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Effective nucleus-nucleus potentials for heavy-ion fusion reactions

NUCLEAR PHYSICS AND INTERDISCIPLINARY RESEARCH

Effective nucleus-nucleus potentials for heavy-ion fusion reactions

Ning Wang
Jin-Ming Chen
Min Liu
Nuclear Science and TechniquesVol.36, No.2Article number 24Published in print Feb 2025Available online 10 Jan 2025
14302

Based on the Skyrme energy density functional and reaction Q-value, this study proposed an effective nucleus-nucleus potential for describing the capture barrier in heavy-ion fusion processes. The 443 extracted barrier heights were well reproduced with a root-mean-square (RMS) error of 1.53 MeV and the RMS deviations with respect to 144 time-dependent Hartree–Fock capture barrier heights was only 1.05 MeV. Coupled with the Siwek–Wilczyński formula, wherein three parameters were determined by the proposed effective potentials, the measured capture cross sections at energies around the barriers were reasonably well reproduced for several fusion reactions induced by nearly spherical nuclei as well as by nuclei with large deformations, such as 154Sm and 238U. The shallow capture pockets and small values of the average barrier radii resulted in the reduction of the capture cross sections for 52,54Cr-and 64 Ni-induced reactions, which were related to the synthesis of new super-heavy nuclei.

Nucleus-nucleus potentialFusion reactionsSuperheavy nucleiCapture cross sections
1

Introduction

The investigation of heavy-ion fusion reactions is important for the synthesis of new superheavy nuclei (SHN) [1-14] and extremely proton-rich nuclei [15-17] and the exploration of nuclear structures [18-22]. In the case of fusion reactions involving light and intermediate nuclei, approaches such as fusion-coupled channel calculations [23-24] and empirical barrier distribution methods [25-30] have been adopted to calculate capture (fusion) cross sections. These calculations are typically based on the static or dynamic nuclear potentials [31-37]. Static potentials are typically characterized using models, such as the liquid drop model, energy density functional, or double-folding concept, coupled with a sudden approximation. The precise characterization of the nucleus–nucleus potential, particularly at short distances, is essential for comprehending the fusion mechanism.

A previous study [27] proposed a static entrance channel nucleus-nucleus potential to describe heavy-ion fusion reactions. They used the Skyrme energy density functional [38] combining the extended Thomas-Fermi (ETF) approach [39-41] and the sudden approximation for densities. By introducing an empirical barrier distribution composed of a combination of two Gaussian (2G) functions to consider the dynamic effects in the fusion processes, the most probable barrier heights VB0.946B0 (with frozen barrier height B0) and fusion excitation functions for various reactions can be described reasonably well [27, 28, 37]. Although certain measured fusion cross sections can be accurately reproduced, the realistic nucleus–nucleus potential in fusion processes, particularly at short distances, remains unclear. In addition, for certain fusion reactions related to the synthesis of super-heavy nuclei such as 64Ni+238U [42, 43], the extracted capture cross sections from the measured mass-total kinetic energy (TKE) distributions at energies above the Bass barrier [32] are significantly smaller than the predicted results of the classic fusion cross-section formula σcap=πRB2(1VB/Ec.m.) and the results of ETF+2G approach mentioned above. Owing to the measurements being highly time-consuming for reactions yielding elements 119 and 120, an accurate prediction of the capture cross sections and the evaporation residue (EvR) cross sections [44-48] is required.

