用于加速器质谱测量的长寿命核素182Hf标准样品的制备

介绍了用于加速器质谱(AMS)测量的182Hf标准样品的研制过程.主要包括四个步骤:1、放射性核素的人工合成;2、同位素比值的准确测定;3、标准样品的稀释;4、AMS测量样品HfF4的制备.目前,合成标样的起始同位素比182Hf/180Hf的TIMS测定结果为(2.33±.07)×10-6,并研制出了一系列标准样品,182Hf/180f的比值从10-6到10-13,并且给出了不同比值标准样品的不确定度.     

3 MV加速器质谱测量36Cl

在端电压为3 MV的AMS装置上实现³⁶Cl及其他中重核素的高灵敏测量是AMS技术发展的重要方向之一。为进一步提高充气飞行时间探测方法中³⁶S的压低能力,本文研究了³⁶S和³⁶Cl在P10、异丁烷和丙烷气体中的能量歧离和角度歧离。在32 MeV的入射能量下测量了几个地下水样品中³⁶Cl的[JP2]含量,测量结果与72 MeV能量下的测量结果相符。测量结果表明,采用充气飞行时间探测方法在3 MV的串列加速器上测量³⁶Cl时,探测限为³⁶Cl/Cl≈10^-14,当样品中³⁶Cl/Cl≈10^-13时测量不确定度为30%。     

95Zr-95Nb活度比确定核事件零时

裂变产物活度比可确定核事件的零时。本文系统研究了通过测量⁹⁵Zr-⁹⁵Nb活度比计算核事件零时的方法。研究表明,⁹⁵Nb^m分支对零时计算影响较小, ⁹⁵Zr-⁹⁵Nb活度比可准确计算核事件零时。在零时后100 d内测量样品,零时计算结果与参考值在1 d内符合;零时后1 a内测量样品,计算的零时与参考值相差小于10 d。零时不确定度随样品开测时刻至零时的时间间隔的增加迅速增加,不确定度区间是不对称的,不确定度正值大于不确定度负值,当⁹⁵Zr-⁹⁵Nb接近平衡时,零时的不确定度正值趋向于无穷大。     

用0.5 MV端电压的串列AMS装置开展10Be测量方法研究

本文通过对¹⁰Be离子在加速器质谱计（CAMS）高能端束流传输进行模拟计算,确定了¹⁰Be离子束流传输的优化设计。设计安装了测量⁹Be束流的法拉第筒、能量吸收膜（SiN膜）装置、ΔE-E_res气体探测器等,结果表明,改进后的CAMS可进行¹⁰Be测量,¹⁰Be测量总传输效率约为2%,测量本底约为4×10^-14。     

加速器质谱法测量含铀微粒中铀同位素比的方法研究

准确测定含铀微粒同位素比在核保障中有重要的应用价值。本文采用将含铀微粒溶解并加入高纯Fe粉烘干的方法制样,采用中国原子能科学研究院的HI-13串列加速器质谱测量靶样中的同位素比。通过对CRM铀系列同位素标准样品的分析表明,该方法可测定高于10^-5的²³⁶U/²³⁸U同位素比;对于²³⁵U/²³⁸U同位素比在10^-4～10^-1范围内的含铀微粒,²³⁵U/²³⁸U同位素比相对扩展不确定度均小于10%。     

加速器质谱测量岩石样品中41Ca的初步研

⁴¹Ca在核天体物理及地质年代学方面可能具有较高的应用价值。为测量天然岩石样品中⁴¹Ca的本底水平,探讨了⁴¹Ca-AMS测量中岩石样品的CaF₂制备,提出了二次氟化的制备方法。在此基础上,通过对导电介质与靶锥的改进,设计了一种提高CaF^-₃束流引出强度的方案。该方案可有效提高CaF^-₃束流引出强度。实验结果表明,天然岩石样品中⁴¹Ca/⁴⁰Ca（⁴¹Ca、⁴⁰Ca原子个数比）的本底水平低于8×10^-14。     

