90 Nuclear Instruments and Methods in Physics Research 812 (1985) 90-94 North-Holland, Amsterdam PROTON STOPPING CROSS SECTIONS FOR CARBON, ALUMINIUM AND GOLD: NEW EXPERIMENTAL DATA AND CRITICAL ANALYSIS OF THE VALIDITY OF EMPIRICAL FIT FORMULAS F. SCHULZ Gesellschaft ftir Strahfen - und Vmweltforschung mbH, Physika fisch -Technische Abteilung, D - 8042 Neuherberg, Fed. Rep. Germany J. SHCHUCHINSKY Radiation and Solid State Laboratory, New York University, 4 Washington Place, New York, NY 10003, USA Received 22 January 1985 and in revised form 18 February 1985 We report new experimental data for the stopping cross section S of protons in carbon, aluminium and gold at energies between 8 and 300 keV. The data are found to exhibit largely the same energy dependence as previously reported data. Using empirical fit functions we have analysed available experimental data in terms of the ratios SC,,,&, from which we derive scaling factors b applicable to various sets of experimental data. These scaling factors, which typically range from 0.9 to 1.1, are attributed to deviations of the true foil thickness from the assumed one. Using b-corrections all sets of experimental data can be adjusted to fall on the same target specific stopping power curve (maximum deviation f 3%). While the adjusted data are well described by the respective fit function (Al: Andersen and Ziegler) or tabulation (Au: Janni) the empirical data for carbon apparently deserve further improvements. 1. Introduction The stopping cross sections for swift ions in matter are still not known with sufficient accuracy. Inspection of stopping power compilations for hydrogen fl] and helium [2] in all elements shows that available experimental data frequently differ by up to 50%. New experiments at low velocities [3-61 indicate that the empirical fit formulas proposed by Andersen and Ziegler [l] and Ziegler 121deserve further improvement. More recently Janni [7] presented proton stopping power and range tables which, for energies between 20 keV and 1 MeV, were obtained by statistically evaluating the accuracy of the available experimental information (up to June 1979) and then performing least square curve fits. Almost at the same time Montenegro et al. [S] presented a “universal” equation for the electronic stopping of ions in solids. The model is based upon the effective charge concept. Although this approach approach to be questionable for protons, the agreement obtained in ref. [S] between the proposed analytical fit function and selected experimental data looks convincing (at first sight). We have carried out measurements of the stopping cross sections for protons in carbon, alu~nium and gold at (incident) energies between 8 and 300 keV. The original motivation of this work was to determine pro0168-583X/85/$03.30 0 Elsevier Science Publishers B.V. (North-Holland Physics Publishing Division) ton stopping powers under the same conditions as those employed in recent measurements of He, N, Ne and Ar stopping in the same or similar foils [lo]. Proton and heavy ion stopping powers derived under identical condition constitute the ultimate experimental data base for a comparison of experimental and theoretical [ll] effective charge fractions of heavy ions. Another purpose of this study was to assess the validity of empirical stopping power formulas or tables [1,7,8]. Using the present and previously reported data we have evaluated systematic deviations of the energy dependence of empirical stopping powers from the experimentally observed trends. This procedure allows the derivation of “adjusted” stopping cross sections which appear to be accurate to within k 3% or better. The measurements were performed at NYU. The experimental set-up was described briefly in ref. [lo]. A detailed description will be given elsewhere [12]. A noteworthy improvement of the vacuum system was accomplished by the incorporation of cryopumps in place of the diffusion pumps originally in use [10,12]. The velocity loss spectra were measured with a 90” magnetic spectrometer (momentum resolution Ap/p = F. Sckult, f. Shchuchimky / Proton sropping crms sections for C, Al and Au 5 x 10e4). In order to detect the analysed protons with