The flux of226Ra from deep-sea sediments

The flux of²²⁶Ra from bottom sediments has been determined from patterns of²²⁶Ra/²³⁰Th disequilibrium in ten deep-sea cores from the world oceans. Values range from ? 0.0015 dpm/cm² yr (in the Atlantic) to 0.21 dpm/cm² yr (in the north equatorial Pacific). The flux is poorly related to sediment type, but is inversely correlated in a non-linear fashion with sediment accumulation rate. There is a direct relationship between the production rate of²²⁶Ra near the sediment-water interface (i.e. the integrated²³⁰Th activity in the biologically mixed zone) and the²²⁶Ra flux. The²²⁶Ra concentration in near-bottom water follows the geographic variation in the²²⁶Ra flux. The high flux from north equatorial Pacific sediments especially is reflected in the high bottom water²²⁶Ra concentrations in that area. The data suggest that both rate of circulation and the magnitude of the radium flux influence the near-bottom²²⁶Ra concentration.     

230Th,226Ra and222Rn in abyssal sediments

A model that predicts the flux of²²²Rn out of deep-sea sediment is presented. The radon is ultimately generated by²³⁰Th which is stripped from the overlying water into the sediment. Data from many authors are compared with the model predictions. It is shown that the continental contribution of ionium is not significant, and that at low sedimentation rates, biological mixing and erosional processes strongly affect the surface concentration of the ionium. Two cores from areas of slow sediment accumulation, one from a manganese nodule region of the central Pacific and one from the Rio Grande Rise in the Atlantic were analyzed at closely spaced intervals for²³⁰Th,²²⁶Ra, and²¹⁰Pb. The Pacific core displayed evidence of biological mixing down to 12 cm and had a sedimentation rate of only 0.04 cm/kyr. The Atlantic core seemed to be mixed to 8 cm and had a sedimentation rate of 0.07 cm/kyr. Both cores had less total excess²³⁰Th than predicted.Radium sediment profiles are generated from the²³⁰Th model. Adsorbed, dissolved, and solid-phase radium is considered. According to the model, diffusional losses of radium are especially important at low sedimentation rates. Any particulate, or excess radium input is ignored in this model. The model fits the two analyzed cores if the fraction of total radium available for adsorption-desorption is about 0.5–0.7, and ifK, the distribution coefficient, is about 1000.Finally, the flux of radon out of the sediments is derived from the model-generated radium profiles. It is shown that the resulting standing crop of²²²Rn in the overlying water may be considered as an added constraint in budgeting²³⁰Th and²²⁶Ra in deep-sea sediments.     

226Ra in the Pacific Ocean

A total of 29 vertical Ra profiles has been measured from the Pacific as part of the GEOSECS program. These profiles are located on an east-west section along ～30°N, and a north-south section, close to the western boundary of the major basins in the western Pacific. Profiles from the northeast Pacific show a deep Ra maximum, with an excess concentration relative to the potential temperature and salinity. This maximum extends westward in the direction with decreasing Ra content, and finally vanishes completely in the northwest Pacific near Japan.Ra profiles along the western boundary show a mid-depth maximum around 3 km and a near-bottom minimum due to southward intrusion of the high-Ra Pacific Deep Water and a northward spreading of the low-Ra Antarctic Bottom Water. The contrast between the maximum and the minimum intensifies toward the south, where the benthic front has clearly separated these two water masses. Ra is thus a useful tracer for the studies of oceanic mixing and circulation in the Pacific.     

The distribution of 226Ra in the Atlantic Ocean

Based on results obtained during the GEOSECS program the primary features of the distribution of²²⁶Ra in the Atlantic Ocean can be defined. Outside the Antarctic no significant variation has been found in the²²⁶Ra content of surface waters. Eighty samples yield an average of 7.4 dpm/100 kg (normalized to a salinity of 35.00‰). Deep waters in the central Atlantic have²²⁶Ra contents several dpm/100 kg higher than expected from the mixing of Antarctic Bottom Water (21.3 dpm/100 kg) and basal North Atlantic Deep Water (10.3 dpm/100 kg). These excesses correlate well with deficiencies in O₂ and excesses in SiO₂. The intermediate water²²⁶Ra maximum in the South Atlantic is associated with the inflow of low-oxygen Circumpolar Intermediate Water beneath the Antarctic Intermediate Water.     

