Plutonium as a chronomarker in Australian and New Zealand sediments: a comparison with Cs

The construction of high resolution chronologies of sediment profiles corresponding to the last 50-100 years usually entails the measurement of fallout radionuclides ²¹⁰Pb and ¹³⁷Cs. The anthropogenic radionuclide, ¹³⁷Cs, originating from atmospheric nuclear weapons testing can provide an important “first appearance” horizon of known age (1954-1955), providing much-needed validation for the sometimes uncertain interpretations associated with ²¹⁰Pb geochronology. However, while ¹³⁷Cs usually provides a strong signal in sediment in the northern hemisphere, total fallout of ¹³⁷Cs in the southern hemisphere was only 25% that of the north and the low activities of ¹³⁷Cs seen in Australian and New Zealand sediments can make its horizon of first appearance somewhat arguable. Low ¹³⁷Cs fallout also limited the size of the 1963-1964 fallout peak, a peak that is usually seen in northern hemisphere sediment profiles but is often difficult to discern south of the equator.This paper shows examples of the use of nuclear weapons fallout Pu as a chronomarker in sediment cores from Australia (3 sites) and New Zealand (1 site). The Pu profiles of five cores are examined and compared with the corresponding ¹³⁷Cs profiles and ²¹⁰Pb geochronologies. We find that Pu has significant advantages over ¹³⁷Cs, including greater measurement sensitivity using alpha spectrometry and mass spectrometric techniques compared to ¹³⁷Cs measurements by gamma spectrometry. Moreover, Pu provides additional chronomarkers associated with changes in the Pu isotopic composition of fallout during the 1950s and 1960s. In particular, the ²³⁸Pu/^239+240Pu activity ratio shows distinct shifts in the early 1950s and the mid to late 1960s, providing important known-age horizons in southern hemisphere sediments. For estuarine and near-shore sediments Pu sometimes has another significant advantage over ¹³⁷Cs due to its enrichment in bottom sediment relative to ¹³⁷Cs resulting from the more efficient scavenging of dissolved Pu in seawater by sediment particles.     

Determining the Chernobyl impact on sediments of a pre-Alpine lake with a very comprehensive set of data

Man-made and natural radionuclides in Lake Wallersee were determined in the pre-Alpine environment at the northern slope of the Alps, which was heavily affected by the Chernobyl fallout in May 1986. The objective of this study was to get knowledge of location and quantity of man-made radionuclide input (especially (137)Cs) generated in the Chernobyl accident to lake sediments. Eleven sediment cores were sampled and activity depth profiles of (137)Cs and (210)Pb were determined with 5mm depth-resolution. The Chernobyl fallout produced an extreme (137)Cs peak in the sediment cores providing an excellent time marker. The chronological interpretation of deeper sediment layers was done by radiochemical analysis of (90)Sr and (239+240)Pu, which were released during atmospheric weapons' tests in the 1950s and 1960s. This allowed a complete chronological analysis of the sediment cores with a very compact set of data.     

Application of the Weibull extrapolation to 137Cs geochronology in Tokyo Bay and Ise Bay, Japan

Considerable doubt surrounds the nature of processes by which 137Cs is deposited in marine sediments, leading to a situation where 137Cs geochronology cannot be always applied suitably. Based on extrapolation with Weibull distribution, the maximum concentration of 137Cs derived from asymptotic values for cumulative specific inventory was used to re-establish 137Cs geochronology, instead of original 137Cs profiles. Corresponding dating results for cores in Tokyo Bay and Ise Bay, Japan, by means of this new method, are in much closer agreement with those calculated from 210Pb method than the previous method.     

Use of 210Pb and 137Cs to simultaneously constrain ages and sources of post-dam sediments in the Cordeaux reservoir, Sydney, Australia

Environmental radionuclides can be employed as tracers of sediment movement and delivery to water bodies such as lakes and reservoirs. The chronologies of sediments that have accumulated in the Cordeaux reservoir in Sydney, Australia, were determined by the rate of change of (210)Pb(ex) with depth and indicate slow accretion in the reservoir. The ratio of enrichment of radionuclides in sediment cores to (210)Pb(ex) and (137)Cs concentrations in a reference soil sample within the Cordeaux catchment indicates that the dominant source of sediment in the Cordeaux reservoir is surface erosion (detachment and removal of sediment at depths less than 30 cm). However, in the Kembla Creek arm of the reservoir a mixture of sources was detected and includes sheet and rill erosion together with sub-soil contributions. Implications for the utility of these radionuclide sedimentation assessments, especially where samples are limited, are that well-constrained chronologies and sources of soil erosion are facilitated.     

