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At least 19 records

Description of the Fission Process: Nuclear Models for Fission Dynamics

Nuclear fission is the splitting of a heavy nucleus into two or more fragments, a process that releases a substantial amount of energy. It is ubiquitous in modern applications, critical for national security, energy generation and reactor safeguards. Fission also plays an important role in understanding the astrophysical formation of elements in the universe. Eighty years after the discovery of the fission process, its theoretical understanding from first principles remains a great challenge. In this paper, we present promising new approaches to make more accurate predictions of fission observables.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Improved Cumulative Fission Yield Measurements with Fission Spectrum Neutrons on 235 U

Two isotopically-characterized targets of high-purity (99.84±0.03%) 235 U-oxide and a neutron dosimetry package were exposed to a pulsed neutron irradiation using the Godiva critical assembly at the National Criticality Experiments Research Center. Following irradiation, the fissioned targets were counted with a broad-energy germanium detector. Estimates of the total fissions for each target were made using measurements of well-known fission products. The total fission values were then used to measure the fission yields of 21 fission products with half-lives between 636 and 119,700 seconds. Mean values of seventeen of the measured fission products fell within the 95% confidence level of the Evaluated Nuclear Data Files VII.1/b (ENDF/B-VII.1) using the larger of the two uncertainties: 84g Br, 89 Rb, 91 Sr, 93 Y, 97 Zr, 101 Mo, 105 Ru, 128 Sn, 129 Sb, 130g Sb, 131 Sb, 131m Te, 133 I, 135 I, 141 Ba, 142 Ba, and 142 La. Seven isotopes were measured to better precision than is listed in the ENDF/B-VII.1 database: 89 Rb, 93 Y, 128 Sn, 129 Sb, 130g Sb, 131m Te, and 133 I. Four of the measured isotopes were found to be statistically different from the ENDF/B-VII.1 database: 94 Y, 134 Te, 134 I, and 138 Xe. Two of the isotopic analyses conducted in this paper fit the parent and daughter data simultaneously. The parent-daughter pairs measured in this way were the 134 Te/I and 142 Ba/La pairs. The fission yield results obtained in this way are unique, especially for 134 I, because the parent and daughter half-lives are so close. Here, given the limited number of direct measurements of the 134 Te/I pair from fast neutron induced fission and the seemingly high estimate for 134 Te from previous work, it is likely that the value in this paper is more accurate; however, additional measurements of this pair are needed to validate this assertion.

42 ENGINEERING↗

Prompt fission neutron spectra from fission induced by 1 to 8 MeV neutrons on {sup 235}U and {sup 239}Pu using the double time-of-flight technique

Prompt fission neutron spectra from {sup 235}U and {sup 239}Pu were measured for incident neutron energies from 1 to 200 MeV at the Weapons Neutron Research facility (WNR) of the Los Alamos Neutron Science Center, and the experimental data were analyzed with the Los Alamos model for the incident neutron energies of 1-8 MeV. A CEA multiple-foil fission chamber containing deposits of 100 mg {sup 235}U and 90 mg {sup 239}Pu detected fission events. Outgoing neutrons were detected by the Fast Neutron-Induced {gamma}-Ray Observer array of 20 liquid organic scintillators. A double time-of-flight technique was used to deduce the neutron incident energies from the spallation target and the outgoing energies from the fission chamber. These data were used for testing the Los Alamos model, and the total kinetic energy parameters were optimized to obtain a best fit to the data. The prompt fission neutron spectra were also compared with the Evaluated Nuclear Data File (ENDF/B-VII.0). We calculate average energies from both experimental and calculated fission neutron spectra.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The Need for Precise and Well-documented Experimental Data on Prompt Fission Neutron Spectra from Neutron-induced Fission of {sup 239}Pu

The spectrum of neutrons emitted promptly after {sup 239}Pu(n,f)—a so-called prompt fission neutron spectrum (PFNS)—is a quantity of high interest, for instance, for reactor physics and global security. However, there are only few experimental data sets available that are suitable for evaluations. In addition, some of those data sets differ by more than their 1-σ uncertainty boundaries. We present the results of MCNP studies indicating that these differences are partly caused by underestimated multiple scattering contributions, over-corrected background, and inconsistent deconvolution methods. A detailed uncertainty quantification for suitable experimental data was undertaken including these effects, and test-evaluations were performed with the improved uncertainty information. The test-evaluations illustrate that the inadequately estimated effects and detailed uncertainty quantification have an impact on the evaluated PFNS and associated uncertainties as well as the neutron multiplicity of selected critical assemblies. A summary of data and documentation needs to improve the quality of the experimental database is provided based on the results of simulations and test-evaluations. Given the possibly substantial distortion of the PFNS by multiple scattering and background effects, special care should be taken to reduce these effects in future measurements, e.g., by measuring the {sup 239}Pu PFNS as a ratio to either the {sup 235}U or {sup 252}Cf PFNS.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Analysis of fission-product energy release after thermal-neutron fission of {sup 235}U and {sup 239}Pu by scale-6.1.3 with recently available fission product yield data - 14419