加速器质谱测量^182Hf等长寿命重核素标准样品的制备

通过对长寿命重核素^182Hf、^151Sm等的测量可以确定某些场合的中子注量，能够确定长寿命放射性核素的迁移行为，对核废物安全处置研究具有重要意义。加速器质谱(AMS)技术是实现^182Hf、^151Sm等高灵敏测量的有效方法(测量灵敏度可达到10^-15)，但AMS测量是一种与标准样品比对的相对测量，市场上无所需标样，需自行制备。     

AMS-14C样品制备系统的研制及其性能研究

为了开展加速器质谱仪（accelerator mass spectrometry, AMS）在¹⁴C测量方面的研究,研制了可采用锌法、氢法、氢化钛法制备¹⁴C样品的装置,该制样系统以石英玻璃为主要结构材料,分为以下三个单元：系统真空维护单元、CO₂纯化单元和CO₂还原单元。为验证此装置的可靠性,进行了系列 ¹⁴C样品的制备实验,得到的石墨产率基本达到80%,同时对商业碳粉、树木的含碳量与实验过程中测量区域对应的CO₂量进行了线性拟合,结果呈现明显的线性关系。对一批标准样品和本底样品进行AMS测试,结果显示每个样品¹²C^-的引出束流均大于20 μA,系列空白样品的测量结果表明,¹⁴C/¹²C丰度比平均值为1.061×10^-15,样品制备系统稳定且在制样过程中引入的碳污染较小,符合制样要求,现代木头样品的AMS绝对测量值为（9.13±0.05)×10^-13,与预期值~9.0×10^-13相符合。上述结果表明,该系统结构紧凑,能避免相互污染,高效且便于操作,满足AMS对¹⁴C样品的测试要求。     

240Am半衰期的测量

²⁴⁰Am的半衰期对准确测量²⁴¹Am(n,2n)²⁴⁰Am反应截面具有重要作用,当前评价的数据50.8(3) h是对²⁴⁰Am的987.8 keV γ射线用Ge(Li)探测器跟踪测量6 d的结果,测量时间不到3个半衰期,使得测量结果的不确定度偏大。本文利用Geant4模拟软件建立了阱型HPGe探测器的测量模型,模拟计算了不同Pb吸收厚度下²⁴⁰Am高能γ射线的探测效率,确定使用阱型HPGe探测器配合吸收X射线和低能γ射线的Pb吸收体可有效提高²⁴⁰Am高能γ射线的探测效率。根据Geant4模拟计算的结果,Pb吸收体厚度为1 mm时,对²⁴⁰Am的888.8 keV和987.8 keV两条特征γ射线的探测效率分别为14.1%和13.3%。在中国原子能科学研究院的HI-13串列加速器上通过²⁴²Pu(p,3n)反应生产了²⁴⁰Am,制备了约700 Bq的²⁴⁰Am测量源,用上述方法跟踪测量²⁴⁰Am的888.8 keV和987.8 keV两条特征γ射线的强度,时间超过18 d,用最小二乘法拟合得到其半衰期为50.79(5) h,结果与评价结果一致,但减小了不确定度。     

用于C6D6测量系统的高精度权重函数计算方法研究

本文基于中国散裂中子源(CSNS)反角白光中子束线(Back-n)的C₆D₆测量系统,以重要核素²⁰⁹Bi为研究对象,利用蒙特卡罗方法研究了样品厚度对权重函数求取精度的影响,并发展了求解C₆D₆探测器的点态权重函数技术。研究结果表明,目前Back-n上的C₆D₆测量系统权重函数的系统不确定度会随实验样品厚度的增加而迅速增加,而本工作得到的点态权重函数的系统不确定度在样品厚度增大到6 mm时仍小于0.5%,有利于提高厚样品实验数据的精度。本工作为将来在Back-n上开展如²⁰⁹Bi等高原子序数、小截面核素的中子辐射俘获截面的实验测量奠定了技术基础。     