137Cs in the Danish Wadden Sea: contrast between tidal flats and salt marshes

The 137Cs activity of salt marsh and tidal flat sediments of the northern part of the European Wadden Sea was studied based on a comprehensive dataset of 210Pb dated cores. The 137Cs inventory of salt marsh sediments shows a major peak corresponding to the Chernobyl accident in 1986, and a minor peak located in the late 1960s interpreted as the combined effect of atmospheric testing of nuclear weapons. Emissions from the nuclear reprocessing plant Sellafield are not reflected as peaks in 137Cs activity, but may contribute to the rising 137Cs activity in the years prior to 1986. The 137Cs activity of tidal flat sediments differs from salt marsh sediment in two respects. First, the activity is much lower and, second, the major peak in the 1980s is located in the beginning instead of in the middle of the decade. The differences in 137Cs inventory between the two environments are interpreted to result from repeated cycles of deposition/resuspension and mixing on tidal flats. A simple model illustrating the consequence of mixings returns an apparent shift of major peaks in 137Cs activities backwards in time corresponding to the mixing depth divided by the deposition rate.     

Evaluation of 137Cs fallout from the Chernobyl accident in a forest soil and its impact on Alpine Lake sediments, Mercantour Massif, S.E. France

The Boréon area in the Mercantour Massif, S.E. France, was contaminated by radionuclides after the Chernobyl accident in the first days of May 1986. Sediments from a small mountain lake in this area were collected, as well as forest soils in its vicinity, in order to obtain 137Cs and 210Pb profiles. Calculated from the 210Pb inventory in a soil of a horizontal area, the flux is high in the area (0.06 Bqcm(-2)y(-1)) probably because of the great frequency of rain and uranium ores outcropping in the massif. The comparison of the 137Cs soil inventories and the unsupported 210Pb suggests that the 137Cs fallout due to the Chernobyl accident in the study site (Boréon) was at least 3.5 Bqcm(-2), more probably the double. The recent lake sediments still undergo a rather strong contamination by 137Cs and the sediment profiles show that the residence time of 137Cs in the catchment area is long. The study area is frequented by many inhabitants of the city of Nice and other cities at the Mediterranean coast during week-end and during summer and winter holidays. Thus the 137Cs external exposure impact was evaluated at 2 mSvy(-1) for 2002 in the most contaminated point.     

Estimating the date corresponding to the horizon of the first detection of 137Cs and 239+240Pu in sediment cores

The anthropogenic bomb fallout nuclides 137Cs and plutonium isotopes (240Pu, 239Pu) are important chronometers for the determination of recent sediment accumulation rates using sediment cores collected from various water bodies. One of the crucial time horizons used to date sediment core profiles corresponds to the date of first detection of these nuclides. Although atmospheric nuclear testing began during the mid-1940s, the year corresponding to a nuclide's first detection when measured in 2006 depends on a number of factors including fallout history, radioactive half-life, gamma/alpha detection limits, geographic latitude and the accumulated thickness of the sediment section. This paper reports estimations of the year of first detection in sediment profiles of fallout 137Cs and Pu measured by gamma and alpha spectrometry, respectively. We find that for the latitude 30-40 degrees south of the equator the year of first detection for 137Cs is 1955. The date is earlier in the northern hemisphere due to higher fallout rates. Due to better measurement sensitivity first detection of Pu is generally earlier than 137Cs by 1-2 years.     

