Relationship between 237Np Mössbauer parameters and bond distances in nitrogen coordinated [NpO2(acac)2py]

We now report the ²³⁷Np Mössbauer spectra for [NpO₂(acac)₂py] I. The neptunium(VI) ion in I is coordinated by six oxygen atoms and the one nitrogen atom of pyridine. The isomer shift value obtained for I is ?40 mm/s, which falls in the range for the Np(VI) oxidation state. The relationship between the isomer shift and Np–O bond distance of the neptunyl group for oxygen coordination compounds is in good agreement with the reported structure of I. It is well known that the mean Np–O bond distance of the neptunium compounds is shorter by 0.01 Å than that of analogous uranium compounds. The good agreement in the ²³⁷Np–Mössbauer parameters and the Np–O distance has indicated that the reported analogous [UO₂(acac)₂py] structure may have some inaccuracies. Therefore, we have re-determined the crystal structure of [UO₂(acac)₂py]. The U–O bond distance we have obtained is reasonable.     

Transmutation of 129I, 237Np, 238Pu, 239Pu, and 241Am using neutrons produced in target-blanket system ‘Energy plus Transmutation’ by relativistic protons

Target-blanket facility ‘Energy + Transmutation’ was irradiated by proton beam extracted from the Nuclotron Accelerator in Laboratory of High Energies of Joint Institute for Nuclear Research in Dubna, Russia. Neutrons generated by the spallation reactions of 0.7, 1.0, 1.5 and 2 GeV protons and lead target interact with subcritical uranium blanket. In the neutron field outside the blanket, radioactive iodine, neptunium, plutonium and americium samples were irradiated and transmutation reaction yields (residual nuclei production yields) have been determined using γ-spectroscopy. Neutron field's energy distribution has also been studied using a set of threshold detectors. Results of transmutation studies of ¹²⁹I, ²³⁷Np, ²³⁸Pu, ²³⁹Pu and ²⁴¹Am are presented.      

Isomer-shift analogue in neutron resonances

For the first time, the recently predicted chemical shift of neutron resonances, to be regarded as an analogue to the Mössbauer isomer shift, has been experimentally observed studying the 6.67 eV resonance of ²³⁸U. The experimental shifts were determined by a chi-square fitting technique from the time-of-flight transmission spectra of metallic uranium and four uranium compounds measured at the Dubna IBR-30 pulsed reactor. A computational method has been applied to estimate, and compensate for, the influence of the crystal-lattice vibrations on the experimental values thus obtained. The electron density differences at the nucleus have been calculated for the various sample pairs using available data on chemical X-ray shifts in uranium compounds, on Mössbauer isomer shifts in isovalent neptunium compounds and on free-ion electron densities. The resonance shift results lead to the conclusion that the mean-square charge radius of ²³⁸U diminishes by 1.7_?0.8^+1.2 fm² upon capturing the resonance neutron.     

Resonance ionization mass spectroscopy for trace analysis of neptunium

Resonance ionization mass spectroscopic (RIMS) measurements for trace analysis and spectroscopy of ²³⁷Np, the ecologically most important isotope of neptunium, are described. The chemical procedure for the separation of neptunium from aqueous samples as well as the preparation of filaments for RIMS are outlined. Several two- and three-step excitation schemes have been investigated in order to find suitable conditions for the sensitive detection of ²³⁷Np. Using a three-step, three-color excitation and ionization scheme an overall detection efficiency of 3×10^–8 was obtained, resulting in a detection limit of 4×10⁸ atoms (160 fg) of ²³⁷Np. The hyperfine structure splittings of the levels under investigation, which influence the detection limit, were measured. A new method to determine the first ionization potential (IP) was applied to neptunium yielding a value of IP=6.2655(2) eV.     

Radiochemical determination of 237NP in soil samples contaminated with weapon grade plutonium

The Palomares terrestrial ecosystem (Spain) constitutes a natural laboratory to study transuranics. This scenario is partially contaminated with weapon-grade plutonium since the burnout and fragmentation of two thermonuclear bombs accidentally dropped in 1966. While performing radiometric measurements in the field, the possible presence of ²³⁷Np was observed through its 29 keV gamma emission. To accomplish a detailed characterization of the source term in the contaminated area using the isotopic ratios Pu-Am-Np, the radiochemical isolation and quantification by alpha spectrometry of ²³⁷Np was initiated. The selected radiochemical procedure involves separation of Np from Am, U and Pu with ionic resins, given that in soil samples from Palomares ^239+240Pu levels are several orders of magnitude higher than ²³⁷Np. Then neptunium is isolated using TEVA organic resins. After electrodeposition, quantification is performed by alpha spectrometry. Different tests were done with blank solutions spiked with ²³⁶Pu and ²³⁷Np, solutions resulting from the total dissolution of radioactive particles and soil samples. Results indicate that the optimal sequential radionuclide separation order is Pu-Np, with decontamination percentages obtained with the ionic resins ranging from 98% to 100%. Also, the addition of NaNO₂ has proved to be necessary, acting as a stabilizer of Pu-Np valences.     

