Introduction
To date, the synthesis of 11 isotopes – 149Lu [1], 207Th [2], 251,264Lr [3, 4], 166Pm, 168Sm, 170Eu, 172Gd [5], 204Ac [6], 39Na [7], and 286Mc [8] – in the last year has brought the total count to 3,327 known nuclei in the nuclide chart. This comprises 288 natural nuclides (254 stable isotopes with lifespans longer than the Earth’s age and 34 unstable nuclides) and 3,039 species of nuclei synthesized in global laboratories. These syntheses utilize techniques such as fusion-evaporation (FE), multinucleon transfer (MNT), deep inelastic reactions (DIR), projectile fragmentation (PF), spallation, fission (SF), neutron capture (NC), and thermonuclear tests (TT) [9]. However, various theoretical models predict the existence of an additional 8,000 to 10,000 unknown bound isotopes in the nuclei chart [10-12]. This suggests that at least over 5,000 nuclides remain to be discovered by nuclear experimentalists, particularly in the realms of nuclear drip lines and the stability islands of superheavy nuclei.
In recent years, laboratories across the globe have made significant advancements in nuclear synthesis. From an experimental standpoint, several new nuclear species have been produced: 207Th, 235Cm, 214U, 222Np, 211Pa, 280Ds[2, 13-15], and others via fusion-evaporation (FE) reactions; 110Zr, 121Tc, 129Pd, and more through projectile fragmentation (PF)[16]; and 223,229Am, 233Bk[17], among others, using multinucleon transfer (MNT) reactions. This study has garnered significant attention from leading research facilities, including the Lanzhou Heavy Ion Research Facility (HIRFL) in China, Joint Institute for Nuclear Research (JINR) in Russia, Helmholtz Centre for Heavy Ion Research (GSI) in Germany, Grand Accëlërateur National d’Ions Lourds (GANIL) in France, and Argonne National Laboratory (ANL) in the USA, actively working towards the synthesis of new nuclides in regions near the drip lines and within the superheavy region.
In efforts to elucidate the damped collision mechanism and predict the synthesis cross-sections of target nuclides, theorists have crafted intricate yet pragmatic models to represent the multinucleon transfer reactions occurring at incident energies close to the Coulomb barrier. Notable among these are the GRAZING model[18-20], the dinuclear system (DNS) model[21-30], and a dynamical model anchored in the Langevin equations[31, 32]. There are also microscopic methods that account for the degrees of freedom inherent to nucleons. Examples include the time-dependent Hartree (TDHF) approach[33-35] and the improved quantum molecular dynamics model (ImQMD)[36, 37]. Although each model possesses its distinctive attributes, they are all capable of faithfully replicating available experimental data. The DNS model, in particular, offers a comprehensive view, considering factors, such as the shell effect, dynamic deformations, fission, quasi-fission, deep-inelastic mechanisms, and the odd-even effect. Furthermore, it stands out for its exceptional computational efficiency.
In this study, we compared the calculated cross-sections of target-like fragments resulting from MNT reactions of 132,136Xe + 248Cm at incident energies proximate to the Coulomb barriers with the available experimental data, using the DNS model as a basis. To delve into the interplay between the Coulomb force and shell effect in the MNT process, we selected isobaric projectiles with a mass number A=208A=208 in proximity to the double magic nucleus 208Pb. These projectiles were directed to bombard targets 232Th and 248Cm at energies consistent with the Coulomb barrier. Our analysis further explores the production cross-sections of yet-to-be-identified actinide isotopes in isobaric collisions. The structure of this study is as follows: In Sec. 2, we provide a concise overview of the DNS model. Sec. 3 presents the calculation results and subsequent discussion. Finally, a summary and conclusions drawn from our study are detailed in Sec. 4.
Model Description
Initially, Volkov introduced a concept to depict deep inelastic heavy-ion collisions[38]. Later on, Adamian incorporated a quasi-fission component into the massive fusion process[39, 40]. Subsequent enhancements, including modifications to the relative motion energy and angular momentum of the colliding nuclei, in tandem with nucleon transfer, were developed within the DNS framework by the Lanzhou Group[41]. The production cross-sections of superheavy nuclei (SHN), quasi-fission, and fusion–fission dynamics have been comprehensively examined within the dynamical DNS model. The dynamic evolution of the colliding system involves sequential processes: overcoming the Coulomb barrier to form the DNS, adjusting the relative motion energy, angular momentum, mass, charge asymmetry, among other factors, within the potential energy surface, and finally, the de-excitation of primary fragments[42]. The production cross-section of the MNT fragments was determined as follows:
In the DNS model, the solution for nucleon transfer and relative motion involves a set of microscopic derivations, and the master equations distinguish between protons and neutrons. The fragment distribution probability,
The excited DNS creates a valence space where the valence nucleons are symmetrically distributed around the Fermi surface. Only particles in states within this valence space participate actively in nucleon transfer. The local excitation energy and nucleon transfer influence the transition probability. These are microscopically determined from the interaction potential within the valence space, as detailed in [47, 48].