Inventories of fallout 210Pb and 137Cs radionuclides in moorland and woodland soils around Edinburgh urban area (UK)

Inventories of fallout (210)Pb and (137)Cs have been measured in moorland and woodland soils around the Edinburgh urban area, using a high purity germanium detector. The (210)Pb inventories in moorland soils were relatively uniform, with a mean value of 2520+/-270Bqm(-2). The mean (137)Cs inventory in moorland soils varied greatly from 1310 to 2100Bqm(-2), with a mean value of 1580+/-310Bqm(-2). The variability was ascribed mainly to the non-uniform distribution of fallout Chernobyl (137)Cs. The mean (210)Pb and (137)Cs inventories in woodland canopy soils were found to be 3630+/-380Bqm(-2) and 2510+/-510Bqm(-2), respectively. At sites for which both moorland and woodland data were available, the mean inventories provided fairly similar average enhancements of (47+/-7)% and (46+/-18)% of (210)Pb and (137)Cs under woodland canopy soils relative to open grassland soils, respectively. The enhancement factors are broadly in line with other independent findings in literature. Enhancement of both (210)Pb and (137)Cs in woodland soils relative to moorland soils is, in part, due to deposition by impaction during air turbulence, wash-off, gravitational settling and deposition during leaf senescence. Results of this study suggest that these processes affect both (210)Pb and (137)Cs carrier aerosols in a similar way.     

Radionuclide tracing of water masses and processes in the water column and sediment in the Algerian Basin

Caesium-137 and (239,240)PU were analysed in the water column along the Algerian coast. The (137)Cs activity concentration in surface water increased from the west to the east from 1.6 to 3.3 mBq L(-1), documenting a presence of Modified Atlantic Water (MAW) in the region. Higher concentrations observed in deep waters may be due to an intrusion of Levantine Intermediate Water (LIW), which has been carrying higher levels of (137)Cs from Chernobyl accident. The (239,240)Pu sub-surface concentration peaked at about 250 m water depth as a result of biogeochemical processes in the water column. The observed (239,240)Pu/(137)Cs activity ratio at the surface (0.003) was significantly lower than that in global fallout (0.04). This decrease exceeds that expected from radioactive decay of (137)Cs, and confirms that Pu due to its adsorption on sinking particles is more effectively removed from surface layers than is (137)Cs. An increase of the (239,240)Pu/(137)Cs activity ratio with depth suggests that (239,240)Pu, similarly as (137)Cs, should be also transported by advection to maintain the observed ratios in deep waters. An intrusion of LIW may enhance therefore both the (137)Cs and (239,240)Pu concentrations in deep waters. The average (238)Pu/(239+240)Pu activity ratio in seawater was 0.03+/-0.02, confirming a global fallout origin of Pu in the Algerian Basin. Caesium-137 and (239,240)Pu inventories in the water column were estimated to be from 2.7+/-0.5 kBq m(-2) to 3.8+/-0.7 kBq m(-2), and from 13.8+/-2.6 Bq m(-2) to 41+/-7B qm(-2), respectively. The (137)Cs massic activities in surface sediment were almost constant, the average activity was 9.0+/-0.8 Bq kg(-1). Sedimentation rates obtained using the (210)Pb method were from 0.1 to 0.7 cm y(-1), and resulting penetration depths of (137)Cs in the sediment cores were from 15 to over 40 cm. The (137)Cs peaks found in the sediment cores were associated with the Chernobyl accident (1986) and global fallout (1964). The (137)Cs inventories in the sediment were increasing from the west (180 Bq m(-2)) to the east (350 Bq m(-2)).     

Physical resuspension and vertical mixing of sediments on a high energy continental margin (Sydney, Australia)

Four sediment cores from the continental margin adjacent to Sydney were analyzed for 210Pb, 137Cs, trace metals (Ag, Cd, Co, Cu, Mn, Ni, Pb, Zn), iron, dry bulk density, mud and moisture content. The concentrations of trace metals in the total sediment are low at all sites, although slightly elevated concentrations of Ag, Cu, Pb and Zn are present in the fine fraction of sediment (< 62.5 microns) near a major ocean outfall. Concentrations of trace metals in the fine fraction of sediment are similar in the upper 10-15 cm, indicating strong vertical mixing of the sediments, whereas an upward coarsening grain size in the upper 1-3 cm of sediment supports physical resuspension during storms. Sediment accumulation rates on the middle shelf adjacent to Sydney were estimated from downcore profiles of 210Pb and 137Cs and range between 0.2 and 0.4 cm yr-1. Although the mass fluxes of Cu, Pb and Zn within a distance of 2 km from the outfall (up to 36.1, 30.8 and 86.2 micrograms cm-2 yr-1, respectively) are greater than 20 km north of the outfall (< 23.5 micrograms cm-2 yr-1), the low concentrations of trace metals in sediments near the outfall support an efficient dispersal of anthropogenic contaminants on this continental margin.     

