PAPER www.rsc.

org/jem | Journal of Environmental Monitoring

Re-construction and updating our understanding on the global weapons

tests 137Cs falloutw
Michio Aoyama,* Katsumi Hirose and Yasuhito Igarashi
Received 6th September 2005, Accepted 16th February 2006
First published as an Advance Article on the web 9th March 2006
DOI: 10.1039/b512601k

Global nuclear weapons tests fallout of 137Cs in the northern hemisphere has been documented in
the UNSCEAR (United Nations Scientific Committee on the Effect of Atomic Radiation) reports.
However, many questions have arisen during the past three to four decades; e.g. the water column
inventory of 137Cs in the North Pacific Ocean was two to three time higher than the cumulative
decay corrected fallout at the same latitude as stated in the UNSCEAR reports. Here we show
more precise spatial distribution of global 137Cs fallout primarily on the basis of global
measurements in rain, seawater and soil, as data from 101
101 grids. A typical feature of
geographical distribution is that two high global 137Cs fallout areas exist in the northern
hemisphere, where the highest 137Cs fallout was observed in the globe. These areas correspond to
crossovers of areas where larger precipitation amounts were expected and where higher
stratosphere–troposphere exchange was expected. Our new estimate of 765  79 PBq as global
137
Cs fallout for the northern hemisphere is 1.4 times higher than that of 545 PBq in the
UNSCEAR reports.

Introduction
The fallout from the atmospheric nuclear weapons tests in the
late 1950s and early 1960s is the main source of artificial
radionuclides in the terrestrial environment. In this context,
‘‘fallout’’ refers to the radioactive debris originated from
atmospheric nuclear weapons tests dispersed via troposphere
or stratosphere circulation from nuclear test sites throughout
the world. Our knowledge of global fallout phenomena largely
depends on the result of the collaborative efforts of the United
Nations Scientific Committee on the Effect of Atomic Radia-
tion (hereafter UNSCEAR) reports. The UNSCEAR re-
ports1–3 describe the global data and show how radionuclide
deposition was dependent on latitude. On the other hand, it
was noticed that water column inventories of 137Cs (see eqn (2)
for definition) in the North Pacific Ocean were greater than the
global fallout at the same latitude described in the UN-
SCEAR.4–6 Aoyama et al.,7 however, revealed that the water
column inventories of 137Cs at three stations around 29–351 N,
140–1601 E during the period from 1973 to 1997 correspond to
93–74% of cumulative decay corrected fallout (see eqn (1) for
definition) for Tokyo at the time of sampling. This result
means that the 137Cs water column inventory in the ocean was
comparable with global 137Cs fallout at the adjacent land
stations, while the cumulative decay corrected fallout in Tokyo
was about two times larger than that estimated in the UN-
SCEAR reports. Although 99Tc/137Cs ratios in seawater near
Geochemical Research Department, Meteorological Research Institute,
305-0052, Japan. E-mail: maoyama@mri-jma.go.jp; Fax: +81-29-
853-8728; Tel: +81-29-853-8719
w Electronic supplementary information (ESI) available: tables of
fallout data and a map of sampling locations. See DOI: 10.1039/
b512601k
Japan coincide with theoretical value8 of 1.4
104, the 99Tc
inventory in Japanese soils derived from 137Cs deposition
based on the estimation in the UNSCEAR1 at the latitude
30–401 N show that an estimate of cumulative decay corrected
fallout of 137Cs by the UNSCEAR might be lower by a factor
about two (Tagami, personal communication). These findings
suggest that the 137Cs in water column inventories in the mid-
latitude of the western North Pacific and 99Tc inventory in the
Japanese soils were comparable with the cumulative decay
corrected fallout in the corresponding area originating from
global fallout.
On the other hand, Renaud and Louvat9 confirmed that
137
Cs fallout observed at a few sites in France was in good
agreement with that at the same latitude reported in the
UNSCEAR. This means that the 137Cs fallout at continental
land stations might be well described by the UNSCEAR
model.
Sigurgeirsson et al.,10 however, found that, on the average, a
137
Cs inventory in soils (see eqn (3) for definition) in Iceland
was 2000 Bq m2, whereas the UNSCEAR reports have given
1300 Bq m2 to the same area at the time of sampling. Their
finding also suggests that UNSCEAR underestimates of 137Cs
deposition in the 60–701 N latitude band.
Simon et al.11 recently presented a geographical pattern of
137
Cs global fallout in the continental US. They showed the
geographical pattern of 137Cs global fallout as of 1971; high in
the eastern US and low in the western US in which primarily it
was reflecting the greater long-term average precipitation rates
in the eastern US compared to the western US within the
continental US. Their result shows that on a continental scale,
fallout at the same latitude might vary by a factor of two or
more. Therefore, it is important to create a global geographi-
cal pattern of 137Cs deposition including lands and oceans. It is