加速器质谱测量用HfF_4的固相合成研究

HfO2样品通过分离纯化流程后,与NH4HF2进行固相反应制成HfF4,并用加速器质谱进行测量。结果表明:α-安息香肟萃取是降低182W含量的重要步骤;固相合成法制备的HfF4样品中180HfF5-的引出束流强度是同等条件下液相合成法的3-4倍;制样方法(固相合成法、液相合成法)对182W/Hf值影响不大;HfF4中182W/Hf值低至10-11g·g-1量级。     

Excitation functions for some W, Ta and Hf radionuclides obtained by deuteron irradiation of Ta up to 40 MeV

Experimental excitation functions for deuteron induced reactions up to 40 MeV on mono-isotopic Ta (¹⁸¹Ta) were measured with the activation method using a stacked foil irradiation technique. From high resolution gamma spectrometry and X-ray analysis cross-section data for the production of ¹⁸¹W, ^{177,178g,180g,182m+g}Ta, and ^179m2,180mHf were determined. Comparison with the scarce earlier published data are presented and results for values predicted by different theoretical codes, adapted for more reliable calculations for d-induced reactions, are included. Thick target yields for ^{182m+g,180g,178g}Ta and ¹⁸¹W were calculated from a fit to our experimental excitation curves. Using dose conversion factors and irradiation scenarios, possible occupational doses to maintenance or scientific personnel around high power accelerators where Ta based structural elements (collimators, beam stoppers, shielding) are present could be derived.     

Determination of the Be half-life by multicollector ICP-MS and liquid scintillation counting

A new method was designed and used for determining the half-life of the isotope ¹⁰Be. The method is based on (1) accurate ¹⁰Be/⁹Be measurements of ⁹Be-spiked solutions of a ¹⁰Be-rich master solution using multicollector ICP mass spectrometry (MC-ICP-MS) and (2) liquid scintillation counting (LSC) using the CIEMAT/NIST method for determining the activity concentrations of the solutions whose ¹⁰Be concentrations were determined by mass spectrometry. Important requirements for the success of this approach (a) was the previous coating of glass ampoules filled for counting experiments with ⁹Be, thereby reducing the risk of the adsorptive loss of ¹⁰Be; (b) the removal of Boron from solutions to be measured by MC-ICP-MS by cation chromatography without the introduction of mass fractionation and (c) the accurate determination of the mass bias of ¹⁰Be/⁹Be measurements by ICP-MS which are always affected by the space-charge effect. The mass bias factor was determined to be 1.1862 ± 0.071 for ¹⁰Be/⁹Be from careful fitting and error propagation of ratios of measured Li, B, Si, Cr, Fe, Cu, Sr, Nd, Hf, Tl and U standard solutions of known composition under the same measurement conditions. Employing this factor, an absolute ¹⁰Be/⁹Be ratio of 1.464 ± 0.014 was determined for a first dilution of the ¹⁰Be-rich master solution. This solution is now available as an absolute Be ratio standard in AMS measurements. Finally, a half-life of (1.386 ± 0.016) My (standard uncertainty) was calculated. This value is much more precise than previous estimates and was derived from a fully independent set of experiments. In a parallel, fully independent study using the same master solution, Korschinek et al. [35] have determined a half-life of (1.388 ± 0.018) My. The combined half-life and uncertainty amounts to (1.387 ± 0.012) My. We suggest the use of this value in nuclear studies and in studies that make use of cosmogenic ¹⁰Be in environmental and geologic samples.     

Nuclear Data Sheets for A=182

Nuclear spectroscopic information for known nuclides of mass number 182 (Lu,Hf,Ta,W,Re,Os,Ir,Pt,Au,Hg, Tl,Pb) with Z=71 to 82 and N=111 to 100 have been evaluated and presented together with adopted energies and Jπ of levels in these nuclei. No excited state data are yet available for ¹⁸²Lu, while only limited structure information is available for ¹⁸²Pb and ¹⁸²Tl. Rotational band structures are known for ¹⁸²Hg and ¹⁸²Au but spin-parity assignments remain largely tentative. The decays of ¹⁸²Lu, ¹⁸²Hg, ¹⁸²Au and ¹⁸²Tl are not well established. The ¹⁸²Hf isotope is of geophysical and astrophysical interest. This evaluation supersedes previous full evaluations of A=182 published by 1988Fi05 and 1975Sc13, and a selected (mainly high-spin) update of A=182 published by 1995Si04.     

