Content of plutonium,thorium and protactinium in sea water and recent coral in the North Pacific

The contents of plutonium isotopes (²³⁹Pu and²³⁸Pu), thorium isotopes (²³²Th,²³⁰Th and²²⁸Th) and protactinium-231 in sea water collected in the North Pacific, the East China Sea and the Japan Sea were determined. These nuclides were sequentially analyzed byα-ray spectrometry after separating them mainly with solvent extraction technique. The contents of²³⁹Pu in surface sea water ranged from 0.6 to 1.6 pCi/10001,²³⁸Pu/²³⁹Pu activity ratios being 0.2～0.7. The²²⁸Th/²³²Th activity ratios for the North Pacific waters varied between 7.6 and 30, whereas the sample from the East China Sea showed the very high value, 65. The contents of²³¹Pa are less than 6 percent of that in equilibrium with its parent²³⁵U. Furthermore, the analysis of plutonium isotopes in recent coral from Yoron Island was carried out and it was confirmed that plutonium isotopes have concentrated in recent coral with the concentration factor of about 1～2×10³.     

Sinking fluxes of particulate U-Th radionuclides in the East Sea (Sea of Japan)

A record of radionuclide fluxes at a deep marginal sea of the Northwest Pacific Ocean (39°40′N 132°24′ E, Japan Basin, East Sea/Sea of Japan) was obtained from analysis of a 1-year continuous collection of sediment-trap samples. The trap was placed at a depth of 2800 m, 500 m above the sea floor, and the samples were recovered at the end of one year. Concentrations of ²³⁸U, ²³⁴U, ²³²Th, ²³⁰Th and ²²⁸Th were measured in the trapped material. All of the radionuclide fluxes showed seasonal variations that were in phase with the variations in total particle flux, which were shown in earlier work to be closely tied to the primary production in the surface water. The formation of authigenic ²³⁸U appears to be less than in other open ocean regimes. The residence time of particulate thorium isotopes were of the order of a year, resulting in an average settling rate of a meter per day. Comparison of the measured ²³⁰Th_ex flux with that of the theoretical production in the overlying water column yielded about 40% surplus of ²³⁰Th, indicating that lateral advection contributes ²³⁰Th to this sampling site.     

Different partitioning among thorium isotopes in seawater of the Northern North pacific

Each about 400 l of seawater sample was collected in the northern North Pacific and filtered through a membrane filter. Four radioisotopes of thorium,²³²Th,²³⁰Th,²²⁸Th and²³⁴Th, were determined for the two FractionsF (filtrate) andP (particles on the filter). In the percentages of FractionP in the subsurface water,²³⁰Th was significantly larger than other 3 isotopes, and²³²Th was significantly smaller than other 3 isotopes. The former finding can be explained by the slower rates in the reversible change between the FractionsF andP. The latter one, however, cannot be explained if thorium isotopes in the FractionF are truly dissolved with the same chemical form. This suggests that major part of the FractionF of²³²Th is not identical with those of other radiogenic thorium isotopes, and it should not be composed of simple dissolved ions. The removal of radiogenic²³⁴Th was related to the biological activity, but there was a deviation, between the FractionP and radioactivity deficiency of²³⁴Th in their vertical profiles. The deviation was similar to that between the chlorophylla and phaeo-pigments contents including their maximum depths.     

Radioactive disequilibrium of thorium series nuclides in surface waters of the Seto Inland Sea

Surface samples of sea water collected in the Seto Inland Sea were analyzed for²³²Th and²²⁸Th. The concentrations of²³²Th were generally less than 2 dpm/1,0001 and these values are probably an upper limit for the²³²Th concentration in surface waters of the Seto Inland Sea. The²²⁸Th concentrations ranged between 4.2 to 42.3 dpm/1,0001. Remarkable seasonal and temporal variations in²²⁸Th concentrations were found, in comparison with the minimal variations in²²⁸Ra concentrations reported previously. The activity ratios of²²⁸Th/²²⁸Ra were about 0.18 in the southern part of the Kii and the Bungo Channels, and decreased markedly from the open ocean toward the central region of the Seto Inland Sea. The average value of the²²⁸Th/²²⁸Ra ratio in the central region of the Seto Inland Sea was 0.032±0.020. This suggests that removal residence time of²²⁸Th can be estimated to be about 34±22 days in surface waters of the Seto Inland Sea.     