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also important to be able to distinguish global fallout from
other sources of man-made radioactivity, and therefore to
have a good estimation qualifying the level of global fallout in
areas where it has not previously been measured.10
Among the radionuclides originating from the atmospheric
nuclear weapons tests, long-lived radionuclide 137Cs (half life
30 years) is regarded as one of the most important radio-
nuclides from the point of view of radioactive contamination
due to its longer half life. It is also important that 137Cs is one
of the useful tracers for oceanographic studies for the decadal
time scale.12,13 Therefore time-series data of 137Cs deposition
on the sea surface as a source term for Ocean General
Circulation Models is essential for oceanographic studies.
Smith et al.14 studied a river runoff of 137Cs in a global scale
using the UNSCEAR zonal averaged data, however, we
believe that it is better to use more realistic data such as
101
101 grid data.
Here, we present re-constructed global 137Cs fallout as 101

101 grid data and discuss fuller geographical description of
137
Cs global fallout.
Methods of construction of 101
101 data
We have been collecting literature to construct databases for
the study of global 137Cs fallout and other anthropogenic
radionuclides and have created the ‘‘Historical Artificial
Radionuclides in the Pacific Ocean and its Marginal Seas’’
database15 including 90Sr, 137Cs and 239,240Pu concentration
data in the seawater of the Pacific Ocean and its marginal seas.
The data in the HAM database have been collected from
about 90 documents, consisting of published papers,16–71
annual reports by the Hydrographic Department, Maritime
Safety Agency, Japan,72–104 and unpublished data provided by
individuals (K. M. Wong, V. E. Noshikin and H. D. Living-
ston; personal communication). The present HAM database
includes 7737 records of 137Cs concentration data, 3972 re-
cords of 90Sr concentration data and 2666 records of 239,240Pu
concentration data.
The Integrated Global Fallout Database (IGFD) includes
information on worldwide fallout data. This database contains
monthly fallout 90Sr, 137Cs and 239,240Pu at more than 200
stations around the world during the period from 1954 to
1998. The data in the IGFD database have been collected from
45 documents.105–150
The Integrated Global Soil Database (IGSD) provides
information on the 137Cs concentrations and inventories in
the soil for 397 stations. The data in the IGSD database have
been collected from 72 published papers.151–222 We also ob-
tained the 137Cs inventories in the icecore at 3 stations.223–225
To estimate 137Cs cumulative decay corrected fallout, CDtr,
water column inventory of 137Cs, IWt, and 137Cs inventory in
soil, ISt, we calculated these values using eqn (1), (2) and (3) as
follows.
(1) 137Cs cumulative decay corrected fallout at year tr
(with tr = 1969):
X
tr
CDtr ¼ Dt elðtrtÞ ð1Þ
t¼1945
432 | J. Environ. Monit., 2006, 8, 431–438
CDtr: cumulative decay corrected fallout at year tr (Bq m2),
l: radioactive decay constant of 137Cs, Dt: annual deposition
of 137Cs at year t (Bq m2).
(2) 137Cs water column inventory at the time of sampling:
X
N 1
1
IWt ¼ ðwiþ1 þ wi Þðdiþ1  di Þ ð2Þ
2
i¼1
IWt: water column inventory (Bq m2), wi: 137Cs concentra-
tion in water at depth i (Bq m3), di: i-th sampling depth of sea
water (m), N: number of sampling layer, (3) 137Cs inventory in
soil at the time of sampling.
X
N1
1
ISt ¼ ðSiþ1 þ Si Þðdiþ1  di Þ ð3Þ
i¼1
2
ISt: soil inventory (Bq m2), Si: 137Cs concentration in soil at
depth i (Bq m3), di: i-th sampling depth of soil (m), N:
number of sampling layer.
The method used to estimate the global deposition of 137Cs
comprises three steps.
137
Step 1. Fallout Cs at the end of 1969
We chose ‘‘at the end of 1969’’ as a primary target because
decay corrected accumulative 137Cs fallout had reached a
maximum between 1968 and 1972. Observed deposition data
were used to calculate radioactive cumulative decay corrected
fallout using eqn (1) up to the end of 1969. Only a few stations
have a complete history to obtain cumulative decay corrected
fallout at the end of 1969 for the fallout time series. Much of
the data shows an incomplete history, so we estimated cumu-
lative decay corrected fallout assuming that the fallout history
at the target station was proportional to that at the Meteo-
rological Research Institute at the same time.
137
Cs data for seawater were used to calculate 137Cs inven-
tory in the water column using eqn (2) at the time of sampling
and radioactive decay was corrected to the end of 1969. For
the 137Cs inventory in seawater, we used only the data between
1963 and 1969 to avoid effects of relatively rapid movement of
137
Cs in the ocean interior.7
137
Cs concentrations in the soil were used to calculate 137Cs
inventory using eqn (3) at the time of sampling and radioactive
decay was corrected to the end of 1969. To avoid the effect of
soil erosion and accretion, we used the data at sites stated as
reference site or not disturbed site in the literature. We used
the data between 1963 and 2001. In case when Chernobyl
fallout affected the 137Cs inventory in soil, we corrected data
obtained after 1985 by subtracting the Chernobyl fallout
portion.
For the 137Cs inventory in the ice core, radioactive decay
was also corrected to the end of 1969. A map of 137Cs
deposition in Russia (Fig. 3.6 in Izrael146) was published and
we obtained a grid datum of 137Cs deposition from the map.
It became feasible to merge 137Cs cumulative decay cor-
rected fallout and 137Cs inventories in water column, in soil
and in icecore at this stage. 713 data items had obtained to
construct geographic pattern of 137Cs fallout. The locations
for 713 data are shown in Fig. 1 in the ESI.w
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Step 2. 101 by 101 grid data
The 713 data items were converted to grid data in 101 latitude
by 101 longitude by averaging the data within the same grid.
For the northern hemisphere, observed values cover 154 of 324
grids. The values at 57 grids within residual 170 grids were