Si AMS measurement with ΔE-Q3D method

Accelerator mass spectrometry (AMS) is one of the most promising methods for the measurement of trace amount of ³²Si for its advantages of small sample size, short measurement time and extremely high sensitivity. However, the isobaric interference from ³²S often badly hinders the AMS measurement of ³²Si. The ΔE-Q3D detection technique established in this work brought about an overall suppression factor of larger than 10¹² for ³²S. As a result, a sensitivity of better than 1 × 10⁻¹⁴ (³²Si/Si) has been achieved, based on the measurement of a blank sample.     

Nuclear data sheets for A = 180

The 1965 version of the Nuclear Data Sheets has been revised according to experimental data received prior to May 1974, including approximately 120 papers.Data are presented for nine nuclei (Lu, Hf, Ta, W, Re, Os, Ir, Pt, and Hg). Only alpha decay data are available for Hg and Pt. No excited states or gamma transitions are definitely assigned to Lu or Ir. A tentative decay scheme for Ir is presented. The decay schemes for Lu(5.7 m), Ta (>10¹³ y and 8.1 h), and Re(2.43 m) are well established. The Os(22-m) decay scheme is still rather uncertain because of a lack of precision gamma-ray energies and intensities.The Hf level scheme includes 46 levels (23 J^π-values), although only the ground-state rotational band has been established. Branching ratios for ¹⁷⁹Hf(n,γ), ^180mHf(5.5-h) decay, and ¹⁸⁰Lu(5.7-m) decay have been compared, and several disagreements are noted. The W level scheme includes 32 levels (16 J^π-values) with three proposed rotational bands, although several assignments are not well established. The Re level scheme includes 10 levels (3 J^π-values), all due to Os decay. The Os level scheme includes 10 levels with J^π-values available only for the ground-state band.The most important deficiency in the data is that very few charged-particle reaction data are available except for (d,p) to Hf and (p,t) to W. Suggested reactions are:     

A sensitive method for Sr-90 analysis by accelerator mass spectrometry

ABSTRACT

Strontium-90 is one of the most important fission products due to the potential health risks of its uptake and retention in the human body. Conventional analysis techniques involve β counting, which requires ingrowth of ⁹⁰Y over a period of two weeks. Accelerator mass spectrometry (AMS) has the potential to shorten the analysis time while offering a lower limit of detection than β counting. Here, Sr in samples was recovered as SrF₂ to provide sufficient negative ions in the caesium-sputtering ion source. In the sample preparation step, 95–98% of Sr was recovered and 99–100% of Zr removed by ion-exchange separation. Sr recovery was ~30% in the precipitation process, and this can be improved. A maximum 500 nA beam current of SrF₃ ^– ions was obtained from SrF₂ samples mixed with PbF₂. A five-anode gas ionization detector was used to avoid isobaric interference from ⁹⁰Zr. The ⁹⁰Sr/Sr atomic ratio background of ~6 × 10^–13 (~3 mBq ⁹⁰Sr) was comparable with that achieved at other AMS facilities. Good linearity in ⁹⁰Sr/Sr atomic ratios was obtained from 1.75 × 10^–10 to 3.38 × 10^–9. Suitable techniques for sample preparation and measurement were thus achieved for ⁹⁰Sr analysis by AMS.     

U measurement with accelerator mass spectrometry at CIAE

²³⁶U is a long-lived radioactive isotope which is produced principally by thermal neutron capture on ²³⁵U. ²³⁶U may be potentially applied in geological research and nuclear safeguards. Accelerator mass spectrometry is presently the most sensitive technique for the measurement of ²³⁶U and a measurement method for long-lived heavy ion ²³⁶U has been developed. The set-up uses a dedicated injector and the newly proposed ²⁰⁸Pb¹⁶ molecular ions for the simulation of ²³⁶U ion transport. A sensitivity of lower than 10⁻¹⁰ has been achieved for the isotopic ratio ²³⁶U/²³⁸U in present work.