H. C. Jain

Determination of isotopic composition of boron

Investigations were carried out on the determination of isotopic composition of boron using Cs2BO2+ ion and thermal ionisation mass spectrometry. The results show distinct advantage over the normally used Na2BO2+ ion.

A comparative study of different methods of preparation of sources for alpha spectrometry of plutonium

Abstract A comparative study of different methods of preparation of sources for alpha spectrometry of plutonium is presented. Typical values of the percentage tail contribution per unit alpha activity ratio 238 Pu /( 239 Pu + 240 Pu ) , fwhm and peak to valley ratios are given for (1) drop deposited sources from aqueous medium without using a spreading agent, (2) drop deposited sources from aqueous medium by using tetraethylene glycol (TEG) as a spreading agent, (3) drop deposited sources from organic medium using TTA extraction and (4) electrodeposited sources. Results obtained on the determination of 238 Pu /( 239 Pu + 240 Pu ) alpha activity ratios in isotopic reference material SRM-947 and in a synthetic mixture of plutonium isotopes using an AuSi surface barrier detector for recording alpha spectra and geometric progression (GP) method for the evaluation of alpha spectra are presented. It is seen that preparation of drop deposited sources from TTA involves minimum effort and the quality of alpha spectra from these sources is comparable to those from the electrodeposited sources. Further, it is recommended that the uncertainty on 238Pu in SRM-947 can be considered as 0.8% (3σ) compared to 2% quoted by the National Bureau of Standards.

Determination of the half-lives of transactinium isotopes by relative activity method

Relative activity method offers the potentiality of providing half-life values over a wide range in a short time for different α-emitting transactinium isotopes. The method involves the preparation of a synthetic mixture using another isotope of the same element followed by the determination of atom ratio and α-activity ratio by thermal ionization mass spectrometry and α-spectrometry, respectively. A double dilution technique is described which helps in maintaining the atom ratios as well as α-activity ratios close to unity so that these could be determined with high precision and accuracy. Results obtained on the half-lives of232U,238Pu,242Pu and243Am using double dilution technique in relative activity method are summarized. Requirements, advantages and applications of this technique for determining the half-lives of other transactinium isotopes are presented.

Determination of K-factors for isotope abundance measurements of uranium and plutonium by thermal ionisation mass spectrometry

K-factors (= certified isotope ratio/observed isotope ratio) are determined for the isotope abundance measurements of uranium and plutonium by thermal ionisation mass spectrometry. An mdf of 0.07% and 0.18% per mass unit differing by a factor of about 3, is obtained for uranium and plutonium, respectively, employing double rhenium filament assembly in the ion source and Faraday cup as the detector using the presently available isotopic reference materials of uranium and plutonium.

Precision and accuracy in the determination of plutionium-239 /uranium-233, americium-241/ uranium-233 and curium-244 /uranium-233 alpha activity ratios by alpha spectrometry

Determination of239Pu/233U,241Am/233U and244Cm/233U alpha activity ratios is required when using233U as a tracer for the determination of plutonium, americium and curium by alpha spectrometry. Precision and accuracy in the determination of these alpha activity ratios was evaluated by preparing synthetic mixtures from solutions of enriched isotopes of239Pu,241Am,244Cm and233U. Separate synthetic mixtures were prepared for each of the three alpha activity ratios. The sources from the synthetic mixtures were prepared by direct evaporation method using tetra ethylene glycol /TEG/ as a spreading agent, alpha spectra were recorded by employing solid state silicon surface barrier detectors coupled to a 4 K analyzer and the alpha spectra were evaluated by a method based on the geometric progression decrease for the far tail of the spectrum. Large area detector /i.e. 450 mm2/ was observed to reduce the effect of nonhomogeneous distribution, if any, of the two elements present in the source. Precision and accuracy of about 1% is demonstrated for the determination of239Pu/233U,241Am/233U and244Cm/233U alpha activity ratios using large area silicon surface barrier detector.

Alpha spectrum evaluation method for the simultaneous determination of plutonium, americium and curium

A method based on the geometric progression decrease of the counts in the far tail of the alpha spectrum is described for the simultaneous determination of plutonium, americium and curium by alpha spectrometry. For evaluating the precision and accuracy, synthetic mixtures were prepared from solutions of enriched isotopes and sources were prepared by direct evaporation method using tetraethylene glycol /TEG/ as a spreading agent and electropolished stainless steel discs as the backing material. Precision and accuracy of about 1% is demonstrated in the determination of244Cm/239Pu,241Am/239Pu,244Cm/233U,241Am/233U and239Pu/233U alpha activity ratios using a 450 mm2 silicon surface barrier detector.

Determination of the plutonium concentration by isotope dilution mass spectrometry using239Pu as a spike

A method is described for the determination of plutonium concentration in the presence of a bulk of other impurities by isotope dilution mass spectrometry /IDMS/ using239Pu as a spike. The method involves the addition of239Pu spike /≥ 90 atom%/ to samples with239Pu /≤ 70 atom%/ and vice versa. After ensuring chemical exchange between the sample and the spike isotopes, plutonium is purified by conventional anion exchange procedure in 7M HNO3 medium.239Pu/240Pu atom ratio in the purified spiked sample is determined with high precision /better than 0.1%/ using a thermal ionization mass spectrometer. Concentration of plutonium in the sample is calculated from the changes in239Pu/240Pu atom ratio in the spiked mixture. Results obtained on different plutonium samples using239Pu as a spike are compared with those obtained by the use of242Pu spike. Precision and accuracy comparable to those achieved by using242Pu are demonstrated. The method provides an alternative in the event of non-availability of enriched242Pu or244Pu required in IDMS of plutonium and at the same time, offers certain advantages over the use of242Pu or244Pu spike.

A gamma-spectrometric method for the determination of plutonium isotope ratios

A gamma-spectrometric method using an intrinsic high resolution germanium detector has been developed for the determination of isotope ratios of plutonium from samples in solution form. The method is based on the assay of low energy gamma-rays of238Pu,239Pu,240Pu and241Pu and does not require the use of branching intensities or the knowledge of detection efficiencies for different gamma rays. Since low energy gamma-rays are used, the effect of241Am has also been studied. It is found that results are not affected up to 0.5 wt% of241Am in plutonium samples. An accuracy of 3% is achievable in the determination of240Pu/239Pu and241Pu/239Pu atom ratios as demonstrated by carrying out measurements on isotopic standards of plutonium.

Determination of alpha activity ratios by alpha spectrometry in the presence of large amounts of uranium

A direct evaporation method is described for the preparation of sources using stainless steel as the backing material and tetraethylene glycol (TEG) as a spreading agent in the presence of large amounts of uranium. It is shown that FWHM and tail contribution at the low energy peak due to energy degradation of the high energy peak can be optimized by heating the source under controlled conditions in a furnace at 500–600°C for about 15 min. An accuracy of 0.5–1% is demonstrated for the determination of238Pu/(239Pu+240Pu) alpha activity ratio in the U/Pu range of 10 to 1500 generally encountered in dissolver solution of irradiated fuel.