In addition to static nuclear potentials, certain microscopic dynamics models [49], such as the time-dependent Hartree–Fock (TDHF) [50-52] and improved quantum molecular dynamics (ImQMD) model [53, 54] have also been widely adopted in studies focused on heavy-ion fusion reactions, wherein the time evolution of the densities of the composite system can be self-consistently described. Recently, the capture thresholds for 144 fusion reactions induced by nearly spherical nuclei have been systematically studied using TDHF calculations [55]. In conjunction with the Siwek-Wilczyński (SW) cross-section formula, which incorporates the classic cross-section formula by folding it with a Gaussian barrier distribution, the experimentally measured fusion cross sections at energies around the barriers can be reproduced well for certain fusion reactions such as 132Sn+40,48Ca. Moreover, the reaction Q-value can influence the fusion cross sections at sub-barrier energies in reactions with nearly spherical nuclei [55]. However, for fusion reactions involving strongly deformed nuclei, such as 154Sm, 238U, and 243Am, the effective consideration of both the Q-value and nuclear static deformations in the calculation of capture cross sections remains an unresolved issue. Furthermore, as microscopic TDHF calculations are extremely time-consuming, a time-saving nucleus-nucleus potential with high accuracy needs to be developed for the systematic study of fusion reactions.

In this work, we attempt to proposed an effective nucleus-nucleus potential based on the Skyrme energy density functional (EDF) and the reaction Q-value for a systematic description of heavy-ion fusion reactions, particularly reaction systems with well-deformed nuclei.

2

Effective nucleus-nucleus potential

In this study, we first calculated the frozen nucleus–nucleus potential based on Skyrme EDF. The entrance-channel nucleus–nucleus potential V(R) between two nuclei is expressed as [27, 56] V(R)=Etot(R)E1E2, (1) where R is the center-to-center distance between the two fragments, Etot(R) denotes the total energy of the nuclear system, and E1 and E2 denote the energies of the reaction partners at an infinite distance. The total energy of a nuclear system can be expressed as an integral of the Skyrme EDF H(r) using the frozen density approximation: Etot(R)=H[ρ1p(r)+ρ2p(rR),ρ1n(r)+ρ2n(rR)]dr. (2) The energies E1 and E2 are expressed as E1=H[ρ1p(r),ρ1n(r)]dr, (3) E2=H[ρ2p(r),ρ2n(r)]dr. (4) where ρ1p, ρ2p, ρ1n, and ρ2n are the frozen proton and neutron densities of the projectile and target described by spherically symmetric Fermi functions. When calculating the energies and corresponding densities of the reaction partners, Skyrme EDF with the parameter set SkM*[57] was adopted. Further, the extended Thomas-Fermi (ETF2) approach was used to describe both the kinetic energy density and spin-orbit density within the EDF.

Based on the entrance nucleus–nucleus potential V(R), the frozen barrier height B0 and depth of the capture pocket Bcap can be obtained [56]. The solid curve in Fig. 1(a) denotes the calculated V(R) value for the reaction 40Ca+144Sm. Certain microscopic dynamics simulations have indicated that the frozen potential barrier is reduced in the fusion process owing to the dynamic deformations of the reaction partners and nucleon transfers. In a systematic study of 16O-induced fusion using the ImQMD model in [54], the dynamic barrier height was lower than the frozen barrier height by approximately 5%.

Fig. 1
(a) Nucleus-nucleus potential for 40Ca + 144Sm. The solid and dot-dashed curves denote the frozen and effective potentials, respectively. The short dashed lines denote the position of the frozen barrier R0 and that of the pocket Rs. (b) Empirical barrier distribution for 40Ca + 144Sm proposed in [27]
pic

To consider the influence of the dynamic effect, we proposed an effective potential (EP) VD (R) for fusion systems in the regions before the contact of the two nuclei: VD(R)=V(R)[1kerfc(RR0s1)], (5) with two parameters of k=0.027 and s=1.0 fm. With an increase in R between the two nuclei, the Coulomb excitation becomes negligible, and VD(R) is consequently close to V(R). The dot-dashed curve in Fig. 1(a) denotes the effective nucleus-nucleus potential for 40Ca+144Sm. The barrier height was reduced from B0=150.57 MeV to VB=143.32 MeV, and in the region R >13.5 fm, one had VD(R)V(R). Figure 1(b) shows the empirical barrier distribution with the superposition of the two Gaussian functions proposed in [27]. Notably, the value of VB approached the average barrier height owing to the distribution function. Further, the effective barrier radius RB was slightly larger than the frozen radius R0.

