. S I OFI ORNL P 1336 . del .. . : EEEEEEEE MICROCOPY RESOLUTION TEST CHART NATIONAL BUREAU OF STANDARDS -1963 m 7S 4. C w w w . -. . - N . -:::..siu i . No ... . . . .. ... . . :iie', or ..., - 1 LEGAL NOTICE This report was prepared as an account of Government sponsored work. Neither the United States, nor the Commission, nor any. person acting on behalf of the Commission: A. Makes any warranty or representa- tion, expressed or implied, with respect to the accuracy, completeness, or usefulness of the information contained in this report, or that the use of any information, appa- ratus, method, or process disclosed in this report may not infringe privately owned | rights; or B. Assumes any liabilities with respect to the use of, or for damages resulting from the use of any information, apparatus, method, or process disclosed in this report. As used in the above, “person acting on behalf of the Commission” includes any em- ployee or contractor of the Commission, or employee of such contractor, to the extent that such employee or contractor of the Commission, or employee of such contractor prepares, disseminates, or provides access to, any information pursuant to his employ- ment or contract with the Commission, or his employment with such contractor. : * . . . . . : Serie :: .. .... 2 ORAL-P-1336 CONF-6506.37-/ MASTERS metri intotiwa new windo* CHANNELING EFFECTS ON THE ENERGY LOSS OF HIGH ENERGY (20-80 Mev) 79Br AND 1271 IONS IN GOLD* W O XIDALANCA ommummomarganyapo matuohon JUN 24 1965 8. Datz, T. S. Noggle and C. D. Moak Oak Ridge National Laboratory Oak Ridge, Tennessee *-.she -Win!;. isinin birincisini, Do's. ; . tiim m e . .. ........ .... .. ....... The channeling effect of an ordered crystal lattice on the trajectory of energetic ions was first predicted in the computer calculations of Robinson and Oen on the ranges of multikilovolt ions in copper. These effects were observed in the transmission of 75 Kev protons through gold and by precise range measurements with low energy heavy ions. 5.4 Evidence has been found for channel- ing effects with (por) and (p, n) reactions and in studies of yields of x-rays induced by proton bombardment.”- Other observations with fast light particles in Si have been reported by Dearnaley, Erginsoy, Wegner and Gibson and Schiffer and Holland. 10 In the present work we have used multicomponent beams of Br and I ions from the Oak Ridge tandem accelerator with energies up to 80 Mev to study the effect of crystalographic orientation ...-','1 5-7 ',catiep . . . Dearnalev. 8 . on energy losses in thin gold single crystals. The application of the tandem van de Graaf accelerator to the production of heavy ion beams with energies from 10-120 Mev was deve loped at ORNL by Moak and co-workers." The experimental arrangement is shown in Fig. 1. Negative Br or I ions are injected from the source, accelerated to 7 Mev at the stripper gas canal. From the canal they may emerge with'ionic charge of 4*, 5* or *Research sponsored by the U. 3. Atomic Energy Commission under se to LBSTERIAI IR ARDPRODEANPROCEDURES contract with the Union Carbide Corporation. THE PUBLICSTA AREM EILE IN THE RECC:VING SECTION, · perhaps higher. At this point, a departure from usual procedure is made. If the gas pressure in the accelerator tune is high enough, some of the particles will continuously lose electrons by collision, reaching higher and higher charge states. As the energy increases the most probable charge state increases, and as the charge increases the rate of acceleration or acceleration per unit voltage increases. This leads to a kind of energy compounding so that a few of the particles reach energies as high as 120 Mev with charges up to 20+. The beam energy distribution thus attains continuous high energy tail which extends above 100 Mev.. The useful aspect is that high energies and high ionic charges go together so that the magnetic rigidity of each energy region of the beam is about the same. Note: . ME from the equation - KH“, that if the magnet is set to pass . charge 57 at 25 Mev, then it will simultaneously pass charge 67 at 36 Mev, charge 7+ at 49 Mev, charge 8+ at 64 Mev, etc. A different magnet setting simply changes the series of