FISSION PRODUCTS IN THE ATMOSPHERE AND RAIN 605 This excess was then determined by titrating with a standard KMnO, solution. A blank experiment was also performed. The chemicalyield of manganese was usually between 25 and 50%. RESULTS AND DISCUSSIONS Isotopic Ratios in Rain Figure 1 shows the variation of the concentration of *°Sr in individual rains as well as in the bimonthly average concentrations. The data show a marked seasonal variation. Figure 2 shows the variation of the ‘°Ba/sr and ‘Ba/®sr ratios in rain since November 1961. Owing to the short half-life of 40Ba, these ratios are sensitive to the injection of fresh nuclear debris. During a test moratorium period, the isotope ratios decay linearly on a semilog scale, as can be seen in the figure, The response of the 40Ba/%Sr ratio to the late December nuclear explosions appears to have been delayed almost two months, and the “°Ba/*Sr ratios in rain reached the straight line ab in Fig. 2 only after March 1964, A very similar trend is seen in the °Ba/®%Sr ratio data. The straight line cd has a slope corresponding to the difference between the decay of '*°Ba and ®%sr, The observed data may be explained as being due to the fact that some of the nuclear explosions that occurred in the late fall of 1962 were high-altitude shots, and hence the debris did not reach the lower atmosphere immediately, Figure 3 shows the ®Sr/%Sr ratios in rain. Data obtained at Lemont, Ill.,° and at Milford Haven, England,® are also plotted, Accu- rate measurement of the ®%Sr/Sr in nuclear debris is tedious and difficult. The radiochemical techniques involved in the determination of the "sr/*sr ratio in nuclear debris have recently been thoroughly reinvestigated by Hodges,’ and, as a result of improvementin technique, the recent data are probably more accurate than old data, A rather large scatter of the experimental points seen in the data prior to 1962 might be at least partly due to experimental errors. The straight line ab in Fig. 3 has a slope corresponding to the 50.4-day half-life of **Sr. The **Sr/Sr ratios in rain after the Decem- ber 1962 nuclear explosions approached the straight line ab asymptotically and joined it at the end of April. By a comparison of this trend with those observed in the cases of the “°Ba/*Sr and the “°Ba/**Sr ratio data, shown in Fig, 2, an impression is obtained that the response of the ®*Sr/%Sr ratios to the late December 1962 nuclear explosions were somewhat slower than those of the “°Ba/Sr and the “°Ba/®%Sr ratios.

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