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Investigation of the Environmental Fate of Tritium in the Atmosphere

Investigation of the Environmental Fate of Tritium in the Atmosphere

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INVESTIGATION OF THE ENVIRONMENTAL FATE OF TRITIUM IN THE ATMOSPHERE<br />

re-evaporation from cont<strong>in</strong>ental water bodies are similar to those occurr<strong>in</strong>g <strong>in</strong> <strong>the</strong> orig<strong>in</strong>al<br />

precipitation, particularly for small water bodies. By comparison, precipitation deposit<strong>in</strong>g<br />

on <strong>the</strong> ocean or on o<strong>the</strong>r deep water bodies is rapidly mixed, and greatly diluted, result<strong>in</strong>g<br />

<strong>in</strong> lower tritium concentrations <strong>in</strong> re-evaporated water vapour compared to <strong>the</strong> levels <strong>in</strong> <strong>the</strong><br />

orig<strong>in</strong>al precipitation.<br />

Concentrations <strong>of</strong> tritium <strong>in</strong> <strong>the</strong> atmosphere are also known to vary across latitudes and<br />

seasons (e.g., Hauglusta<strong>in</strong>e and Ehhalt, 2002). For example, <strong>in</strong> addition to <strong>the</strong> observed<br />

difference <strong>in</strong> cont<strong>in</strong>ental water versus oceanic tritium levels, differences also occur as<br />

dictated by <strong>the</strong> latitud<strong>in</strong>al movement <strong>of</strong> air masses. Specifically, tritium concentrations are<br />

typically higher <strong>in</strong> precipitation orig<strong>in</strong>at<strong>in</strong>g from air masses with trajectories from <strong>the</strong> north<br />

and west, compared to those orig<strong>in</strong>at<strong>in</strong>g from <strong>the</strong> south and east, likely primarily due to<br />

latitud<strong>in</strong>al differences <strong>in</strong> tritium transfer rates from <strong>the</strong> stratosphere (Brown, 1964).<br />

Vapour exchange processes are thought to account for approximately two-thirds <strong>of</strong> <strong>the</strong> tritium<br />

removal <strong>in</strong>to <strong>the</strong> oceans (Erikkson, 1965), and also account for much <strong>of</strong> <strong>the</strong> tritium transfer<br />

to terrestrial soil water. Additional exchange can occur between atmospheric tritium and<br />

precipitation, as dictated by ra<strong>in</strong>fall <strong>in</strong>tensity, as well as <strong>the</strong> size and correspond<strong>in</strong>g surface<br />

area <strong>of</strong> precipitation droplets. Precipitation <strong>the</strong>n transfers tritium to <strong>the</strong> earth’s surface.<br />

In <strong>the</strong> case <strong>of</strong> light ra<strong>in</strong>fall, tritium levels <strong>in</strong> precipitation are thought to be representative<br />

<strong>of</strong> those occurr<strong>in</strong>g at lower heights <strong>in</strong> <strong>the</strong> atmosphere, whereas for moderate to heavy ra<strong>in</strong>s,<br />

exchange at <strong>the</strong> lower levels is considered to be <strong>in</strong>significant (Bol<strong>in</strong>, 1961). As noted by<br />

Sejkora (2006), light, long-duration ra<strong>in</strong>fall events can yield higher tritium concentrations <strong>in</strong><br />

<strong>the</strong> ground water, run<strong>of</strong>f, storm dra<strong>in</strong>s and soils than heavy, short-duration events. This may<br />

be important when consider<strong>in</strong>g <strong>the</strong> <strong>in</strong>fluence <strong>of</strong> severe storm events and <strong>the</strong> potential<br />

<strong>in</strong>fluence <strong>of</strong> climate change on this phenomenon.<br />

<strong>Tritium</strong> concentrations <strong>in</strong> precipitation (as HTO) have been found to <strong>in</strong>crease with length<br />

<strong>of</strong> <strong>the</strong> travel path through <strong>the</strong> air mass. For example, comparisons <strong>of</strong> tritium levels <strong>in</strong><br />

precipitation with meteorological factors (such as type <strong>of</strong> storm, radar height <strong>of</strong> precipitation<br />

formation, ra<strong>in</strong>fall duration and <strong>in</strong>tensity, and <strong>the</strong> type and orig<strong>in</strong> <strong>of</strong> <strong>the</strong> air mass) have<br />

revealed <strong>in</strong>creases <strong>in</strong> precipitation tritium levels as <strong>the</strong> depth <strong>of</strong> <strong>the</strong> air mass be<strong>in</strong>g traversed<br />

by <strong>the</strong> precipitation <strong>in</strong>creases (Brown, 1964).<br />

Related to <strong>the</strong> <strong>in</strong>tensity <strong>of</strong> <strong>the</strong> precipitation, <strong>the</strong> size and surface area <strong>of</strong> <strong>the</strong> ra<strong>in</strong> droplets<br />

can also <strong>in</strong>fluence tritium exchange between water vapour and ra<strong>in</strong> drops dur<strong>in</strong>g <strong>the</strong> process<br />

<strong>of</strong> film diffusion across <strong>the</strong> droplets (Chamberla<strong>in</strong> and Eggleton, 1964). In general, <strong>the</strong><br />

tritium specific activity <strong>of</strong> ra<strong>in</strong> drops that have passed through a plume that is contam<strong>in</strong>ated<br />

with tritium is very dependent upon <strong>the</strong> size <strong>of</strong> <strong>the</strong> droplet, with decreases <strong>in</strong> tritium<br />

concentrations <strong>in</strong> larger ra<strong>in</strong> drops due to <strong>the</strong> smaller surface area-to-volume ratio <strong>of</strong><br />

larger droplets. This essentially leads to relatively greater tritium dilution <strong>in</strong> larger droplets.<br />

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