energies for which the various charge states pass. Thus, once the magnet constant kis precisely determined from proton thresholds and resonances, we have a multi-component beam consisting of a whole series of accurately known energies. Incidence of this beam onto a si surface barrier detector produces a pulse height spectrum characteristic of the beam energy distribution. In practice it is necessary to divert the main accelerator beam which would burn up our detector if it happened to come through the analyzer. For this reason we connect the slit regulator system up backwards so that the terminal voltage 3 will avoid those values which cause a main beam to come round through the magnet onto the slits. A portion of the resulting spectrum for 1271 ions is shown in the upper part of Fig. 2. Each of the lines is broadened because of the rather poor energy resolution which solid state detectors exhibit for very heavy ions. Were it not for this effect the lines would be a lmost ten t.imes as sharp. A number of sharp, low energy peaks is present in all the spectra, due to oxygen, nitrogen and other light contaminant ions. The spectrum for Br ions is similar except that double peaks are observed due to the mixture of 79Br and 81Br isotopes. However, with suitable adjustment of the ion source tuning and slit system, either one or the other isotope can be a lmost completely eliminated. For a measurement of the stopping power of any material, it is only necessary to place the material between the accelerator and the detector and measure what happens to each peak in the spectrum. Notice that we are not concerned with the height of the peaks. No attempt is made to regulate the accelerator voltage, so the exact composition of the high energy tail distribution will vary from run to run. Our only concern is with the shapes and positions of the various peaks. The spectra shown in the lower half of Fig. 2 were obtained for a polycrystalline gold foil approximately 200 ug/cm² thick and for 12'1 ions." Notice that the peaks are shifted and somewhat broadened. Such spectra can be used to give accurate estimates of dE/dx for various materials. Since the peaks are well separated, the use of . 1- 2NS R . " ete CU hi multicomponent beams with energy sensitive detectors permits us to perform several experiments at different energies at one time. For single crystal experiments, the absorber was mounted on a goniometer so that it could be rotated in the beam for the experi- ments being reported here, only one direction of rotation was available for each crystal. The gold crystals used were epitaxially grown on freshly cleaved, ratiation-hardened rock-sa ít faces. The rock salt was dissolved away and the crystals were mounted free. An x-ray map was used to determine the crystal axes and to analyze the imperfections in each crystal. The crystals were formed with a (100) plane parallel to their surfaces and were 1.1 mg/cm thick (ca. 2000 atoms) as determined by a particle energy loss measurements and by weighing. One foil was mounted with the goniometer axis lying on a (100) crystal axis in the plane of the foil; a second foil was mounted with the goniometer axis lying on a (110) axis in the plane of the foil. The goniometer axis was parallel to the (100) planes within 0.2° and was perpendicular to the beam axis within 0.2º. The angular position error was I 0.1°. The foil dianeter was 3 mm, and this defined the beam divergence of approximately 1.5 mm in 10 meters (ca. 0.01°). The collimator arrangement consisted of the target, 3 mm dia., followed by a 1 cm dia. aperture at a distance of 10 cm, followed by the 2 cm dia. detector at a distance of 5 cm from the aperture. An illustration of the crystal orientation available is shown in Fig. 3. The two axes of rotation are shown in the upper figure. With the goniometer set at oº, a square channel is seen for both crystals. Since the crystal is 2000 atoms deep, an extremely accurate angle sitting would be required for any sort of trans- parency to occur; fortunately, this is quite unnecessary for the appearance of strong channeling effects. As the crystals are rotated away from oº, planes are viewed edge-on and for most angles the picture is as shown in the figures marked planar channel. Por the (100) axis rotation, a very large diamond shaped (110) channel opens up at 45º. Finally, for the (100) rotation the rectangular 1112) channel is exposed at 35° 16', A number of experiments on channel effects on energy losses of light ions have been previously reported. 