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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Elucidating Actinide–Pertechnetate and Actinide–Perrhenate Bonding via a Family of Th–TcO 4 and Th–ReO 4 Frameworks and Solutions

Technetium-99, a β-emitter produced from 235 U fission, poses a challenge for the nuclear industry due to co-extraction of pertechnetate (TcO 4 – ) with the actinides (An) during nuclear fuel reprocessing. Previous studies suggested that direct coordination of pertechnetate with An plays an important role in the coextraction process. However, few studies have provided direct evidence for An–TcO 4 – bonding in the solid state, and even fewer in solution. The present study describes synthesis and structural elucidation of a family of thorium(IV)-pertechnetate/perrhenate (ReO 4 – , nonradioactive surrogate) compounds, which is obtained by dissolution of thorium oxyhydroxide in perrhenic/pertechnic acid followed by crystallization, with or without heating. For reaction ratios of 3:1, 4:1, and 6:1 MO 4 – /Th(IV) (M = Tc, Re), the crystallized compounds reflect the same ratio, suggesting facile and flexible coordination. Furthermore, nine structures reveal 1-dimensional and 2-dimensional frameworks with varying topologies. While a multitude of compounds isolated from 4:1 (and 6:1) reaction solutions feature Th monomers linked by MO 4 – , the 3:1 reaction solution yielded the well-known dihydroxide-bridged thorium dimer, linked, and capped by MO 4 – . Density functional theory calculations on ReO 4 – /TcO 4 – isomorphs suggest similar bonding characteristics in the solid state, but experimental solution characterization noted differences. Specifically, small-angle X-ray scattering studies suggest the bonding of Th–TcO 4 – persists in solution, while Th–ReO 4 – bonding is less apparent.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Synthesis and Computational Analysis of Uranium(III)-Pnictogen Bonds

In this report, we describe the synthesis and characterization of two novel complexes that contain uranium(III)-pnictogen (P: 1-PMes 2 ; As: 1-AsMes 2 ) bonds to elucidate the degrees of covalency among these bonds. To our knowledge, this is the first reported uranium(III)-arsenic complex to be synthesized and characterized. Analysis of the phosphorus and arsenic bonds reveals a similar electronic environment, assessed by UV–vis NIR, that is comparable to other previously reported uranium(III) complexes. A computational analysis of these compounds and their congeners, N, Sb, and Bi, was performed to identify trends in the overall bonding character of the complexes. This analysis shows that bond covalency decreases as the pnictogen becomes heavier and that overall the interaction energy and its components decrease down the group. Here, this study provides an in-depth analysis and understanding of the nature of bonding between hard actinide and soft pnictogen centers.

Actinides↗
DOE OSTI2021

Electron–Nucleus Hyperfine Coupling Calculated from Restricted Active Space Wavefunctions and an Exact Two-Component Hamiltonian

Exact two-component (X2C) relativistic nuclear hyperfine magnetic field operators were incorporated in X2C ab-initio wavefunction calculations at the multi-reference restricted active space (RAS) level for calculations of nuclear hyperfine magnetic properties. Spin-orbit coupling was treated via RAS state interaction (SO-RASSI). The method was tested by calculations of electron – nucleus hyperfine coupling constants. The approach, implemented in the OpenMolcas program, overcomes a major limitation of a previous SO-RASSI implementation for hyperfine coupling that relied on non-relativistic hyperfine operators [J. Chem. Theor. Comput. 2015, 11, 538–549] and therefore had only limited applicability. Furthermore, results from calculations on systems with light and heavy main group elements, transition metals, lanthanides, and one actinide complex, demonstrate reasonably good agreement with experimental data, where available, as long as the active space can generate sufficient spin polarization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Lipophilic ternary complexes in liquid-liquid extraction of trivalent lanthanides

