The purposes of this study are to understand and compare: the distributions of the particulate and dissolved 210Po and 210Pb in the northern South China Sea and in the east and west sides of the Luzon Strait; the associated biogeochemical processes, including their mechanisms and rates involved in the area; and the disequilibrium between 226Ra and the 210Pb as observed in profiles. Seawater samples were collected from three stations in the northern South China Sea (station I, J, and F) and one station to the east of the Luzon Strait (station S5) using a Rosette sampling system during three Ocean Researcher I cruises (ORI-688 in July, 2003, ORI-707 in February, 2004, and ORI-734 in October, 2004). The dissolved 210Pb in surface water generally displays higher activities (around 14-28 dpm/100kg) relative to deep water, reflecting atmospheric input. The dissolved 210Pb profile as seen at station F displays a maximum of 26 dpm/100kg at 200 m and lower values at about 10 dpm/100kg below 1500 m. Highest value at 28 dpm/100kg was observed at S5 surface water. It is probably due to being on the path of the Kuroshio which has accumulated atmospheric 210Pb continually from the northern Equatorial Current on its way. The mean residence time with respect to particle scavenging is about 0.62 years for total 210Po within a 50 m mixed layer, and ranges between 0.34 to 1.13 years for total 210Pb in the mixed layer. 210Po is deficient relative to 210Pb in most profiles, suggesting that 210Po is more readily scavenged. The mean scavenging residence time is about 87 years for total 210Pb in the deep water at station F, and 60 years at station J. This residence time is longer than that in both the Pacific and East China Sea deep waters, i.e. a lower scavenging rate in the South China Sea. As the upwelling rate is much higher in the South China Sea than in the Pacific, it may effectively reduce the sinking rate of the sinking particulates, resulting in higher 210Pb residence time in the water columns of the South China Sea.

Po-210 and Pb-210 are particle-reactive natural radionuclides which can be removed from seawater by their incorporation with various particulate materials, resulting in radioactive disequilibria with respect to their parent nuclides. Previous studies showed that Po-210/Pb-210 activity ratio in surface seawater ranges from about 0.2 to 1 due to atmospheric input of Pb-210 and effects of biological productivity and upwelling. In order to evaluate the effects of plankton on Po-210 and Pb-210 distributions, plankton samples were collected by surface-trawling of plankton net in Taiwanese water. These plankton samples were analyzed for Po-210 and Pb-210 in order to obtain their concentrations and activity ratio, which may indicate the enrichment or discrimination of these nuclides in the marine planktonic phase around Taiwan. The results show that the Po-210/Pb-210 activity ratio of planktonic samples ranges from 23.06 to 51.40 in northeastern Taiwan, whereas the activity ratio in southwest Taiwan varies within and outside of the sampleing locations: stations 1, 2, 3 and 4 yield range of 10.72-43.90, 16.40-47.87, 13.86-23.37 and 9.35-13.82, respectively. Two marine algae (Sargassum polycystum C.Agardh and Hypnea charoides Lamouroux) yield values of 2.24-8.57, and 3.72-5.96, respectively. These Po-210/Pb-210 activity ratios are much greater than unity, and their activities comparison to those of inorganic particulates support the contention that the plankton preferentially incorporates Po-210 but discriminates against Pb-210. However, the mechanism or process of Po-210 to be incorporated in the plankton remains unclear. In comparison of the activities between Po-210 and Pb-210 in organic particulates, one finds that Po-210 is effectively enriched while Pb-210 is clearly discriminatied by the organic particulates. These results are consistent with those reported in literatures.

Pb-210 and Po-210, a parent-daughter pair, are particle-reactive radionuclides. Pb-210 tends to be associated with inorganic particles but Po-210 prefers organic particles. In the context of these characteristics the purpose of this study is to determine Po-210 and Pb-210 in the surface water plankton of the northern South China Sea (SCS) and the Luzon Strait (LS) areas in order to understand their temporal and spatial distributions and the extent of their radioactive disequilibrium. As the LS has provided a pathway for the exchange between the Kuroshio and the SCS waters, the study area has the characteristics of an open ocean and a marginal sea. The plankton Po-210 activities in the study area are about 10~400 dpm/g, but may reach 1200dpm/g in an El Nino year, the effect of which on Po-210 is not clear at present. The Po-210 in the plankton is mainly affected by the surface water Po-210 , biomass concentration, and the Po-210 in the surface water as well as plankton transported from other area(s). If the biomass concentration (as indicated by Chlorophyll-a) increases, the Po-210 in the plankton decreases, i.e. they are inversely correlated. Based on the planktonic Po-210 distribution, the Kuroshio water which has both high Po-210 and high Po-210-bearing plankton has evidently intruded into the northern SCS. The Pb-210 activities of in the plankton vary from 5 to 25dpm/g; the variation trend is similar to that of Po-210 but with much lower activity, resulting in a Po-210/Pb-210 ratio much greater than unity. Compared to the suspended particles, the plankton is highly enriched in Po-210 but it strongly repels Pb-210. Based on earlier studies and this one, the extent of Po-210 enrichment (as indicated by the Po-210/Pb-210 activity ratio) in various organisms increases sequentially from plankton to mussel, large swimmer and then to marine fish, i.e. the higher the level of organism in the food chain, the higher the ratio becomes. However, the Po-210 and Pb-210 activities per unit mass of these organisms are generally lower than those of plankton. Organisms of higher food-chain level may accumulate Po-210 in the digestive system, but part of it may be excreted. Po-210 accumulation does not occur in other parts of these organisms. In terms of adsorption, the plankton with greater surface area to volume ratio, can adsorb more Po-210 resulting in a higher specific activity, whereas large organisms with smaller surface area to volume ratio can adsorb less Po-210 yielding a lower specific activity. The enrichment of Po-210 in various organisms must have been achieved by absorption and adsorption with unknown proportion. Based on a simple box model calculation for the northern SCS water within the upper 100m layer, the excess Po-210 in the planktonic biomass can account for about 70% of the total deficit in this layer. But in the LS area, the excess and the deficit are balanced. This suggests that the Po-210 deficit in this surface water is due to absorption and adsorption by organisms as evidenced by their large Po-210 enrichment.

