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Systematic study on the proton radioactivity of spherical proton emitters

NUCLEAR PHYSICS AND INTERDISCIPLINARY RESEARCH

Systematic study on the proton radioactivity of spherical proton emitters

Dong-Meng Zhang
Lin-Jing Qi
De-Xing Zhu
Yang-Yang Xu
Song Luo
Xiao-Hua Li
Nuclear Science and TechniquesVol.34, No.4Article number 55Published in print Apr 2023Available online 19 Apr 2023
39903

In this study, based on a two-potential approach, we systematically investigated the proton radioactivity half-lives of spherical proton emitters with 69≤ Z ≤ 81 from the ground and/or isomeric state, choosing the nuclear potential to be a modified Woods–Saxon potential that contains the isospin effect of the daughter nucleus. It was found that the calculated half-lives could reproduce the experimental data well. Furthermore, we extended this model to predict the half-lives of 17 proton-emitting candidates whose radioactivity is energetically allowed or observed but not yet quantified in NUBASE2020. For comparison, the unified fission model, Coulomb potential and proximity potential model, universal decay law for proton emission, and new Geiger–Nuttall law were also used. All the predicted results are consistent with each other.

Proton radioactivitySpherical nucleiTwo-potential approachModified Woods–Saxon potentialHalf-lives
1

Introduction

Proton radioactivity, the spontaneous process in which a nucleus with a large excess of protons transforms into the stable state by emitting an individual proton, was first observed by Jackson et al. [1, 2] from an isomeric state of 53Co. In the early 1980s, Hofmann et al. [3] and Klepper et al. [4] further discovered proton emission from the nuclear ground states of 151Lu and 147Tm, respectively. With the advancement of diverse infrastructures and radioactive beam installations, more than 40 proton emitters have been provenly illustrated in the proton number range 51≤ Z ≤ 83 from the ground state or low-lying isomeric state during the last decades [5-10]. Proton radioactivity can be used as an effective probe to identify nuclei near the proton drip line and explore diverse nuclear information, such as the released energy, half-lives, branching ratio, and wave function of the parent nucleus [11-14]. However, the study of proton-rich nuclei far from the β-stability line has become an extremely hot topic in nuclear physics.

Proton radioactivity shares the same decay mechanism as α decay [15-20], two-proton radioactivity [21-29], and cluster radioactivity [30, 31], that is, barrier penetration. These processes can be dealt with using the Wentzel–Kramers–Brillouin (WKB) approximation. To date, many models and/or formulae have been proposed to calculate the half-life of proton radioactivity, which can be divided into the following two categories: The first are theoretical models, including the effective interactions of density-dependent M3Y [32, 33], single-folding model [21], unified fission model (UFM) [34, 35], Gamow-like model [36], Coulomb and proximity potential model [37-39], generalized liquid-drop model [7, 40-42], and modified two-potential approach [11, 43, 44]. The second are empirical formulae proposed in the form of the Geiger–Nuttall (G-N) law [45], such as the universal decay law for proton emission (UDLP) [46], the new Geiger-Nuttall law (NG-N) [47], the four-parameter empirical formula of Zhang and Dong [12], and the screened decay law for proton emission [48]. Calculations using these theoretical methods provide excellent estimates of the lifetime of proton radioactivity and improve our understanding of the proton radioactivity phenomenon.

For proton radioactivity, it is well known that the emitted particle–nucleus interaction potential is extremely crucial to improving the accuracy of half-life calculations. In 2008, based on the Skyrme-energy-density-function approach, taking into account the isospin effect of the nuclear potential, Wang et al. [49, 50] proposed a modified Woods–Saxon potential to describe a large number of heavy-ion elastic or quasi-elastic scattering and fusion reactions. Later, it was widely used to study α decay and cluster radioactivity [51, 52]. Whether this modified potential can be extended to investigate proton radioactivity is an interesting topic. To this end, based on the two-potential approach within the modified Woods–Saxon potential (TPA-MWS), we systematically studied the half-lives of 32 spherical proton emitters. The results indicate that our calculations are consistent with the experimental data. In addition, we extended this model to predict the half-lives of 17 proton-emitting candidates whose radioactivity is energetically allowed or observed but not yet quantified in NUBASE2020.