The formation of ternary complexes between lanthanide ions [Nd(III) or Eu(III)], octyl(phenyl)-N,N-diisobutyl-carbamoylmethylphosphine oxide (CMPO), and bis-(2-ethylhexyl)phosphoric acid (HDEHP) was probed by liquid-liquid extraction and spectroscopic techniques. Equilibrium modeling of data for the extraction of Nd(III) or Eu(III) from lactic acid media into n-dodecane solutions of CMPO and HDEHP indicates the predominant extracted species are of the type [Ln(AHA){sub 2}(A)] and [Ln(CMPO)(AHA){sub 2}(A)], where Ln = Nd or Eu and A represents the DEHP{sup -} anion. FTIR (for both Eu and Nd) and visible spectrophotometry (in the case of Nd) indicate the formation of the [Ln(CMPO)(A){sup 3}] complexes when CMPO is added to n-dodecane solutions of the LnA{sub 3} compounds. Both techniques indicate a stronger propensity of CMPO to complex Nd(III) versus Eu(III).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Effect of competition of spherical and deformed shells in quasifission of superheavy nuclei

Quasifission and fusion-fission represent the two most likely reaction outcomes to occur postcapture in collisions leading to superheavy nuclei. As such, understanding these mechanisms and how they relate to one another is key to understanding the intricate dynamics that drive the formation (or dissociation) of the nascent compound nuclei formed in fusion reactions. This understanding directly translates to a more informed picture of suitable reaction partners and can provide vital information for experimental efforts to study the physics and chemistry of superheavy elements. In this work we report results from time-dependent simulations of 48 Ca + 238 U and 50 Ti + 236 Th reactions at incident energies just above the Coulomb barrier with a focus on the quasifission process that prevent the formation of a fully equilibrated 286 Cn compound nucleus. We study these reactions systematically and consider a wide range of initial configurations to extract a robust estimate of primary fragment yields for the quasifission process. Multiple preferred exit channels are observed, with both spherical and deformed shell effects in the heavy and light fragments driving contributions to the production yields depending on the initial configuration of the system. Orientation effects of the deformed actinide targets are found to be a primary driver of which exit channels are populated. Here, the impact of moving away from a doubly magic projectile is explored with implications towards the reactions considered for current and future superheavy searches.

Gumbel, Richard [Michigan State University, East L↗
DOE OSTI2018

Advanced Waste Management Concepts for Uranium and Plutonium Multi-Recycling - 18533

The multiple recycling of plutonium and uranium will play a major role in gradually achieving a fully closed nuclear fuel cycle in the future, once the first Generation IV fast reactors (FR) are deployed in the NPP fleet. To reach this objective, optimizations of current processes and technologies and, in some cases, the development of innovative concepts are required to meet the scientific, technical and economic challenges imposed by the treatment of spent fuels with an increasingly higher Pu content. Based on the significant past experience acquired by France in LWR and FR MOX fuel treatment, the CEA is running R and D studies to develop new efficient processes for Pu recycling and for FR MOX fuel fabrication. More compact and economically competitive processes, ensuring the safety/security of the facilities (particularly as regards criticality and proliferation resistance) have to be developed taking into account that the amounts of plutonium involved will be one order of magnitude higher than in UOX fuels. New concepts of head-end treatment, dissolution, and separation have been proposed. Consequently, effluent and waste management must be adapted to these processes and to the characteristics of fast reactor MOX fuels. New waste treatment processes are suggested: 1) Cladding waste and undissolved metallic particles could be treated simultaneously in a melting process. The molten metal could be decontaminated by a specific slag and the oxides recovered, in particular PuO{sub 2}, would be recycled at the frond-end of the process, 2) Fission Products and Actinides (FPA) containment glass will also be optimized to accommodate significant amounts of iron, nickel and chromium coming from hull corrosion, and / or decontamination slag coming from the metal melting process. 3) New peraluminous-type glass formulations are under development to accept increased amounts of FPA, as well as iron, nickel, and chromium. The first trials to evaluate the melting process have indicated that metallic compounds from the dissolution residues could be easily incorporated into a molten metal at levels of 1, 2 and 3 w%. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Exploring high temperature phenomena related to post-detonation using an electric arc