high sensitivity, even at energies of a few keV, the solid state detectors alloyed for the heavy ion work [IO&?] were replaced by channeltrons. The areal density of the target foils (amorphous carbon, polycrystalline aluminium and gold) was determined with an accuracy of approximately k 10% as described in ref. [lo] (carbon: 10.6 and 13.6 &g/cm’; alumitium: 26 pg/cm’; gold: 130 and 140 y g/cm')_ Among other methods, thickness calibration involved measurements of the energy loss of 300 keV He and the use of the respective stopping cross sections according to Ziegler’s empirical fit [2] (at 300 keV, the stopping powers in C, Al and Au, reported by different groups, agree to within about + 10% [2]). -. - -- - - , ( / ) ,$,,) , . ! Jonni AndersensZiegler Montenegro et al. ti: 1 B 01 0‘7 91 ( / , 1 ,,,( , # , k ,,,J IQ2 IO ENERGY/ MASS lo3 IkeVfu) Fig. 2. As fig. 1 but for aluminiurn. 3. Results The measured proton velocity loss spectra exhibited u&modal distributions. For carbon and alurninium the loss peaks were almost Gaussian in shape_ In the case of gold the loss peaks exhibited a tail OR the high-energy side which is attributed to channeling [lO,f3]. This tail could be removed by offsetting the angle of observation by l-3” from the direction of beam propagation [IO]. Because of the absence of a channeled loss component, the mean random energy loss n = E, - EoU, and the corresponding stopping cross sections could be de termined unambiguously and rather precisely ( E, is the incident ion energy and Ena, the mean ion energy after passage through the foil). The experimental results of this work are presented in figs. 1-3 (full circles). The measured cross sections S are plotted versus the appropriate “mean” ion energy/mass, E,/M, in the foil. If the stopping cross section can be described, in the interval i& c E < E, H--Au e this work -.---- Jonni Andenen & Ziegfef Montenegro et al. $00 lo3 1 ENERGYi MASS lkeVlut Fig. 3. As fig. 1 but for gold. by S(E) = kEP, the correct value for E, is [12] ; I E I& 0 0 $ 9 5 s 5 IOL % m 8 5% (3 In this study the error intr~uced the power p is less than 1%. H-C by ~ncert~nties of * this work 4. Discussion - ,---- t E Oo !7J 1 Jonni Andersen 8 Ziegter Montenegro et al 10 ENERGY/MASS lo2 (keV/uI lO> Fig. 1. Proton stopping cross section for carbon versus the appropriate mean energy of the protons in the target foil (see text). Previously reported empirical fit functions [1,7,8] are shown for comparison. In figs. 1-3 the results of this study are compared with the fit formulas suggested in refs. [1,7,8]. The extent to which the experimental data and the fit functions agree depends on the target material. The agreement is seen to be best for aluminium (fig. 2) and less satisfactory for carbon (fig. 1) and gold (fig. 3). Even in the latter case, however, the maximum relative deviation does not exceed 20%. Considering the fit formulas one will note that the curves of Andersen and Ziegler [l] and Janni [7] generally agree rather well with each other (except for gold STOPPfNC POWER WORKSHOP F. Schulz, J. Shchuchinsky / Proton stopping cross sections for C, Al and Au 92 around the maximum of the stopping cross section, cf. fig. 3). The maximum in the fit functions of refs. [1,7] is located at almost the same energy, i? = E( S = S_). This emperical number 8,, [1,7] is in accordance with observed in this study. The agreement with i? of R, Montenegro et al. [8] is not as good, notably in the case of carbon and gold where the calculated ,6 is apparently too low. As pointed out in sect. 2 the thickness of the foils used in this study was known with an estimated accuracy of &-lo%. Accordingly part of the discrepancy between our experimental data and the fit formulas can be attributed to deviations between the assumed and the true foil thickness. If we multiply our data for aluminium by a factor of 1.05 the agreement with the Andersen-Ziegler fit is almost perfect. A similar agreement cannot be achieved for carbon and gold, i.e., in these cases the observed energy dependence of the stopping cross section deviates significantly from the empirical fits (cf. figs. 1 and 3). In order to check the quality of our data with respect to their