In order to understand the source, transport pathway and sink of settling particulates in the sea off northeast Taiwan, three moorings with six sediment traps (about 100 m and 300 m above bottom) were deployed on the northern slope of the Ilan ridge (T17S and T18S) and in the South Okinawa trough (T19S). The mooring deployed at T17S was lost due to a connecting ring which was rusted and broken. The duration of the mooring was 6 months (late November, 1999 to early May, 2000) with sampling intervals at 15 days each. When the moorings were recovered, seawater samples were collected for filtration near each station and a box core at T19S was also taken so that the settling particulates, suspended particulates and bottom sediments can be compared for their characteristics. The results show that higher apparent mass fluxes were observed in January, February and early April, 2000 at T18S. The apparent mass fluxes vary between 11 and 91 g/m2/d at T18S, and between 6 and 22 g/m2/d at T19S. The time-series variations of the Pb-210 activity are between 46 and 76 dpm/g at T18S, and between 79 and 122 dpm/g at T19S, the values of which are much higher than those of T18S. The temporal Po-210 variations range between 18 and 90 dpm/g at T18S, and from 65 to 193 dpm/g at T19S. The Po-210 activity and its variation are greater at T19S than at T18S. The 210Po/210Pb activity ratios are less than unity at about 0.8 at T18S, and greater than unity at about 1.3 at T19S. The total Po-210 activity in all water columns varies between 0.2 and 16 dpm/100kg while the total Pb-210 activity varies between 28 and 43 dpm/100kg. The mean total 210Po/210Pb activity ratio is about 0.3, indicating that Po-210 was easily scavenged and removed from water columns by particulate matter. The box core taken at T19S has Po-210 activity ranging from 54 to 121 dpm/g and Pb-210 activity from 51 to 90 dpm/g. The 210Po/210Pb activity ratio is greater than unity in the upper 6 cm, indicating an excess of Po-210 activity. Below 6 cm Po-210 and Pb-210 are nearly at equilibrium. The 210Po/210Pb activity ratios in the water columns observed after the first deployments were higher than those observed after the second deployments. However, the 210Po/210Pb activity ratios of the settling particulates collected from the first trap deployments were lower than those from the second trap deployments. These changes might be attributed to earthquakes which occurred mainly before the second mooring period. These earthquakes could have caused a large quantity of terrigenous particulates with higher 210Po/210Pb activity ratio to be transported out to the study area in addition to resuspended shelf and slope sediments. These settling particulates, being enriched in organic matter with higher activity ratio, could preferentially scavenge Po-210 from the water column, resulting in much higher 210Po/210Pb activity ratios.

The purposes of this study are to understand the variations of the particulate and dissolved Pb-210 and Po-210 in profiles in the South China Sea and to estimate the residence time of these nuclides through their extent of radioactive disequilibrium. The profiles of Pb-210 and Po-210 in particulate and dissolved phases were measured at four stations in the northern South China Sea (station B, C, D and F) and three in the Bashi Channel (stations W2, W3 and W5) from four Ocean Researcher I cruises (ORI-575, ORI-580, ORI-588 and ORI-606). At Station C two profiles were taken, one before and the other after a typhoon to see its effect, if any, during the ORI-588 cruise. As the associated Ra-226 profiles were not measured their relations to Pb-210 profiles are not available for discussion in this thesis. The mean suspended particulate matter (SPM) concentration for each station is about 0.2 mg/kg with small deviations. Activities of Pb-210 and Po-210 in the northern South China Sea were all higher than those in the sea off NE Taiwan easured during the KEEP program. The dissolved Pb-210 profiles generally display a maximum around 15 to 25 dpm/100kg in the surface layer due to atmospheric input, and a minimum of about 5 to 15 dpm/100kg from 300 to 1000 m. The activities below 1000 m vary only slightly with a deep maximum as high as 20 dpm/100kg around 2000 to 3000 m, as seen at Station C. The particulate Pb-210 is around 3 to 5 dpm/100kg with small variation for the entire water column. The dissolved Po-210 profiles are somewhat similar to the dissolved Pb-210 profiles, but lower by about 5 to 10 dpm/100kg in activity. The mean residence time is about 0.76 year for total Po-210 in the entire water column, and 0.35 to 2.13 years for total Pb-210 in the mixed layer. At each station, Po-210 is deficient relative to Pb-210 in either the particulate or dissolved phase. The mean total Po-210/Pb-210 activity ratio is about 0.58, indicating that Po-210 is more effectively scavenged. It is imperative to understand the fate and pathway of the missing Po-210. Judging from its biophilic nature, Po-210 may have been absorbed or consumed by biomass and enriched in various tropic levels in the food chain, in addition to being scavenged and removed by sinking particles.