226Ra distribution in the Antarctic Ocean

²²⁶Ra data on eleven vertical profiles taken during the GEOSECS program from the Antarctic Ocean and its vicinity in both the Atlantic and the Pacific are presented. Replicate measurements were made on each sample using the Rn-emanation method. The precision (1 σ) based on triplicate analyses averages about ±2.5%. Waters all around the Antarctic continent below 2 km depth appear to exhibit a uniform²²⁶Ra concentration of 21.5 ± 1dpm/100kg, except perhaps locally such as the Ross Sea and the Drake Passage where small variations may be present. Higher in the water column, the²²⁶Ra contents decrease toward the surface with gradients which vary as a function of the influence exerted by the Antarctic Convergence. Across this oceanic front, a north-to-south increase of²²⁶Ra occurs (the increase being the largest near the surface: from 8 to 18 dpm/100 kg), reflecting the combining effect of deep-water upwelling and meridional water mixing. The core layer of the Antarctic Intermediate Water contains about 14 dpm/100 kg of²²⁶Ra and that of the Circumpolar Intermediate Water (O₂ minimum and local T maximum) about 18 dpm/100 kg. To a first approximation,²²⁶Ra covaries with Si in the circumpolar waters.     

226Ra chronology of a coastal marine sediment

Unsupported²²⁶Ra (t₁₂ = 1620years) in marine sediments can provide a basis for measuring rates of accumulation of the order of centimeters per thousand years. The excess radium apparently enters the sediments incorporated in phytoplankton. The sensitivity of the method depends upon the initial value of the unsupported²²⁶Ra and of the value of²³⁰Th, a parent of²²⁶Ra, in the sedimentary components.²²⁶Ra dating was applied to a sediment taken from the slope of the San Clemente Basin in the Southern California coastal region. Rates of sedimentation over two half-lives of the nuclide were found to be either 5.2 or 5.3 cm/1000 years depending upon which of two models for the geochronology is used. One model assumes that the²³⁰Th brings to the deposit an amount of²²⁶Ra in equilibrium with it. The other is based upon the growth of the²²⁶Ra from the²³⁰Th in the sedimentary components.^238+239Pu and²¹⁰Pb levels in the upper strata indicated sedimentation rates of the order of 100–500 cm/1000 years, i.e. much faster accumulations. We suggest these derived rates are spurious and reflect bioturbative activities of surface-living organisms.     

210Pb/226Ra disequilibrium in the Santa Barbara Basin

The vertical distributions of²¹⁰Pb and²²⁶Ra in the Santa Barbara Basin have been measured. The²¹⁰Pb/²²⁶Ra activity ratio is close to unity in surface water, but ranges from 0.2 to 0.6 in deep water with a mean value of 0.3 (d > 250m), suggesting rapid removal of²¹⁰Pb from the water column. The²¹⁰Pb concentrations in the particulate phase at different water depths indicate that the removal of²¹⁰Pb is due to adsorption on settling particles.It is estimated that the particulate²¹⁰Pb contributes about 50–70% of the total²¹⁰Pb measured on unfiltered water samples of the Santa Barbara Basin. The fate of²¹⁰Pb (and Pb) in the water column is thus strongly controlled by the settling particles, which have a mean residence time of one year or less in the basin. Material balance calculation for²¹⁰Pb in the basin suggests that there is an external source supplying about 70–80% of the²¹⁰Pb observed in particulate material or sediments. This excess²¹⁰Pb is most likely provided by particles entering the basin loaded already with²¹⁰Pb.     