Recent atmospheric lead deposition recorded in an ombrotrophic peat bog of Great Hinggan Mountains, Northeast China, from Pb and Cs dating

Radioactive markers are useful in dating lead deposition patterns from industrialization in peat archive. Peat cores were collected in an ombrotrophic peat bog in the Great Hinggan Mountains in Northeast China in September 2008 and dated using ²¹⁰Pb and ¹³⁷Cs radiometric techniques. The mosses in both cores were examined systematically for dry bulk density, water and ash content. Lead also was measured using atomic emission spectroscopy with inductively coupled plasma (ICP-AES). Both patterned peat profiles were preserved well without evident anthropogenic disturbance. Unsupported ²¹⁰Pb and ¹³⁷Cs decreased with the depth in both of the two sample cores. The ²¹⁰Pb chronologies were established using the constant rate of supply model (CRS) and are in good agreement with the ¹³⁷Cs time marker. Recent atmospheric ²¹⁰Pb flux in Great Hinggan Mountains peat bog was estimated to be 337 Bq m⁻² y⁻¹, which is consistent with published data for the region. Lead deposition rate in this region was also derived from these two peat cores and ranged from 24.6 to 55.8 mg m⁻² y⁻¹ with a range of Pb concentration of 14-262 μg g⁻¹. The Pb deposition patterns were consistent with increasing industrialization over the last 135-170 y, with a peak of production and coal burning in the last 50 y in Northeast China. This work presents a first estimation of atmospheric Pb deposition rate in peatlands in China and suggests an increasing trend of environmental pollution due to anthropogenic contaminants in the atmosphere. More attention should be paid to current local pollution problems, and society should take actions to seek a balance between economic development and environmental protection.     

Physico-chemical and toxicological characterization of the historic estuarine sediments: a multidisciplinary approach

The accumulation rates, the geochronology of metals and PAH contamination, and the Microtox toxicity are studied in five sediment cores (50 cm length) covering different areas of the Santander Bay, Northern Spain. Chronology given by (210)Pb and (137)Cs reveals significant differences in accumulation rates between sites (0.2-1.1 cm/year), as well as a variable degree of anthropogenic enrichment factors for Fe, Mn, Cu, Pb, Zn, Ni (from 1 to 15) and concentrations of summation Sigma 16PAHs (from 0.01 to 23.84 mg/kg dw) in sediments over the last 90 years. The results indicate the increasing contamination pressure from industrial and urban activities along the Bay. No toxic results from the Microtox test are obtained either with pore water or with normalised sediment aqueous extracts (European Norm EN 12457), suggesting low water solubility and low availability of contaminants in the studied sediments. However, the EC50 values from the Microtox Basic Solid Phase Test (BSPT) ranged from 0.03% to 2.35%, showing vertical toxicity profiles in accordance with metal and PAHs behaviour. The correlation degrees of Microtox BSPT toxicity to chemical concentration in sediment profiles are widely variable showing a high site-dependent toxicity. The oligochaete Limnodrilus hoffmeisteri has been used as a chronic bioassay over surface sediments of two of the studied sites, showing results coherent with the Microtox BSPT acute test results. Global results of the present work provide regional geochemical baselines for metals and PAHs and toxicological data now make it possible to obtain a preliminary quality assessment of the Santander Bay sediment profiles.     

210Pb as a tool for establishing sediment chronologies: examples of potentials and limitations of conventional dating models

For aquatic sediments, the use of ²¹⁰Pb originating from the decay of atmospheric ²²²Rn is a well-established methodology to estimate sediment ages and sedimentation rates. Traditionally, the measurement of ²¹⁰Pb in soils and sediments involved laborious and time-consuming radiochemical separation procedures. Due to the recent development of advanced planar (‘n-type’) semi-conductors with high efficiencies in the low-energy range which enable the gamma-spectrometric analysis of the 46.5 keV decay line of ²¹⁰Pb, sediment dating using this radionuclide has gained renewed interest.In this contribution, potentials and limitations of the ²¹⁰Pb methodology and of the models used for estimating sediment ages and sedimentation rates are discussed and illustrated by examples of freshwater and marine sediments. Comparison with the use of ¹³⁷Cs shows that the information which may be gained by these two tracers is complementary. As a consequence, both radionuclides should be used in combination for dating of recent sediments. It is shown that for various sedimentation regimes additional information from other sources (e.g. sediment lithology) may be needed to establish a reliable chronology. A strategy for sediment dating using ²¹⁰Pb is recommended.     

