JOURNAL OF GEOPHYSICAL RESEARCH: ATMOSPHERES, VOL. 118, 10201027, doi:10.

1029/2012JD018485, 2013

Detection of radioactive 35S at Fukushima and other Japanese sites

Antra Priyadarshi,1 Jason Hill-Falkenthal,1 Mark H. Thiemens,1 Naohiro Yoshida,2
Sakae Toyoda,3 Keita Yamada,2 Arata Mukotaka,2 Ayako Fujii,3 Mitsuo Uematsu,4
Shiro Hatakeyama,5 Izumi Noguchi,6 Yukihiro Nojiri,7 and Hiroshi Tanimoto7
Received 16 July 2012; revised 29 October 2012; accepted 25 November 2012; published 30 January 2013.

[1] The Fukushima nuclear power plant was severely damaged by an earthquake and
concomitant tsunami during March 2011. An effect of this disaster was secondary
formation of radioactive 35S via the 35Cl(n,p)35S reaction, when neutrons from the partially
melted reactor cores activated the coolant sea water. Here we report the rst measurements
of 35S in sulfate aerosols and rain water collected at six Japanese sampling sites, Hokkaido,
Tsukuba, Kashiwa, Fuchu, Yokohama, and Fukushima, during March-September 2011.
The measured 35SO24 concentrations in aerosols vary signicantly. The Kashiwa (AORI)
4
3
site shows the highest 35SO24 concentration (6.1
10  200 atoms/m ) on 1 April 2011,
which is nearly 100 times higher than the natural background activity. Considering the
percentage loss of 35SO24 resulting from dry and wet deposition and dilution of the
radiation plume in the boundary layer during transport, it was determined that the surface
5
3
air concentration of 35SO24 at the Fukushima would have been 2.8
10 atoms/m during
the week after the earthquake, which is in agreement with the model prediction
[Priyadarshi et al., 2011a]. 35SO24 activity in rain water collected during March-May 2011
at Tokyo Tech Yokohama varies from 1.1
105 to 9.8
105 atoms/liter, whereas stream
water collected near Fukushima was found to have 1.2
105 atoms/liter during April. Even
4
3
after 6 months, 35SO24 activity remains very high (9.9
10  770 atoms/m ) in the marine
boundary layer in the Fukushima region, which implies that the reactor core was producing
radioactive sulfur.
Citation: Priyadarshi, A., et al. (2013), Detection of radioactive 35S at Fukushima and other Japanese sites, J. Geophys.
Res., Atmos., 118, 10201027, doi:10.1029/2012JD018485.

1. Introduction
[2] On 11 March 2011, a magnitude 9.0 earthquake
occurred in the western Pacic Ocean, with its epicenter
approximately 72 km east of the Oshika peninsula of
Tohoku Japan (see http://earthquake.usgs.gov/earthquakes/eqinthenews/2011/usc0001xgp/). The earthquake
triggered a catastrophic tsunami with severe collateral

1
Department of Chemistry and Biochemistry, University of California
San Diego, La Jolla, California, USA.
2
Department of Environmental Chemistry and Engineering, Tokyo
Institute of Technology, Yokohama, Japan.
3
Department of Environmental Science and Technology, Tokyo
Institute of Technology, Yokohama, Japan.
4
Atmosphere and Ocean Research Institute, University of Tokyo, Chiba,
Japan.
5
Institute of Agriculture, Graduate School of Agriculture, Tokyo
University of Agriculture and Technology, Tokyo, Japan.
6
Institute of Environmental Sciences, Hokkaido Research Organization,
Sapporo, Japan.
7
National Institute for Environmental Studies, Tsukuba, Japan.

Corresponding author: A. Priyadarshi, Department of Chemistry and

Biochemistry, University of California San Diego, 9500 Gilman Drive,
La Jolla, CA 92093, USA. (fantra@ucsd.edu)
2012. American Geophysical Union. All Rights Reserved.
2169-897X/13/2012JD018485