The motion of the nucleons in the interacting potential is governed by a single-particle Hamiltonian[41, 50]:
The total kinetic energy (TKE-mass) of the primary fragment was evaluated using the following expression:
The survival probability
Results and Discussion.
We calculated the production cross-sections of actinide isotope chains with atomic number Z = 93-100 in the collisions of 132,136Xe + 248Cm at incident energy Elab = 699-790 MeV, as shown in Fig. 1. Compared with the available experimental data for 129,132,136Xe + 248Cm, which are represented by a solid red star, solid blue circle, and solid black squares with error bars, respectively, our calculation of 136Xe + 248Cm, marked by solid black lines, and 132Xe + 248Cm, marked by dashed red lines, could reproduce the tendency of the cross-sectional distribution of actinide isotopic chains. From experimental data[59, 60], it was determined that projectile 129,132,136Xe isotopes induced reactions with the target 248Cm to provide actinide products that have a large overlap distribution area in the neutron-rich region. This was not clearly distinguishable as expected. From our calculation in terms of the deep-inelastic mechanism, relative proton-rich projectile 132 Xe-induced reactions tend to shift to the proton-rich region when compared to the experimental results. Based on the data presented in Figs. 1, target-like fragments have production cross-sections of magnitude levels from 100 millibarns to 10 nanobarns. When significantly distanced from the target, the formation cross-section of products below the target declines more gradually than that of trans-target products. This suggests that quasi-fission plays a more dominant role in these collisions. It is worth noting that our calculations have limitations: they rely on a model with free parameters both for calculating the primary fragment cross-section and for estimating the survival probability against fission.
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To investigate the competition between the Coulomb repulsive potential and shell effect in MNT reactions, we calculated the reactions of isobaric projectiles with A=208 bombarding targets 248Cm and 232Th at incident energy Ec.m.=1.1× VB. The calculation details of these collisions are presented below. The interaction potential between the colliding partners was combined with the Coulomb and nuclear potentials. In Fig. 2(a), interaction potential VCN of 208Pt + 248Cm, 208Hg + 248Cm, 208Pb + 248Cm, 208Po + 248Cm, and 208Rn + 248Cm reactions were marked by solid black, dashed red, dash-dot blue, dash-dot-dot green, and short dashed olive lines, respectively. The tendencies of VCN distributions for these collisions were similar. A larger Coulomb potential results in a larger interaction potential VCN. Specifically, VCN increases exponentially with decreasing distance R decreasing in the attraction region of the nuclear force, where it increases slowly. Nucleon transfer occurred in the touch configuration. Based on the deflection function, the sticking times of the colliding partners are calculated for all impact parameters [49], as shown in Fig. 2(b), which decreases exponentially as angular momentum increases. In these collisions, a relatively large Coulomb potential resulted in a longer sticking time with a fixed impact parameter. During the sticking time, the kinetic energy dissipates into the composite system to heat with the internal excitation energy, which increases exponentially with reaction time and reaches equilibrium at approximately 2× 10-21 s, as shown in Fig. 2(c).
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After the colliding partners are captured, the dissipated kinetic energy, combined with the angular momentum in the DNS, allows them to diffuse along the potential energy surface (PES). This is followed by nucleon rearrangement between the colliding entities, determined by solving a set of master equations. The PES and driving potential were derived using Eqs.(12). These are composed of the Coulomb potential, binding energy, and nuclear potential. They are calculated using the Wong formula, the liquid-drop model with shell correction, and the double folding method, respectively, as cited in [42]. The driving potential of projectiles 208Hg, 208Pb, and 208Po on targets 248Cm and 232Th during tip-tip collision at a fixed distance is plotted as a function of mass asymmetry, denoted as η. Here,
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Open circles and stars represent the projectile–target injection points. Panels (a) and (e) show that the tendencies of the driving potential trajectories for these collisions are similar. Two pockets appeared at η = 0.2, 0 to derive the potentials of the target 248Cm-based reactions. One pocket in the driving potentials for the target 232Th-based reactions appears at η = 0.2. The neutron subshell number N=162 can potentially play a crucial role in pocket formation. For projectiles, such as 208Po, which are distant from the β- stable line, their initial points of interaction lie significantly away from their respective driving potential trajectories. As diffusion starts, they quickly converge toward the driving potential path. Generally, using the PES, one can broadly predict the spectral distribution trend across each isotope chain.