Following projectile-target contact at energies around the barrier height VB, the frozen density approximation is no longer applicable because of the dynamic evolution of the neck. For a light fusion system, the compound nucleus is formed directly after the fusion barrier is overcome because the fission barrier is sufficiently high to render fission an improbable decay mode at incident energies close to the fusion barrier, and the potential VD should approach -Q when the distance between the two fragments becomes very small. For heavy systems, such as the reactions leading to SHN, the influence of quasi-fission becomes evident. This implies that the effective entrance-channel nucleus-nucleus potential VD(R) for heavy systems could be significantly larger than the value of -Q at short distances. Moreover, nucleon transfer through the neck becomes an important method to form the compound nucleus, as described in the dinuclear system (DNS) model [45, 47, 58-61]. In the regions following the projectile-target contact, the effective potential (EP) is expressed as VD=Vs+ΔUQVs1+exp[(RR2)/s]+(V1Vs)exp(RR1s), (6) where Vs and V1 are the corresponding effective potentials obtained using Eq. (5) at distance R=RBΔR and at the touching point R=R1, respectively. Further, ΔR=R0Rs and R2=Rs/2. R0 and Rs are the barrier radius and position of the capture pocket in the frozen nucleus-nucleus potential V(R), respectively (indicated by the dashed lines in Fig. 1). In this study, the touching point R1 was considered as R1={R0:ΔR<1.5fmR0ΔR/2:ΔR1.5fm (7) where ΔU=(VB+Q)(VBsym+Qsym) denotes the difference between the driving potential at the entrance channel and that of the corresponding symmetric system (i.e., the mass asymmetry of the projectile-target combination is approximately zero). According to the DNS model, the nucleon transfer is primarily governed by the driving potential. Here, we introduce the truncation for fusion reactions, that is, ΔU0 and VsQ, considering that the energy of the composite system after the projectile-target contact should be larger than that of the compound nucleus at its ground state for fusion reactions with heavy nuclei.

Figure 2 shows the calculated effective potentials for the reactions 16O + 208Pb, 48Ca + 208Pb, 30Si + 238U, and 70Zn + 209Bi. The frozen nucleus–nucleus potentials (solid curves) are also presented for comparison. In a previous study [62], the fusion barrier parameters for 367 reaction systems were systematically extracted based on 443 datasets of measured fusion/fission cross sections. The green squares denote the extracted barrier heights [62]. As evident, the capture barrier heights VB obtained from the effective potential (EP) were consistent with the experimental values. In this study, the calculated VB with the proposed EP was systematically compared with the extracted barrier heights. The root-mean-square (RMS) deviations with respect to the 443 extracted barrier heights was 1.53 MeV, which is smaller than the Bass [32, 33] and BW91 [34] potentials. For 16O + 208Pb and 48Ca + 208Pb, the EP results approached the corresponding TDHF capture thresholds [55]. The RMS deviations with respect to the 144 capture barrier heights [55] predicted by TDHF calculations was only 1.05 MeV. Considering that microscopic TDHF calculations are extremely time-consuming, the proposed effective nucleus-nucleus potentials with similar accuracy would be useful for the systematic study of fusion reactions.

Fig. 2
Similar to the situation presented in Fig. 1(a), albeit for 16O + 208Pb, 48Ca + 208Pb, 30Si+ 238U and 70Zn + 209Bi. The green squares denote the extracted barrier heights [62]. The gray lines in (b) and (d) indicate the energies of VE=0.99 VB. VBTDHF indicates the predicted capture barrier height in the TDHF calculations [55]
pic

Figure 2 shows that for the intermediate fusion system 16O + 208Pb, the EP evidently decreased with a decrease in R after the projectile-target contact and gradually approached the value of -Q=46.5 MeV. However, for the heavy fusion system 70Zn + 209Bi, the EP slightly decreased by BcapD=1.71 MeV after projectile-target contact, and at very short distances, the potentials were even higher than VB by approximately 2 MeV. This implied that the formation of the compound nuclei was a relatively slow process, and competition among fusion, quasi-fission, and deep-inelastic scattering was evident for this system. The gray lines in (b) and (d) denote the energies VE=0.99 VB below which elastic scattering was the dominant process. Figure 2(d) also indicates the difficulty in forming compound nuclei in the reaction 70Zn + 209Bi at energies lower than VE based on the barrier penetration concept. This is because the potential barrier becomes extremely thick. In addition, compared with the EP for 30Si + 238U, wherein the depth of the capture pocket BcapD=9.38 MeV was considerably larger than that of 70Zn + 209Bi, the quasi-fission and deep-inelastic scattering events were considerably greater in 70Zn + 209Bi at energies around the capture barriers.

