贫化铀/聚乙烯球壳交替系统中铀-238中子俘获率的测量与分析

为校验次临界能源堆的概念设计,建立了贫化铀/聚乙烯球壳交替系统, 采用活化法测量²³⁸U的中子俘获率. 贫化铀片置于系统内与入射D离子束成90^o的方向上活化 ,用HPGe探测器测量²³⁸U俘获中子衰变产生的²³⁹Np 衰变产生的277.6 keV特征γ射线计数,实验修正了贫铀片对277.6 keV γ射线的自吸收, 得到了交替系统中²³⁸U (n, γ)反应率的径向分布,反应率的相对不确定度为3.5%-3.7%, 并计算得到系统上整个贫铀区中²³⁸U的总中子俘获率为2.24 ± 0.09. 用MCNP5程序在常用ENDF库下进行了模拟计算, ²³⁸U (n, γ)反应率分布计算与实验一般在5%以内符合, 总俘获率在1%以内符合.     

铀氧化物中238U含量的定量研究

准确定量铀氧化物样品中238U的含量对于裂变产额测量等工作具有重要意义,其定量方法的研究对于涉及238U的绝对测量的诸多实验都具有参考价值。利用四川大学2.5 MeV质子静电加速器产生的准单能中子对八氧化三铀样品进行中子活化,用高纯锗探测器测量活化产物的β衰变子体239Np的277.6 keV特征γ射线,利用已知的活化截面,算出样品中238U的质量占比为79.1%,不确定度为6.2%。利用电感耦合等离子体质谱法对样品中238U的含量进行了测量,其质量占比为59.2%。此外,基于EA3000元素分析仪、卡尔费休电位滴定仪和TGA-DSC2同步热分析质谱联用仪,测知样品中不含N元素,含水量在2.2%以下。并利用PIXE方法排除了样品中含有Al元素以上杂质,利用EPBS方法测知样品中U/O原子数比为1:3.6,误差约2%,推知样品中238U质量占比为80%,验证了活化法测得的238U含量。最终测得样品中238U的质量占比为79.1%,不确定度6.2%。对照按U3O8分子式折算的84.5%,考虑到水分含量等,此结果合理。The accurate quantification of 238U in uranium oxides is of great importance for measurements of fission yield. The study for the method of 238U quantification has significance to lots of experiments involving absolute measurement of 238U. The reaction (n, γ) in the triuranium octoxide samples was induced by T(p,n)3He quasi-monoenergetic neutrons provided by the 2.5 MeV proton electrostatic accelerator in Sichuan University. The 277.6 keV characteristic γ ray of 239Np that comes from β-decay of the activation product 239U was detected by a HPGe detector. With the known (n, γ) cross section, the mass percentage of 238U in samples was determined to be 79.1%, with the uncertainty of 6.2%. ICP-MS was also used in the quantification of 238U in samples, its result was 59.2%. Meanwhile, the samples were analyzed by other several methods and the results showed that less than 2.2% H₂O, no nitrogen, and no other impurity elements above Al were contained in the samples. EPBS was used to measure the atomic ratio of U and O and it was found that the mass percentage of 238U in samples was about 80%, verifying the result 79.1% of INAA.     

Excited levels of Pa

The -decay spectrum of ²³⁷Np was measured with a semiconductor spectrometer of 18 keV effective resolution (FWHM). Over 13 new lines were identified. The γ-ray spectrum of ²³⁷Np and ²³³Th from 20 to 1000 keV was studied with high-resolution Ge(Li) and Si(Li) detectors. From these data and previous results, a more complete level scheme of ²³³Pa is constructed.

Nilsson assignments for rotational bands based on levels at 0, 86.6 and 237.7 keV are confirmed. A new band whose lowest member is the level at 170.3 keV is identified and new levels with probable vibrational character are studied.     