We report a study of materials recovered from a uranium-containing plasma generated by an electric arc. The device used to generate the arc is capable of sustaining temperatures of an eV or higher for up to 100 μs. Samples took the form of a 4 μm-thick film deposited onto 8 pairs of 17 μm-thick Cu electrodes supported on a 25 μm-thick Kapton backing and sandwiched between glass plates. Materials recovered from the glass plates and around the electrode tips after passage of an arc were characterized using scanning and transmission electron microscopy. Recovered materials included a variety of crystalline compounds (e.g., UO{sub 2}, UC{sub 2}, UCu{sub 5},) as well as mixtures of uranium and amorphous glass. Most of the materials collected on the glass plates took the form of spherules having a wide range of diameters from tens of nanometers to tens of micrometers. The composition and size of the spherules depended on location, indicating different chemical and physical environments. A theoretical analysis we have carried out suggests that the submicron spherules presumably formed by deposition during the arc discharge, while at the same time the glass plates were strongly heated due to absorption of plasma radiation mainly by islands of deposited metals (Cu, U). The surface temperature of the glass plates is expected to have risen to ∼2300 K thus producing a liquefied glass layer, likely diffusions of the deposited metals on the hot glass surface and into this layer were accompanied by chemical reactions that gave rise to the observed materials. These results, together with the compact scale and relatively low cost, suggest that the experimental technique provides a practical approach to investigate the complex physical and chemical processes that occur when actinide-containing material interacts with the environment at high temperature, for example, during fallout formation following a nuclear detonation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Alkali Counterion-Dependent Crystallization of Uranium(IV)–Chloro Structural Units

The synthesis, structural characterization, and spectroscopic properties of five tetravalent uranium (U) phases including Li 6 [U 4 (μ 3 -O) 2 Cl 18 (H 2 O) 2 ]·10H 2 O (1), [U(H 2 O) 4 Cl 4 ] (2), [U(H 2 O) 4 Cl 4 ]·KCl (3), Rb 2 UCl 6 (4), and Cs 2 UCl 6 (5) are reported. Notably, a change in the U 4+ solid-state structural unit was observed based on the identity of the alkali counterion used in the synthesis. Li 1+ yielded a tetranuclear oxo-bridged cluster, [U 4 (μ 3 -O) 2 Cl 18 (H 2 O) 2 ] 6– , Na 1+ and K 1+ yielded two structurally distinct [U(H 2 O) 4 Cl 4 ] complexes, and Rb 1+ and Cs 1+ resulted in [UCl 6 ] 2– as the dominant phases. The spectroscopic properties of the compounds were analyzed using Raman and UV–vis–NIR absorption spectroscopy. The UV–vis–NIR spectra of compounds 1–5 exhibited transitions consistent with uranium in the +4 oxidation state. Clear differences in the absorption band splitting were observed and are likely attributed to differences in metal ion coordination, crystal field effects, and outer sphere interactions Overall, this work demonstrates the utility of noncovalent interactions in tuning the crystallization of various metal complexes from otherwise identical reaction solutions and provides further evidence that counterions impact the composition and structure of actinide complexes isolated in the solid state. In this way, this work affords important insight into directing and controlling the structure of actinide complexes and clusters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Actinyl-cation interactions: experimental and theoretical assessment of [Np(vi)O 2 Cl 4 ] 2– and [U(vi)O 2 Cl 4 ] 2– systems

The interaction of the actinyl (AnO 2 2+ ) oxo group with low-valent cations influences the chemical and physical properties of hexavalent actinides, but the impact of these intermolecular interactions on the actinyl bond and their occurrence in solution and solid state phases remain unclear. In this study, we explore the coordination of alkali cations (Li + , Na + , K + ) with the [NpO 2 Cl 4 ] 2– coordination complexes using single-crystal X-ray diffraction, Raman spectroscopy, and density functional theory (DFT) calculations and compare to the related uranyl system. Three solid-state coordination compounds ([Li(12-crown-4)] 2 [NpO 2 Cl 4 ] (LiNp), [Na(18-crown-6)H 2 O] 2 [NpO 2 Cl 4 ] (NaNp), and [K(18-crown- 6 )] 2 [NpO 2 Cl 4 ] (KNp) have been synthesized and characterized using single-crystal X-ray diffraction and Raman spectroscopy. Only Li + cations interact with the neptunyl oxo in the solid-state compounds and this results in a red-shift of the NpO 2 2+ symmetric stretch (ν 1 ). Raman spectra of Np(VI) solutions containing lower Li + concentrations display a single peak at ~854 cm –1 and increasing the amount of Li + results in the ingrowth of a second band at 807 cm –1 . DFT calculations and vibrational analysis indicate the lower frequency vibrational band is the result of interactions between the Li + cation and the neptunyl oxo. Here, comparison to the related uranyl system shows similar interactions occur in the solid state, but subtle differences in the actinyl-cation modes in solution phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Shell effects in quasi-fission for calcium induced reactions forming thorium isotopes