3

Capture cross sections

The couplings between the relative motion of colliding nuclei and the intrinsic degrees of freedom play an important role in heavy-ion fusion reactions. To consider these couplings, Stelson introduced the distribution of barrier heights D(B) in the calculation of the fusion excitation function [63]. A well-known example is the Gaussian distribution of barrier heights predicted from different orientations of colliding nuclei that undergo slow deviations from sphericity [63]. In a previous study [26], an analytical cross section formula was proposed for describing the capture excitation function at energies around the Coulomb barrier by Siwek-Wilczyńska and Wilczyński (SW) under the Gaussian distribution assumption, σcap(Ec.m.)=πRm2W2Ec.m.[Xerfc(X)+1πexp(X2)], (8) where X=(Ec.m.VB)/2W, VB and W denote the centroid and the standard deviation of the Gaussian function, respectively, and Rm denotes the average barrier radius, which is typically set as Rm=RB. In this study, the average barrier radius was Rm=(VDVE)RdR(VDVE)dR. (9) This was calculated using the effective potential VD at energies near the capture barrier height Ec.m.=(1±0.01)VB. Notably, RmRB for most fusion systems (indicated by the positions of the green squares in Fig. 2). In contrast, for reaction systems with very shallow capture pockets, Rm is significantly smaller than RB, which is discussed later.

For fusion reactions induced by heavy target nuclei with a quadrupole deformation of β2, the range of barrier heights ΔBβ2VBRT/RB owing to the different orientations of the deformed nuclei can be derived using an average target radius RT [22]. Therefore, the VB and β2 dependences of W are expected for reactions with deformed nuclei. In contrast, the excitation energy of the compound nuclei (related to the reaction Q-value) at energies around the barrier in the reaction with deformed nuclei is typically larger than that with neighboring spherical nuclei. For example, the Q-value of the reaction 16O+154Sm is higher than that of 16O+144Sm by approximately 12 MeV (which is further discussed later). In addition, for heavy nuclei with large deformations, the excitation threshold εth, defined as the energy of the lowest excited state of the reaction partner, is typically very small. For example, εth =0.082 MeV for 154Sm and εth =0.045 MeV for 238U. The deformation parameter β2 is model-dependent [64, 29]. Thus, it would be interesting to modify the barrier height effects with W having a Q-value and excitation threshold dependence.

Recently, the SW formula was applied to study the fusion excitation functions for reactions involving nearly spherical nuclei with three parameters determined by TDHF calculations [55]. The standard deviation of the Gaussian function W was observed to be related to the reaction Q-value and deformation effects. A relatively higher excitation energy at the capture position can facilitate stronger impacts on the dynamic deformations and nucleon transfer during the capture process, thereby broadening the width of the barrier distribution. Based on the concepts described in [55], we extended the expression of W to intermediate and heavy fusion reactions induced by nuclei with large deformations. The value of W for the fusion reactions induced by nuclei with large deformations is parameterized as W=23W0+13W1, (10) where W0=0.052(VB+Q) for reactions induced by nearly spherical nuclei [55]. In a systematic study of the fusion barrier parameters, Chen et al. determined the value of W(0.014+0.135λB)VB with the reduced de Broglie wavelength λB=/2μVB [62]. Considering the systematic behavior of W, we write W1=(0.048+ηε1/ε2)VB. Here, η=|A1A2|/(A1+A2) denotes the mass asymmetry of the reaction system, where A1 and A2 are the mass numbers of the projectile and target, respectively. Further, ε1 and ε2 denote smaller and larger energies of the lowest excited states for the reaction partners, respectively. Simultaneously, we introduce a truncation of the value of W, that is, W2.5W0. Equation (10) shows that the VB dependence of the barrier distribution width is considered in W1 and the deformation effects are indirectly considered using the Q-value in W0 and the energies of the lowest excited states in W1.

