ON THE LIIMITS OF POSSIBILITIES OF SUPERHEAVY ELEMENT SYNTHESIS IN NUCLEAR REACTIONS WITH HEAVY IONS V.L. Mikheev Flerov Laboratory of Nuclear Reactions Joint Institute for Nuclear Research, 141980 Dubna, Moscow Region, Russia Abstract Experimental data on the bombarding energies of heavy ions with 10 Z 30 in 36 fusion reactions with evaporation of 1-4 neutrons at irradiation of targets with 82 Z 98 have been compared with fusion barriers calculated according to different theoretical models. The experimental fusion barrier was defined as the minimum value of the heavy ion bombarding energy at which neutron evaporation residues were really observed to form. Corrections to the theoretical fusion barriers have been found by least-squares linear fit of calculated and experimental barrier values. The corrected values of the fusion barriers B were calculated for the fusion of 208Pb, 238U, 248Cm, 249Cf with heavy ions with the atomic numbers 6 Z 46. These fusion barriers B were compared with the ground state Q-values for the complete fusion. According to the criterion (B+Q) 0 for complete fusion, the extreme atomic number for the elements producible in complete fusion reactions involving heavy ions is 134. 1. Introduction In the last years, considerable progress has been achieved in the synthesis of superheavy elements. The elements with atomic numbers 114 and 116 were synthesized [1-3]. Experiments to produce element 118 in a 249Cf + 48Ca nuclear reaction were carried out at the Flerov Laboratory of Nuclear Reactions, JINR, Dubna [4]. The results concerning the production of elements 104-112 can be found in surveys [5-8]. The periodic table currently contains 23 man-made elements, of which the latest 14 elements were produced using fusion nuclear reactions involving heavy ions (HI). This raises the question on limits to producing superheavy elements in laboratory conditions. The main restricting factors are: 1) the instability of nuclei first of all with respect to spontaneous fission and 2) the entrance channel limitations for the fusion of the nuclei used to produce new heavy elements. The nuclear properties of superheavy elements were analyzed in many works. According to work [9], the most heavy nuclide with a shell stabilized fission barrier which can be produced using the really available isotopes of elements in the Mendeleev’s Table is 329134. In work [10] the spontaneous fission half-lives larger than 0.1 s were calculated for the elements with atomic numbers up to 120. The alpha and beta decay properties of the nuclei with atomic numbers up to 136 have been estimated in work [11]. By now, a large body of data on the complete fusion of heavy ions with heavy targets has been accumulated. One of the key factors to be dealt with in planning and analyzing experiments is the fusion barrier, which basically owes its existence to Coulomb repulsion. The fusion barrier is known to be the minimum value of entrance channel energy for colliding nuclei to overcome their mutual Coulomb repulsion and fuse. Below the fusion barrier, complete fusion can occur only with a low probability owing to the quantum-mechanical penetrability of a potential barrier. The nucleus-nucleus interaction potential and the near barrier fusion cross section are determined by many factors [12-14]. For heavy targets, experimental values for fusion barriers are usually deduced from the corresponding excitation functions for fusion-fission and for the summary yield of evaporation residues. For most heavy systems target + heavy ion, the problems connected with fast fission, incomplete fusion-fission and the sharply decreasing fusion cross section make identification of real complete fusion-fission events very difficult. An event of complete fusion can be most reliably identified by direct registration of