damage. In addition to a signicant loss of life and infrastructure destruction, the tsunami caused damage to the
Fukushima Di-ichi nuclear power plant (http://www.iaea.
org). Immediately after the earthquake, the reactors at the
Fukushima nuclear power plant were automatically shut
down and boroncarbon control rods inserted between
the fuel columns to absorb neutrons and halt the nuclear
chain reaction. Even after the shutdown, the reactor core
required a prolonged cooling, because the uranium fuel
continues to decay into radioactive byproducts and to
release heat. A preliminary computer model by the U.K.
National Nuclear Laboratory showed that, even after shut
down of the Fukushima nuclear power plant, the radioactive byproducts of the ssion reaction still generated 7
megawatts of heat [Brumel, 2011a]. Because both the
regular and the emergency backup power supply (diesel
generators) that powered the cooling system of the power
plant were severely damaged by the tsunami waves, the
reactor core became sufciently hot that it initiated a melt
down and released hydrogen gas that eventually ignited and
caused explosions. The core damage was estimated to be
55%, 35%, and 30% for Units 1, 2, and 3, respectively
(http://www.iaea.org). Even after 6 months of continuous
cooling, the reactor core was too hot to allow access [Brumel,
2011b]. As the result of these events, a signicant amount of radioactivity was released into the atmosphere [Chino et al., 2011;

1020

PRIYADARSHI ET AL.: 35S MEASUREMENT IN FUKUSHIMA DISASTER

Morino et al., 2011]. Potentially dangerous levels of radiation

were detected nearly 30-40 km away from the nuclear plant.
Approximately 4
1011 neutrons/m2 were emitted during the
rst week following the earthquake, which led to the formation
of radioactive 35S [Priyadarshi et al., 2011a]. During the rst
few weeks (13 March to 26 March 2011) after the earthquake
and tsunami, several hundred tons of sea water were pumped into
the partially melted reactor core as a coolant. Neutrons emitted
from the reactor core were absorbed or captured by the constituents of sea water to produce a variety of radioactive isotopes,
mainly 24Na by interaction of neutrons with stable sodium via
an (n,g) reaction and 35S produced by interaction of neutrons with
stable chlorine via an (n,p) reaction [Dryssen and Nyman, 1955;
Love and Sam, 1962]. Since 24Na has a very short half-life (15 h),
the total radioactivity after a week was due nearly exclusively to
35
S [Dryssen and Nyman, 1955].
[3] Once produced, 35S was oxidized to 35SO2 gas, which
was eventually further oxidized to 35SO24 aerosol in the
atmosphere, similar to the natural atmospheric process
[Brothers et al., 2010; Priyadarshi et al., 2011b; Tanaka
and Turekian, 1991]. It was subsequently transported in
the atmosphere depending on air mass trajectories and
removed from the atmosphere by dry/wet deposition and
radioactive decay. 35S is a unique tracer in that it provides
information on the number of neutrons emitted from the
reactor core and can be used to probe the condition of the
reactor core as well as the containment vessel. Because of
the unavailability of samples from near the Fukushima
power plant, there have been no measurements of 35S until
now. Based on 35S measurements of atmospheric sulfate and

SO2 samples collected at La Jolla, California, and concomitant

model calculations, the concentration of 35SO24 in surface air
was estimated to be 2
105 atoms/m3 at Fukushima during
March 2011 [Priyadarshi et al., 2011a]. Here we report the rst
measurement of radioactive 35S in sulfate aerosols and rain
water collected at different sites in Japan (Figure 1) and compare
the data with the model calculation of Priyadarshi et al.
[2011a].

2. Materials and Methods

[4] Aerosol samples were collected at six different places in
close proximity to the Fukushima nuclear power plant
(37.25 N, 141.02 E; Figure 1): Tokyo Institute of Technology
(Tokyo Tech) Yokohama (35.52 N, 139.48 E); Atmosphere
and Ocean Research and Institute (AORI), University of Tokyo,
Kashiwa, Chiba Prefecture (35.90 N, 139.94 E); Tokyo
University of Agriculture and Technology (TUAT), Fuchu,
Tokyo (35.68 N, 139.48 E); National Institute of Environmental Studies (NIES), Tsukuba, Ibaraki Prefecture (36.05 N,
140.12 E); Hokkaido Research Organization, Sapporo
(43.08 N, 141.34 E); and Kawamata town, Fukushima prefecture (37.40 N, 140.36 E). These sampling sites, except for
Sapporo, are located within a 250 km radius and south of the
Fukushima nuclear plant. The aerosol samples were collected
from March through September 2011 using a high-volume air
sampler. Rain water samples were collected only at Tokyo Tech
during March-May 2011. In addition, a water sample from a local water stream, situated in Fukushima prefecture, nearly
50 km away from the Fukushima nuclear power plant, was