energy dependence we have carried out a detailed comparison with previously reported data. We made the rather reasonable assumption that in all measurements the largest error is introduced by uncertainties in the determination of the foil thickness. In order to assess likely errors in foil thickness we derived ratios of stopping cross sections, S,,,/Sril. Visual inspection of these ratios revealed a common energy dependence. Almost perfect agreement between the various sets of data could be achieved by multiplication with an individual factor b, where b usually ranged from 0.9 to 1.1. The procedure is illustrated in fig. 4 which shows scaled ratios of stopping cross sections b&.,/S,, using the fit function according to Andersen and Ziegler [l], Sri, = S,. Two observations are evident. (i) The energy dependence of S observed in this study agrees quite well with previously reported data. (ii) The common trend in the energy dependence of SeXPis not described properly by the suggested fit functions. In all cases b&,/S,, = f(E) rather than bS,,,/S,, = const (ideally b&,/S,, = 1.0). Accordingly we conclude that presently available fit functions usually deserve an energy dependent correction in order to describe experimental data properly, i.e. with an accuracy of better than f 3%. It should be pointed out that the selection of the respective set of b-values for a given target was not completely arbitrary since, for each target, we tried to arrive at mean value b between 0.97 and 1.03. The use of this “boundary condition” was based upon the idea that the error in foil thickness determination should roughly cancel by averaging over data from different laboratories. Although the choice of the data sets may be considered somewhat arbitrary we based our decision on some practical aspects. (i) The measured stopping cross sections had to cover a sufficiently large range in energy, preferably around the maximum (since this is the region where the employed procedure is most sensitive to systematic differences between different sets of data). (ii) Experimental results of those authors who provided data for more than one target material (out of the three investigated by us) were given preference to those who studied one material only. (iii) Data which revealed systematic energy-dependent deviations from the common trend were not taken into account in the final compilation of stopping cross sections. As discussed 5 % = 3 this work 1x1.091 o vws D 62 1.0.881 A 0 8 0 63 1x0.98) l !j --jl m 1 10 ENERGY/ MASS v 0 q SoZ 65 1x1.103 Ms K 80 (x0.971 MsK 82 1x0.98) 102 (keV/ u) 10- g l ti IO’ ?I & ” B 5-0 c o A v 0 q this work VW L D 62 Oe D 63 Ss 2 65 Ma K 80 Ms K 82 (x1.091 Ix0.88) (x0.981 1x110) 1x0.97) ix0.981 Fig. 4. Scaled ratio of the proton stopping cross section is the fit function suggested by b&,, L&z for carbon (S, Andersen and Ziegler [l]). The factor b for the respective set of data is specified in parentheses. The mean value of b is 1.00. For comparison S,.,,/S, and SJanni/SAz are also plotted. References: M. et al. [8], Janni [7], VW & D 62 [14], 0 & D 63 [El, S St Z 65 [16], M & K 80 [17], M & K 82 [6]. Fig. 5. Adjusted proton stopping cross section for carbon. Experimental data as in fig. 4. The tabulated stopping cross section due to Janni [7] is shown for comparison. F. Schulz, J. Shchuchinsb / Proton stopping cross sections for C, AI and Au 93 5-7. Also shown is that fit function out of refs. [1,7,8] which describes the new set of data best. Whereas for alumiuium (fig. 6) and gold (fig. 7) the fit functions due this work (x1.05) o M&K (xO.8L) q MsK 82 (x0.83) OMD65/H,D(x1.03) l AO 0’ 80 I 10 ENERGY/ MASS I ,,I,, 10' 102 (keV/uI Fig. 6. Adjusted stopping cross section for protons (H) and deuterons (D) in ahnninium. The scaling factors b are specified in parentheses. The mean value of b is 1.00 (counting M & K 80; 82 only once). The empirical fit function due to Andersen and Ziegler (A & Z) [l] is shown for comparison. References: Bii 36 [18], Ma 53 [19], OMD 65 [20], M & K 80 [17], M & K 82 [6]. below the employed procedure may in fact be used to identify these deviations. On the basis of the scaling procedure illustrated in fig. 4 we have derived “adjusted” stopping cross sections, using both our own and previously reported experimental data. The results, Sadj = b&r, together with the employed scaling factors b are presented in figs. H.D - Au to Andersen and Ziegler [l] and Janni [7], respectively, describe the “adjusted” stopping cross sections very well, a sufficient accurate fit is not yet available for carbon. The closest agreement is achieved using Janni’s fit (fig. 5). Whilst it is evident from figs. 5-7 that the scaled experimental data generally agree to within better than f3% the procedure illustrated in fig. 4 may also serve to identify “unusual” data. For example, the results recently reported by Mertens and Krist [6] for aluminium exhibit a rather rapid drop at energies above 200 keV (cf. fig. 6). This drop is at variance with the present and all previously reported data. A similar, though not as pronounced fall-off is seen in their results for carbon and gold [18] (figs. 4, 5 and 7; clearly evident for gold in a data analysis corresponding to fig. 4). The origin of this unusual energy dependence is not easy to assess without a knowledge of all details of the experimental approach as well as of the method employed for deriving stopping cross sections from measured energy loss spectra. As another example we like to mention that the stopping cross sections for gold reported by Bader [24] (scaling factor b = 0.98) exhibit a shift towards higher energies by about 10 to 20%. This shift raises some doubt whether the terminal voltage of the accelerator employed was calibrated properly. In view of this uncertainty Bader’s data are not included in fig. 7. Last but not least, a comment on the quality of our own thickness determination is in order. According to figs. 4-7 the true foil thickness was 5 to 11% smaller than anticipated. Since recent heavy ion stopping power measurements at NYU were carried out using the same and similar foils (and the same procedure for thickness calibration) we suspect that the data reported in ref. [lo] have to be corrected by the scaling factors given in figs. 4-7. Janni l this work (xl.lll .ri”-, ;;F;iZ;,,,,j 10 ENERGY/MASS lo2 (k&‘/u) 10’ Fig. 7. Adjusted stopping cross section for protons (H) and deuterons (D) in gold. The scaling factor b is specified in parentheses. The mean value of b is 1.03. The tabulated cross section due to Janni [7] is shown for comparison. References: Ba 36 [18], vWMB 71 [21], T & P 80; 81 [22,5], M & K 80; 82 [17,6], BSG 84 [23]. 5. Conclusion Based upon a critical analysis of new and previously reported proton stopping cross sections for carbon, aluminium and gold we have derived sets of “adjusted” experimental data which appear to be accurate to within *3% or better. The new data provide means for a critical test of previously suggested fit functions or tabulated data. Corrections to the empirical stopping cross sections are desirable in the case of carbon. The improvements accomplished by determining and critically analysing ratios of stopping cross sections, Se,+/&, are evident. Therefore we suggest that this procedure should be employed in evaluations of the STOPPING POWER WORKSHOP 94 F. Schulz, J. Shchuchinsky / Proton stopping cross sections for C, Al and Au quality of new experimental data as well as in attempts to derive optimum sets of stopping cross sections from experimental data of different sources. This work was initiated by the late Prof. W. Brandt to whom we are grateful for his enthusiastic encouragement and advice in course of the measurements. Thanks are due to C. Peterson (NYU) for technical support during the experiments and to K. Wittmaack (GSF) for the numerous discussions and assistance during the preparation of this paper. Part of this work was supported by the US Department of Energy. References [l] H.H. Andersen and J.F. Ziegler, Hydrogen stopping powers and ranges in all elements (Pergamon, New York, 1977). [2] J.F. Ziegler, Helium stopping powers and ranges in all elements (Pergamon, New York, 1977). [3] H. Oetzmann and S. Kalbitzer, Radiat. Effects 47 (1980) 73. [4] R. Blume, W. Eckstein and H. Verbeek, Nucl. Instr. and Meth. 168 (1980) 57. [5] D.A. 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