neutron evaporation residues with Z=Z1+Z2, where Z1 and Z2 are the atomic numbers of target and projectile nuclei. In this work, the experimental fusion barrier B(exp) is defined as a minimum value of heavy ion bombarding energy at which neutron evaporation residues corresponding to the minimum number of evaporated neutrons were really observed to form. This definition is not so rigorous. But it permits to extract B(exp) values from the data on the synthesis of the heaviest elements when the measurements were performed at one value of projectile energy and the number of registered events was a few units. Comparing the experimental values of fusion barriers derived from (HI, xn) reactions with existing theoretical calculations allows corrections to be found to the initial theoretical barrier values. Due to that, it is possible to obtain more reliable estimations of fusion barriers for various combinations of targets and projectiles. The aim of the present work is to estimate what is the maximum Z value of the element which can be synthesized in fusion reactions from the really available quantities ( ~1 mg) of initial atoms of the elements (natural or man-made) required for producing targets and beams. For this purpose, a comparison of the fusion barriers and the compound nucleus ground state Q-values was made for different target + projectile combinations. 2. Calculated and experimental fusion barriers Potential energy calculations can be carried out now in multidimensional approaches using many parameters. But one-dimensional models allow to reveal more clearly the general tendencies in changing fusion barriers for the wide ranges of Z1 and Z2. From among many approaches to calculating entrance channel potential (see, for example, [14] and the references cited therein) those approaches were chosen that use a minimum number of adjustable parameters. The classical potential model by Bass [15] is much used to calculate the fusion barriers for heavy ion reactions,. Heavy ion collisions were analysed in detail by W. Wilcke et al. [16]. The fusion barriers have been calculated for s-waves using the BSS Coulomb potential [17] and the nuclear proximity potential [18]. Myers and Swiatecki [19] have revised the nuclear parameters used for proximity potential calculations. However for heavy targets, the results of works [16,18] and [19] differ only slightly. This work makes use of the parameterization from works [16,18]. K. Siwek-Wilczynska and J. Wilczynski [20] suggested for the description of fusion barriers the adiabatic fusion potential with the nuclear part of the Woods-Saxon shape. The fusion barriers can be expressed in terms of the Coulomb potential alone, B(Coul.)=Z1Z2e2/r0(A11/3+A21/3). The radius parameter r0 is a handy variable for comparing fusion barriers for various combinations of nuclei. In this work r0 =1.44 fm. The experimental and calculated fusion barriers are listed in Table 1. The used experimental data include 36 nuclear reactions involving heavy ions with 10 Z 30 and heavy targets with 82 Z 98. Only those experiments were selected in which the incident energy in the middle of the thin target was exactly determined. The data have been arranged corresponding to the experimental fusion barrier magnitudes. Table 1 Fusion barriers (MeV) deduced from the experimental data on (HI,xn) reactions, compared with the Coulomb barriers and with the barriers calculated by theoretical models [15, 16, 20]. Reaction Ref. B(exp) B(Coul) B(Bass) B(Wilcke) B(Wilcz.) 