226Ra and210Pb in the Weddell Sea

²²⁶Ra and²¹⁰Pb were measured in sections and profiles collected in the Weddell Sea during the International Weddell Sea Oceanographic Expedition in 1973. The results can be correlated with the circulation and mixing schemes deduced from hydrographic observations. Along the surface cyclonic gyre the Ra activities are fairly uniform at about 17 dpm/100 kg, quite similar to those of the Circumpolar surface water south of the Antarctic Convergence. The²¹⁰Pb activities in the northern flank of the gyre, probably influenced by the high²¹⁰Pb-bearing Circumpolar Deep Water in the north, are as high as 12 dpm/100 kg. At the central gyre and its southern flank, the surface water²¹⁰Pb activities are about 7 dpm/100 kg. The warmer surface water at the central gyre has a Ra activity of about 19 dpm/100 kg, slightly higher than the colder surface water at the flanks. Thus lower²¹⁰Pb/²²⁶Ra activity ratios are observed in the central gyre, and higher ratios in its flanks. Similar relationships between Ra and Pb are noted in the Weddell Sea Bottom Water (WSBW): lower Pb associated with higher Ra in the center; higher Pb with slightly lower Ra in the flanks.Vertical profiles along the cyclonic gyre show lower Ra and Pb activities in the southwestern Weddell Basin where lower temperature and lower silicate are observed. Similar to Ba, both Ra and Si are non-conservative in the Weddell Sea, with significant input from the bottom sediments and particulate dissolution during subsurface mixing.Each water mass or type in the Weddell Sea is well characterized by its Ra content, but not well by its Pb content. Ra and Si are crudely correlated with a slope of about 7 × 10^?4 dpm Ra per μmole of Si. The fact that the WSBW values fall on the slope suggests that the net input rate for Ra (corrected for the decay rate) is proportional to that of Si. The linear extrapolation to zero Si gives a Ra value of 13 dpm/100 kg. These relationships are quite similar to those observed in the Circumpolar waters.     

226Ra, 210Pb and 210Po disequilibria in the Western North Pacific

²²⁶Ra,²¹⁰Pb and²¹⁰Po were measured in oceanic profiles at two stations near the Bonin and Kurile trenches.²¹⁰Po is depleted by 50% on average relative to²¹⁰Pb in the surface water. In the deep water,²¹⁰Pb is about 25% deficient relative to²²⁶Ra. Based on the deficiency,²¹⁰Pb residence time with respect to removal by particulate matter was estimated to be less than 96 years in the deep water.²¹⁰Pb deficiency in the bottom water was significantly greater than that of the adjacent deep water, indicating more effective removal near or at the bottom interface.²¹⁰Pb,²¹⁰Po and Th appear to have similar overall rate constants of particulate removal throughout the water column.     

210Pb and226Ra distributions in the Circumpolar waters

²¹⁰Pb and²²⁶Ra profiles have been measured at five GEOSECS stations in the Circumpolar region. These profiles show that²²⁶Ra is quite uniformly distributed throughout the Circumpolar region, with slightly lower activities in surface waters, while²¹⁰Pb varies with depth as well as location or area. There is a subsurface²¹⁰Pb maximum which matches the oxygen minimum in depth and roughly correlates with the temperature and salinity maxima. This²¹⁰Pb maximum has its highest concentrations in the Atlantic sector and appears to originate near the South Sandwich Islands northeast of the Weddell Sea. Concentrations in this maximum decrease toward the Indian Ocean sector and then become fairly constant along the easterly Circumpolar Current.Relative to²²⁶Ra, the activity of²¹⁰Pb is deficient in the entire water column of the Circumpolar waters. The deficiency increases from the depth of the²¹⁰Pb maximum toward the bottom, and the²¹⁰Pb/²²⁶Ra activity ratio is lowest in the Antarctic Bottom Water, indicating a rapid removal of Pb by particulate scavenging in the bottom layer and/or a short mean residence time of the Antarctic Bottom Water in the Circumpolar region.²²⁶Ra is essentially linearly correlated with silica and barium in the Circumpolar waters. However, close examination of the vertical profiles reveals that Ba and Si are more variable than²²⁶Ra in this region.     

