysis, the re£ection and decay probabilities are determined from other sources, whereas A and B are treated as free parameters. We assume an exponential decay law pD exp u=vz , where u is a constant velocity and vz v sin c is the vertical velocity of the projectile. It can readily be shown that u 2dGL is obtained as the double passage of the jellium edge region within the lifetime of the hollow Ne atom. Both the velocity u and the re£ection probability pR were determined from an independent analysis of the atomic Ne** Auger peak observed at 22 eV (exhibited in the electron spectra of, e.g., Refs. [6,13]). Finally, the sum dYA =dO dYB =dO was ¢tted to the experimental data treating A and B as adjustable parameters for each incident energy. The results are plotted in Fig. 2 where apart from the sum (solid lines) also the individual yields dYA =dO (dashed lines) and dYB =dO (dashed dotted lines) are given. It is seen that the theoretical data compare well with experiment providing con¢dence for the essential features of the present model. The comparison explains detailed features of the experimental results. For instance, the existence of a minimum in the electron yields and its shift with the projectile energy can be associated with the onset of specular re£ection of the projectiles at the surface. The main goal of the present analysis is the (approximate) separation of above and below surface contributions to the plasmon yield. We note that these contributions are governed by the parameters A and B, respectively, which # Physica Scripta 2001 229 are obtained as asymptotic electron yields A dYA c ! 0=dO and B dYB c 0=dO. It is found that the parameters A and B have opposite energy dependencies. It can readily be veri¢ed from Fig. 2 that A decreases slightly, whereas B increases signi¢cantly with increasing projectile energy. This appears to con¢rm potential energy e¡ects to be responsible for the above-surface processes, whereas the below-surfaces processes are expected to be in£uenced by kinetic energy e¡ects. In view of this ¢nding, future work is needed to verify the opposite energy dependencies of the contributions to plasmon production above and below the surface. References 1. Lindhard, J., Kgl. Danske Videnskab. Mat-fys. Medd. 28, Nr. 8 (1954). 2. Pines, D., ``Elementary excitations in solids'', (W.A. Benjamin Inc., New York, 1964). 3. RÎsler, M., Scan. Micr. 8, 3 (1994). 4. Hasselkamp, D. and Scharmann, A., Surf. Sci. 119, L388 (1982). 5. Almulhem, A. A. and Girardeau, M., Surf. Sci. 210, 138 (1989). 6. Baragiola, R. A. and Dukes, C. A., Phys. Rev. Lett. 76, 2547 (1996). 7. Niemann, D., Grether, M., RÎsler, M. and Stolterfoht, N., Phys. Rev. Lett. 80, 3328 (1998). 8. Monreal, R. C., Surf. Sci. 388, 231 (1997). 9. Gutierrez, F. A., Jouin, H., Jequier, S. and Riquelme, M., Surf. 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