Th isotopes in the Santa Monica basin: Temporal variation,long-term mass balance and model rate constants

Distribution and flux of²³⁴Th,²³²Th and²³⁰Th in the water column of central Santa Monica basin observed over a period of seven years show seasonal and interannual variabilities. A steady-state model is applied to the integrated data to calculate long term average flux and model rate constants of Th isotopes. Mass balance calculations show that the basin acts like a closed system for short-lived²³⁴Th, but not for the long-lived isotopes²³⁰Th and²³²Th. Most²³⁰Th in the basin is transported from elsewhere. Of the incoming Th, 40–55% of the²³⁰Th and 14–26% of the²³²Th enter the surface water in dissolved form. In the upper 100 m, the residence time of dissolved Th with respect to adsorption onto suspended particulates, 70–80 days, is about one order of magnitude higher than the residence time of suspended particles with respect to aggregation into sinking particles, 7–10 days.     

Th and Pa isotopes in the waters of the western margin of the pacific near Japan: Evidence for release of228Ra and227Ac from slope sediments

Using the moored MnO₂-fiber method, we have obtained 38 determinations of Th and Pa isotope concentrations from 18 sites along the margin of the western North Pacific near Japan, from water depths of 1,330 to 5,873 m. From our data, we are able to show that (1)²²⁸Ra and²²⁷Ac are being supplied to the seawater from the slope sediments of Honshu, Japan, (2) our²³⁰Th and²³¹Pa concentrations match those obtained byin situ pumping with a MnO₂-fiber adsorber in the Japan and Izu-Ogasawara trenches but are significantly higher than those from the Panama and Guatemala basins, and (3) our²³²Th concentrations show a similar systematic decrease with depth as do those of trace metals like Mn, Al, Te and Bi whose concentrations are strongly controlled by particulate matter scavenging.In contrast, our data fail to show (1) that enhanced removal of²³⁰Th and²³¹Pa by scavenging from the water column is taking place near the western margins and (2) that²³¹Pa is being removed in preference to²³⁰Th from the water column to the marginal sediments. This is probably due to rapid mixing of the deep waters as compared to the scavenging rates of²³⁰Th and²³¹Pa in the water column and at the sediment/seawater interface.     

沉积物中钍同位素分析样品的处理方法比较研究

分别用HCl浸取和HF全溶法分析研究沉积物中的同位素^232Th、^230Th、^228Th，并对所分析的结果进行全面的对照比较，盐酸浓度、温度及样品的矿物组分都能影响这3种同位素的酸浸取效率，对于一种确定的沉积物来说，在相同的浸取条件下，^228Th的酸浸取效率总是高于^232Th，这是由于α辐射子体同位素的反冲作用造成的，与HCl浸取法比较，HF全溶法更可靠、更准确。     

228Ra in surface water of the Seto Inland Sea

The concentrations of²²⁸Ra in surface waters of the Seto Inland Sea were determined. Surface waters from the central region of the Seto Inland Sea, Hiuchi Nada and Bingo Nada, contained concentrations of²²⁸Ra of 655–811 dpm/1000 l which were 100 times higher than those obtained in the Pacific Ocean. These high concentrations of²²⁸Ra must be supported by a²²⁸Ra flux from the bottom sediment. The lower limit of this flux was estimated to be more than 0.16 dpm cm^–2 y^–1. The²²⁸Ra concentrations decreased markedly from central regions of the Seto Inland Sea to about 18 dpm/1000 l in the Kii and the Bungo Channels as salinity increased. Using a box model and the²²⁸Ra data, the mean residence time of sea water in the Seto Inland Sea with respect to the exchange with the open ocean water was estimated to be less than 10 y, and the most probable value is the order of several years.     

Radium-228 in the Japan Sea

The distribution of²²⁸Ra in surface and subsurface waters in the Japan Sea was studied. The concentrations of²²⁸Ra in surface waters were around 100 dpm/1000l which were much higher than those reported for Pacific surface waters. The concentrations of²²⁸Ra decreased with increasing depth to less than 10 dpm/1000l in the Japan Sea Proper Water. Based on the comparison between observed values of²²⁸Ra and calculated profile through the near-surface water mass and the underlying main water mass in the Japan Sea, the apparent vertical eddy diffusion coefficient was estimated to be about 2 cm² s^–1.     