Table 1 lists the calculated barrier parameters of the reactions under consideration. The barrier height VB and average barrier radius Rm were obtained using Eqs. (5) and (9), respectively. The standard deviation of the Gaussian function W was obtained using Eq. (10). The reaction Q-value for unmeasured super-heavy system was obtained from the prediction of the Weizsäcker-Skyrme (WS4) mass model [65] with which the known masses can be reproduced with an RMS error of ~0.3 MeV [66] and the known α-decay energies of SHN can be reproduced with deviations smaller than 0.5 MeV [6, 12].

Table 1
Barrier parameters with the effective potential. Q denotes the reaction Q-value
Reaction VB (MeV) W (MeV) Rm (fm) Q (MeV)
16O+144Sm 60.51 1.66 10.66 -28.54
16O+154Sm 59.42 2.66 10.87 -16.43
32S+154Sm 114.34 4.61 11.31 -60.60
48Ca+154Sm 137.93 4.36 11.75 -90.74
30Si+238U 138.42 4.51 12.24 -93.01
48Ca+238U 191.19 3.95 12.71 -160.78
52Cr+232Th 225.26 4.92 8.15 -187.40
52Cr+248Cm 237.90 4.41 6.13 -203.95
54Cr+243Am 235.49 3.68 5.98 -207.20
64Ni+238U 263.37 3.22 5.42 -238.61
Show more

Figure 3 presents the effective potentials and fusion excitation functions for the reactions 16O + 144,154Sm. As shown in Fig. 3(a), the calculated barrier heights were consistent with the experimental values. The fusion barrier height for the neutron-rich system 16O + 154Sm was lower than that of 16O + 144Sm by 1.09 MeV. At very short distances, the potentials approached the corresponding values of -Q. From Fig. 3(b), it can be observed that the measured fusion cross-sections for both 16O + 144Sm and 16O + 154Sm were well reproduced.

Fig. 3
(a) Similar to situation presented in Fig. 2, albeit for 16O + 144,154Sm. The data for the barrier heights are obtained from [62]. (b) Fusion excitation functions for 16O + 144,154Sm. The scattered symbols denote the experimental data taken from [67] and the curves denote the predicted results with Eq. (8)
pic

Figure 4 shows the calculated capture excitation functions for reactions with the deformed nuclei 154Sm and 238U. The scattered symbols represent experimental data. The solid curves and short dashes denote the results of the effective potential coupled with the SW formula (Eq. (8)) and the results of the ETF+2G approach [27], respectively. Notably, at energies near the capture barriers, the experimental data were reasonably well reproduced by both approaches. For 48Ca + 238U, the measured cross-sections at the sub-barrier energies were reproduced considerably better using the EP+SW approach. Here, we emphasize that the SW formula was obtained from the folding of the Gaussian barrier distribution and the classic over-barrier fusion cross-section expression, which is not applicable to deep sub-barrier energies because it does not consider the barrier penetration effect. Figure 3 and 4 indicate that the measured capture cross sections at energies near the barrier were well reproduced by the SW formula. Thus, the folding of a suitable barrier distribution plays a role in describing the capture cross sections around barrier energies. In addition, the Wong formula [31], which considers the quantum mechanical tunneling effect, was used to fold the two-Gaussian barrier distribution in the ETF+2G calculations. As evident, the results from the two approaches were similar for the reactions 32S + 154Sm, 30Si + 238U, and 48Ca + 154Sm, which also indicates the importance of the barrier distribution.