208 22 Pb( Ne, 4n) 21 92 94.0 92.5 95.8 89.8 232 Th(22Ne,4n) 22 92 100.6 99.6 103.1 92.9 208 20 Pb( Ne, 4n) 21 93 94.9 93.6 95.9 92.5 238 22 U( Ne,4n) 23 96 102.2 101.3 104.9 94.6 242 22 Pu( Ne,4n) 24 99 104.1 103.2 106.9 97.1 236 U(22Ne,4n) 25 102 102.4 101.5 103.5 95.1 243 22 Am( Ne,4n) 26 103 105.1 104.3 108 98.1 248 22 Cm( Ne,4n) 27 107 105.7 105.0 107.3 98.5 232 Th(26Mg, 4n) 25 117 118.6 118.5 122.6 110.2 207 Pb(34S,3n) 28 138 143.3 144.7 149.3 139.1 206 40 Pb( Ar,2n) 29,30 155 158.3 160.5 165.6 155.5 208 40 Pb( Ar,2n) 5,30 157 157.9 160.1 165.3 155.3 209 Bi(40Ar,2n) 31 159 157.8 162 167.2 157.4 208 48 Pb( Ca,1n) 32 171 171.6 174.5 180.0 174.5 206 48 Pb( Ca, 2n) 28 173 171.9 174.8 180.3 174.5 204 Pb(48Ca,2n) 28 173 172.3 175.2 180.7 174.3 207 48 Pb( Ca,2n) 28 174 171.7 174.6 180.2 174.6 208 50 Pb( Ti,1n) 6,33 185 187.7 191.9 198.1 189.5 209 50 Bi( Ti,1n) 33 187 189.8 194.2 200.4 192.2 232 Th(48Ca,3n) 34 189 184.1 188 194.0 183.6 238 48 U( Ca,3n) 34 192 187.2 191.3 197.3 187.4 242 48 Pu( Ca, 3n) 34 196 190.6 195.0 201.3 191.8 244 48 Pu( Ca,3n) 1 197 190.2 194.7 201.0 191.1 209 Bi(51V,2n) 35 199 198 203 209.5 198.4 248 48 Cm( Ca,4n) 3 201 193.6 198.4 204.7 195.6 208 54 Pb( Cr,1n) 6 202 202.8 208.1 214.8 205.1 249 Cf(48Ca, 3n) 4 206 197.5 202.6 209 201.4 209 54 Bi( Cr,1n) 36 208 205.1 210.6 217.3 208.3 207 58 Pb( Fe,1n) 6,37 218 217.9 224.7 231.6 221.8 208 58 Pb( Fe,1n) 6,37 219 217.6 224.4 231.4 221.4 209 Bi(58Fe,1n) 6 223 220.1 227.2 234.1 223.4 208 64 Pb( Ni,1n) 6 236 231.3 239.3 246.6 237.0 208 62 Pb( Ni,1n) 6 237 232.3 240.6 247.8 236.0 207 Pb(64Ni,1n) 38,39 239 231.6 239.6 246.9 237.5 209 64 Bi( Ni,1n) 6,39 240 233.9 242.2 249.5 240.1 208 70 Pb( Zn,1n) 6,39 255 244.9 254.1 261.8 252.6 Fig. 1(a) shows the difference between the experimental fusion barriers and the barriers calculated by theoretical models [15,16,20] as well as the Coulomb barriers. It is seen this difference to be as much as ~13 MeV. To decrease this discrepancy, least squares linear fit of calculated and experimental fusion barriers was made. The formulae for calculating the corrected fusion barriers are as follows: B(Coul. corr.)= -10.61 + 1.068 B(Coul.); standard deviation SD=3.2MeV B(Bass corr.)= -2.54 + 1.00B(Bass); SD=3.1 MeV B(Wilcke corr.)= -2.61+ 0.97B(Wilcke); SD=3.3 MeV B(Wilcz. corr.)=5.60+ 0.974B(Wilcz.); SD=3.3 MeV 30 [B(calc. corr.) - B(exp)] / MeV [B(calc) -B(exp)] / Mev 25 80 100 120 140 160 180 200 220 240 260 B(Bass) B(Coulomb) B(Wilcke) B(Wilczynski) (a) 20 15 (1) 30 25 20 15 10 10 5 5 0 0 -5 -5 -10 -10 -15 -15 -20 30 -20 30 25 25 (b) 20 20 15 15 10 10 5 5 0 0 -5 -5 -10 -10 -15 -15 -20 80 100 120 140 160 180 200 220 240 260 -20 B(exp) / MeV Fig.1 (a) The difference between the calculated and experimental fusion barriers versus B(exp) values for the nuclear reactions from Table 1. (b) The same as in (a), but the theoretical barriers are corrected by formulae (1). Fig. 1(b) demonstrates the effect of introducing corrections to the initial theoretical fusion barriers. Based on experimental data, these corrections include possible effects of extra push energy, nuclear static and dynamic deformations, different entrance channels coupling and so on. The fusion barriers calculated by formulae (1) differ from the experimental fusion barriers by no more than 5 MeV. An essential part of this difference may be aroused owing to the errors in the B(exp) values connected with target thickness, incomplete measurement of the excitation function, the accuracy of HI energy measurement. Table 2 Number of evaporated neutrons 1 2 3 4 Dissipated energy, MeV 6.32.2 9.13.5 10.83.7 13.36.1 Table 2 shows the mean values of dissipated energy E* for presented in Table 1 (HI, xn) reactions x E*=(B(exp) + Q - Bi ), i 1 x where Bi is the binding energy of evaporated neutrons. i 1 The Q-values and neutron binding energies were calculated using mass tables [40-42]. According to the way experimental fusion barriers were determined, the E* value for x=1 corresponds to the maximum of the excitation function and that for x 1 corresponds to the low energy edge of the excitation function or the sole projectile energy at which the evaporation residue was observed. 