Anomalous Large Scavenging of 230Th and 231Pa Controlled by Particle Composition in the Northwestern North Pacific

We report the role of particle composition and lateral particle movement that influences the oceanic distribution of ²³¹Pa and ²³⁰Th. Settling particles were collected during sediment trap experiments. These and surface sediments were obtained from five stations along 38 to 44°N in the northwestern North Pacific. The high total mass flux and seasonal variations in the marginal area of the western North Pacific are controlled by the supply of lithogenic materials and primary productivity. The high content of the lithogenic material in the settling particles in this area contributes to ²³⁰Th_ex fluxes that exceed the local rate of supply. The lithogenic materials are important as a carrier of ²³⁰Th and contribute to the fractionation between ²³⁰Th and ²³¹Pa in the ocean, as the ²³¹Pa_ex/²³⁰Th_ex ratio in the settling particles decreases with increasing ²³²Th concentration. The ²³¹Pa_ex/²³⁰Th_ex ratio in the settling particles collected in the abyssal basin decreases with water depth, which indicates that lateral transport of the lithogenic particles from the marginal area and/or shallower depth plays an important role in determining the ²³¹Pa_ex/²³⁰Th_ex ratio in a population of settling particles and remineralization. This indicates that lateral redistribution of particles and sediment focusing influence the ²³¹Pa_ex/²³⁰Th_ex ratios in surface sediments. Thus, the observations reported here mean that the use of the sediment ²³¹Pa_ex/²³⁰Th_ex ratio as a paleoproductivity proxy will be problematic in the northwestern North Pacific. This revised version was published online in July 2006 with corrections to the Cover Date.     

Determination of thorium isotopes in seawater by moored MnO2-fiber method

A method is described for the determination of Th isotopes (²³²Th,²³⁰Th,²²⁸Th and²²⁷Th) in seawater through analysis of Th adsorbed on MnO₂-impregnated fiber that has been moored in the deep sea for up to 10 months. Since the MnO₂-fiber adsorbs Th from seawater at a constant rate, natural²³⁴Th can be used as a yield monitor by making a correction for its decay during the period of deployment. The results obtained by the method showed good reproducibility and accuracy. The method has the advantage over the chemical coprecipitation method that the time and labor for sampling and processing a large-volume of seawater is reduced.     

Measuring low concentrations of Th in water and sediment

²³⁴Th/²³⁸U disequilibria have been used extensively in studies of particle dynamics and the fate and transport of particle-reactive matter in marine environments. Similar work in low salinity, estuarine, and freshwater systems has not occurred primarily because the lower concentrations of both parent and daughter nuclides that are typical of these systems often render established methods for the analysis of ²³⁴Th inadequate. The application of this radionuclide tracer technique to these systems, however, has great potential. To this end, we present a method for measuring low activities of ²³⁴Th in relatively small samples (<200 l) using low background gas-flow proportional counters, a ²²⁹Th yield monitor, and empirical corrections for the interferences from real and apparent betas that are emitted by other thorium isotopes and their progeny. For samples with low ²³⁴Th/²²⁸Th activity ratios, we improve upon current beta counting methodologies that rely on immediate sample counting, weak beta absorption, or multiple beta counts so that, using the analytical approach outlined here, it should be possible to measure ²³⁴Th activities (i) as low as 1.5 dpm/total sample, (ii) up to 2 weeks after radiochemical purification of thorium, and (iii) with only one sample count for alpha and beta activity.     

Seasonal variation of <Superscript>228</Superscript>Ra/<Superscript>226</Superscript>Ra ratio in surface water from the East China Sea and the Tsushima Strait

A total of 21 surface water samples were collected on the east side of the East China Sea (ECS) (3 sites) and at the Tsushima Strait (1 site), and ²²⁶Ra and ²²⁸Ra activities were measured using low-background γ-spectrometry. The ²²⁸Ra/²²⁶Ra ratios among the samples exhibited notable seasonal variation (²²⁸Ra/²²⁶Ra = 0.2–2.6) accompanying changes of salinity (31.7–34.7). Seasonal water circulation within the ECS is hypothesized to cause the change by altering the mixing ratio of ²²⁸Ra-rich continental shelf water and ²²⁸Ra-poor Kuroshio water.     

Radiochemical studies of deep-sea manganese nodules

Five manganese nodules collected from the Northern Mid - Pacific have been analysed for their U and Th isotopes.lt is found that the enrichment of thorium compared to uranium is universal in deep- sea manganese, nodules and in the top sides of the nodules there are large excesses of Th and Pa decreasing exponentially with depth. For each of the nodules, the concordant growth rates are obtained from three different methods: 230Thex 230Thex/232Th and 231Paex.The growth rates of manganese nodules are closely related to the chemical compositions of the nodules and the types of the underlying sediments. The growth rates of five nodules are determined to be in the range of 0.79-7.4 mm/106a, in agreement with those predicted from the chemical compositions of the nodules. By the comparison of the extrapolated 230Thex,230Thex/232 Th and 231PaeX data from the top and bottom surfaces of the nodule from Site M21 yields, the nodule turnover time is (9.83-13.7)×104a.     

