新同位素235Am的产生与鉴别

一种缺中子新同位素２３５Ａｍ通过２３８Ｐｕ（ｐ,４ｎ）２３５Ａｍ反应而产生．产物借助Ｈｅ－ｊｅｔ系统的传输,快化学分离以及γ、Ｘ射线和γ－Ｘ（γ）符合测量等得到鉴别,测得其半衰期为１５±５ｍｉｎ． A new neutron deficient isotope 235 Am was produced via 238 Pu(p,4n) 235 Am reaction. The products were identified by means of the transporting of He jet system, separating of rapid radiochemical method and measuring of γ and X rays as well as X γ coincidence. The measured half life of 235 Am is 15±5min.     

Production of neutron-deficient nuclei around N = 126 by proton-induced spallation

Many isotopes of Np, Pu, Am, and Cm around the N = 126 shell still have not been produced in the laboratory. This study aims to investigate the cross sections and yields of the neutron-deficient nuclei of Np, Pu, Am, and Cm produced in the proton-induced spallations of transuranium elements. The isospin-dependent quantum molecular dynamics (IQMD) model is applied to study the dynamical process of reaction, and the subsequent decay process is simulated by the GEMINI++ model. The IQMD-GEMINI++ model is applied to calculate the cross section, kinetic energy, and angular distribution of the isotopic productions around N = 126. The Lindhand, Scharff, and Schiott theory is applied to calculate the energy loss of different heavy nuclei in the target material. A comparison between the data and the calculations shows that the IQMD-GEMINI++ model can reproduce the production cross sections of the neutron-deficient nuclei in spallation within approximately 1.5 orders of magnitude. The maximum cross section of the undiscovered isotopes of Np, Pu, Am, and Cm is about 10^?5 mb, while the kinetic energies of the productions are all less than 16 MeV. The angular distribution shows that the emission direction of production is mostly at a backward angle. The range of production in the target is within the range of 10^?7 to 10^?5 cm. This range is the effective target thickness for the online identification of undiscovered isotopes. Based on the effective thickness of the target and assuming an intensity of 120 μA for the proton beam, the yields of the undiscovered neutron-deficient nuclei are calculated. Productions of the undiscovered isotopes of Np, Pu, Am, and Cm by the proton-induced spallations of transuranium elements are feasible. However, experimental techniques for online identification of neutron-deficient nuclei produced in proton-induced spallation should be developed.     

Alphaspektrometrische Isotopenverdünnungsanalyse von Plutoniumisotopen in Kernbrennstofflösungen

In einer bestrahlten Kernbrennstofflösung wurde die Plutoniumaktivität mit Hilfe der Isotopenverdünnungsanalyse bestimmt. Dabei wurde ²³⁸Pu als Tracerisotop verwendet. Die Abtrennung des Plutoniums wurde durch Extraktion und die Aktivitätsmessung mit Hilfe der Alphaspektrometrie unter Verwendung von Si-Halbleiterdetektoren vorgenommen. Die Störung durch ²⁴¹Am wurde durch gammaspektrometrische Messung berücksichtigt. Die Genauigkeit der ²³⁸Pu-Aktivitätsmessung und die der Messung der Gesamtaktivität beträgt ungefähr 1,5%. Die Bestimmung des ²³⁹Pu zu ²⁴⁰Pu Verhältnisses war nur mit einem groβen Fehler möglich, entsprechend der nahezu gleichen Alphaenergien dieser Isotope und der komplizierten Peakform. ²⁴¹Pu wurde durch alphaspektrometrische Differenzmessung der nachgebildeten ²⁴¹Am Aktivität bestimmt.

In irradiated nuclear fuel solution plutonium isotops were determined with the help of isotope dilution analysis. ²³⁸Pu was used as a tracer isotope. Plutonium was separated by extraction and the activity was measured by alphaspectroscopy using silicon detectors. Interfering ²⁴¹Am was recognized by gamma spectroscopic measurements. The accuracy of ²³⁸Pu determination and the determination of the total activity amounts to about 1-5%. For the ²³⁹Pu ratio we obtained a value with a large systematic error due to the similar alpha energies of these isotopes in the complicated shape of the peaks. The ²⁴¹Pu activity was determined by alphaspectroscopic difference measurement, and was calculated from the ingrown of ²⁴¹Am activity.     

