ABSTRACT
In this Letter, inspired by the ghost imaging technique, we propose a wavefront shaping technique based on the third-order correlation of light fields (TCLF). Theoretically, we prove that if the light field fluctuation can be modeled by a complex Gaussian random process with a non-zero mean, the conjugate complex amplitude of the object and a focusing phase factor can be obtained by TCLF when using a single-point detector, which can support wavefront shaping. Experiments demonstrate that TCLF can achieve high-resolution wavefront shaping for scattered fields and scattering-assisted holography without additional operations such as optimization and phase shifting.
ABSTRACT
In this Letter, we propose a simple and robust method that we have named an optimal accumulation algorithm (OAA) to modulate a scattered light field. Compared with the simulated annealing algorithm (SAA) and genetic algorithm (GA), the OAA is very robust, that is to say it has a strong anti-disturbance capability. In experiments, the scattered light field through ground glass and a polystyrene suspension was modulated, where the polystyrene suspension supported a dynamic random disturbance. It was found that, even if the suspension is too thick to see the ballistic light, the OAA can still modulate the scattered field effectively, while the SAA and GA completely failed. In addition, the OAA is so simple that only addition and comparison are needed, and it can achieve multi-target modulation.
ABSTRACT
Organic compounds of actinyls and their bonding features have attracted extensive attention in nuclear waste separation due to their characteristics of separating fission products. Herein, detailed studies on the binding sites of [AnO2(COOH) n (H2O) m ]2-n (An = U, Np, Pu, and Am; n = 1-3; m = 0, 2, 4; 2n + m = 6) complexes toward Cs are predicted by calculation, and their electronic excitation characteristics were illustrated, providing theoretical supports for the design of Cs adsorbents. The quantum theory of atom in molecules and electron localization function have been implemented to analyze the chemical bonding characterization. The covalent character of An-OC bonds become weaker with increasing COOH- ligands, and the covalent interaction in An-OC bonds is more obvious than that in An-OH bonds. Total and partial population density of state suggest that the 2p orbits of O have more significant contribution in the low-energy region atoms and the 6d/5f orbits of An have more significant contribution in the high-energy region. The Cs+ best adsorption site on [UO2(COOH)2(H2O)2] and [UO2(COOH)3]- is the adjacent oxalates, and the [UO2(COOH)3]- complexes have better adsorption capacity. Besides, the electronic excitation characteristics of Cs+ adsorption on the UO2(COOH)2(H2O)2 complex were analyzed by the UV-vis spectrum and hole-electron distribution.
ABSTRACT
Actinide sulfides are especially significant in actinide chemistry because of their potentials that are used as nuclear fuel and the wide variety of their stoichiometries and physical properties. It is essential for studying the synthesis mechanism of actinide sulfides. In this study, the reactions of thorium cation Th2+ with the facile sulfur-atom donor OCS to produce thorium sulfides have been systematically explored by using density functional. The detailed insights of the primary reaction and secondary reaction paths are reported. We investigated that the multiple bonding characters and complexes involved in reaction exhibit significant covalent character. The reaction rate indicated that the tunneling effect is small compared with the effect of temperature on the rate. This study addresses some of the current limitation in understanding the detailed reaction information of Th2++OCS.
ABSTRACT
Exploring the bonding features between organics and actinide elements is a fundamental topic in nuclear waste separation. In this work, [AnO2(C2O4) n](2 n-2)- (An = U, Np, Pu, and Am; n = 1-3) complexes have been characterized by density functional theory. The actinyl oxalate complexes are found to exhibit the typical An-Oyl, An-Oeq bonds and Oyl-An-Oyl angles. Interatomic interaction analyzed by electron density difference, charge decomposition analysis, charges population, bond order, electron localization function, and quantum theory of atom in molecules indicates that An-Oeq bonds are ionic (closed-shell) bonding interaction with a small degree of covalent character. The similarities and differences between isomers have been discussed in the actinide coordination chemistry, and the orbital interactions also have been investigated through total, partial, and overlap population density of state diagrams. Besides, the electrostatic potential was used to predict the adsorption sites on the molecular vdW surface.
ABSTRACT
Activation of prototypical bonds by actinide atoms is an important aspect of material activity, and the results can be used for the study of nuclear material storage. In this study, the activation of the P-H bonds of the PH3 molecule by U or Th to form uranium or thorium hydride phosphorus has been systematically explored using density functional theory. A detailed description of the reaction mechanism which includes the potential energy profiles and the properties of bond evolution is presented. There are two types of reaction channels, isomerization and dehydrogenation in U + PH3 and Th + PH3. The difference between the two reactions is the process of the first P-H bond dissociation. The evolution characteristics of the chemical bonds along reaction pathways is analyzed by using electron localization functions, quantum theory of atoms in molecules, Mayer bond orders and natural bond orbitals. The reaction rate constants are calculated at the variational transition state level, and rate-determining steps are predicted.