8-10 The typical result with channe led light ions in Si single crystals in the reports published until now was characterized by an emergent particle spectrum consisting of a peak due to normal energy loss with a high energy tail due to channe led particles which did not lose as much energy as they would have lost in amorphous or polycrystalline material. The high · energy particle spectrum usually exhibited a sma 11 component of rather definite energy loss consisting of a peak in the distribution at an energy loss which was always more than half the normal loss. The experiments being reported here give lor the first time some indication of what channeling effects are for fast, multiply charged, very heavy ions. The particles ''Br and 1271 simulate rather well the masses and energies of fission fragments, and thus give an idea of the crystalline effects to be expected with fission . . 24. fragments. . IF - E Typical spectra obtained with "Br ions incident on a single crystal gold target are shown in F18. 4. The top curve is the . spectrum without absorber. Barllor dx/dx measuromonts on poly- crystalline samples were used to calculate the normal energy losses expected for polycrystalline targets corresponding to the thickness of specimens used in the present work. These expected losses are indicated by the arrows. As can be seen from the figure, channeling offects are quito pronounced and often they completely predominate over all other types of energy loss. · The spectrum of Fig. 4c iliustrates the effects produced when the 1001) crystal direction was aligned to a ''Br bean. The energy losses for the various groups are characterized by single peaks. The losses are substantially less than corresponding normal (poly- crystalline) l08808 for a foil of this thickness. Although the peaks are asymmetric, the fraction of particles with normal energy loss was less than 0.1. Almost identical patterns have been observed for bombardment in the (110) and the (112) directions. This type of channeling, associated with all low index crystal directions observed, has been named pipe channeling. For the case of the (111) direction, the spectra were unusable because the excessive sample thickness, due to the oblique angle, caused overlap of the energy groups. The spectrum of Fig. 4b was obtained with the crystal rotated 9° about a (110) axis from the (001) direction; in this case the (110) planes were "edge-on" to the bean. Each peak has shifted and broken up into two distinct groups, and in this case some of the ions are channeled between shexts of atons. The spectrum consists of double peaks, one set of which corresponds to the normal energy lossor. This spectrum 19 typical of all those taken at angles .. . .. . . Some corresponding spectra obtained for I ions are shown in Pig. 5. Once again single peaks of reduced energy loss occur for pipe channel directions, Fig. 5c; for planar channels, Fig. 5b, double peaks appear corresponding to reduced energy loss and normal enorgy loss The fact that these double peaks are resolvable into two groups is demonstrated in Fig. 6, which shows a computer analysis of the data shown in Fig. 4b. The analysis consisted of a non-linear least-squares fit of gaussian distributions, and indicated that the observed distributions could be very closely described by a set of gaussian peaks. The effect of planar channel dimension is shown in Fig. 7 for 1211 in the (100) and (110) planes. In the wider (100} planar channel, the fraction channeled is higher and the difference in the energy loss for channeled and unchanns les particles, as can be seen from the distance between the two peaks in a given group, is greater. The effect of small displacements from a pipe channel direction is shown dramatically in Figs. 8 and 9. In Fig. 8 we explored the region of (110) direction with ''Br cons. It can be seen that just a 0° 30' displacement is