Sediment accumulation rate and radiological characterisation of the sediment of Palmones River estuary (southern of Spain)

Chemical analyses and radioecological methods were combined in order to estimate the sediment accumulation rate in the upper 20 cm depth of the Palmones River estuary. Organic matter, total carbon, C:N and (137)Cs vertical profiles showed changes at 13 cm depth. These changes could be associated with the decrease in river input since 1987 when a dam situated in the upper part of the estuary started to store water. Using 1987 as reference to date the sediment, accumulation rate was 1.2 cm yr(-1). As alternative method, two layer model of (210)Pb(xs) vertical distribution showed a sedimentation rate of 0.7 cm yr(-1) with a surface mixing layer of 7 cm thickness. The high ammonium, potassium and sodium content in pore water and the strong correlation between (137)Cs activities and organic matter in dry sediment suggests that (137)Cs (the only anthropogenic product detected) is mainly accumulated in the estuary associated with the particulate organic material from the catchment area.     

210Pb and 137Cs as chronometers for salt marsh accretion in the Venice Lagoon - links to flooding frequency and climate change

Five salt marsh sediment cores from different parts of the Venice Lagoon were studied to determine their depositional history and its relationship with the environmental changes occurred during the past approximately 100 years. X-radiographs of the cores show no disturbance related to particle mixing. Accretion rates were calculated using a constant flux model applied to excess (210)Pb distributions in the cores. The record of (137)Cs fluxes to the sites, determined from (137)Cs profiles and the (210)Pb chronologies, shows inputs from the global fallout of (137)Cs in the late 1950s to early 1960s and the Chernobyl accident in 1986. Average accretion rates in the cores are comparable to the long-term average rate of mean sea level rise in the Venice Lagoon ( approximately 0.25 cm y(-1)) except for a core collected in a marsh presumably affected by inputs from the Dese River. Short-term variations in accretion rate are correlated with the cumulative frequency of flooding, as determined by records of Acqua Alta, in four of the five cores, suggesting that variations in the phenomena causing flooding (such as wind patterns, storm frequency and NAO) are short-term driving forces for variations in marsh accretion rate.     

Distribution and inventories of fallout radionuclides (239+240Pu, 137Cs) and 210Pb to study the filling velocity of salt marshes in Doñana National Park (Spain)

Within an extensive multinational and multidisciplinary project carried out in Do?ana National Park (Spain) to investigate its preservation and regeneration, the filling velocity of the salt marshes has been evaluated through the calculation of their average sediment accumulation rates. (239+240)Pu and (137)Cs from weapons testing fallout and total (210)Pb distribution profiles and inventories have been determined in some of the most characteristic zones of the park, namely, the ponds (or "lucios") and the waterjets (or "ca?os"). Plutonium inventories range from 16 to 101 Bq m(-2), (137)Cs values fluctuate between 514 and 3,758 Bq m(-2) and unsupported (210)Pb values comprise between 124 and 9398 Bq m(-2). Average sedimentation rates range from 3 to 5 mm y(-1) (1952-2002). These data are higher than those obtained by carbon dating for the period 6,500 AD-present, estimated as 1.5-2 mm y(-1), suggesting an increase in the accumulation of sediments and the alteration of the park's hydrodynamics caused by the re-channeling of the major rivers feeding the salt marshes.     

Sedimentation rates and trace metal input history in intertidal sediments from San Simón Bay (Ría de Vigo, NW Spain) derived from 210Pb and 137Cs chronology

(210)Pb and (137)Cs dating methods, accompanied by a high-resolution geochemical study, were applied to intertidal sediments containing both fine and coarse-grained particles and also, anthropogenic Pb in order to establish sedimentation rates and historical trends in heavy metal input. Sedimentation rates were established according to the "Constant Flux:Constant Sedimentation" (CF:CS) (210)Pb dating model, which was preferred rather than the "Constant Rate of Supply-Minimum Variance" (CRS-MV) model. Variations in sediment grain-size were accounted for by application of several normalization procedures. Al was selected for grain-size correction. Corrected sedimentation rates obtained from (210)Pb dating were corroborated through a second independent radionuclide tracer and by comparison of peak trace metal inputs into the environment with peaks in the sediment. The Chernobyl maximum was identified in the normalized (137)Cs activity profile. Sedimentation rates of 6.2+/-1.2 mm y(-1) and 3.1+/-0.5 mm y(-1) for the upper (two muddy layers) and 6.0+/-2.0 mm y(-1) for the lower (sandy) intertidal mud flat deposits of San Simón Bay were determined. According to the established chronology, human-induced environmental changes were detected in total metal concentrations (Cu, Pb, Zn) and in sediment grain-size and composition.     