3. Fusion barriers and Q-values for the synthesis of nuclei with the highest Z numbers The up-to-date theoretical approaches [43-45] are not capable of predicting the values of the formation cross sections of superheavy elements with a good accuracy [43]. Therefore, from the practical point of view, while planning experiments to produce superheavy elements, it is very important to choose an optimal target + projectile combination and the value of incident energy. The only question arises then on the maximum sensitivity of experiments. The Q-value is the very important parameter in nuclear processes. The use of the corresponding Q-values and Coulomb barriers allows unified systematization of the probabilities of spontaneous fission, alpha decay and cluster decay of heavy nuclei [46]. To some extent, the fusion of heavy ion with a target nucleus is the inverse process to the cluster decay [47]. It seems reasonable to analyze the entrance channels of nuclear reactions leading to superheavy elements by comparing the entrance fusion barriers and the Q-values for the compound nuclei formed. 3.1 Main points of approach proposed 1) The necessary condition for fusion to occur is (B+Q) 0 (Q 0 for all the considered nuclear reactions), which provides a gradient of potential (driving force) between the initial double nuclear system and the final compound nucleus. In terms of statistical model, it means that compound nucleus excitation energy is greater than zero for the incident energy equal to B. 2) Formulae (1) are used to calculate the B value that does correspond to the complete fusion. 3) The sum of Coulomb and nuclear potentials must have a pocket on the way of radial motion towards fusion. The only s-wave absorption is considered owing to the fact that the nuclear systems involved in the formation of superheavy nuclei are highly fissionable. 4) At (B+Q) 0, an increase in the initial kinetic energy over B will not result in compound nucleus formation. The additional kinetic energy is thermalized [20]. 5) Since superheavy elements have small formation cross sections ( pb), only the isotopes of elements available in quantities no less than ~1 mg are considered to make it possible to produce the targets and beams required. 3.2 Calculations for 208Pb, 238U, 248Cm, 249Cf These nuclides were chosen as the most suitable targets for producing the elements with Z much greater than 100. 252Cf and 254Es can be used also, but they give no appreciable advantage in comparison with 248Cm and 249Cf. Moreover, 252Cf produces an extremely high spontaneous fission background and 254Es, available in small quantities (~0.1 mg) only, has a half-life less than 1 year. Figs. 2-5 show the (B+Q) values as a function of the atomic number of the projectile, the projectile being either the heaviest or the lightest isotope of the element with Z number plotted. As can be seen from the figures, the (B+Q) values with B calculated by the various models and corrected by formulae (1) are close to one another. The increasing projectile Z number results finally in cold fusion for all the targets considered. 50 0 40 4 8 12 16 20 24 28 32 40 44 48 B(Bass) B(Coulomb) B(Wilcke et al) B(Wilczynski) (a) 30 (B + Q) / MeV 36 20 40 30 20 10 10 0 0 -10 -10 208 Pb + the heaviest projectile isotopes -20 -30 -20 -30 -40 50 -40 50 40 (B + Q) / MeV 50 40 (b) 30 30 20 20 10 10 0 0 -10 -10 208 Pb + the lightest projectile isotopes -20 -30 -40 0 4 8 12 16 20 24 28 -20 -30 32 36 40 44 48 -40 Projectile Z number Fig. 2. (a) The sum of the fusion barriers calculated by formulae (1) and the Q-values for the fusion of 208 Pb (arbitrary taken to be the target) and the heaviest isotope of the elements with the Z numbers plotted on the horizontal axis. (b) The same as in (a) for the lightest isotope 