The remainder of this paper is organized as follows: In Sect. 2, the theoretical framework of the two-potential approach and two different empirical formulae are introduced in detail. The results and discussion are presented in Sect. 3. Finally, a brief summary is provided in Sect. 4.

2

Theoretical framework

2.1
Two potential approach

The proton radioactivity half-life, T1/2, which is an important indicator of nuclear stability, is determined by T1/2=ln2Γ, (1) where is the reduced Planck constant, and Γ represents the proton radioactivity width. In the framework of the two-potential approach [53-55], Γ can be expressed as Γ=Sp2FP4μ, (2) where μ=mpmd/(mp+md)938.272×Ad/(Ad+Ap) MeV/c2 represents the reduced mass of the emitted proton and daughter nucleus, with mp, md, Ap, and Ad as the masses of the emitted proton and daughter nucleus, and the mass numbers of the emitted proton and daughter nucleus, respectively. Sp is the formation probability of the emitted proton–daughter system, which is related to the probability that the orbit of the emitted proton is empty in the daughter nucleus [7]. In this study, based on Ref. [34], we chose Sp=1. F is the normalized factor describing the collision frequency of the emitted proton in the potential barrier. This satisfies the condition Fr1r212k(r)dr=1. (3) P, the penetration probability of the emitted proton penetrating the barrier, is calculated using the semiclassical WKB approximation. It can be expressed as P=exp[2r2r3k(r)dr], (4) where k(r)=2μ2|QpV(r)| is the wavenumber, and V(r) is the total interaction potential between the emitted proton and daughter nucleus, with r as the mass center distance between the emitter proton and daughter nucleus. In Eq. 3 and 4, r1, r2, and r3 represent the classical turning points. These satisfy the condition V(r1)=V(r2)=V(r3)=Qp, where Qp denotes the released energy. It can be obtained by Qp=ΔM(ΔMd+ΔMp)+k(ZεZdε), (5) where the experimental data of the mass excess Δ M, Δ Md, and Δ Mp are taken from the latest atomic mass table NUBASE2020 [56], representing the mass excesses of the parent and daughter nuclei and emitted proton, respectively. The term k(ZεZdε) denotes the screening effect of atomic electrons, with Z and Zd being the proton number of the parent and daughter nuclei, for Z lt;60, k=13.6 eV, ε=2.408, and for Z ≥ 60, k = 8.7 eV, ε=2.517 [57, 58].

In this study, the total interaction potential V(r) was composed of the nuclear potential VN(r), Coulomb potential VC(r), and centrifugal potential Vl(r) (see Fig. 1). It can be expressed as V(r)=VN(r)+VC(r)+Vl(r). (6) For VN(r), we chose the modified Woods–Saxon potential [49, 50], which can be parameterized as VN(r)=V01+exp[(rR0)/a]. (7) Here, R0 is the effective nuclear radius, which can be expressed as R0=Rd+Rp1.37, (8) where Rd=1.27Ad1/3 is the radius of the daughter nucleus. Rp=0.875 represents the proton radius [59]. a=0.4+0.33Id is the diffuseness of the nuclear potential [60]. V0 denotes the potential depth, which can be parameterized as V0=44.16[10.4(Id+Ip)]Ad1/3Ap1/3Ad1/3+Ap1/3, (9) where Id=(NdZd)/Ad and Ip=(NpZp)/Ap are the isospin asymmetries of the daughter nucleus and emitted proton with Zd, Nd and Zp, Np being the proton and neutron number of the daughter nucleus and emitted proton, respectively.