sufficient to change the pattern from the typical pipe channel single distribution in the lower curve to a typical planar channol distribution of the upper eurvo. In the case of 1271 (Fig. 9), the situation is more complex because the position of the normal energy loss group from a given initial energy actually lies below the channe led loss portion of the preceding energy group. This mixing of groups leads to a maximum in confusion abouč 1° away from the (110) direction. However, when the channel 18 in line we again see the single group characteristic of pipe channeling energing (patterns obtained at 469 and 47° are identical to those obtained at 44º and 43°, respectively). For the experiments reported here, two axes of rotation were not available simultaneously. Without rotation around two axes, sna11 risalignments could not be corrected. Although these mis- #lignments are thought to be less than 0.1°, several spectra have indicated that even these small errors might affect the relative populations of channeled and unchanneled groups. It will be neces- sary to perform rotations around two axes in order to obtain the detailed structure of channel acceptance angles. In spite of the possible wise ligament, it is noteworthy that in the cases studied where planar channeling was involved a major portion of the ions were channeled. As can be seen from the relative peak heights for a given energy group in Figs. 7, 46 and 5b, the fraction of the long which are channe led decreases with increasing ion energy. These results seem to give at least qualitative verification to arguments of Lindhard's, which indicate an expected (v) a dependence for channel acceptance angle. For direct incidence into a pipe channel, the fraction undergoing normal loss is too small to be measured accurately at any of the incident energies; at ang les slight ly oft Dishes * * * itoestro w n - - . * .. * *** .. r.* ' .-, , ..... . .. . axis (1.e., 0° 30'), a normal loss component became observable which increased with increasing energy. These observations suggest a positive channeling mechanism as opposed to a simple trans- parency model and indicates that the probability of channeling decreases with increasing transverse momentum of the incident ion. Moreover, the fact that two distinct groups were observed, rather than a' continuum of energy losses, implies that most of the channeled particles were channeled a lmost immediately upon entering the crystal and remained in channels during the remainder of their trajectory through the solid. Channeling of ions involves correlated collisions with rows of atoms which steer the ions on paths with reduced proba- bility of low impact parameter events; however, the effective size of the "strings"ds of atoms, in this energy range, is too sma 11 to confine a particle to a single channel. Thus, in a pipe channel direction, movement of the particle to adjacent channels is essentially unhindered. Interplanar movements are more restricted because wander- ing is limited to only one direction. Although the trajectory of the particle is controlled by nuclear ...... .. . - - wo collisions, the energy loss suffered by the Cons in this energy range . ... . is primarily due to electronic stopping and the decreased energy loss associated with channeling iherefore reflects the lower average electron density encountered by the channeled particle. However, if the ions are merely conc irained to stay away from strings, it is curious that the channe led group of ions displays such a definite energy loss, as opposed to a continuum on the high energy side of the normal loss group. Of course, if the transverse oscillations . "Wimmo- n irin intermed mari the content ee it will s 10 were damped, all the ions would tend to settle into common pathways, but we have been unable to find any mechanism which would cause damping. Detector resolution in these experiments was insufficient to allow obafrvation of the detailed structure and shape of the channe led and unchanneled groups of ions; however, in those cases where the two groups appeared to be well separated, a set of numbers called the channel energy loss fraction (f - AE channe led/AE normal) was derived from the data. The