given by interpolation using the values of the adjacent grids
and the values at 3 grids were given by extrapolation.
Step 3. Assume a proportional relationship between precipitation
and deposition
To estimate the 137Cs deposition in the remaining grids in
which data was not available in step 2, we applied propor-
tional relationships between precipitation and deposition.
We could estimate 137Cs deposition at 110 grids in the
northern hemisphere from the relationships between precipita-
tion and deposition at the adjacent grids. Recent progress of
the study of the precipitation on the earth’s surface provides a
global data set of the precipitation. The data set is ‘‘The
Global Precipitation Climatology Project (hereafter GPCP)
data’’ which is an element of the Global Energy and Water
Cycle Experiment (GEWEX) of the World Climate Research
program (WCRP).226 It provides monthly mean precipitation
data on a 2.5
2.51 latitude–longitude grid for the period
1987–1998. The GPCP data was accomplished by merging
infrared and microwave satellite estimates of precipitation
with rain gauge data from more than 30 000 stations. An
annual mean precipitation amount in each 10
101 latitu-
de–longitude grid was calculated for this study to adjust the
grid size between precipitation data and fallout data.
Although these climatologies of global precipitation for the
period from 1987 to 1998 might not the same as the climato-
logies for our study period of 1945 to 1970, we believe that
GPCP data used in this study could presently be one of the
best present datasets for estimating global precipitation. It
should be also noted that the method described here empiri-
cally contain contribution of dry deposition. The estimates for
fallout in the arid area are likely to be over-estimated.
Finally, we fill 324 grids with 101 by 101 longitude–latitude
in the northern hemisphere. We could fill only 144 grids north
of 401 S in the southern hemisphere due to less availability of
raw data. 101 by 101 longitude–latitude grid data are shown in
Tables 1-1, 1-2, 1-3 and 1-4 in the ESI.w
Estimation of uncertainty
Uncertainty of fallout 137Cs in 101
101 data obtained in this
study had been estimated from the standard deviations (one
sigma) at each grid. As mentioned above, 154 of 324 grids in
the northern hemisphere were filled with the observations. The
raw data numbers in each grid ranged from 1 to 99 with an
average of 3.8, while the standard deviations ranged from
2.4% to 200%. We corrected radioactive decay to the end of
1969 for 137Cs inventory in the water column, in the soil and in
the icecore as described in the method section. This radioactive
decay correction to a reference date of 1969 for the inventories
for different years between 1963 and 2001 might produce a
discrepancy of several percent in the values in the manner by
cumulative decay corrected fallout up to 1969. The inventories
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for the water column, the soil and the icecore observed
between 1963 and 1985 would have discrepancies within 5
percent and about half of the raw data of inventories in water
column and in soil exist within these years. This 5 percent
discrepancy was small enough for those of the variability of
137
Cs fallout within a 101 by 101 grid. Therefore this effect was
neglected in our dataset. For the inventories in soil affected by
Chernobyl fallout after 1986, we subtracted 10% as combined
effect of Chernobyl fallout and decay correction from the
corresponding data.
Since the fallout of 137Cs in each grid and the size of the area
of each grid were varied as functions of latitude, fallout 137Cs
was converted to total depositions with the uncertainty as
expressed by standard deviation at the grids where raw data
were available. Then the uncertainty for integrated fallout in
the northern hemisphere was calculated by propagation of
‘‘error’’ and it was 6.0%, 386  23 PBq for sum of 153 of 324
grids in which observed values exist.
The interpolation (57 grids), estimation from GPCP pre-
cipitation (111 grids) and extrapolation (3 grids) would give
larger uncertainty rather than 6.0% based on the observations
as mentioned above. When we assume 20% uncertainty for the
other half of 324 grids, as 379  76 PBq, a combined
uncertainty for 324 grids in the northern hemisphere would
be 10%. Then we finally estimate that the uncertainty for
integrated fallout in the northern hemisphere would be
765  79 PBq.
Results and discussion
Global distribution
The geographical distribution of global 137Cs fallout is shown
in Fig. 1. A typical feature of geographical distribution in the
northern hemisphere is that two localized regions of the ocean
with higher global 137Cs fallout than in adjacent regions. One
is the Kuroshio and the Kuroshio extension areas at the
latitude of 20–401 N in the Pacific Ocean. Another is in the
Gulf Stream areas at the latitude of 30–501 N in the Atlantic
Ocean. These regions are crossroad of larger precipitation
region and higher stratosphere–troposphere exchange region.
Beekmann et al.227 showed that stratosphere–troposphere
exchange concentrated in the latitude band 40–701 with re-
gional maxima in the east of North America and Asia and in
Europe.227 Stratosphere–troposphere exchange was a main
source of 137Cs in the troposphere air during the periods in
1960s. For the 137Cs depositions on the land stations, a good
positive relationship between deposition and precipitation
amount was widely accepted.228 Aoyama and Hirose229 re-
cently revealed that a good positive relationship between
deposition and precipitation amount was also existent over
the ocean.
The global pattern of precipitation reflects the heat and
fresh water flux from the Equator towards the North Pole
along the Kuroshio and the Gulf Stream. Therefore we can
conclude that crossing of large precipitation amounts and
higher stratosphere–troposphere exchange would be the main
cause to produce the localized regions of ocean appearing at
the Kuroshio and the Gulf Stream regions as shown in Fig. 1.
J. Environ. Monit., 2006, 8, 431–438 | 433
 137
Table 1 Summary of global Cs deposition in the form of the
UNSCEAR model