By solving a set of master equations, we derived the production probabilities of primary fragments with their respective excitation energies. These equations categorized the fragments based on mass number and kinetic energy as delineated in Eq. (16). These distributions are illustrated in Figs. 4, with driving potential trajectories represented as solid grey lines. From Fig. 4, we observe two prominent peaks in the high kinetic regions, situated around the projectile–target injection points. Additionally, cross-sections tend to concentrate in the valleys of the driving potential trajectories. Reactions involving projectiles 208Hg, 208Pb, and 208Po with targets 248Cm and 232Th at the incident energy Ec.m. = 1.1 × VB exhibited TKE-mass distributions that were both symmetric and expansive. The TKE-mass distribution spans broadly within the kinetic range of 500–800 MeV and mass range of 160–-280 MeV, suggesting a potential transfer of more than 30 nucleons.
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Utilizing the statistical evaporation program, we calculated the survival probability of the excited primary fragments, which in turn determined the production cross-sections of the secondary fragments. The production cross-sections of primary and secondary fragments, delineated by mass and charge numbers in the collisions from projectiles 208Hg, 208Pb, and 208Po with target 248Cm at Ec.m. = 1.1 × VB, are depicted in Fig. 5 panels (a) through (f). The solid blue and dashed red lines represent secondary and primary fragments, respectively, while regions of superheavy nuclei are highlighted with rectangular shading. Our findings show that primary fragments span a vast charge spectrum, even reaching the superheavy regions. Conversely, secondary fragment production was significantly dampened by de-excitation. This reduction is attributed to the fact that highly excited primary trans-target fragments, having minimal fission barriers, are prone to undergoing fission. Our predictions indicate cross-sections for superheavy nuclei (with atomic numbers Z = 104-116) exceeding 10 picobarns. The neutron subshell N=162 may be particularly influential, especially in the 208Po + 248Cm collision.
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Secondary production cross-sections for actinide target-like fragments, including isotopes of Actinium, Thorium, Protactinium, Uranium, Neptunium, Plutonium, Americium, Curium, Berkelium, Californium, Einsteinium, Fermium, Mendelevium, Nobelium, and Lawrencium, have been calculated. These calculations pertain to collisions involving projectiles 208Pt, 208Hg, 208Pb, 208Po, 208Rn, and 208Ra bombarding on targets 248Cm at Ec.m. = 1.1 × VB. The line representations for these projectiles in Fig. 6 are as follows: solid black for 208Pt, dashed red for 208Hg, dash-dot green for 208Pb, dashed-dot-dot blue for 208Po, and short dashed olive for 208Rn. Observations indicate that collisions characterized by a smaller Coulomb force lean towards the neutron-rich region, whereas those with a more substantial Coulomb force gravitate to neutron-deficient areas. Numerous previously unidentified actinide isotopes are predicted from reactions 208Pt+248Cm, 208Hg+248Cm, 208Pb+248Cm, 208Po+248Cm, 208Rn+248Cm, and 208Ra+248Cm. These predictions are detailed in Table 1. For the new neutron-rich actinide isotopes, 208Pt+248Cm reactions produce the largest cross-sections. However, 208Pt remains unclear. Notably, unknown actinide products are highly dependent on the Coulomb potential. The 208Rn+248Cm reactions result in the largest cross-sections for new neutron-deficient actinide isotopes. The open circles represent the new neutron-rich actinide nuclides.