The distribution of radionuclides and some trace metals in the water columns of the Japan and Bonin trenches

Presented here is the first detailed geochemical data set on the U/Th series Th, Pa, Ac, and Pb isotopes and artificial fallout radionuclides (⁹⁰Sr, ¹³⁷Cs, and Pu isotopes), and some trace elements (V, Zn, Cd, Cu, Mn, and Ni) in two water columns of the Japan and Bonin trenches down to the bottom depths of 7585 m and 9750 m, respectively. Hydrographic properties such as temperature, salinity, dissolved oxygen, and nutrient content within the trench valley remain constant at the same levels as those in the bottom water of the Northwest Pacific basin (typically ∼6000 m in depth). The radionuclide activities and most trace metal concentrations are also not very different from those in the overlying water at depths of around 5000–6000 m. This means that any chemical alteration which sea water undergoes during its residence within the trench was not obviously detected by the techniques used here. The suggestion follows that the trench water is rather freely communicating by isopycnal mixing with the bottom water overlying the Northwest Pacific abyssal plain. The trench waters contain high ^{239, 240}Pu activities throughout, indicating that Pu is actively regenerating from rapidly sinking, large particles at the bottom interface, probably due to a change in the oxidation state. On the other hand, the vertical profiles of ²¹⁰Pb and ²³¹Pa show lower activities within the trench than those in the overlying deep waters, suggesting that the effect of boundary and bottom scavenging is significant in controlling their oceanic distributions. However, none of the trace metals studied here obviously follows the behaviour of the above nuclides. The ²²⁸Th data show scattering within the Bonin Trench that is largely ascribable to analytical errors. If, however we accept that the scatter of ²²⁸Th data is real and the variation is caused solely by decay of its parent ²²⁸Ra, we can set an upper limit of ∼5 years for the renewal time of the trench water.     

Impact of the Mediterranean Outflow Water on particle dynamics in intermediate waters of the Northeast Atlantic, as revealed by Th and Th

Over the last decade ²³⁴Th has become increasingly used to study particle transport in the ocean on a timescale of weeks. The application of ²³⁴Th is mainly focused on the determination of particle and associated carbon fluxes from oceanic surface water. However, ²³⁴Th is also suitable for investigating particle dynamic from the upper ocean down to interface sediments, as illustrated by the present work which reports unexpected behavior of ²³⁴Th in intermediate waters associated with the Mediterranean Outflow Water (MOW). Concentration profiles of dissolved ²³⁸U and ²²⁸Ra, and dissolved and particulate ²³⁴Th and ²²⁸Th were measured in the Mediterranean Outflow Water (MOW) near the Gibraltar Straits and at two sites (36°30′N–15°35′W, Nicole; 36°27′N–10°35′W, Yseult) which had hydrographic characteristics of Meddies, i.e. MOW that propagates as eddies in the Northeastern Atlantic at intermediate depths.There are marked differences in the distribution of thorium between MOW and the surrounding Atlantic waters. At the youngest Meddy Nicole salinity maximum at 1000 m depth, ²³⁴Th(total) : ²³⁸U and ²²⁸Th(total) : ²²⁸Ra activity ratios are significantly lower than radioactive equilibrium, indicating an unusual deficit of short half-life thorium nuclides. This implies an export of thorium, presumably on particles, from intermediate Meddy Nicole waters. This process is supported by an increase of particulate thorium fluxes measured in sediment traps deployed for two weeks above and within Meddy Nicole. In contrast, offshore Meddy Yseult has more typical profiles of both thorium nuclides that are nearly in equilibrium with their parents. These results indicate that at intermediate depths, the presence of MOW affects the exchange of reactive elements between particles and dissolved forms and enhances the downward flux of particles from intermediate waters in the Northeast Atlantic.     