Fig. 1
(color online) Variation in the total V(r) and nuclear VN(r) potentials for the parent nucleus 170Au as a function of the nuclear radius.
pic

VC(r) is the Coulomb potential, which is taken as the potential of a uniformly charged sphere. It can be expressed as VC(r)={ZdZpe22R[3r2R2],rR,ZdZpe2r,r>R, (10) where e2 ≈ MeVfm denotes the square of the electronic elementary charge [61]. R denotes the sharp radius. For convenience, it can be taken as the effective nuclear radius R0 of the modified Woods–Saxon potential [62].

For the centrifugal potential Vl(r), we chose the Langer modified form because l(l+1)(l+1/2)2 is an essential correction for one-dimensional problems [63]. It can be expressed as Vl(r)=2(l+12)22μr2. (11) Here, l is the angular momentum removed by the emitted proton, which satisfies the spin–parity conservation laws. It can be expressed as l={ Δjfor even Δj and π=πd,Δj+1for even Δj and ππd,Δjfor odd Δj and ππd,Δj+1for odd Δj and π=πd, (12) where Δj=|j-jd-jp|, with j, π, jd, πd, jp, πp denoting the spin and parity values of the parent and daughter nuclei and emitted proton, respectively.

2.2
Two different empirical formulae
2.2.1
Universal decay law for proton emission

Based on the R-matrix theory of the cluster decay process and the microscopic mechanism of charged-particle emission, Qi et al. [64, 65] proposed a universal decay law that improves the accuracy of cluster radioactivity half-lives. Because proton radioactivity shares the same decay mechanism as α decay and cluster radioactivity, considering the influence of the centrifugal barrier, this formula was later extended to investigate proton radioactivity [46]. It is expressed as log10T1/2=aχ'+bρ'+c+d(l+1)l/ρ', (13) where χ=ZpZdApAd(Ap+Ad)Qp and ρ=ZpZdApAd(Ap1/3+Ad1/3)Ap+Ad. a=0.386, b=-0.502, c=-17.8, and d=2.386 are adjustable parameters.

2.2.2
New Geiger–Nuttall law

In the form of the G–N law [45], considering the contributions of the orbital angular momentum l and the charge of the daughter nucleus Zd, Chen et al. [47] proposed a two-parameter empirical formula to study proton radioactivity in a unified way, which is expressed as log10T1/2=a(Zd0.8+l)Qp1/2+b, (14) where the parameters a=0.843 and b=-27.194 were determined by fitting 44 experimental data points of the proton radioactivity half-lives from the ground state and/or isomeric state.

3

Results and discussion

In this study, we systematically investigated the half-lives of 32 spherical proton emitters based on the TPA–MWS. For comparison, the UFM [35], Coulomb potential and proximity potential model with the Guo-2013 formalism (CPPM) [66], UDLP [46] and NG-N [47] were also used. The detailed numerical results are listed in Table 1. In this table, the first three columns contain the proton emitter, proton radioactivity released energy Qp, and angular momentum l removed by the emitted proton. The last six columns contain the logarithmic form of the experimental half-lives and theoretical half-lives calculated using three models and two different empirical formulae denoted as Exp, TPA-MWS, UFM, CPPM, UDLP, and NG-N. As shown in Table 1, the calculated proton radioactivity half-lives obtained using our model can well reproduce the experimental data. To visually present their deviations, we plotted the differences between the experimental proton radioactivity half-lives and the calculated values using these five models and/or formulae in logarithmic form in Fig. 2. From this figure, we can see that the deviations are in the range of ±1. Overall, all of the calculated proton radioactivity half-lives were consistent with the experimental data. Nevertheless, it should be noted that the logarithmic deviation between the experimental and calculated half-lives was large, corresponding to the special case 177Tlm. Its deviations in logarithmic form were –0.889, -0.802, -1.176, -0.881, and -0.826 using TPA-MWS, UFM, CPPM, UDLP, and NG-N, respectively. Exploring the causes of such a large deviation is crucial for further investigation of proton radioactivity. As we know, the selection of the proton radioactivity released energy Qp and angular momentum l is important in proton radioactivity. In our previous study, we discussed that the effect of angular momentum on the half-life is larger than the released energy [67]. The result indicated that the calculated half-life of proton radioactivity for 177Tlm was closer to the experimental data when l = 6 [67]. Therefore, we chose l =6 and calculated its logarithm proton radioactivity half-life as -2.779 with a deviation of 0.567, which has a higher consistency with the experimental data than the calculated value of -4.235 when the value of l is set as 5. In addition, the proton number of 177Tlm is close to the magic number Z = 82, and the proton shell effect may be another reason for this phenomenon.