Identification of the new isotope 241Bk

A new neutron-deficient berkelium isotope ²⁴¹Bk produced in the ²³⁹Pu(⁶Li, 4n) reaction has been identified using a gas-jet coupled on-line isotope separator. Cm K and L X-rays associated with the EC decay of ²⁴¹Bk were observed in the mass-241 fraction, and three γ transitions were attributed to the EC decay of ²⁴¹Bk through X-γ coincidences. The half-life of ²⁴¹Bk was determined to be 4.6±0.4 min which is 1/2-1/4 of that of theoretical predictions. The half-life value and the observed γ transitions can be consistently explained as a consequence of the allowed EC transition of π7/2⁺[633] → ν7/2⁺[624]. Received: 14 October 2002 / Accepted: 6 November 2002 / Published online: 17 January 2003 RID="a" ID="a"e-mail: asai@tandem.tokai.jaeri.go.jp Communicated by J. ?yst?     

EC and α decays of 235Am

EC and decays of ²³⁵Am have been studied using a gas-jet coupled on-line isotope separator. Excited states in ²³⁵Pu have been established for the first time by means of -ray spectroscopy following the EC decay of ²³⁵Am. The deduced log ft value suggests that the ground state of ²³⁵Am should have the 5/2^-[523] configuration. The - coincidence result has revealed that the 5/2^-[523] state in ²³¹Np populated by the favored transition of ²³⁵Am is located at < 15 keV, which allows us to precisely determine the Q value of ²³⁵Am.     

Beta decay of 93Pd

The very neutron-deficient isotope ⁹³Pd was produced in fusion-evaporation reactions of a ⁴⁰Ca beam on a ⁵⁸Ni target. The reaction products were separated at the GSI Online Mass Separator, using ion sources of the FEBIAD type. The -decay properties of ⁹³Pd were studied by detecting -delayed protons and -delayed -rays. The feeding of excited levels in the daughter nucleus ⁹³Rh and the -decay half-life of ⁹³Pd were determined. The experimental results are discussed in comparison to shell model predictions. Received: 19 April 2000 / Accepted: 17 June 2000     

Pu and Am determination in the environment—method development

A high resolution inductively coupled plasma mass spectrometric (HR-ICP-MS) method for the determination of plutonium isotopes, Am and the ²⁴⁰Pu/²³⁹Pu isotope ratio utilising modification of Pu-02-RC Plutonium in Soil Samples, Pu-03-RC Plutonium in Soil Residue—Total Dissolution Method, Pu-11-RC Plutonium Purification—Ion Exchange Technique, Pu-12-RC Plutonium and/or Americium in Soil or Sediments, HASL-300 was developed. Total plutonium concentrations (^239+240Pu) measured in environmental samples by this HR-ICP-MS method were in good agreement with recommended data obtained from a-spectrometry. It was achieved the decreasing of the time to analyze the samples over than 33%.     

Determination of Separated Plutonium,Americium and Curium in Environmental Samples by Sequential Extraction Techniques

A simple, reliable and practical radiochemical method for sequential isolation and determination of plutonium, americium and curium in a wide variety of environmental samples including soils, river sediments and water was developed. The isotopes determined are: ²³⁸Pu, ^239,240Pu, ²⁴¹Am, ²⁴²Cm and ²⁴⁴Cm. The methods involve leaching of soil or sedimental samples with concentrated nitric acid using a pressure digestion technique. Subsequent concentration and separation of nuclides of interest from major matrix elements and other interfering alpha-emitters are carried out by coprecipitation with ferric hydroxide and solvent extractions. Sources suitable for alpha-spectrometry are prepared by electrodeposition from acidic ammonium chloride solution. ²⁴²Pu and ²⁴³Am are used as tracer isotopes of plutonium and americium-curium elements, respectively. Some results of analysis of soils, sediments and water are given. The alpha peaks from ²³⁸Pu, ^239,240Pu and ²⁴²Pu as well as ²⁴¹Am, ²⁴⁴Cm, ²⁴²Cm and ²⁴³Am are well resolved. The entire analytical procedures for plutonium, americium and curium are completed in less than sixteen hours.     