60 0 50 4 8 12 16 20 24 28 36 40 44 60 B(Bass) B(Coulomb) B(Wilcke et al) B(Wilczynski) (a) 40 (B + Q) / MeV 32 30 50 40 30 20 20 10 10 0 0 238 U+ the heaviest projectile isotopes -10 -10 -20 60 -20 60 (B + Q) / MeV 50 50 (b) 40 40 30 30 20 20 10 10 0 Fig. 3. The same as in Fig. 2, but the target is 238U 0 238 U+ the lightest projectile isotopes -10 -20 0 4 0 4 8 12 16 20 24 -10 28 32 36 -20 44 40 Projectile Z number 60 50 8 12 16 20 24 28 (B + Q) / Mev 36 40 B(Bass) B(Coulomb) B(Wilcke et al) B(Wilczynski) (a) 40 30 60 50 40 30 20 20 10 10 0 0 248 Cm + the heaviest projectile isotopes -10 -20 -10 -20 -30 -30 60 60 50 (B + Q)/ MeV 32 50 (b) 40 40 30 30 20 20 10 10 0 0 248 -10 -20 -30 -10 Cm + the lightest projectile isotopes 0 4 8 12 16 20 24 -20 28 Projectile Z number 32 36 40 -30 Fig. 4. The same as in Fig. 2, but the target is 248Cm 0 4 8 12 16 20 24 28 (a) 40 30 (B + Q) / MeV 32 36 40 B(Bass) B(Coulomb) B(Wilcke et al) B(Wilczynski) 50 40 30 20 20 10 10 0 0 249 Cf + the heaviest projectile isotopes -10 -20 -10 -20 -30 -30 50 50 (b) 40 (B + Q) / MeV 50 40 30 30 20 20 10 10 0 0 249 -10 -20 -30 -10 Cf + the lightest projectile isotopes 0 4 8 12 16 20 24 -20 28 32 36 40 -30 Projectile Z number Fig. 5. The same as in Fig. 2, but the target is 249Cf. Reaction with the heaviest isotope 208 Pb +82Se 238 U + 88Sr 248 Cm + 82Se 249 Cf+82Se Table 3 Compound Reaction with the lightest nucleus isotope 290 208 116 Pb +84Sr 326 238 130 U + 90Zr 330 248 130 Cm+84Sr 331 249 132 Cf+78Kr Compound nucleus 292 120 328 132 332 134 327 134 Table 3 shows the combinations of nuclei that satisfy the criterion (B+Q) 0 and result in producing compound nuclei with the largest Z values. The results obtained for odd Z projectiles are similar to the results for even Z projectiles shown in Figs. 2-5 and didn’t provide for the possibility of the synthesis of elements with Z134. From entrance channel consideration, combinations of a light isotope of the less heavy element and a heavy isotope of the heavier element are a bit more advantageous for producing nuclei with the extreme atomic number in complete fusion reactions. Fig. 6 shows the driving potential per one projectile mass unit (B+Q)/Aproj. for fusion reactions involving heavy targets. As can be seen, it is close to zero for the projectile mass number A ~80. The calculations were carried out using the Wilczynski model [20]. The other models give similar results. [B(Wilcz.)+Q]/A, MeV/(m. u.) 4.0 0 10 20 30 40 50 60 70 80 90 100 110 120 4.0 3.6 3.6 3.2 3.2 2.8 208 b Pb 2.4 238 U 248 Cm 1.6 Cf 1.2 2.0 1.6 249 1.2 2.8 2.4 2.0 0.8 0.8 0.4 0.4 0.0 0.0 -0.4 -0.4 0 10 20 30 40 50 60 70 80 90 100 110 120 Projectile mass number A Fig. 6. Driving potential per one projectile mass unit versus Aproj.. The B was calculated by the Wilczynski model and corrected by formulae (1). The targets were 208Pb, 238U, 248Cm and 249 Cf .For every projectile Z, there are two dots referring to the heaviest and the lightest isotopes. 4. Conclusion Formulae (1) allow us to obtain fusion barrier values based on a large body of experimental data on (HI, xn) reactions including those used for the synthesis of the heaviest elements produced up to now. Analysis based on the (B+Q) criterion ensures an optimum choice of fusion reaction intended to be used for producing new elements. It can be illustrated with the situation about element 118, which was intended to be produced in a 208Pb(86Kr,1n) reaction. The production cross section was predicted to be 670 pb [45]. The observed events corresponded to cross section of ~2pb [48] and were retracted later [49]. From the standpoint of our approach, these experiments had very little chance for success since (B+Q) 0 for that reaction and fusion process is suppressed (see Fig. 2(a)). 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