Table 1
Comparison of experimental proton radioactivity half-lives with the calculated values using different theoretical models and/or formulae. The symbol m denotes the first isomeric state. The experimental proton radioactivity half-lives, spin, and parity are taken from Ref. [56]. The released energy is given by Eq. 5, with the exception of the Qp value for 159Re, 161Rem, 164Ir, and 177Irm, which are taken from Ref.[6].
Nucleus AZ Qp(MeV) l Log10T1/2(s)
      Exp TPA-MWS UFM CPPM UDLP NG-N
144Tm 1.724± 0.016 5 5.5690.0007+0.0017 –4.962 –4.937 –5.138 –4.687 –5.212
145Tm 1.754± 0.007 5 5.4990.027+0.027 –5.174 –5.145 –5.415 –4.871 –5.401
146Tm 0.904± 0.006 0 0.8100.105+0.105 –0.912 –0.685 –0.600 –0.610 –1.272
146Tmm 1.214± 0.008 5 1.1370.006+0.006 –0.660 –0.645 –0.695 –0.896 –0.999
147Tm 1.072± 0.003 5 0.5870.022+0.022 1.046 1.058 1.001 0.614 0.681
147Tmm 1.133± 0.006 2 3.4440.048+0.048 –3.197 –3.010 –2.911 –2.859 –2.455
150Lu 1.285± 0.033 5 1.3470.029+0.029 –0.896 –0.868 –0.953 –1.132 –1.219
150Lum 1.305± 0.055 2 4.3980.005+0.007 –4.485 –4.294 –4.206 –4.050 –3.633
151Lu 1.255± 0.0018 5 0.8960.011+0.011 –0.593 –0.562 –0.699 –0.862 –0.910
151Lum 1.315± 0.004 2 4.7960.027+0.027 –4.598 –4.402 –4.380 –4.150 –3.722
155Ta 1.466± 0.015 5 2.4950.165+0.225 –2.154 –2.112 –2.321 –2.269 –2.397
156Ta 1.036± 0.004 2 0.8260.016+0.016 –0.645 –0.444 –0.300 –0.624 –0.180
156Tam 1.126± 0.009 5 0.9330.005+0.005 1.476 1.514 1.479 0.947 1.101
157Ta 0.946± 0.010 0 0.5270.017+0.017 –0.211 0.050 –0.072 –0.038 –0.657
159Re 1.816± 0.020 5 4.6780.092+0.076 –4.381 –4.332 –4.642 –4.270 –4.496
159Rem 1.816± 0.020 5 4.6650.087+0.087 –4.381 –4.332 –4.640 –4.269 –4.494
160Re 1.276± 0.007 2 3.1630.048+0.079 –3.064 –2.866 –2.803 –2.841 –2.353
161Re 1.216± 0.005 0 3.3570.010+0.010 –3.331 –3.077 –2.953 –2.895 –3.277
161Rem 1.338± 0.052 5 0.6780.009+0.009 –0.465 –0.416 –0.599 –0.806 –0.747
164Ir 1.844± 0.009 5 3.9470.139+0.190 –4.172 –4.110 –4.376 –4.114 –4.247
165Irm 1.727± 0.007 5 3.4330.087+0.087 –3.374 –3.311 –3.611 –3.408 –3.482
166Ir 1.167± 0.008 2 0.8240.091+0.091 –1.196 –0.984 –0.904 –1.188 –0.688
166Irm 1.347± 0.010 5 0.0760.026+0.026 –0.061 –0.004 –0.136 –0.475 –0.344
167Ir 1.087± 0.004 0 1.1200.025+0.025 –1.045 –0.780 –0.640 –0.865 –1.347
167Irm 1.262± 0.045 5 0.8420.009+0.009 0.865 0.923 0.757 0.348 0.546
170Au 1.487± 0.012 2 3.4870.060+0.075 –4.104 –3.895 –3.927 –3.845 –3.254
170Aum 1.767± 0.018 5 2.9710.028+0.035 –3.252 –3.187 –3.443 –3.333 –3.330
171Au 1.464± 0.010 0 4.6520.151+0.185 –4.803 –4.535 –4.527 –4.298 –4.460
171Aum 1.718± 0.014 5 2.5870.013+0.013 –2.905 –2.836 –3.144 –3.026 –2.992
176Tl 1.278± 0.018 0 2.2080.012+0.025 –2.287 –2.012 –1.910 –2.059 –2.361
177Tl 1.173± 0.019 0 1.1740.121+0.121 –0.975 –0.700 –0.624 –0.875 –1.274
177Tlm 1.967± 0.026 5 3.3460.076+0.076 –4.235 –4.148 –4.522 –4.227 –4.172
Show more
Fig. 2
(color online) Deviations between the experimental proton radioactivity half-lives and the calculated values using three models and two different empirical formulae for spherical nuclei. The rhombi, circles, triangles, inverted triangles, and squares correspond to the results obtained using the UFM, CPPM, UDLP, NG-N, and TPA-MWS, respectively.
pic