226Ra,210Pb and210Po in the Red Sea

Profiles of²²⁶Ra and dissolved²¹⁰Pb have been measured at several stations in the Red Sea. At one station in the central Red Sea an expanded profile was measured including²²⁶Ra and dissolved and particulate²¹⁰Pb and²¹⁰Po. These profiles show several distinct features: (1)²²⁶Ra displays a mid-depth maximum of about 13 dpm/100 kg at about 500 m; (2) dissolved²¹⁰Pb concentrations are uniformly low at about 2 dpm/100 kg with little lateral or vertical variation; (3) the surface-water²¹⁰Pb excess which is commonly observed in low-latitude open ocean regions is entirely lacking; (4)²¹⁰Pb and²¹⁰Po activities are essentially identical to each other in both particulate and dissolved phases although²¹⁰Po activities appear somewhat lower; (5) about 20% of the²¹⁰Pb and²¹⁰Po in the water column residues on particulate matter.Assuming the atmospheric²¹⁰Pb flux to be in the dissolved form and at the lower level of the normal range i.e. 0.5 dpm/cm² yr, the residence time of the dissolved Pb is about 1.5 years. However, if the same atmospheric flux is entirely in particulate form, then the residence time of the dissolved Pb is about 5 years. The residence time of Pb in the particulate phase is less than 0.4 years if all the Pb is removed only by sinking particles.     

Desorption of Ba and226Ra from river-borne sediments in the Hudson estuary

The pronounced desorption of Ba and²²⁶Ra from river-borne sediments in the Hudson estuary can be explained quantitatively by the drastic decrease in the distribution coefficients of both elements from a fresh to a salty water medium. The desorption in estuaries can augment, at least, the total global river fluxes of dissolved Ba and²²⁶Ra by one and nine times, respectively. The desorptive flux of²²⁶Ra from estuaries accounts for 17–43% of the total²²⁶Ra flux from coastal sediments. Two mass balance models depicting mixing and adsorption-desorption processes in estuaries are discussed.     

226Ra behavior in the Pee Dee River-Winyah Bay estuary

Concentrations of dissolved²²⁶Ra in Winyah Bay, South Carolina, and in the adjacent Atlantic Ocean are augmented by the desorption of radium from sediments in the low-salinity area of the estuary and diffusion from bottom sediments. Desorption of²²⁶Ra is reflected by lower concentrations in suspended sediments from higher-salinity regions of the estuary. Bottom sediments from the high-salinity region have lower²²⁶Ra/²³⁰Th activity ratios than those from the low-salinity end.The shape of the dissolved²²⁶Ra vs. salinity profile is influenced by the river discharge. During average-discharge conditions, desorption of²²⁶Ra from suspended and bottom sediments increases the dissolved²²⁶Ra concentrations by a factor of 3.5 as the water passes through Winyah Bay. High river discharge produces an initial increase of dissolved²²⁶Ra by a factor of 2 to 3 and apparently reflects only desorption from suspended sediments. By driving the salt wedge down the estuary and reducing the zone of contact of salt water with bottom sediments, the high-flow conditions sharply reduce the flux of²²⁶Ra from bottom sediments.     

210Pb/226Ra and 210Po/210Pb disequilibria in seawater and suspended particulate matter

The distribution of²¹⁰Po and²¹⁰Po in dissolved (<0.4 μm) and particulate (>0.4 μm) phases has been measured at ten stations in the tropical and eastern North Atlantic and at two stations in the Pacific. Both radionuclides occur principally in the dissolved phase. Unsupported²¹⁰Pb activities, maintained by flux from the atmosphere, are present in the surface mixed layer and penetrate into the thermocline to depths of about 500 m. Dissolved²¹⁰Po is ordinarily present in the mixed layer at less than equilibrium concentrations, suggesting rapid biological removal of this nuclide. Particulate matter is enriched in²¹⁰Po, with²¹⁰Po/²¹⁰Pb activity ratios greater than 1.0, similar to those reported for phytoplankton. Box-model calculations yield a 2.5-year residence time for²¹⁰Pb and a 0.6-year residence time for²¹⁰Po in the mixed layer. These residence times are considerably longer than the time calculated for turnover of particles in the mixed layer (about 0.1 year). At depths of 100–300 m,²¹⁰Po maxima occur and unsupported²¹⁰Po is frequently present. Calculations indicate that at least 50% of the²¹⁰Po removed from the mixed layer is recycled within the thermocline. Similar calculations for²¹⁰Pb suggest much lower recycling efficiencies.Comparison of the²¹⁰Pb distribution with the reported distribution of²²⁶Ra at nearby GEOSECS stations has confirmed the widespread existence of a²¹⁰Pb/²²⁶Ra disequilibrium in the deep sea. Vertical profiles of particulate²¹⁰Pb were used to test the hypothesis that²¹⁰Pb is removed from deep water by in-situ scavenging. With the exception of one profile taken near the Mid-Atlantic Ridge, significant vertical gradients in particulate²¹⁰Pb concentration were not observed, and it is necessary to invoke exceptionally high particle sinking velocities to account for the inferred²¹⁰Pb flux. It is proposed instead that an additional sink for²¹⁰Pb in the deep sea must be sought. Estimates of the dissolved²¹⁰Pb/²²⁶Ra activity ratio at depths greater than 1000 m range from 0.2 to 0.8 and reveal a systematic increase, in both vertical and horizontal directions, with increasing distance from the sea floor. This observation implies rapid scavenging of²¹⁰Pb at the sediment-water interface and is consistent with a horizontal eddy diffusivity of 3?6 × 10⁷ cm²/sec. The more reactive element Po, on the other hand, shows evidence of rapid in-situ scavenging. In filtered seawater,²¹⁰Po is deficient, on the average, by ca. 10% relative to²¹⁰Pb; a corresponding enrichment is found in the particulate phase. Total inventories of²¹⁰Pb and²¹⁰Po over the entire water column, however, show no significant departure from secular equilibrium.     

