146 HAINES AND MUSGRAVE Recent results of Begemann® show that the T/H ratio in the northern-hemisphere methane has been essentially constant from 1958 to 1963; during this time the tritium content of atmospheric hydrogen increased by a factor of 2 to 4. This observation makes it seem most probable that the tritiated methane was of synthetic origin and not due to the incorporation of HT into methane in the atmosphere. A final determination of the source of tritium in methane may not be possible; it will be apparent, however, that there are sufficient sources in the nuclear industry to account for the increase in the T/H ‘yatio in atmospheric hydrogen prior to 1952 and that these same sources were releasing tritiated methane during this period, Although the methane and the HT may be from a common or a Similar source, there is no particular significance to be given to an apparent exponential T/H increase in methane or hydrogen in the northern hemisphere. CAUSE OF THE T/H INCREASE IN ATMOSPHERIC HYDROGEN PRIOR TO 1952 Fairly detailed information is available from the tritium produc- tion techniques employed at Los Alamos Scientific Laboratory.'* The system involved a thermal-diffusion column that included seven massspectrometer leaks for controlling the feed and for withdrawing tritium from the column. The combined leak total was about 10 ml of tritium per day, mostly as T,. The depleted tritium was reprocessed, with the depleted fraction from the second cycle being exhausted into the atmosphere. At the minimum estimated rate of operation of the system, the reprocessing released another 10 mi of tritium per day. It is stated that the final stripped product was “vented with safety.” It can be as- sumed that the vacuum systems connected to the mass spectrometers and those used for final sample storage were vented in a like manner. The rate of tritium release estimated for this thermal-diffusion column fits the increase in the T/H ratio reported for hydrogen be- tween 1949 and 1952. Examining this rate of release from a different approach, we can estimate the minimum amount of tritium that even- tually must have been released by the time of the 1954 Operation Castle test series. For the production system to release the amount of tritium that was estimated to have been released by the Ivy and Castle tests, the minimum amount released should have been 9 to 12 g. This corre- sponds to a T/H ratio of approximately 0.2 to 0.3 x 10° tritium units (T.U.) as of 1954. The amount released may have been as high as 22 g; this would give a T/H ratio of 0.5 10° T.U. for the 1954 level. The values measured® were in the range of 0.4 to 1.2 x 10° T.U. for 1954 and 1955. The highest of these values was from a sample taken before the Castle test series.

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