Cesium, americium and plutonium isotopes in ground level air of vilnius

Systematic observations of radionuclide composition and concentration in the atmosphere have been carried out at the Institute of Physics in Vilnius since 1963. Increases in activity concentration of radionuclides in the atmosphere were observed after nuclear weapon tests and the Chernobyl NPP accident. At present the radiation situation in Lithuania is determined by two main sources of radionuclides, forest fire and resuspension products transferred from highly polluted region of the Ukraine and Belarus. The activity concentrations of ¹³⁷Cs were measured in two to three days samples while plutonium and americium in monthly samples. The extremely high activity concentrations of ²³⁸Pu, ^239,240Pu, ²⁴¹Am determined in the atmosphere during the Chernobyl accident can be explained by transport of “hot particles” of different composition. Activity concentration in 1995–2003 of ²⁴¹Am and ^239,240Pu isotopes ranged from 0.3 to 500 and from 1 to 500 nBq/m³, respectively. ²³⁸Pu/^239,240Pu activity ratio in measured samples differs from 0.03 to 0.45. A decrease in ²⁴⁰Pu/²³⁹Pu atomic ratio from 0.30 to 0.19 was observed in 1995–2003.     

Cesium,americium and plutonium isotopes in ground level air of Vilnius

Systematic observations of radionuclide composition and concentration in the atmosphere have been carried out at the Institute of Physics in Vilnius since 1963. Increases in activity concentration of radionuclides in the atmosphere were observed after nuclear weapon tests and the Chernobyl NPP accident. At present the radiation situation in Lithuania is determined by two main sources of radionuclides, forest fire and resuspension products transferred from highly polluted region of the Ukraine and Belarus. The activity concentrations of ¹³⁷Cs were measured in two to three days samples while plutonium and americium in monthly samples. The extremely high activity concentrations of ²³⁸Pu, ^239,240Pu, ²⁴¹Am determined in the atmosphere during the Chernobyl accident can be explained by transport of “hot particles” of different composition. Activity concentration in 1995–2003 of ²⁴¹Am and ^239,240Pu isotopes ranged from 0.3 to 500 and from 1 to 500 nBq/m³, respectively. ²³⁸Pu/^239,240Pu activity ratio in measured samples differs from 0.03 to 0.45. A decrease in ²⁴⁰Pu/²³⁹Pu atomic ratio from 0.30 to 0.19 was observed in 1995–2003.     

Structures in far-out asymmetric mass distributions in low energy fission

The far-out asymmetric mass distributions for ²³⁵U(n_th, f), ²³⁹Pu(n_th, f), ²⁴³Am(n_th, f) and ²⁵²Cf(sf) have been determined. The structures in these data and those in the existing results on ²³⁸U, ²³⁴Np and ²³⁵Np have been analysed in a systematic way in terms of the static scission-point model of Wilkins et al. The model explains well all the structures seen in very asymmetric fission.     

Photofission of americium isotopes in the energy range 6–12 MeV

By means of the reference method, the cross sections for the fission of the ²⁴¹Am, ^242m Am, and ²⁴³Am isotopes were measured at the microtron of the Institute of Physics and Power Engineering (Obninsk). These measurements, which employed the cross section for ²³⁸U photofission as a reference, covered the energy range 6–12 MeV scanned with a variable step of 50 to 200 keV. Data on ^242m Am photofission in the energy range 6–12 MeV and ²⁴³Am photofission in the region between 6 and 7 MeV were obtained for the first time. New results for ²⁴¹Am reveal that the cross sections for ²⁴¹Am photofission from previous studies of the present author were exaggerated. The new results for this isotope comply well with data of other authors. It is not confirmed that the fissility of ²⁴¹Am is less than the fissility of ²⁴³Am. The energy dependences of the fissilities of the americium isotopes from photofission data are compared with those that were obtained for these fissilities from data on direct reactions like ²⁴⁰Pu(³He, df)²⁴¹Am. The results of this comparison show that the observed fission thresholds and the plateaulike dependences at energies above 7.5 MeV from the two types of studies comply well. The present data show evidence that, in the energy region around 6 MeV, the photofission cross section has a maximum, which is associated, in all probability, with the low-energy resonance structure in the cross section for dipole photoabsorption.     