To obtain further insight into the agreement between the experimental and calculated data, the root-mean-square deviation σ was used to estimate the calculated capabilities of the above five models and/or formulae for the proton radioactivity half-lives. It can be defined as σ=1Ni=1N(log10T1/2cal.ilog10T1/2exp.i)2, (15) where log10T1/2cal.i and log10T1/2exp.i denote the experimental proton radioactivity half-life and the calculated half-life in logarithmic form for the i-th nucleus, respectively. For comparison, the specific results of σ for the five theoretical models and/or formulae are listed in Table 2. From this table, we can clearly see that the standard deviation σ obtained using TPA-MWS (σTPA-MWS=0.341) was smaller than that of the others. This means that the present model can better reproduce the experimental proton radioactivity half-lives than the others for spherical emitters.

Table 2
Standard deviations σ between the experimental and calculated half-lives using different theoretical models and/or formulae.
Type TPA-MWS UFM CPPM UDLP NG-N
σ 0.341 0.376 0.410 0.406 0.423
Show more

A single line of the universal curve for α decay and cluster radioactivities could be manifested by plotting the decimal logarithm of the half-life versus the negative decimal logarithm of the penetration probability through the barrier [68, 69]. Whether this linear correlation can be extended to investigate proton radioactivity is an interesting topic [69]. Therefore, we plotted the correlation between the decimal logarithm of the experimental half-life against the negative decimal logarithm of penetrability in Fig 3. The penetrability was calculated theoretically in the framework of the semiclassical WKB approximation. As shown, the decimal logarithm of the experimental half-life had a clear linear dependence on the negative decimal logarithm of the penetrability, which implies that our calculations and the present methods are valid and reliable.

Fig. 3
(color online) Decimal logarithm of the experimental half-lives plotted against log10P for proton radioactivity. The slope and intercept of the fitted solid line for each case are shown in the corresponding figure.
pic

Considering the good agreement between the experimental half-lives and those calculated using the present model, we extended our model to predict the half-lives of proton radioactivity in the proton number region 51Z83. For comparison, the UFM, CPPM, UDLP, and NG-N were also used. The detailed predictions are listed in Table 3. In this table, the first three columns contain the possible proton radioactivity candidates, released energy Qp, and orbital angular momentum l. The last five columns contain the predicted proton radioactivity half-lives obtained using the five models and/or formulae. From this table, we can clearly see that the magnitude of all results using our model is consistent with those calculated using the other four models and/or formulae, validating the predictive power of this method. Taking 116La as an example, the predictions were –10.256, –10.117, –9.963, –9.000, and –9.126. To further test the reliability of the predictions, we obtained a linear relationship between the quantities log10T1/2pre and (Zd0.8+l)Qp1/2 based on the NG-N [47] in Fig. 4. The results show that the predictions are consistent with the NG-N, which indicates that our predictions of the proton radioactivity half-lives are valid and reliable. These predictions may provide valuable information for when searching for new nuclides with proton radioactivity in the future.