Cross sections for 209Bi, 232Th, 235U, 238U, and 237Np fission induced by intermediate-energy protons and deuterons

The cross sections for ²⁰⁹Bi, ²³²Th, ²³⁵U, ²³⁸U, and ²³⁷Np fission induced by protons of energy in the range 1.0–3.7 GeV and by deuterons of energy 1.0 GeV were measured. The results are compared with data from other experiments, with available estimates, and with the predictions of theoretical models.     

237Np separation from environmental matrices by extraction chromatography method

Aliquat-336 anchored on hydrophobized silica gel was used for effective separation of ²³⁷Np from soil matrices and from model solutions. Alpha spectrometry for ²³⁷Np determination was used. The interfering radionuclides present in environmental samples such as ²³⁴U, ²³²Th, ²³¹Pa and ^239+240Pu were removed by separation with nitric acid solutions containing formic acid and ferrous sulfamate as reducing agents. Spiking samples with ^238,234U, ²³²Th and ²³⁸Pu were used to check separation effectiveness. A separation yield of ²³⁷Np from soil matrices was checked by measuring of added known amount activity and was found to be about 15%. The yield of separation for model solutions was about 56%. Different parameters of eluant on recovery of ²³⁷Np from column were studied.     

The study of prompt and delayed muon induced fission

The ratios of prompt to delayed fission yields for the isotopes²³³U,²³⁴U,²³⁵U,²³⁶U,²³⁸U,²³⁷Np,²⁴²Pu, and²⁴⁴Pu and the fission probabilities relative to each other have been investigated experimentally. Using the value of the total fission probability for²³⁷Np the absolute probabilities for prompt and delayed fission have been determined. The fission probabilities per muon captureP _fc have been derived for all the isotopes and compared with an evaluation based on excitation functions from theory.     

237Np and 57Fe Mössbauer study of NpFeGa5

⁵⁷Fe and ²³⁷Np Mössbauer ōmeasurements have been performed for NpFeGa₅, which is one of the so-called neptunium 1-1-5 compounds. The ⁵⁷Fe Mössbauer spectra below T _N = 118 K show the magnetically ordered state. The magnitude of the hyperfine magnetic field at the ⁵⁷Fe nucleus is determined to be 1.98 ± 0.05 T at 10 K. From the ²³⁷Np Mössbauer spectrum at 10 K, the hyperfine magnetic field at the ²³⁷Np nucleus is 203 T and the hyperfine coupling constant is determined to be 237 T/μ_B using the Np atomic magnetic moment of 0.86 μ_B determined by the neutron diffraction study.     

Systematic trends in the237neptunium Mössbauer isomer shift: Overlap of IV,V and VI neptunium oxidation states and correlation between isomer shift and crystal structure

The influence of the neptunium ion environment on the²³⁷Np Mössbauer isomer shifts has been studied in various metal coordination complexes: fluorides, oxides, oxide fluorides and polycarboxylates. A linear dependence between the isomer shift and the mean neptunium-ligand distance in a series of hexavalent Np compounds has been evidenced and the feasibility of overlapped isomer shift areas, namely Np(IV), Np(V) and Np(VI) has been established.     

The E1 and E2 strength in the electrofission of some heavy elements

Measurements of the electrofission cross section for ²³²Th, ²³⁸U and ²³⁷Np have been made for an electron energy range from 20 to 120 MeV. A comparison is made between the electrofission and photofission cross sections using the concept of virtual photons. It is deduced that the electrofission reaction for these elements proceeds through a significant E2 contribution as well as an E1 transition mode.     

Photofission of 238Pu, 240Pu, and 242Pu in the energy range 5–10 MeV

The cross sections for the photofission of plutonium isotopes ²³⁸Pu, ²⁴⁰Pu, and ²⁴²Pu in the energy range 5–10 MeV have been measured by using a beam of bremsstrahlung photons from the microtron installed at the Institute of Physics and Power Engineering (Obninsk). The energy regions below the fission barrier and above 6 MeV have been scanned with pitches of 0.05 and 0.1 MeV, respectively. In deriving the absolute cross section for ²³⁸Pu photofission, ²³⁸U photofission has been employed as a reference reaction. In measurements involving ²⁴⁰Pu and ²⁴²Pu nuclei, the neptunium isotope ²³⁷Np, which is characterized by a more regular dependence of the photofission cross section on excitation energy than ²³⁸U, has been chosen for the first time as a reference nucleus. The measured cross sections as functions of energy show resonance structures in the vicinity of the fission threshold that are consistent with those previously observed in the energy dependences of fissilities for corresponding direct reactions. The partial-wave cross sections for the J ^π K = 1^?0, 1^?1, and 2⁺0 photofission channels have been determined as functions of energy. At energies below some 5.5 MeV, the total cross section for photofission of each plutonium isotope being studied receives a significant contribution from quadrupole interaction. Within the one-dimensional model of a two-humped fission barrier, the parameters of the barriers for ²³⁸Pu, ²⁴⁰Pu, and ²⁴²Pu have been extracted from data and have then been compared with estimates based on previous measurements.     