Gamma rays of primary fission products from 235U(n,f) and 239Pu(n,f)

Gamma rays of primary fission products in thermal-neutron-induced fission of ²³⁵U and ²³⁹Pu were investigated. Isotopic assignments of several lines were made by comparing fission yield ratios and relative γ-ray intensities of the two fissioning nuclei. Differences between ²³⁵U and ²⁵²Cf fission product γ-ray lines are discussed.     

Spontaneous fission of neutron-deficient fermium isotopes and the new nucleus 241Fm

Spontaneous fission of neutron-deficient fermium isotopes (N ≤ 144) was investigated. The nuclei were produced in fusion-evaporation reactions of ⁴⁰Ar beams with ^{204,206–208}Pb targets. Excitation functions of the two-and three-neutron evaporation channels were measured. The new isotope ²⁴¹Fm was identified, and its decay properties were determined. A previously made assignment of a 0.8 ms spontaneous-fission activity to the isotope ²⁴²Fm could not be confirmed. Isomeric states were not observed in any of the investigated isotopes. The experiments were performed at the velocity filter SHIP of GSI in Darmstadt.     

New nuclides228,229Pu

In continuation of our work on investigation of the neutron-deficient plutonium isotopes [1] we carried out the experiments aimed to produce new isotopes^228,229Pu. The isotope²²⁸Pu has been produced in the bombardment of the²⁰⁸Pb target with a beam of²⁴Mg and the isotope²²⁹Pu — in the reactions of^207,208Pb targets with²⁶Mg projectiles. The isotopes were identified after in-flight separation from the beam and target-like particles by the VASSILISSA electrostatic separator [2] and implantation into silicon strip detectors. The assignment of unknown -decays was made by establishing their genetic position and time correlations with those belonging to known -decay chains. The -decay energies of^228,229Pu were measured to be (7810±20) keV and (7460±30) keV, respectively.     

Measurements of delayed-neutron yields from thermal-neutron-induced fission of 235U, 233U, 239Pu, and 237Np

The experimental results on delayed-neutron yields from thermal-neutron-induced fission of some actinides in the IBR-2 pulsed reactor are presented. A method of periodic irradiation without displacement of the sample was used. The measurements of delayed-neutron total yields in thermal-neutron-induced fission of ²³⁹Pu, ²³³U, and ²³⁷Np and in cold-neutron-induced fission of ²³⁵U, ²³³U, and ²³⁹Pu were carried out. All values were obtained with the use of the value of β₀ for (n _th+²³⁵U) as a reference. Precise measurements of decay curves in the time interval 5–350 ms for ²³⁵U and ²³⁹Pu were performed.     

Evidence for a J = 0 first excited state of Zr through a measurement of internal conversion electrons from fission products

An investigation of conversion electrons from fission fragments and fission products of the ²³⁵U(n, f) reaction has revealed a strong E0 transition in some isotope at Z=40. Strong evidence that this transition depopulates the first excited state of ⁹⁸Zr is presented.     

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.     

The emission of Long-Range α-particles in the thermal neurtron induced fission of233U,235U,and239Pu

The yields of the long-range α-particles (LRA) in the thermal neutron induced fission 0f²³³U,²³⁵U, and²³⁹Pu have been determined relative to the corresponding binary fiassion yield. The measurements were performed with surface harrier detectors on a thermalized reactor beam. We obtained for²³³U,²³⁵U and²³⁹Pu binary-to-LRA ratios the values 485±20 respectively 615±20, 475±20. Some of the discrepancies between the published data were explained and experimental indications for²³⁵U(n, α)- and²³⁹Pu(n, α)-reactions are present. Finally the LRA-yield was correlated with some other fission characteristics.     

Recent status of radiochemical analysis of irradiated trans-uranium targets

We have developed a sequential radiochemical separation method (SRCS) in order to isolate each trans-uranium element (TRU) contained in a TRU target (or fuel) irradiated in the experimental fast reactor JOYO. The chemical separation procedures for SRCS consist of the following steps: