Monte Carlo Analysis of the Accelerator-Driven System at Kyoto University Research Reactor Institute

An accelerator-driven system consists of a subcritical reactor and a controllable external neutron source. The reactor in an accelerator-driven system can sustain fission reactions in a subcritical state using an external neutron source, which is an intrinsic safety feature of the system. The system can provide efficient transmutations of nuclear wastes such as minor actinides and long-lived fission products and generate electricity. Recently at Kyoto University Research Reactor Institute (KURRI; Kyoto, Japan), a series of reactor physics experiments was conducted with the Kyoto University Critical Assembly and a Cockcroft-Walton type accelerator, which generates the external neutron source by deuterium-tritium reactions. In this paper, neutronic analyses of a series of experiments have been re-estimated by using the latest Monte Carlo code and nuclear data libraries. This feasibility study is presented through the comparison of Monte Carlo simulation results with measurements.clos

Design of singlet fission chromophores with cyclic (alkyl)(amino) carbene building blocks

We use MRSF-TDDFT and NEVPT2 methods to design singlet fission chromophores with the building blocks of cyclic (alkyl)(amino)carbenes (CAACs). CAAC dimers with C2, C4, and p-phenylene spacers are considered. The substitutions with trifluoromethyls and fluorine atoms at the α C position are investigated. The electronegative substituents enhance the π accepting capability of the α C, while maintaining it as a quaternary C atom. The phenylene-connected dimers with the two substitutions are identified as promising candidates for singlet fission chromophores. The cylindrically symmetric C2 and C4 spacers allow for substantial structural reorganizations in the S0-to-S1 and S0-to-T1 excitations. Although the two substituted dimers with the C4 spacer satisfy (or very close to satisfy) the primary thermodynamics criterion for singlet fission, the significant structural reorganizations result in high barriers so that the fission is kinetically unfavorable

Physics Study of Canada Deuterium Uranium Lattice with Coolant Void Reactivity Analysis

This study presents a coolant void reactivity analysis of Canada Deuterium Uranium (CANDU)-6 and Advanced Canada Deuterium Uranium Reactor-700 (ACR-700) fuel lattices using a Monte Carlo code. The reactivity changes when the coolant was voided were assessed in terms of the contributions of four factors and spectrum shifts. In the case of single bundle coolant voiding, the contribution of each of the four factors in the ACR-700 lattice is large in magnitude with opposite signs, and their summation becomes a negative reactivity effect in contrast to that of the CANDU-6 lattice. Unlike the coolant voiding in a single fuel bundle, the 2 ?? 2 checkerboard coolant voiding in the ACR-700 lattice shows a positive reactivity effect. The neutron current between the no-void and voided bundles, and the four factors of each bundle were analyzed to figure out the mechanism of the positive coolant void reactivity of the checkerboard voiding case. Through a sensitivity study of fuel enrichment, type of burnable absorber, and moderator to fuel volume ratio, a design strategy for the CANDU reactor was suggested in order to achieve a negative coolant void reactivity even for the checkerboard voiding case.ope

Computation of Molecular Electron Affinities Using an Ensemble Density Functional Theory Method

The computation of electron attachment energies (electron affinities) was implemented in connection with an ensemble density functional theory method, the state-interaction state-averaged spin-restricted ensemble-referenced Kohn–Sham (SI-SA-REKS or SSR) method. With the use of the extended Koopmans’ theorem, the electron affinities and the respective Dyson orbitals are obtained directly for the neutral molecule, thus avoiding the necessity to compute the ionized system. Together with the EKT-SSR (extended Koopmans’ theorem-SSR) method for ionization potentials, which was developed earlier, EKT-SSR for electron affinities completes the implementation of the EKT-SSR formalism, which can now be used for obtaining electron detachment as well as the electron attachment energies of molecules in the ground and excited electronic states. The extended EKT-SSR method was tested in the calculation of several closed-shell molecules. For the molecules in the ground states, the EKT-SSR energies of Dyson’s orbitals are virtually identical to the energies of the unoccupied orbitals in the usual single-reference spin-restricted Kohn–Sham calculations. For the molecules in the excited states, EKT-SSR predicts an increase of the most positive electron affinity by approximately the amount of the vertical excitation energy. The electron affinities of a number of diradicals were calculated with EKT-SSR and compared with the available experimental data. With the use of a standard density functional (BH&HLYP), the EKT-SSR electron affinities deviate on average by ca. 0.2 eV from the experimental data. It is expected that the agreement with the experiment can be improved by designing density functionals parametrized for ionization energies

Structural or population dynamics: what is revealed by the time-resolved photoelectron spectroscopy of 1,3-cyclohexadiene? A study with an ensemble density functional theory method

Time-resolved photoelectron spectra during the photochemical ring-opening reaction of 1,3-cyclohexadiene (CHD) are modeled by an ensemble density functional theory (eDFT) method. The computational methodology employed in this work is capable of correctly describing the multi-reference effects arising in the ground and excited electronic states of molecules, which is important for the correct description of the ring-opening reaction of CHD. The geometries of molecular species along the non-adiabatic molecular dynamics (NAMD) trajectories reported in a previous study of the CHD photochemical ring-opening were used in this work to calculate the ionization energies and the respective Dyson orbitals for all possible ionization channels. The obtained theoretical time-resolved spectra display decay characteristics in a reasonable agreement with the experimental observations; i.e., the decay (and rise) of the most mechanistically significant signals occurs on the timescale of 100–150 fs. This is very different from the excited state population decay characteristics (τ _(S1) = 234 ± 8 fs) obtained in the previous NAMD study. The difference between the population decay and the decay of the photoelectron signal intensity is traced back to the geometric transformation that the molecule undergoes during the photoreaction. This demonstrates the importance of including the geometric information in interpretation of the experimental observations