Quantum shell effects induce an asymmetric fission mode in actinides, which disappears in neutron deficient isotopes. Quasi-fission, characterized by a significant mass transfer in heavy ion collisions at low-energies, is expected to be affected by similar shell effects. This is studied in 40−56 Ca+176 reactions with the time-dependent Hartree-Fock approach. All reactions exhibit a mass equilibration process that stops when a heavy fragment with 𝑍 ≃ 54 protons is formed. Unlike the fission of thorium compound nuclei, quasi-fission does not exhibit a transition to symmetric modes in neutron deficient systems. This observation is interpreted in terms of potential energy surfaces that show a persistence of an asymmetric valley with an increasing barrier preventing its population in fission of the most neutron deficient thorium isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2016

Uranium(iii) and thorium(iv) alkyl complexes as potential starting materials

The synthesis and characterization of a rare U(iii) alkyl complex, U[η 4 -Me 2 NC(H)C 6 H 5 ] 3 , using the dimethylbenzylamine (DMBA) ligand has been accomplished. While attempting to prepare the U(iv) compound, reduction to the U(iii) complex occurred. In the analogous Th(iv) system, C-H bond activation of a methyl group of one dimethylamine was observed yielding Th[η 4 -Me 2 NC(H)C 6 H 5 ] 2 [η 5 -(CH 2 )MeNC(H)C 6 H 5 ] with a dianionic DMBA ligand. The utility of these complexes as starting materials has been analyzed using a bulky dithiocarboxylate ligand to yield tetravalent actinide species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

The role of surfaces, chemical interfaces, and disorder on plutonium incorporation in pyrochlores

Pyrochlores, a class of complex oxides with formula A 2 B 2 O 7 , are one of the candidates for nuclear waste encapsulation, due to the natural occurrence of actinide-bearing pyrochlore minerals and laboratory observations of high radiation tolerance. In this work, we use atomistic simulations to determine the role of surfaces, chemical interfaces, and cation disorder on the plutonium immobilization properties of pyrochlores as a function of pyrochlore chemistry. We find that both Pu 3+ and Pu 4+ segregate to the surface for the four low-index pyrochlore surfaces considered, and that the segregation energy varies with the chemistry of the compound. We also find that pyrochlore/pyrochlore bicrystals A 2 B 2 O 7 /A 2 'B 2 'O 7 can be used to immobilize Pu 3+ and Pu 4+ either in the same or separate phases of the compound, depending on the chemistry of the material. Finally, we find that Pu 4+ segregates to the disordered phase of an order/disorder bicrystal, driven by the occurrence of local oxygen-rich environments. However, Pu 3+ is weakly sensitive to the oxygen environment, and therefore only slightly favors the disordered phase. This behavior suggests that, at some concentration, Pu incorporation can destabilize the pyrochlore structure. Together, these results provide new insight into the ability of pyrochlore compounds to encapsulate Pu and suggest new considerations in the development of waste forms based on pyrochlores. Particularly, the phase structure of a multi-phase pyrochlore composite can be used to independently getter decay products based on their valence and size.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Transmission Electron Microscopy Characterization of Fuel Cladding Chemical Interaction between Minor Actinides bearing U-Pu-Zr Fuel and AIM1 Cladding

Minor actinides (MA) significantly contribute to the long-term radiotoxicity of spent nuclear fuel (SNF). Separating MA from SNF and incorporating it into metallic fuels for fast reactor transmutation is a potential method to reduce this radiotoxicity. Here, this study focuses on transmission electron microscopy characterization of two samples from the fuel cladding chemical interaction (FCCI) region of an americium (Am) and neptunium (Np)-bearing (MA-bearing) uranium-plutonium-zirconium (U-Pu-Zr) fuel irradiated in the Phenix fast reactor to 9.5 % FIMA burnup at approximately 550 °C cladding temperature. The results show that despite the complex chemical interactions between MA and AIM1 cladding elements, excessive FCCI was not induced, and Am penetration depth in the cladding limited to less than 4 µm. Np remained mostly inside fuel. The Zr-rich compounds layer effectively limited the accumulation of lanthanide on the inner cladding surface. Overall, the FCCI behavior between investigated MA-bearing U-Pu-Zr fuel and AIM1 cladding is benign.