248Cm + | 208Pt | 208Hg | 208Pb | 248Cm+ | 208Pt | 208Hg | 208Pb | 248Cm+ | 208Pt | 208Hg | 208Pb |
---|---|---|---|---|---|---|---|---|---|---|---|
237Ac | 6.8 μb | 24 nb | 254Pu | 1.3 μb | 261Es | 16 μb | 2.2 μb | 7.6 nb | |||
238Ac | 2.6 μb | 6.9 nb | 255Pu | 0.2 μb | 262Es | 0.2 μb | 0.1 μb | 0.3 nb | |||
239Ac | 1 μb | 1.8 nb | 256Pu | 8.4 nb | 263Es | 0.3 μb | 22 nb | 0.1 nb | |||
240Ac | 28 nb | 0.1 nb | 248Am | 11 mb | 50 mb | 56 μb | 264Es | 23 nb | 1.1 nb | 30 pb | |
241Ac | 2.8 nb | 0.5 pb | 249Am | 4.5 mb | 1 mb | 1.1 μb | 265Es | 9.2 nb | 30 pb | ||
239Th | 20 μb | 0.2 μb | 0.34 nb | 250Am | 3.9 mb | 0.3 mb | 74 nb | 260Fm | 1.3 μb | 2.1 μb | 0.3 μb |
240Th | 8.4 μb | 64.8 nb | 0.04 nb | 251Am | 1.1 mb | 14 μb | 6.6 nb | 261Fm | 2.4 μb | 1.4 μb | 0.1 μb |
241Th | 5 μb | 9.6 nb | 252Am | 0.4 mb | 1.5 μb | 262Fm | 1.6 μb | 0.4 μb | 16 nb | ||
242Th | 0.7 μb | 0.94 nb | 253Am | 0.3 mb | 0.2 μb | 263Fm | 0.7 μb | 0.1 μb | 2.8 nb | ||
243Th | 0.1 μb | 0.02 nb | 254Am | 72 μb | 16 nb | 264Fm | 0.1 μb | 5.8 nb | 0.08 nb | ||
244Th | 26 nb | 255Am | 17 μb | 1.9 nb | 265Fm | 34 nb | 0.9 nb | ||||
245Th | 2.8 nb | 256Am | 2.7 μb | 40 pb | 266Fm | 7 nb | 0.1 nb | ||||
246Th | 0.3 nb | 257Am | 0.3 μb | 267Fm | 0.9 nb | 10 pb | |||||
240Pa | 0.5 mb | 7.8 μb | 20. nb | 258Am | 9.7 nb | 261Md | 0.9 μb | 1.9 μb | 1.7 μb | ||
241Pa | 0.4 mb | 4.9 μb | 5.5 nb | 252Cm | 0.8 mb | 0.6 mb | 43 nb | 262Md | 0.6 μb | 0.6 μb | 0.2 μb |
242Pa | 0.2 mb | 1.1 μb | 0.5 nb | 253Cm | 0.2 mb | 47 μb | 1.9 nb | 263Md | 2.3 μb | 1.2 μb | 0.5 μb |
243Pa | 10 μb | 0.2 μb | 5 pb | 254Cm | 0.1 mb | 9.7 μb | 0.2 nb | 264Md | 0.5 μb | 0.2 μb | 62 nb |
244Pa | 28 μb | 17 nb | 255Cm | 97 μb | 2.8 μb | 2 pb | 265Md | 0.4 μb | 74 nb | 18 nb | |
245Pa | 3.3 μb | 1 nb | 256Cm | 28 μb | 0.3 μb | 266Md | 35 nb | 3.7 nb | 0.9 nb | ||
246Pa | 0.4 μb | 20 pb | 257Cm | 11 μb | 40 nb | 267Md | 23 nb | 1.1 nb | 40 pb | ||
247Pa | 74 nb | 258Cm | 1.4 μb | 1.7 nb | 268Md | 1.6 nb | 40 pb | ||||
248Pa | 7.3 nb | 259Cm | 0.1 μb | 40 pb | 269Md | 0.7 nb | 8 pb | ||||
249Pa | 0.6 nb | 260Cm | 0.8 nb | 261No | 6.3 nb | 54 nb | 47 nb | ||||
250Pa | 9 pb | 252Bk | 0.2 mb | 0.7 mb | 36 μb | 262No | 12 nb | 64 nb | 219 nb | ||
243U | 0.9 mb | 9.1 μb | 18.4 nb | 253Bk | 0.3 mb | 0.9 mb | 1.9 μb | 263No | 0.1 nb | 206 nb | 68 nb |
244U | 0.7 mb | 2.2 μb | 2.2 nb | 254Bk | 0.2 mb | 0.1 mb | 0.1 μb | 264No | 0.2 nb | 131 nb | 47 nb |
245U | 2.2 mb | 0.5 μb | 70 pb | 255Bk | 0.1 mb | 46 μb | 14 nb | 265No | 0.1 nb | 86 nb | 5.4 nb |
246U | 46 μb | 29 nb | 256Bk | 81 μb | 12 μb | 1.5 nb | 266No | 62 nb | 16 nb | 0.15 nb | |
247U | 10 μb | 2.6 nb | 257Bk | 0.1 mb | 5.2 μb | 0.3 nb | 267No | 16 nb | 2.6 nb | 0.01 nb | |
248U | 1.7 μb | 0.3 nb | 258Bk | 36 μb | 0.4 μb | 3 pb | 268No | 6 nb | 0.4 nb | ||
249U | 0.2 μb | 259Bk | 22 μb | 46 nb | 269No | 1.3 nb | 70 pb | ||||
250U | 14 nb | 260Bk | 2.5 μb | 2. nb | 267Lr | 86 nb | 31 nb | 15 nb | |||
251U | 1.1 nb | 261Bk | 0.1 μb | 20 pb | 268Lr | 12 nb | 2.1 nb | 0.6 nb | |||
245Np | 3.3 μb | 1 nb | 261Bk | 6.1 nb | 269Lr | 17 nb | 1.5 nb | 0.1 nb | |||