Average/ Integral/ Range/ UNSCEAR/

Latitude/1 Bq m2 PBq Bq m2 Bq m2
Northern hemisphere
85 900 3.5 820–990 280
75 1970 22.8 880–5280 800
65 3420 64.5 1110–8060 2050
55 5040 128.9 2770–7910 3430
45 5090 159.8 1540–10230 3830
35 4100 149.0 700–10630 2780
25 2620 105.0 120–6430 2110
15 1820 77.6 380–7280 1420
5 1300 57.3 410–3860 970
Southern hemisphere
5 800 35.1 100–1210 510
15 530 22.8 120–1060 440
25 470 18.7 170–830 750
35 580 21.1 150–1430 810
45 NA
55 NA
65 NA
75 NA
85 NA

the northern hemisphere. Since UNSCEAR1 stated 545 PBq

Fig. 1 Re-constructed global 137
Cs fallout as of 1 January, 1970
(Bq m2).
In the Arctic region, lower global fallout occurred in the
northern hemisphere. Lower 137Cs fallout regions were ob-
served at the desert and arid areas. In the lower latitude at
10–201 N latitude, the relatively higher 137Cs fallout regions
were observed. Although weaker stratosphere–troposphere
exchange was expected, the largest precipitation amount in
the east of the Indian peninsula and South China Sea would
cause the relatively higher 137Cs fallout at these regions.
and Playford et al.231 stated 574 PBq for the corresponding
value, respectively, our newly estimated global fallout of 137Cs
in the northern hemisphere was 1.4 times higher than those by
the previous studies. For the southern hemisphere, it was
difficult to estimate a cumulative amount of global fallout
because fewer data for south of 401 latitude were available.
Acknowledgements
The authors thank Kayono Yamamoto for her work on
constructing the databases of global fallout of anthropogenic
radionuclides.

Meridional distribution
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shown in Table 1, our re-constructed spatial distribution of
global 137Cs fallout shows a different figure from the previous
one. In the Pacific regions, the 137Cs fallout was high along the
Kuroshio and the Kuroshio extension regions around 10–
501 N latitude in the Pacific Ocean. The 137Cs fallout in the
Atlantic Oceans, however, was high along the Gulf Stream
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137
Total amount of Cs fallout in the northern hemisphere
We integrated 137
Cs fallout grid data in the northern hemi-
sphere to estimate the total amount of fallout. The value of
765  79 PBq was estimated as the total amount of fallout in
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