The fission-product energy release after the reactor shutdown has been an important issue from the perspective of the nuclear reactor safety in a very short time. The energy release from the decay of fission products can be estimated using a summation calculation method implemented in various burnup and depletion programs. The method generally depends on the nuclear structure data such as the decay and fission product yield data. In this study, the decay heat measurements after thermal-neutron fission of {sup 235}U and {sup 239}Pu have been evaluated by the ORIGEN-S with the decay and fission product yield libraries included in the SCALE-6.1.3 code package. In order to verify the importance of the fission product yield data when estimating the decay heats, new fission product yields libraries for ORIGEN-S have been generated based on the recently available fission product yield data such as ENDF/B-VII.1, JEFF-3.1.1, JENDL/FPY-2011, and JENDL-4.0. The new libraries were applied to the decay heat calculations, and the results were compared with those of the reference calculation based on the yield library that belongs to the SCALE-6.1.3. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Microscopic theory of singlet exciton fission. III. Crystalline pentacene

We extend our previous work on singlet exciton fission in isolated dimers to the case of crystalline materials, focusing on pentacene as a canonical and concrete example. We discuss the proper interpretation of the character of low-lying excited states of relevance to singlet fission. In particular, we consider a variety of metrics for measuring charge-transfer character, conclusively demonstrating significant charge-transfer character in the low-lying excited states. The impact of this electronic structure on the subsequent singlet fission dynamics is assessed by performing real-time master-equation calculations involving hundreds of quantum states. We make direct comparisons with experimental absorption spectra and singlet fission rates, finding good quantitative agreement in both cases, and we discuss the mechanistic distinctions that exist between small isolated aggregates and bulk systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nuclear Fission: from more phenomenology and adjusted parameters to more fundamental theory and increased predictive power

Two major recent developments in theory and computational resources created the favorable conditions for achieving a microscopic description of fission dynamics in classically allowed regions of the collective potential energy surface, almost eighty years after its discovery in 1939 by Hahn and Strassmann [1]. The first major development was in theory, the extension of the Time-Dependent Density Functional Theory (TDDFT) [2–5] to superfluid fermion systems [6]. The second development was in computing, the emergence of powerful enough supercomputers capable of solving the complex systems of equations describing the time evolution in three dimensions without any restrictions of hundreds of strongly interacting nucleons. Thus the conditions have been created to renounce phenomenological models and incomplete microscopic treatments with uncontrollable approximations and/or assumptions in the description of the complex dynamics of fission. Even though the available nuclear energy density functionals (NEDFs) are phenomenological still, their accuracy is improving steadily and the prospects of being able to perform calculations of the nuclear fission dynamics and to predict many properties of the fission fragments, otherwise not possible to extract from experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Singlet fission efficiency in tetracene-based organic solar cells

Singlet exciton fission splits one singlet exciton into two triplet excitons. Using a joint analysis of photocurrent and fluorescence modulation under a magnetic field, we determine that the triplet yield within optimized tetracene organic photovoltaic devices is 153% ± 5% for a tetracene film thickness of 20 nm. The corresponding internal quantum efficiency is 127% ± 18%. These results are used to prove the effectiveness of a simplified triplet yield measurement that relies only on the magnetic field modulation of fluorescence. Despite its relatively slow rate of singlet fission, the measured triplet yields confirm that tetracene is presently the best candidate for use with silicon solar cells.

36 MATERIALS SCIENCE↗

Preliminary Evaluation and Uncertainty Quantification of the Prompt Fission Neutron Spectrum of {sup 239}Pu

Low evaluated uncertainties were obtained in a previous evaluation of the {sup 239}Pu prompt fission neutron spectrum and associated covariances for incident neutrons of 0.5 MeV, which were enlarged a-posteriori before being incorporated into ENDF/B-VII.1. These low evaluated uncertainties triggered an in-depth study and improved estimate of experimental as well as model uncertainties. Here, we will summarize these efforts and show that the improved estimate of experimental and model uncertainties leads to corresponding evaluated uncertainties in good agreement with uncertainties obtained in a statistical analysis based primarily on experimental information.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Slow light enhanced singlet exciton fission solar cells with a 126% yield of electrons per photon

Singlet exciton fission generates two triplet excitons per absorbed photon. It promises to increase the power extracted from sunlight without increasing the number of photovoltaic junctions in a solar cell. We demonstrate solar cells with an external quantum efficiency of 126% by enhancing absorption in thin films of the singlet exciton fission material pentacene. The device structure exploits the long photon dwell time at the band edge of a distributed Bragg reflector to achieve enhancement over a broad range of angles. Measuring the reflected light from the solar cell establishes a lower bound of 137% for the internal quantum efficiency.

14 SOLAR ENERGY↗