Table 3
Comparison of the predicted half-lives for possible radioactivity candidates whose proton radioactivity is energetically allowed or observed but not yet quantified in NUBASE2020. The symbols m and n denote the first and second isomeric states, respectively. The released energy is given by Eq. 5.
Nucleus AZ Qp MeV l log10T1/2(s)
      TPA-MWS UFM CPPM UDLP NG-N
103Sb 0.979 2 –6.985 –6.872 –6.522 –5.948 –6.009
104Sb 0.509 2 1.373 8.284 –0.783 3.154 2.187
105Sb 0.331 2 4.871 8.688 1.503 8.002 9.240
111Cs 1.740 2 –11.511 –11.383 –11.299 –10.094 –10.375
116La 1.591 2 –10.256 –10.117 –9.963 –9.000 –9.126
127Pm 0.792 2 –0.856 –0.696 –0.757 –0.620 –0.239
137Tb 0.843 5 3.351 3.342 2.677 2.714 2.974
146Tmn 1.144 5 0.150 0.166 0.142 –0.177 –0.206
159Re 1.606 0 –7.019 –6.772 –6.749 –6.227 –6.381
165Ir 1.547 0 –6.051 –5.791 –5.779 –5.387 –5.530
169Irm 0.782 5 8.750 8.799 5.590 7.362 8.043
171Irm 0.403 5 14.420 23.326 8.456 20.337 21.891
169Au 1.947 0 –8.421 –8.156 –8.249 –7.572 –7.478
172Au 0.877 2 4.145 4.357 2.752 3.578 3.983
172Aum 0.627 2 7.658 10.880 4.835 9.433 9.678
185Bi 1.541 5 –0.596 –0.505 –0.784 –1.030 –0.732
185Bin 1.721 6 –0.664 –0.690 –1.069 –1.171 –1.512
Show more
Fig. 4
(color online) Linear relationship between the quantities log10T1/2pre and (Zd0.8+l)Qp1/2 based on the NG-N.
pic

Furthermore, recent studies have shown that nuclear deformation plays an important role in proton radioactivity [37, 44, 48, 69]. Barrier penetration can be affected by the deformation of daughter nuclei during the proton emission process [70]. The deformation effect can result in the reduction of Coulomb and centrifugal barriers, which can influence the penetrability and reduce the theoretical half-lives [11]. In addition, some methods can be used to calculate the proton radioactivity half-lives of deformed proton emitters. In 2016, based on the WKB tunneling approximation, Qian and Ren et al. [44] proposed a simple formula including the deformation term to evaluate the proton radioactivity half-lives of the deformed nuclei. In 2022, the deformation dependence of the screened decay law for proton radioactivity was proposed by Budaca et al. [48] to systematically study proton radioactivity. Inspired by this, we will also discuss the influence of the deformation effect on the estimation of proton radioactivity half-lives in more detail in future work.

4

Summary

In summary, we present a systematic study of the proton radioactivity half-lives for 32 spherical proton emitters based on the TPA-MWS, which contains the isospin effect. It was found that the calculated results could reproduce the experimental data well. In addition, we extended this model to predict the proton radioactivity half-lives for 17 possible candidates. The predicted results are in reasonable agreement with those obtained using the UFM, CPPM, UDLP, and NG-N. This study may provide useful and reliable information for when predicting the existence of new proton emitters above the proton drip line, which may be detected in the future.

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