A deep226Ra maximum in the Northeast Pacific

Seven vertical profiles of²²⁶Ra have been measured along an east-west traverse at about 30°N from San Diego to northwest of Hawaii. These profiles show that there is a distinct core of Ra maximum spreading westward as a tongue in the northeast Pacific deep water. This core starts in the east with 21.1 Ra units (1Ra unit= 10^?14g/kg) at 3.9 km depth at about 130°W, and deepens westward to 4.1 km with its Ra reduced to 18.3 units at 150°W. A similar core with some uncertainty due to possible sampling errors extends westward near the bottom at 5.2 km depth from 19.4 Ra units at 150°W to 15.9 units at about 180° longitude. In addition, these profiles appear to be correlated with each other in structure above the cores of Ra maximum. These cores indicate that the Ra input depends locally on the type and composition of sediments and so the flux varies over the ocean bottom. On the basis of a one-dimensional diffusion-decay model, a horizontal diffusion coefficient of 10⁶ cm²/sec has been computed along these cores. Although this value appears to be slightly lower, it is not inconsistent with those derived from other physical methods.     

A226Ra section across the East Pacific Rise

Four vertical Ra profiles have been measured across the East Pacific Rise (EPR) from Callao to Tahiti. These profiles show that Ra in the deep water (below 2 km depth) increases toward the EPR. However, this increase does not necessarily indicate a Ra source on the EPR. The increase from Tahiti toward the EPR reflects the general trend of the Pacific Ra distribution. The decrease from the EPR eastward to the Peru Basin is probably due to the continental effect with higher sedimentation rates.The hydrography, especially potential temperature and oxygen, indicates significant differences below about 3 km depth between the east and west flanks of the EPR indicating the effect of the cold bottom water to the west of the EPR. The benthic front is identified at 3.9 km depth at the westernmost station near Tahiti. Silicate and salinity data are by no means unique and reflect a complicated local circulation and mixing pattern with a minor intrusion of the Antarctic Bottom Water from the south into the Peru Basin.The θ-Ra and Ra-Si relationships both indicate an enrichment of Ra in the deep water below 2 km depth probably due to input from the underlying sediments. Above 2 km depth, Ra covaries almost linearly with θ as well as Si, mimicking a stable conservative property. This suggests that the radiodecay rate is nearly balanced by the input rate within the water column between 1 and 2 km depth in which θ is linearly correlated withS.Simple vertical model calculations show that the in-situ production of Ra by particulate dissolution in the deep water is negligible within a reasonable range of upwelling rates from 2 to 12 m/yr. Thus the Ra profiles show a net decay effect and so the θ-Ra relations are not linear in the deep water. In fact, the composite θ-Ra plots show a break at 25 dpm/100 kg (at 2 km depth) rather than a smooth curve, while theθ-S plots are essentially linear. A maximum Ra production rate of about 8 × 10^?3 (dpm/100 kg) yr^?1 is obtained from all the profiles with minimum upwelling rates between 0.7 and 3.5 m/yr.     