Intermediate Circulation in the Northwestern North Pacific Derived from Subsurface Floats

In order to examine the formation, distribution and synoptic scale circulation structure of North Pacific Intermediate Water (NPIW), 21 subsurface floats were deployed in the sea east of Japan. A Eulerian image of the intermediate layer (density range: 26.6–27.0σ_θ) circulation in the northwestern North Pacific was obtained by the combined analysis of the movements of the subsurface floats in the period from May 1998 to November 2002 and historical hydrographic observations. The intermediate flow field derived from the floats showed stronger flow speeds in general than that of geostrophic flow field calculated from historical hydrographic observations. In the intermediate layer, 8 Sv (1 Sv ≡ 10⁶ m³s⁻¹) Oyashio and Kuroshio waters are found flowing into the sea east of Japan. Three strong eastward flows are seen in the region from 150°E to 170°E, the first two flows are considered as the Subarctic Current and the Kuroshio Extension or the North Pacific Current. Both volume transports are estimated as 5.5 Sv. The third one flows along the Subarctic Boundary with a volume transport of 5 Sv. Water mass analysis indicates that the intermediate flow of the Subarctic Current consists of 4 Sv Oyashio water and 1.5 Sv Kuroshio water. The intermediate North Pacific Current consists of 2 Sv Oyashio water and 3.5 Sv Kuroshio water. The intermediate flow along the Subarctic Boundary contains 2 Sv Oyashio water and 3 Sv Kuroshio water. This revised version was published online in July 2006 with corrections to the Cover Date.     

Particle flux in the twilight zone of the eastern Indian Ocean: A constraint from 234U–230Th and 228Ra–228Th disequilibria

Total ²³⁰Th and ²²⁸Th vertical distributions were measured in the eastern Indian Ocean. Based on disequilibria of ²³⁴U–²³⁰Th and ²²⁸Ra–²²⁸Th, we estimated the particle flux from the surface to 950 m. The estimated particle flux ranged from 190±60 (150 m in the Southern Ocean) to 8.4±2.5 mg/m²/day (950 m in the West Australian Basin). The particle fluxes correlate well with estimates of nitrate supply by vertical mixing to the euphotic zone, suggesting local control by new production. Flux attenuation at mesopelagic depths appears to be related to biogenic carbonate and silica remineralization based on comparison to alkalinity and dissolved silicate distributions, with possible additional control by lithogenic particle inputs. The particle flux estimates obtained by combining the ²³⁴U–²³⁰Th and ²²⁸Ra–²²⁸Th disequilibria offer advantages over those from ²²⁸Ra–²²⁸Th disequilibrium alone, in that they can account for some aspects of vertical mixing and thus are applicable to a wider range of oceanographic settings.     

A case study of a Kuroshio main path cut-off event and impacts on the South China Sea in fall-winter 2013–2014

This study examines a Kuroshio main path(KMP) cut-off event east of Taiwan Island occurred in fall-winter2013–2014 and its impacts on the South China Sea(SCS) by analyzing satellite altimetry and mooring observations. Satellite altimeter sea level anomaly(SLA) images reveal a complete process that a huge cyclonic eddy(CE) from the Pacific collided with the Kuroshio and the western boundary from 15 October 2013 to 15 January 2014. Mooring observations evidenced that the Kuroshio upper ocean volume transport was cut off more than 82% from 17×106 m~3/s in September to 3×106 m~3/s in November 2013. The KMP cut-off event caused the Kuroshio branching and intruding into the SCS and strengthened the eddy kinetic energy in the northern SCS west of the Luzon Strait. Using the total momentum as a dynamic criterion to determine the role of eddy collision with the Kuroshio reasonably explains the KMP cut-off event.     

吕宋海峡水交换季节和年际变化特征的数值模拟研究

利用ROMS(Regional Ocean Modeling System)建立了一套覆盖西北太平洋的涡尺度分辨率环流模型,并对吕宋海峡附近的环流进行了模拟研究。结果表明,吕宋海峡120.75°E断面净流量季节变化显著,全年均为西向输运,6月份达到最小,为0.40×106 m3/s,然后逐渐增大,在12月份达到最大,为6.14×106 m3/s,全年平均流量为3.04×106 m3/s。在500 m以浅,秋、冬季都有明显的黑潮流套存在,并伴有黑潮分支入侵南海,而春、夏季黑潮南海分支减弱或消失,黑潮入侵不明显。在500 m以深,冬、春季,吕宋海峡以东有非常明显的南向流存在,流速约10 cm/s,而到了夏、秋季该南向流出现明显的减弱,黑潮与南海的水交换主要通过吕宋海峡以北的吕宋海沟进行。在垂向结构上,120.75°E断面浅层呈多流核结构,并且流核的位置和强弱受黑潮的季节性变化影响显著,深层流的季节变化不大。在年际尺度方面,吕宋海峡年际体积输运量异常与Niño3.4滞后6个月相关系数达到41.6%,吕宋海峡水交换与ENSO现象有较为显著的正相关关系,并存在2~3 a和准8 a周期的年际变化。