246Np | 4.3 μb | 20 pb | 257Cf | 27 μb | 12 μb | 0.3 μb | 270Lr | 1.2 nb | 0.1 nb | 6 pb | |
247Np | 74 nb | 258Cf | 24 μb | 4.5 μb | 36 nb | 271Lr | 0.9 nb | 80 pb | 1 pb | ||
248Np | 7.3 nb | 259Cf | 23 μb | 1.6 μb | 6.5 nb | ||||||
249Np | 0.7 nb | 260Cf | 9.2 μb | 0.1 μb | 0.4 nb | ||||||
248Pu | 17 mb | 41 μb | 12.8 nb | 261Cf | 1.4 μb | 15 nb | 7 pb | ||||
249Pu | 2.7 mb | 11 μb | 1.3 nb | 262Cf | 6.1 nb | 0.3 nb | |||||
250Pu | 0.3 mb | 0.2 μb | 0.019 nb | 263Cf | 0.6 nb | ||||||
251Pu | 0.1 mb | 30 nb | 258Es | 7.4 μb | 6.2 μb | 1.1 μb | |||||
252Pu | 48 μb | 2.4 nb | 259Es | 29 μb | 13 μb | 0.3 μb | |||||
253Pu | 13 μb | 10 pb | 260Es | 11 μb | 3 μb | 34 nb |
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Figure 7 shows secondary production cross-sections of all the formed fragments in collisions of 208Os+248Cm, 208Pt+248Cm, 208Hg+248Cm, 208Pb+248Cm, 208Po+248Cm, 208Rn+248Cm, 208Ra+248Cm, and primary production cross-sections of 208Pb+248Cm at the incident energy Ec.m. = 1.1 × VB as N-Z panel. Panels (g) and (h) clearly show the de-excitation effects. Panels (a), (b), (c), (d), (e), (f), and (h) show that many new isotopes are predicted, including neutron-rich and neutron-deficient isotopes and even superheavy nuclei. The projectile-target injection points and all existing isotopes in the nuclide chart are represented by solid black triangles and open squares, respectively.
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Conclusion
Using the DNS model framework, we systematically calculated the production cross-sections of MNT fragments in reactions involving projectiles such as 208Os, 208Pt, 208Hg, 208Pb,208Po, 208Rn, 208Ra, and 132,136Xe colliding with targets 232Th and 248Cm around Coulomb barrier energies. To investigate the isospin diffusion on the formation of actinide products during the MNT process, the same number of projectiles with A=208 were selected. Our calculation for 132,136Xe + 248Cm is consistent with the available experimental data. The sticking time for these colliding systems, inferred from deflection functions, was significantly influenced by the Coulomb force, especially at smaller impact parameters. Furthermore, PES and TKE of these reactions, which can contribute to predicting the tendency of cross-sectional diffusion, are discussed. A relatively large cross-section from TKE appears around the pockets in PES, where the neutron subshell N=162 is evident. The de-excitation process strongly depresses the primary cross-section of actinide isotopes up to four magnitude levels. The production cross-section of the new actinides is highly dependent on the N/Z ratio of the isobaric projectile. It was determined that the Coulomb force coupled with the shell effect plays a crucial role in the production of cross-sections of actinides products in MNT reactions. These five colliding systems predicted a wide array of previously unknown heavy isotopes, with accessible cross-sectional values even for superheavy nuclei within the charge numbers Z=104-110.
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