Electron induced fission of the 238U, 237Np, 239Pu and 243Am nuclei in the energy region 100–1000 MeV

Electrofission cross sections for ²³⁸U, ²³⁷Np, ²³⁹Pu and ²⁴³Am have been measured over the energy range 100–1000 MeV. Relative flssilities are evaluated. Analysis in terms of the virtual photon spectra technique involving a nuclear size effect is made. Contributions of various electronuclear excitation mechanisms in the large-energy region are discussed.     

Die Anwendung der Methode der zeitlich korrelierten assoziierten Teilchen (MEZKAT)

The TCAPM was developed to absolute and precise fission cross section measurement for neutron energies from 2 MeV up to 19 MeV. Experimental results of absolute fission cross section measurements on ²³³U, ²³⁵U, ²³⁸U, -²³⁷Np, ²³⁹Pu and ²¹²Pu are given. Furthermore the TCAPM is suitable for the application of inelastic scattering of neutrons by the analysis of element contents.     

Photofission of heavy nuclei at energies up to 4 GeV

Total photofission cross sections for 238U, 235U, 233U, 237Np, 232Th, and natPb have been measured simultaneously, using tagged photons in the energy range Egamma=0.17-3.84 GeV. This was the first experiment performed using the Photon Tagging Facility in Hall B at Jefferson Lab. Our results show that the photofission cross section for 238U relative to that for 237Np is about 80% over the entire energy range, implying the presence of important processes which compete with fission. If we assume that for 237Np the photofission probability is equal to unity, we observe a significant shadowing effect, starting below 1.5 GeV.     

Systematics of Mössbauer hyperfine parameters in Np intermetallics

Data for intermetallic compounds of neptunium obtained with the 60 keV Mössbauer resonance of²³⁷Np are reviewed. Measurements of temperature, pressure and field dependencies are available. The main questions addressed are: (a) the degree of delocalization of 5f-electrons, (b) the formal charge state of Np, and (c) the influence of the ligand on the neptunium electronic structure. For this purpose, we present an evaluation of systematic behavior concerning mainly the hyperfine field and isomer shift in the cubic Laves phase materials NpX₂, the NaCl-type monochalcogenides and monopnictides, and intermetallics with AuCu₃ and ThCr₂Si₂ structures. Analogies to corresponding rare-earth compounds will be pointed out.     

Symmetric and asymmetric fission modes in proton-induced fission at 660 MeV of <Superscript>238</Superscript>U

Fission product cross sections of intermediate-energy fission of ²³⁸U were used in order to construct the charge and mass yield distributions. Enriched target of ²³⁸U was irradiated by proton beam with energy 660 MeV for several hours at the LNP Phasotron, Joint Institute for Nuclear Research (JINR), Dubna, Russia. The charge distribution of the fission fragments was analyzed for calculation of isobaric cross sections. The mass yield curves were expanded into symmetric and asymmetric components according multimodal fission approach. The fissility values of actinides were calculated at given proton energy. The obtained results have been compared to the same data for targets ²³⁷Np and ²⁴¹Am.     

Iodine- and xenon-isotope yield ratio in photofission fragments of heavy nuclei

The ratios of cumulative yields of the ¹³⁵I isotope and the independent yield of ¹³⁵Xe at photofission of ²³²Th, ²³⁸U, ²³⁷Np, ²⁴³Am, and ²³⁸Cm by bremsstrahlung radiation with a boundary energy of 25 MeV are measured. The selective gas transportation of fission fragments and a measurement of the spectra of their γ radiation were used. A large difference in the ratios of the yields for these targets was discovered: from 34 for ²³⁸U to 1.3 for ²⁴³Am. This difference is discussed based on the known ideas of the formation mechanism of fission fragments.     

Measurement of uranium and its isotopes at trace levels in environmental samples using mass spectrometry

Actinides have widely entered the environment as a result of nuclear accidents and atmospheric weapon testing. These radionuclides, especially uranium, are outstanding radioactive pollutants, due to their high radiotoxicity and long half-lives. In addition to this, since depleted uranium (DU) has been used in the Balkan conflict in 1999, there has been a concern about the possible consequences of its use for the people and environment. Therefore, accurate, precise and simple determination methods are necessary in order to evaluate the human dose and the concentration and effects of these nuclides in the environment. The principal isotopes of uranium e.g. ²³⁵U and ²³⁸U are of primordial origin and ²³⁴U present in radioactive equilibrium with ²³⁸U. ²³⁶U occurs in nature at ultra trace concentrations with a ²³⁶U: ²³⁸U atom ratio of 10⁻¹⁴. Concentrations of uranium in soil samples were determined using inductively coupled plasma mass spectrometry (ICP-MS) and isotope ratios of uranium were measured using a thermal ionisation mass spectrometer. Radioactive dis-equilibrium of ²³⁴/²³⁸U, depletion of ²³⁵/²³⁸U and significant evidence of ²³⁶U/²³⁸U were noticed in soil samples.