226Ra and222Rn contents of Galapagos Rift hydrothermal waters —the importance of low-temperature interactions with crustal rocks

Hydrothermal waters collected by “Alvin” from the Galapagos Spreading Center are enriched in²²²Rn by factors of 50–200 over bottom waters. The²²⁶Ra in the same samples, however, is enriched by less than a factor of four over bottom waters. Enrichments of²²²Rn result primarily from α-recoil from rock surfaces while²²⁶Ra enrichments are dominantly produced by high-temperature alteration of cooling ridge volcanics. The abundances of both nuclides exhibit positive correlations with temperature. The data extrapolate to bottom water temperatures and compositions, demonstrating the importance of seawater mixing. Different vents, however, have different mixing lines, and vents with high²²²Rn have low²²⁶Ra. We propose these patterns result from variations in the extent of low-temperature crustal interaction with the hydrothermal fluids. Low-temperature crustal waters can maintain high steady state²²²Rn contents due to the α-recoil additions to the fluids. The²²⁶Ra, however, is strongly adsorbed at low-temperatures resulting in low concentrations of this nuclide in low-temperature crustal waters. Thus, physical mixing of a crustal water component with hydrothermal waters or variable crustal path lengths of the hydrothermal fluids can account for the variable mixing lines and²²²Rn/²²⁶Ra values of the hot springs.The²²²Rn/²²⁶Ra value appears to be a sensitive indicator of low-temperature crustal interaction. Values > 100 have experienced extensive crustal interaction and are indicative of diffuse hydrothermal flow. Values between 1 and 10 are indicative of primary hydrothermal fluids which have not experienced significant interaction with the crust. Values of²²²Rn/²²⁶Ra between 10³ and 10⁴ are indicative of interaction of the hydrothermal fluids with sediments. Such values are observed in water samples from the Galapagos hydrothermal mounds.     

Meridional distribution of226Ra in the eastern Pacific along GEOSECS cruise tracks

We present the distribution of²²⁶Ra in eight vertical profiles from the eastern Pacific. The profiles are located along a meridional trend near 125°W, from 43°S to 29°N. Surface²²⁶Ra concentrations are about 7 dpm/100 kg, except for the two stations south of 30°S where the higher values are due to the Antarctic influence. Deep waters show a distinctive south-to-north increase in the²²⁶Ra content, from about 26 to 41 dpm/100 kg near the bottom. Unlike in the Atlantic and Antarctic Oceans, the effect of²²⁶Ra injection from bottom sediments is clearly discernible in the area. The presence of this primary²²⁶Ra can be traced up to at least 1–1.5 km above the ocean floor, making this part of the sea bed among the strongest source regions for the oceanic²²⁶Ra. Numerical solutions of a two-dimensional vertical advection-diffusion model applied to the deep (1.2–4 km)²²⁶Ra data give the following set of best fits: upwelling velocity(V_z) = 3.5m/yr, vertical eddy diffusivity(K_z) = 0.6cm²/s, horizontal (north-south) eddy diffusivity(K_y) = 1 × 10⁷cm²/s, and water-column regeneration flux of²²⁶Ra(J) = 3.3 × 10^?5dpmkg^?1yr^?1 as an upper limit. These parametric values are in general agreement with one-dimensional (vertical) model fits for the Ra-Ba system. However, consideration of²²⁶Ra balance leads us to suspect the appropriateness of describing the vertical exchange processes in the eastern Pacific with constantV_z and K_z. If future modeling is attempted, it may be preferable to treat the area as a diffusion-dominant mixing regime with depth-dependent diffusivities.     

10Be in marine sediments

The depth profile of the long-lived radionuclide¹⁰Be in a marine sediment recovered in the vicinity of the Samoan Islands has been precisely assayed with a highly sensitive needle-type gas counter. The obtained irregular pattern of¹⁰Be concentrations with depths ranging from 4.7 to 0.3 dpm/kg dry sediment is interpreted as being due to dilution of¹⁰Be by volcanic eruptions in the past.