Geochronology of anthropogenic radionuclides in Ribeira Bay sediments, Rio de Janeiro, Brazil

Ribeira Bay is located approximately 130 km south of the city of Rio de Janeiro and receives discharges of liquid effluent from the Angra dos Reis nuclear power plant (NPP) site, where two pressurized water reactors are located. To test whether the presence of anthropogenic radionuclides in sediments in Ribeira Bay could be correlated to the NPP operations, we sampled seven sediment cores and determined accumulation rates and chronologies. Only one sediment core did not exhibit a superficial mixing layer; this sample was used for dating purposes. Cesium-137 and ²⁰⁷Bi were observed in this sediment profile, but their presence was associated with atmospheric fall-out rather than the nearby NPP. The exponential decay of ²¹⁰Pb concentration with sediment layer depth was verified below a superficial mixing layer for all other sediment cores. Calculated accumulation rates ranged from 1.2 mm y⁻¹ in the inner bay to 6.2 mm y⁻¹ close to its entrance.     

Determining floodplain sedimentation rates using Cs in a low fallout environment dominated by channel- and cultivation-derived sediment inputs, central Queensland, Australia

Fallout ¹³⁷Cs has been widely used to determine floodplain sedimentation rates in temperate environments, particularly in the northern hemisphere. Its application in low fallout, tropical environments in the southern hemisphere has been limited. In this study we assess the utility of ¹³⁷Cs for determining rates of floodplain sedimentation in a dry-tropical catchment in central Queensland, Australia. Floodplain and reference site cores were analysed in two centimetre increments, depth profiles were produced and total ¹³⁷Cs inventories calculated from the detailed profile data. Information on the rates of ¹³⁷Cs migration through local soils was obtained from the reference site soil cores. This data was used in an advection–diffusion model to account of ¹³⁷Cs mobility in floodplain sediment cores. This allowed sedimentation rates to be determined without the first year of detection for ¹³⁷Cs being known and without having to assume that ¹³⁷Cs remains immobile following deposition. Caesium-137 depth profiles in this environment are demonstrated to be an effective way of determining floodplain sedimentation rates. The total ¹³⁷Cs inventory approach was found to be less successful, with only one of the three sites analysed being in unequivocal agreement with the depth profile results. The input of sediment from catchment sources that have little, or no, ¹³⁷Cs attached results in true depositional sites having total inventories that are not significantly different from those of undisturbed reference sites.     

Reinvestigation of airborne 210Pb, 137Cs and 207Bi in Vienna (Austria) after atmospheric nuclear weapons tests

Reconstruction of atmospheric 210Pb and 137Cs activity concentrations occurring in Vienna immediately after the atmospheric nuclear weapons tests shall answer the question, whether artificial 210Pb has been produced by fusion devices using lead materials. If so, 207Bi also can be expected. In 1962, weekly average values for 210Pb were between 0.08 +/- 0.02 and 1.31 +/- 0.30 mBq/m2, 137Cs amounts up to 5.1 +/- 0.6 mBq/m3. 207Bi remains below the detection limit, viz. < 0.5 mBq/m3. Bimonthly averages for the periods 1962-1964 and 1974-1975 show 137Cs activity concentrations with typical springtime maxima occurring together with low 210Pb values and 207Bi < 0.02 mBq/m3. Annual averages of 210Pb are varying between 0.27 and 0.53 mBq/m3, independent of whether atmospheric tests have been performed or not. Comparison of the activity ratios 207Bi/210Pb, 207Bi/137Cs and 210Pb/137Cs with published data, leads to the conclusion that no evidence exists for a significant production of 210Pb by nuclear explosions, neither after the Soviet tests in 1961-1962 nor after the Chinese tests in 1973-1976.