energy loss fraction in various channels is plotted against incident energy in Fig. 10. The values all 1.9 between 0.5 and 0.85, show a slow rise with energy, and seem to have lower overall values for broader channels. Planar channels seem to . - . --- . -- give the same energy loss as pipe channels of the same dimension. It is also noteworthy that the energy loss fraction in planar channels did not change when the crystal thickness was changed by 40% in accord with the assumption that the ions are channeled early and remain chan- ne led. The loss fraction curve for 79Br ions in a given channel is somewhat higher than that for 1271 ions; an effect which may be caused by the higher velocity of the ''Br ion at a given energy. The fact that the values are larger than those recently measured for protons and a-particles 14 is perhaps caused by the fact that the heavy ions are not bare nuclei but have electrons which spend part of their - .. . - - - - - .. - time in dense regions alongside the channels, while the fact that the values are not constant with energy may indicate that the ion charge states are not following the same schedule which they would follow in amorphous solid matter. This latter effect could be brought about .. . on the by the avoidance of small impact parameter collisions in which the ion would tend to lose electrons. Presumptive evidence for this possibility can be adduced from studies of inelastic collisions in gases in the region 25-100 kev from which 1t has been demonstrated that the charge state increases rapidly as the distance of closest approach decreases. 15, 16 Since the electronic stopping power increases with ionic charge, a decrease in the equilibrium charge state could contribute significantly to the lowered energy loss of the channeled particles. Experiments designed to test this hypothesis are presently . . - - underway. - ... . .. - - - -- - - -- -- - - -... ang amat aman wang ada Shanka siasal maak dan u SLANG - ... .- 12. 12 References 1. M. T. Robinson and 0. 8. Oen, Bull. Am. Phys. soc. ?, 171 (1962); Appl. Phys. Letters 2, 30 (1963); Phys. Rev. 132, 2385 (1963). 2. R. 8. Nelson and M. W. Thompson, Phil. Mag. 8, 1677 (1963). .3. G. R. Piercy, F. Brown, J. A. Davies and M. McCargó, Phys. Rev. Letters 10, 399 ( 1963). ,' 4. H. Lutz and R. Sizmann, Phys. Letters 5, 113 (1963). 5. E. Bøhg, J. A" .e's and K. 0. Nielsen, Phys. Letters 12, 129 ( 1964). M. W. Thompson, Phys. Rev. Letters 13, 756 (1964). Brandt, Khan, Potter, Worley and Smith, Phys. Rev. Letters 14, 42 ( 1965). G. Dearna ley, IEEE Trans. Nucl. Sci. 11., 249 (1964). .. 9. C. Erginsoy, H. E. Wegner and W. M. Gibson, Phys. Rev. Letters 13, 530 ( 1964); Bull. Am. Phys. Soc. 10, 43' (1965). 10. J. P. Schiffer and R. E. Holland, Bull, Am. Phys. Soc. 10, 54 : (1965). 11. Moak, Neiler, Schmitt, Walter and Wells, Revs. Sci. Instr. 34, 853 (1963). 12. C. D. Moak and M. D. Brown, Phys. Rev. Letters 11, 284 (1963). 13. J. Lindhard, Phys. Letters 12 126 ( 1964). Both Erginsoy, Wegner and Gibson, and Sattler and Dearna ley have recently observed proton channel energy losses far below the minimum value of 0.5 predicted by the equipartition rule. Lindhard and A. Winther, Kgl. Danske Videnskab. Selskab, Mat.- Fys. Medd. 34, No. 4 ( 1964). We are indebted to these authors for communication of their data prior to publication. 13 .15. G. H. Morgan and E. Everhart, Phys. Rev. 128, 667 (1962). 16. V. V. Afrosimov, Iu. 8. Gordeev, M. N. Panov, and N. V. Fedorenko, Zh. Tekhn. Fiz. 34 1613, 1624, 1637 (1964). . .......and more . .....L a sim. omnia come i mill . -- - opo-.- .icm ....... .. . 12 . .. . ....... 1 . Figure Captions Fig. 1. Arrangement for the production of multicomponent high-energy heavy ion beams in the tandem van de Graaf accelerator. Fig. 2. 1??1 pulse height spectra obtained with (a) no absorber and (b) an Au polycrystalline absorber (205 Mg/cm). The q values given on the upper curve are the charge states on the ions prior to entering the absorber. The peaks labeled O are due to oxygen ion inpurities. Fig. 3. Representative of a face centered cubic lattice demonstrating the various channeling directions (for Au, a - 4.07 Å). Fig. 4. 