SSNTD and radiochemical studies on the transmutation of nuclei using relativistic ions

Extended targets were irradiated for transmutation studies with relativistic heavy ions. For this, a metal core was surrounded by a paraffin moderator. The metal is either copper or lead and it was irradiated with deuterium, alpha, or carbon beams of 1.5 or 3.7 GeV/u at the SYNCHROPHASOTRON, LHE, JINR, Dubna, Russia. During this irradiation copious amounts of secondary neutrons are produced and studied with SSNTD detectors and radiochemical sensors, for example ¹³⁹La (n, γ) ¹⁴⁰La→β⁻. The yield of reaction products allows an estimation of secondary neutron fluxes. The yields of all kinds of reactions produced with deuterium and alpha beams obey to some extent the law of “limiting fragmentation”, i.e. they show little influence on the energy and the kind of incoming particles. However, one observes with 44 GeV ¹²C ions always enhanced nuclear cross-sections induced by secondary particles. This behavior could not be confirmed with theoretical estimations based on the Dubna Cascade Model in its Cascade Evaporation Model version (DCM-CEM). Finally, some results for transmutation studies on ¹²⁷I and Cu will be presented.     

Nuclear track radiography of “Hot” aerosol particles

Nuclear track radiography was applied to identify aerosol “hot” particles which contain elements of nuclear fuel and fallout after Chernobyl NPP accident. For the determination of the content of transuranium elements in radioactive aerosols the measurement of the -activity of “hot” particles by SSNTD was used in this work, as well as radiography of fission fragments formed as a result of the reactions (n,f) and (γ,f) in the irradiation of aerosol filters by thermal neutrons and high energy gamma quanta. The technique allowed the sizes and alpha-activity of “hot” particles to be determined without extracting them from the filter, as well as the determination of the uranium content and its enrichment by ²³⁵U, ²³⁹Pu and ²⁴¹Pu isotopes. Sensitivity of determination of alpha activity by fission method is 5×10⁻⁶ Bq per particle. The software for the system of image analysis was created. It ensured the identification of track clusters on an optical image of the SSNTD surface obtained through a video camera and the determination of size and activity of “hot” particles.     

Methods of high-sensitive analysis of actinides in liquid radioactive waste

A set of methods has been developed to determine actinides in liquid radioactive waste for solving the problems of radiation, nuclear and ecological safety of nuclear reactors. The main method is based on the radiochemical separation of U, Np–Pu, Am–Cm on ion-exchange and extraction columns. An identification of radionuclides and determination of their content are performed using alpha-spectrometry. The microconcentrations of the sum of the main fissile materials ²³⁵U and ²³⁹Pu are determined with plastic track detectors. An independent method of ²³⁸U content determination is the neutron activation analysis. ²⁴¹Am content is possible to be determined by gamma-spectrometry. A chemical composition of macrocomponents is determined by the atomic-absorption spectrophotometry method.     

Investigation of neutron emission from relativistic heavy ion interactions by nuclear tracks

Fast neutrons produced in 44 and 22 GeV ¹²C+Cu interactions have been recorded and analysed with a CR-39 detector stack. The irradiation of the CR-39 stack to fast neutrons was carried out at the accelerator Synchrophasotron, Joint Institute for Nuclear Research, Dubna, Russia. Areal and volume densities of tracks induced by fast neutrons in the CR-39 at different positions and for different etching time have been measured. The neutron production ratio of 44 GeV to 22 GeV ¹²C+Cu interactions has been obtained, which is 2.17 ± 0.30 by areal track density, or 2. 12±0.33 by step etch technique, or 2.03±0.34 by volume track density measurement. These results confirm that the production rate at 44 GeV ¹²C+Cu interactions is more than theoretical estimation.     

Fission of Th and U in the interaction with negative muons

Muon-induced fission of ²³²Th and ²³⁸U was studied, measuring the time correlation between stopping muons, fission events and electrons.

The measured muon lifetimes are τ_μ(²³²Th) = 77.3±0.3 ns and τ_μ(²³⁸U) = 77.1±0.2 ns. After prompt fission the muon was found to be attached predominantly to the heavy fragment with a lifetime for ²³²Th of 132±7 ns and for ²³⁸U of 134±4 ns. The probability for muon conversion was found to be a few percent per fission event.

Indications were found that the muonic shape isomer is populated in ²³⁸U when the nucleus is excited in a radiationless muonic transition.     

