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On the origin of asymmetric fission of actinides

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 Added by Guillaume Scamps
 Publication date 2018
  fields
and research's language is English




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Nuclear fission of heavy (actinide) nuclei results predominantly in asymmetric mass-splits. Without quantum shells, which can give extra binding energy to these mass-asymmetric shapes, the nuclei would fission symmetrically. The strongest shell effects are in spherical nuclei, so naturally the spherical doubly-magic ${^{132}}$Sn nucleus (${Z=50}$ protons), was expected to play a major role. However, a systematic study of fission has shown that the heavy fragments are distributed around ${Z=52}$ to 56, indicating that ${^{132}}$Sn is not the only driver. Reconciling the strong spherical shell effects at ${Z=50}$ with the different ${Z}$ values of fission fragments observed in nature has been a longstanding puzzle. Here, we show that the final mass asymmetry of the fragments is also determined by the extra stability of octupole (pear-shaped) deformations which have been recently confirmed experimentally around $^{144}$Ba (${Z=56}$), one of very few nuclei with shell-stabilized octupole deformation. Using a modern quantum many-body model of superfluid fission dynamics, we found that heavy fission fragments are produced predominantly with ${52-56}$ protons, associated with significant octupole deformation acquired on the way to fission. These octupole shapes favouring asymmetric fission are induced by deformed shells at ${Z=52}$ and 56. In contrast, spherical magic nuclei are very resistant to octupole deformation, which hinders their production as fission fragments. These findings may explain surprising observations of asymmetric fission of lighter than lead nuclei.



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Fission-fragment mass distributions are asymmetric in fission of typical actinide nuclei for nucleon number $A$ in the range $228 lnsim A lnsim 258$ and proton number $Z$ in the range $90lnsim Z lnsim 100$. For somewhat lighter systems it has been observed that fission mass distributions are usually symmetric. However, a recent experiment showed that fission of $^{180}$Hg following electron capture on $^{180}$Tl is asymmetric. We calculate potential-energy surfaces for a typical actinide nucleus and for 12 even isotopes in the range $^{178}$Hg--$^{200}$Hg, to investigate the similarities and differences of actinide compared to mercury potential surfaces and to what extent fission-fragment properties, in particular shell structure, relate to the structure of the static potential-energy surfaces. Potential-energy surfaces are calculated in the macroscopic-microscopic approach as functions of fiveshape coordinates for more than five million shapes. The structure of the surfaces are investigated by use of an immersion technique. We determine properties of minima, saddle points, valleys, and ridges between valleys in the 5D shape-coordinate space. Along the mercury isotope chain the barrier heights and the ridge heights and persistence with elongation vary significantly and show no obvious connection to possible fragment shell structure, in contrast to the actinide region, where there is a deep asymmetric valley extending from the saddle point to scission. The mechanism of asymmetric fission must be very different in the lighter proton-rich mercury isotopes compared to the actinide region and is apparently unrelated to fragment shell structure. Isotopes lighter than $^{192}$Hg have the saddle point blocked from a deep symmetric valley by a significant ridge. The ridge vanishes for the heavier Hg isotopes, for which we would expect a qualitatively different asymmetry of the fragments.
Ternary fission of actinides probes the state of the nucleus at scission. Light clusters are produced in space and time very close to the scission point. Within the nonequilibrium statistical operator method, a generalized Gibbs distribution is constructed from the information given by the observed yields of isotopes. Using this relevant statistical operator, yields are calculated taking excited states and continuum correlations into account, in accordance with the virial expansion of the equation of state. Clusters with mass number $A le 10$ are well described using the nonequilibrium generalizations of temperature and chemical potentials. Improving the virial expansion, in-medium effects may become of importance in determining the contribution of weakly bound states and continuum correlations to the intrinsic partition function. Yields of larger clusters, which fail to reach this quasi-equilibrium form of the relevant distribution, are described by nucleation kinetics, and a saddle-to-scission relaxation time of about 7000 fm/c is inferred. Light charged particle emission, described by reaction kinetics and virial expansions, may therefore be regarded as a very important tool to probe the nonequilibrium time evolution of actinide nuclei during fission.
The impact of pairing correlations on the fission barriers is investigated in Relativistic Hartree Bogoliubov (RHB) theory and Relativistic Mean Field (RMF)+BCS calculations. It is concluded that the constant gap approximation in the usual RMF+BCS calculations does not provide an adequate description of the barriers. The RHB calculations show that there is a substantial difference in the predicted barrier heights between zero-range and finite range pairing forces even in the case when the pairing strengths of these two forces are adjusted to the same value of the pairing gap at the ground state.
Structure properties of fifty five even-even actinides have been calculated using the Gogny D1S force and the Hartree-Fock-Bogoliubov approach as well as the configuration mixing method. Theoretical results are compared with experimental data.
The systematic investigation of the ground state and fission properties of even-even actinides and superheavy nuclei with $Z=90-120$ from the two-proton up to two-neutron drip lines with proper assessment of systematic theoretical uncertainties has been performed for the first time in the framework of covariant density functional theory (CDFT). These results provide a necessary theoretical input for the r-process modeling in heavy nuclei and, in particular, for the study of fission recycling. Four state-of-the-art globally tested covariant energy density functionals (CEDFs), namely, DD-PC1, DD-ME2, NL3* and PC-PK1, representing the major classes of the CDFT models are employed in the present study. Ground state deformations, binding energies, two neutron separation energies, $alpha$-decay $Q_{alpha}$ values and half-lives and the heights of fission barriers have been calculated for all these nuclei. Theoretical uncertainties in these physical observables and their evolution as a function of proton and neutron numbers have been quantified and their major sources have been identified. Spherical shell closures at $Z=120$, $N=184$ and $N=258$ and the structure of the single-particle (especially, high-$j$) states in their vicinities as well as nuclear matter properties of employed CEDFs are two major factors contributing into theoretical uncertainties. However, different physical observables are affected in a different way by these two factors. For example, theoretical uncertainties in calculated ground state deformations are affected mostly by former factor, while theoretical uncertainties in fission barriers depend on both of these factors.
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