In this study, the settling particulates collected by time-series sediment traps, sediment cores, and seawater samples taken in the western South Okinawa Trough were analyzed for 210Pb and 210Po in order to understand the characteristics of the particulates and sediments based on the distribution of these two nuclides and the extent of their radioactive disequilibrium. Two sediment traps were deployed at T18 (24¢X45'N 122¢X18'E, about 300m and 100m above bottom) from February to August 1999. The results show that higher mass fluxes were observed from February to April, ranging between 16 and 56 g/m2/d. The 210Pb activity increases systematically with time from about 80 to 100 dpm/g, and the upper trap has slightly higher values. Similar to 210Pb, the 210Po activity also increases, but from near zero to only 27 dpm/g for both traps, much lower than the corresponding 210Pb activity. The 210Pb activities are quite different between the settling particulates collected by traps at T18 and the surface sediment taken nearby (the former have a mean activity of about 85 to 90 dpm/g; the latter has a value of only 11 dpm/g). The size distribution and elemental composition are also different between the trapped particulates and the sediment. Thus the underlying sediments were not directly derived from the overlying trapped particulates. Except for T4 core below 15cm and T19 entire core, the 210Po/210Pb activity ratio in the sediments varies greatly, from near zero to 0.7, indicating deficiency of 210Po. Both 210Po and 210Pb activities are much lower in the sediments than in the settling particulates. A T19 both 210Po and 210Pb activities in the core decrease steeply from 120 dpm/g at surface to 60 dpm/g at 4 cm, indicating radioactive equilibrium. This is entirely different from the cores taken at other stations. The total 210Po/210Pb activity ratio in the water column at T17 is nearly constant at about 0.6, but drops to 0.3 below 700m, i.e. 210Po activity is deficient in the entire water column. At T18, the activity ratio is about 1.3 between 100m and 300m, indicating a 210Po excess in this layer. Below 400m, the ratio is about 0.6 to 0.7, showing 210Po deficit again. These observations indicate that the water columns at T17 and T18 are stratified, probably due to lateral transport. Based on the 210Po/210Pb activity ratio the mean residence time of 210Po with respect to particulate scavenging ranges from 3 to 16 months.

The objectives of this thesis were: (1) to develop a mass balance partitioning model of the natural uranium-238 series comprising radium-226, lead-210 and polonium-210 and (2) to apply the model to estimate the source and fate of these radionuclides in freshwater lakes and streams. Samples were collected from Ottawa River watershed tributaries and measured for lead-210 and polonium-210 content to determine the water concentrations that were input to the model. The radium-226 partitioning model was developed by reconstructing and analyzing Quantitative Water, Air, Sediment Interaction (QWASI) models of lead for Lake Ontario and Hamilton Harbour and selecting parameters for an updated QWASI model of lead for a Lake Ontario basin. This study gave insight about model basis definition, and partition coefficient and sediment particle constraint. The radium-226 series model was formulated by connecting separate QWASI modules for radium-226, lead-210 and polonium-210 with decay and ingrowth terms. The radium-226 model was applied to studies of Crystal Lake, Wisconsin; Bickford Pond, Massachusetts; and Clinton River, Michigan, using parameters reported in these and other studies. Model error was evident in the applications to Crystal Lake due to underlying lake heterogeneity, to Bickford Pond due to unidentified sources of lead-210 from sediment diffusion or watershed runoff, and to Clinton River from watershed runoff. The model was applied to seven Laurentian Shield lakes in the Ottawa River watershed using the sample measurements as the basis for water concentration inputs. The application showed that hydrologic flushing rate may be a factor in the proportion of watershed atmospheric deposition and overall Pb-210 input to the water. Laurentian Shield Lakes with the lowest hydrologic flushing rates (<3 a-1) had proportions of Pb-210 losses to sediment greater than 85%. In another application to Judge Sissons Lake, Nunavut, the model indicated that the watershed was the source of about 85% of Pb-210 and 98% of Po-210 input to the water, and that a significant geologic component of Pb-210 input to the lake was likely. The model indicated that most of the Pb-210 in Judge Sissons Lake was lost to outflow, and that most of the Po-210 was lost to sediment. The model showed that sedimentation is a better proxy measurement for atmospheric deposition of Pb-210 to the Laurentian lakes than originally estimated. The model also showed that watershed contributions to Judge Sissons Lake could explain the observed background concentrations of Pb-210 and Po-210.