Isomerism in Ag and non-yrast levels in Pd and Rh, studied in β decay

The β decay of ⁹⁶Ag (Z=47,N=49) was investigated by measuring positrons, X rays as well as β-delayed protons and γ rays. The γ radiation was studied by means of germanium detectors and a NaI total-absorption spectrometer. Two β-decaying isomers in ⁹⁶Ag were established with half-lives of 4.40(6) and 6.9(6) s and tentative spin–parity assignments of (8⁺) and (2⁺), respectively. For both isomers, the intensities of β transitions to low-lying levels of ⁹⁶Pd (Z=46,N=50) and β-delayed proton decays to levels in ⁹⁵Rh (Z=45,N=50) were measured. Several new ⁹⁶Pd levels were firmly established. The level energies, their γ decays and the Gamow–Teller decay of ⁹⁶Ag are compared to shell-model predictions. A new low-lying level in ⁹⁵Rh was found at 680 keV excitation energy. Through a comparison with low-lying states of N=50 isotones, this level is interpreted as the first excited 7/2⁺ state built on the proton 9/2⁺ ground state. The assignments of further excited states in ⁹⁵Rh are discussed.     

The decay scheme of Ag

The γ-radiations following the decay of ¹¹²Ag have been studied with Ge(Li) detectors. The ¹¹²Ag half-life has been measured as 3.16±0.02 h; twenty gamma radiations ranging in energy from 606.7 keV to 2829.6 keV have been observed.

Gamma-gamma coincidence measurements have been performed with Ge(Li) and NaI(Tl) detectors. A decay scheme consistent with the present data is proposed.     

The nature of 0 excitations in Er

Lifetimes of excited 0⁺ states in ¹⁶⁶Er have been measured with the (n,n′γ) reaction. The first and second excited 0⁺ states have no significant collective enhancements of their decays, and their properties are suggestive of pair-type excitations rather than those of a β vibration or phonon excitation built on the γ vibration. The third excited 0⁺ state at 1934 keV has an enhanced decay to the ground state band with B(E2; 0₄⁺ → 2_gsb⁺) = 8.8 ± 0.9 W.u., consistent with that expected for a β vibration.     

Determination of slow neutron flux and spatial distribution using LR-115 2B detectors and radiochemical sensors and comparison of the results with Monte Carlo simulations

The fluence and spatial distribution of slow neutrons on the surface of a cylindrical paraffin moderator, surrounding a Pu/Be neutron source was measured using LR-115 2B detectors via ¹⁰B(n,)⁷Li reaction and ¹³⁹La radiochemical sensors. The obtained results were compared with Monte Carlo simulation using MCNP-4B2 code.     

Man-made plutonium in environment — possible serious hazard for living species

It is pointed out that, contrary to the situation with natural Rn, the growing concentration of man-made Pu in environment — natural water soil plants and food — can provide the serious danger for all kind of animals and especially for mankind. Really, as it was established recently, element Pu is accumulated in human body during all the life and the dangerous concentration estimated to be 10⁻¹² – 10⁻¹³ grapm Pu per gram of human tissues. Unfortunately up to now there are no simple nonexpensive methods of Pu determination at the level of sensitivity 10⁻¹⁴ – 10¹⁵ g/g which can provide the determination of Pu even in 0.2 g of human tissue. We warn that now the average concentration of Pu in human body is not less than 10⁻¹⁴ g/g and much higher for some “hot” regions in Europe and Asia. We propose to discuss the problem of organizing world net exploration of Pu in environment — similarly to Rn exploration program — and personnel Pu monitoring for inhibitions of Pu damaged regions. Our approach to the problem is based on chemical separation of Pu, on determination of Plutonium by high fission cross section with thermal neutrons ²³⁹Pu(n,f) reaction and by control of possible admixture of ²³⁵U isotope by ²³⁸U(γ, f) reaction in Pu preparations. The problem of increasing of sensitivity of Pu analysis up to 10⁻¹⁴ – 10⁻¹⁵ g/g is discussed in detail.     

Observation of the reaction products formed in the interaction of 3.65 A GeV O ions with thick copper target at wide angles

Experiments have been carried out to study the ‘heavy fragments’ emitted at wide angles in the interaction of 3.65 A GeV ¹⁶O ions with a thick Cu target, using a stack of CR-39 track detectors. Diametric distribution in a stack registering ¹⁶O-beam halo are compared with diameters observed in a stack placed downstream at an angle of 25°. There is a strong indication that the heavy fragments are scattered at large angles.     

Reaction filters. Charged-particle multiplicity and linear momentum transfer

The relation between charged-particle multiplicity and linear momentum transfer to heavy reaction residues has been investigated with a 4π charged-particle detector for the reactions ³⁶Ar+²³⁸U at E/A=35 MeV and ¹⁴N+²³⁸U at E/A=50 MeV. The multiplicity of charged particles at backward angles (θ > 35°) incrreases linear momentum transfer while the multiplicity of charged particles in the forward direction is almost independent of the linear momentum transfer.     

Decay of the 55 min and 12 min Te isomers

Gamma rays emitted in the decay of the ¹³³Te isomers, 55.4 min ^133mTe and 12.5 min ^133gTe, have been observed with Ge(Li) detectors. Sources were prepared by separating Sb from fission products, allowing several minutes for decay of 2.7 min ¹³³Sb and then separating the Te daughter activities. A total of 29 γ-rays between 312 and 2541 keV were attributed to decay of ^133gTe and 30 from 74 to 2050 keV to that of ^133mTe. Gamma-gamma coincidences in the decay of ^133gTe were observed with a NaI(Tl)---Ge(Li) set-up. The decay scheme of ^133gTe was constructed, involving placement of 25 of the γ-rays emitted. The decay of ^133gTe populates levels in ¹³³I at 0, 312, 720, 787, 1313, 1333, 1374, 1565, 1718, 2137, 2194 and 2541 keV. The decay of ^133mTe is very complicated, and we have not attempted construction of a complete decay scheme for it; however, levels at 913 and 1561 keV in ¹³³I are definitely populated in ^133mTe decay. The value for Q_β of ¹³³Te was measured as 3.52±0.10 MeV. The low-lying levels of the odd-mass iodine isotopes vary smoothly through the series ¹²⁵I through ¹³³I. The levels of ¹³³I are fitted rather well by predictions based on quasi-particle-phonon coupling.     

On the interpretation of rotational bands in odd actinide nuclei

While the cranked quasiparticle model gives too large alignment of angular momentum for the ground state bands of ²³⁵U and ²³⁷Np, the empirical alignments are well reproduced in a quasiparticle plus rotor model with a rotation dependent interaction between core and quasiparticle. This model also gives better agreement with the data than a cranked quasiparticle model with Coriolis attenuation.     

Search for projectile fragments with fractional charge in relativistic heavy ion collisions

We measured the charge of about 35 000 projectile fragments with Z5e produced by 14.5 GeV/nucleon and 200 GeV/nucleon ¹⁶O beams in a Pb target using CR39 plastic nuclear track detectors. A minimum track length of 3 mm in the detector without nuclear interaction was required. No evidence for fragments carrying a fractional charge was found.     

Ranges of 0.2-1.0 GeV/nucleon heavy ions in nuclear photoemulsion

Heavy nuclei transport in matter are studied experimentally and theoretically. Our experimental range and straggling values of 0.2 – 1.0 GeV/nucleon ²⁰Ne, ⁴⁰Ar, ⁵⁶Fe, ¹⁹⁷Au and ²³⁸U nuclei in BR-2 nuclear photoemulsion are presented and compared with model calculations carried out according to our RANGE-program and the PRAL-model (version of 1987) developed by Ziegler et al. The presented data analysis points at the necessity to take into account Z³-correction in Bete-Bloch formula when ionization losses of very heavy multicharge ions (for example ¹⁹⁷Au and ²³⁸U) are calculated. The comparison of experimental and calculated results showed that RANGE program can correctly calculate the ranges and straggling of heavy ions. The difference between experimental and theoretical data do not exceed 5% in all of the cases examined. PRAL model describes the heavy ion ranges quite adequately, but overestimates the particle range straggling.     

Mesonic and non-mesonic decay widths of ΛC

Results are reported on the precise measurement of the lifetime and the weak-decay branching ratios with charged particle(π⁻ and proton) emission from _Λ¹²C formed via ¹²C(π⁺,K⁺) reaction. The π⁻ mesonic decay width is consistent with the calculations including the pion wave function distortion effect. We observed large contribution of the neutron-stimulated decay widths, Γ(Λ + n → n + n), in the non-mesonic weak decay, which cannot be explained by the current theoretical calculations.