Chemical interaction↗
DOE OSTI2023

Back in bismuth: controlling triplet energy transfer, phosphorescence, and radioluminescence via supramolecular interactions

Five bismuth(III)-organic phases that consist of supramolecular assemblies of Bi-2,6-pyridinedicarboxylate structural units and substituted 1,10-phenanthroline molecules (R-Phen; R = H, 5-methyl, 5-chloro, 2,9-dimethyl, and 2,9-dicholoro) were synthesized. All five compounds exhibited solid-state photoluminescence. Whereas the phases containing 2,9-dimethylphenanthroline (Me 2 Phen) and 2,9-dichlorophenanthroline (Cl 2 Phen) displayed solely phosphorescence, the structures built from 5-methylphenanthroline and 5-chlorophenanthroline showed exclusively fluorescence. The remaining phase, consisting of phenanthrolinium, exhibited both fluorescence and phosphoresence. It was determined that phosphorescence arises from triplet state emission (T 1 → S 0 ) of substituted R-Phen units while fluorescence originates from Bi(III) coordinated pyrdinedicarboxylate ligands. Bismuth induces spin–orbit coupling for triplet state population and additionally acts as a heavy metal attenuator for X-ray luminescence (radioluminescence). The electronic structure was mapped and excitation pathway investigated via density functional theory calculations. Computational findings indicate favorable conditions for triplet energy transfer from donor Bi(III)-organic units to acceptor R-Phen derivatives. It is proposed that for the phosphorescent compounds, strong π–π interactions promote electron transfer, whereas the compounds that exhibit purely fluorescence lack any such π–π interactions and undergo triplet energy transfer. In conclusion, these results provide a useful platform for probing structure–property relationships of luminescent bismuth-organic compounds, and specifically highlights the role of noncovalent interactions in achieving room temperature phosphorescence and radioluminescence.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Design principles and physical properties of two-dimensional heterostructured borides

Principles of design to create dynamically stable transition metal-, lanthanide-, and actinide-based low-dimensional borides are presented. A charge transfer analysis of donor metal atoms to electron deficient honeycombed B lattices allows to predict complex covalent heterostructures hosting Dirac states. The applicable guidelines are supported with the analysis of phonon spectra computed with first-principles calculations to demonstrate the physical stability of nanometer-thick heterostructures. Similar or dissimilar layered borides can be stacked on top of each other in a layer-by-layer fashion creating compounds that can be fundamentally different from the individual layers, opening a rich playground to explore novel physical properties and new materials. Functionalities such as multiple Dirac states, highly dispersive electronic bands, and decoupled acoustic-optical phonon branches are studied. The combination of appealing electronic properties and physical realization makes of predicted layered borides promising materials to integrate a new generation of two-dimensional materials.

2-dimensional systems↗
DOE OSTI2015

Selectivity in ligand binding to uranyl compounds: A synthetic, structural, thermodynamic and computational study

The uranyl cation (UO₂²⁺) is the most abundant form of uranium on the planet. It is estimated that 4.5 billion tons of uranium in this form exist in sea water. The ability to bind and extract the uranyl cation from aqueous solution while separating it from other elements would provide a limitless source of nuclear fuel. A large body of research concerns the selective recognition and extraction of uranyl. A stable molecule, the cation has a linear O=U=O geometry. The short U-O bonds (1.78 Å) arise from the combination of uranium 5f/6d and oxygen 2p orbitals. Due to the oxygen moieties being multiply bonded, these sites were not thought to be basic enough for Lewis acidic coordination to be a viable approach to sequestration. The goal of this research is thus to broaden the coordination chemistry of the uranyl ion by studying new ligand systems via synthetic, structural, thermodynamic and computational methods. It is anticipated that this fundamental science will find use beyond actinide separation technologies in areas such as nuclear waste remediation and nuclear materials. The focus of this study is to synthesize uranyl complexes incorporating amidinate and guanidinate ligands. Both synthetic and computational methods are used to investigate novel equatorial ligand coordination and how this affects the basicity of the oxo ligands. Such an understanding will later apply to designing ligands incorporating functionalities that can bind uranyl both equatorially and axially for highly selective sequestration. Efficient and durable chromatography supports for lanthanide separation will be generated by (1) identifying robust peptoid-based ligands capable of binding different lanthanides with variable affinities, and (2) developing practical synthetic methods for the attachment of these ligands to Dowex ion exchange resins.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Structural and Spectroscopic Trends in Alkali Tris(Acetato)Actinyl(VI) Complexes