79Br pulse height spectra obtained with (a) no absorber, (b) an Au single crystal absorber (1.1 mg/cm², rotated gº about a (110) axis in the (100) surface toward (111) and (c) with the (001) axis in line with the beam. The shifts indicated by the arrows drawn from the peak positions on (a) show the expected energy loss for a polycrystalline Au sample of the same thickness. Fig. 5. 1271 pulse height spectra obtained with (a) no absorber, (b) an Au single crystal absorber rotated gº about a (100) axis toward (110) and (c) with the (001) axis in line with the ion beam direction. Fig. 6. A computer analysis of the data in Fig. 4b. The single curves aro gaussians for a given energy group. The upper curve is the sum of the gaussians and the points are the experimental data smoothed over a 5-point average. (Note that in this curve we are using a linear abscissa as against the logarithmic scales of the other figures.) . . . ( a Fig. 7. A comparison of the (100) and the (110) planar channeling of 1271 tons. Fig. 8. The effect of small rotations on the pulse height spectra of 79Br ions in the region of the (110) pipe channel. . Fig. 9. The effect of small rotations on the pulse height spectra of 1271 ions in the region of the (110) pipe channel. Fig. 10. Fractional energy loss for 1271 and 79Br ions for several channel directions in Au vs incident son energy. within the ministeri memnunarsto sito.hentermine tment and consisting r p a A ORNL-LR-DWG 78271 . Br", 1° ions Br8+, TO 15.+ 19+ TO 19+ 20° ANALYZER MAGNET 90° ANALYZER MAGNET NEGATIVE SLITS MAGNETIC LENS ION SOURCE Br4+, 5+ 14+, 5+. : SLITS HIGH VOLTAGE TERMINAL, 7 Mv STRIPPER GAS CANAL odovodno novoooo. MAGNETIC LENS MOVEABLE ALPHA PARTICLE CALIBRATING SOURCE DETECTOR CONDITION FOR PASSAGE THROUGH ANALYZER MAGNET M = 042 MULTICHANNEL ANALYZER DOUBLE LINE AMPLIFIER CHARGE SENSITIVE PREAMPLIFIER 02 PRECISION PULSE GENERATOR Arrangement for Measuring Heavy Ion Energies in Semiconductor Detectors ORNL-DWG 65-2194 10 20 1271 ION ENERGY (Mev) 40 50 30 60 . 70 80 DETECTOR RESPONSE NO ABSORBER (a) - q=10 9=12 19=8 ------ 4 - COUNTS PER CHANNEL POLYCRYSTALLNET Au 205 kg/cm2 (b) WWWVYVYN 50 400 450 200 250 CHANNEL NUMBER 300 350 400 450 500 ၀ ၆ . ပ. . (wol 0.30 -- Q Q ၀ ၀ ၀ OT ဝ ဝ ဝ O--- (၅၀၀) Po 6 6 O .. - - - - Face Centered Cubic Crystal Viewod Along the (001) Axis * Rotation is Rotation သာ OT CCTOro Cicconcocco OOOO momo BCCO FOCCO COO COO (400) (100) Plarar Channel (110) Planar Channel Od 0 9 999 0.577 | 0 0 0 ဝ CO . ။ 0 o none | 0 5 56 (110) Channel (112) Channel - -- . " Y es » All ! --- -- -.---.. - . - .--. - .-- . .--. -.- -- - VO OriL-Dwc es-2014 WE 79Br ION ENERGY (Men) 30 40 .: 70 DETECTOR RESPONSE NO ABSORBER w COUNTS PER CHANNEL g® FROM 1000 TOWARD A10 . . loou CHANEL 50 - 100 150 200 250 CHANNÉL NUCABER 300 350 450 500 OROL - DWG GS-2033 . 30 - 1277 ION ENERGY (Mor) 40 50 80 DETECTOR RESPONSE NO ABSORBER m COUNTS PER CHANNEL CC 9* FROM 1000 TOWARD (110) IC 1001) CHANNEL 50 100. 150 200 250 300 CHANNEL NUMBER 350 400 450 500 550 WANNCL NUMOCN ORNL-DWG. 65-5601 20- 79Br ION ENERGY ( Mev) 30 40 50 50 . 9° FROM [001) TOWARD (111) OL]LIII Ô Á Ñ Ô : COUNTS PER CHANNEL (X 10-3) 0 0 A . N talo 50100 150 200 300 250 CHANNEL NUMBER 350 400 400 ORNL-DWG 65-2094 1271 ION ENERGY (Mevi 40 20 50 60 70 80 NORMAL ENERGY 9° FROM (001) TOWARD (110) (100) PLANER CHANNEL COUNTS PER CHANNEL © 9° FROM (001) TO''ARD (111) [110] PLANER CHANNEL & o 50 100 150 200 250 300 CHANNEL NUMBER 350 400 450 500 . - . . t ombolisinin in woons ORNL-DWG 55-2092 79Br ION ENERGY (Mev) 30 40 70 -UNSHIFTED PEAK POSITIONS — Oc30' FROM [140] TOWARD [001] COUNTS PER CHANNEL .. [110] DIRECTION 100 150 200 250 CHANNEL NUMBER 300 350 400 450 500 -. ......... .... OR NL - DWG 69-2003 N ENERGY (Mov) 50 . 43° FROM [001] TOWARD (110) Ø 8 map 44• FROM [oo] TOWARD (110) COUNTS PER CHANNEL 08 45. FROM [001] (110) O Ô 50 100 150 200 300 350 250 CHANNEL NUMBER 400 450 500 ORNL-DWG. 65-5390A T O RNE-WO. 65-5809 1271 ..804 (110) PLANAR CHANNEL .70 (001) CHANNEL (100) PLANAR CHANNELHI ENORMAL (110) CHANNEL .40LIIIIII p=0ECHANNELED / .904 7987 (110) PLANAR CHANNEL entamente terrain 7 (001) CHANNEL .604 1112 CHANNEL i t o 20 30 40 50 60 70 80 r O ION ENERGY (Mev) END . 1. DATE FILMED 9/ (10/65 . . .