Fig. 4
Capture excitation functions for the reactions 32S + 154Sm [68], 30Si + 238U [69], 48Ca + 154Sm [70], and 48Ca + 238U [71, 43, 72]. The solid curves and short dashes denote the results of the effective potential coupled with the SW formula (Eq. (8)) and the results of the empirical two Gaussian (2G) barrier distribution approach [27], respectively
pic

Simultaneously, the proposed effective potential (EP) was tested to describe fusion reactions leading to the synthesis of superheavy nuclei. Figure 5 shows the calculated EP for the reactions 30Si,48Ca,64Ni + 238U, and 54Cr+243Am. To observe the depth of the capture pockets more clearly, the potential and distance were scaled by VB and RB, respectively. Notably, the depths of the capture pockets significantly decreased with an increase in the product of the projectile-target charge numbers Z1 Z2. Very recently, Yao et al. found that the yields of fission-like events in the measured mass-TKE distributions and the ratio of capture to deep-inelastic scattering events evidently decreased with a decrease in the depths of the capture pockets Bcap [56]. To understand the underlying physics, we studied the average barrier radius, Rm. Table 1 shows that for the reactions induced by 52,54Cr and 64Ni, the average barrier radii were significantly smaller than those of the other reactions, although the contact distances were larger. With smaller average barrier radii for reactions with 52,54Cr and 64Ni, the corresponding capture cross-sections at the above barrier energies are expected to be reduced. Figure 6 shows the predicted capture cross-sections for the reactions 52Cr+ 232Th, 52Cr+ 248Cm, 54Cr+243Am, and 64Ni+ 238U. The green dashed and blue solid curves denote the results predicted using the empirical 2G barrier distribution and EP+SW approaches, respectively. The solid circles denote the experimental data obtained from [43]. As evident, for 52Cr+ 248Cm and 64Ni+ 238U, the capture cross-sections were significantly overpredicted by the ETF+2G approach. The dot-dashed curves denote the results with the ETF+2G approach but adopt the average barrier radius Rm in the calculations. When using Rm rather than RB in the calculations, the capture cross sections at the above barrier energies were considerably better reproduced. The predicted capture cross sections at sub-barrier energies with the effective potential were evidently smaller than those with the 2G approach for 52,54Cr induced reactions. This implies that the predicted 2n EvR cross sections would be considerably smaller than those obtained using the ETF+2G approach for the reaction 54Cr+243Am.

Fig. 5
Effective nucleus-nucleus potentials for 30Si,48Ca,64Ni + 238U and 54Cr+243Am
pic
Fig. 6
(Color online) Similar to the situation presented Fig. 4, albeit for 52Cr+232Th,248Cm, 54Cr+243Am and 64Ni+238U. The dot-dashed curves denote the results with the 2G approach but with the average barrier radius Rm rather than RB in the calculations. The data are obtained from [43]
pic
4

Summary

Based on the frozen nucleus–nucleus potential from the Skyrme energy density functional, coupled with the extended Thomas-Fermi approach and sudden approximation of densities, this study proposed an effective approach to obtain the capture barrier heights and average barrier radii for heavy-ion fusion reactions. The 443 extracted barrier heights were well reproduced with an RMS error of 1.53 MeV. The effective potential results were very close to the corresponding TDHF capture thresholds for 16O + 208Pb and 48Ca + 208Pb. The RMS deviation with respect to the 144 capture barrier heights predicted using the TDHF calculations was only 1.05 MeV, which provides a useful balance between accuracy and computation cost, facilitating numerous fusion systems in a simple uniform manner. Combined with Siwek-Wilczyński formula, wherein the three parameters are determined by the proposed effective potentials, the measured capture cross-sections at energies around the barriers were well reproduced for several fusion reactions induced by both spherical and well-deformed nuclei. The shallow capture pockets and small values of the average barrier radii led to the reduction of the capture cross-sections for 52,54Cr-and 64 Ni-induced reactions. Moreover, the decrease in the capture pocket depth for the heavy reaction system resulted in an increase in deep inelastic collisions at energies around the capture barrier, which consequently suppressed the production of the compound system.

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Footnote

The authors declare that they have no competing interests.