A series of alkali tris(acetato)actinyl(VI) compounds M[AnO 2 (CH 3 COO) 3 ] (M=Na, K, Rb, Cs and An=U, Np, Pu) is reported, applying a combination of singlecrystal X-ray diffraction, solid-state Raman spectroscopy, and U(VI) luminescence spectroscopy for their structural and spectroscopic characterization. The results show that complexes formed from the same alkali metal but different actinyl ions are mostly isostructural. The symmetric actinyl stretch (ν 1 (An=O yl )) in these isostructural complexes undergoes a redshift within the actinide series despite the shortening of the actinyl bond due to the actinide contraction. Complexes formed from the same actinyl but co-crystallized with different alkali metals show a progression toward lower space group symmetry. While the actinyl bond length remains unmodulated within the alkali series, a small redshift of ν 1 (An=O yl ) is observed, indicating minor changes in the vibrational properties of the actinyl moiety caused by the structural progression towards lower symmetry. This subtle change is also evidenced by a redshift of the U(VI) luminescence spectra within the M[UO 2 (CH 3 COO) 3 ] series.

Raman↗
DOE OSTI2015

Calculated fission-fragment yield systematics in the region 74 <=Z <= 94 and 90 <=N <= 150

Background: In the seminal experiment by Schmidt et al . [Nucl. Phys. A 665 , 221 (2000)] in which fission-fragment charge distributions were obtained for 70 nuclides, asymmetric distributions were seen above nucleon number A ≈ 226 and symmetric ones below. Because asymmetric fission had often loosely been explained as a preference for the nucleus to always exploit the extra binding of fragments near ¹³²Sn it was assumed that all systems below A ≈ 226 would fission symmetrically because available isotopes do not have a proton-to-neutron Z/N ratio that allows division into fragments near ¹³²Sn. But the finding by Andreyev et al . [Phys. Rev. Lett. 105 , 252502 (2010)] did not conform to this expectation because the compound system ¹⁸⁰Hg was shown to fission asymmetrically. It was suggested that this was a new type of asymmetric fission, because no strong shell effects occur for any possible fragment division. Purpose: We calculate a reference database for fission-fragment mass yields for a large region of the nuclear chart comprising 987 nuclides. A particular aim is to establish whether ¹⁸⁰Hg is part of a contiguous region of asymmetric fission, and if so, its extent, or if not, in contrast to the actinides, there are scattered smaller groups of nuclei that fission asymmetrically in this area of the nuclear chart. Methods: We use the by now well benchmarked Brownian shape-motion method and perform random walks on the previously calculated five-dimensional potential-energy surfaces. The calculated shell corrections are damped out with energy according to a prescription developed earlier. Results: We have obtained a theoretical reference database of fission-fragment mass yields for 987 nuclides. These results show an extended region of asymmetric fission with approximate extension 74 ≤ Z ≤ 85 and 100 ≤ N ≤ 120. The calculated yields are highly variable. We show 20 representative plots of these variable features and summarize the main aspects of our results in terms of “nuclear-chart” plots showing calculated degrees of asymmetry versus N and Z. Conclusions: Experimental data in this region are rare: only ten or so yield distributions have been measured, some with very limited statistics. We agree with several measurements with higher statistics. Regions where there might be differences between our calculated results and measurements lie near the calculated transition line between symmetric and asymmetric fission. To draw more definite conclusions about the accuracy of the present implementation of the Brownian shape-motion approach in this region experimental data, with reliable statistics, for a fair number of suitably located additional nuclides are clearly needed. Because the nuclear potential-energy structure is so different in this region compared to the actinide region, additional experimental data together with fission theory studies that incorporate additional, dynamical aspects should provide much new insight.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