Figure 1. Details of the sampling sites. Aerosol samples were collected at six different places in close
proximity to the Fukushima nuclear power plant (37.25 N, 141.02 E): Tokyo Institute of Technology
(Tokyo Tech), Yokohama (35.52 N, 139.48 E); Atmosphere and Ocean Research and Institute (AORI),
University of Tokyo, Kashiwa, Chiba Prefecture (35.90 N, 139.94 E); Tokyo University of Agriculture
and Technology (TUAT), Fuchu, Tokyo (35.68 N, 139.48 E); National Institute of Environmental Studies (NIES), Tsukuba, Ibaraki Prefecture (36.05 N, 140.12 E); Hokkaido Research Organization, Sapporo
(43.08 N, 141.34 E); and Kawamata town, Fukushima prefecture (37.40 N, 140.36 E). These sampling
sites except for Sapporo are located within a 250 km radius and south of the Fukushima nuclear plant.
1021

PRIYADARSHI ET AL.: 35S MEASUREMENT IN FUKUSHIMA DISASTER

collected in April 2011. The samples were analyzed at the

University of California, San Diego. The details of the sample
processing for analyzing 35S activity in sulfate aerosols have
been described by Brothers et al. [2010]. Three or four liters
of rainwater was passed through a pre-prepared anion resin
column to trap sulfate on the resin surface, and 15 ml of HBr
(1 M) was passed through the resin column to elute sulfate ions
from the resin. The solution was then neutralized by adding
Ag2O and oven dried. Sulfate was cleaned of organics as
discussed by Brothers et al. [2010]. The 35S activity was
counted in an ultralow-level liquid scintillation spectrometer
(Wallac 1220 Quantulus) and was corrected for the background
activity (which is 1.07 DPM and probably is due to the radioactivity contributed from vial material and the scintillation gel
used for counting) and the decay time from the sample
collection date. The natural variation in 35SO24 concentration,
as reported by Priyadarshi et al. [2011b, 2012], is from 130
to 900 atoms/m3 and from 200 to 1600 atoms/m3 at Scripps Pier
in southern California and in Antarctica, respectively.

3. Results and Discussion

[5] 35S activities measured in sulfate aerosols collected at
Tokyo Tech, AORI, TUAT, NIES, Hokkaido, and Fukushima
(different aerosol size fraction) are shown in Figures 2 and 3.
Even though the sampling sites are relatively close to each
other (southward direction from Fukushima, except for
Hokkaido), a large variation in 35SO24 activities was observed
during March-April 2011. 35SO24 concentrations were 0.26

103  11.78
103, 0.69
103  61.4
103, 0.51
103 1.42

103, 1.41
103  18.05
103, 0.56
103  2.63
103
atoms/m3 at Tokyo Tech, AORI, TUAT, NIES, and Hokkaido, respectively (Table 1). The 35S activities observed at
Tokyo Tech, AORI and NIES are signicantly higher than
those observed at TUAT, NIES, and Hokkaido sites. At
3
4
Fukushima, 35SO24 varies from 8.1
10 to 9.9
10 atoms/
3
3
m and from 46 to 62 atoms/m in ne and coarse fractions, re4
spectively (Table 2). 35SO24 concentrations at AORI (6.1
10
3
5
3
atoms/m ) and Fukushima (1.2
10 atoms/m ) are the highest
35
S activities ever measured in any atmospheric sample and are
nearly 100 times higher than the natural background.

Figure 2. 35SO2
4 activity measured at ve different sampling sites near Fukushima. The maximum 35SO2
4 activity
(6.1
104 atoms/m3) was observed at AORI on 1 April 2011.

Figure 3. 35SO2
4 measured in different aerosol size fractions (Q5, Q6, Q7, representing aerosol size fraction
between 0.69 and 1.3 mm, between 0.39 and 0.69 mm, and
less than 0.39 mm, respectively) collected at Fukushima
prefecture. 35SO2
in the ne particles (Q7 < 0.39 mm) is
4
nearly 100 times higher than the natural background and
shows that, even after 6 months, of the nuclear disaster, the
reactor core was active and producing 35S.
Radioactive 35S (half-life 87 days) is also produced by the interaction of cosmic rays with 40Ar in the Earths atmosphere [Lal
and Peters, 1967]. The natural background 35SO24 concentration in the atmosphere varies from 300 to 900 atoms/m3
[Brothers et al., 2010; Priyadarshi et al., 2012]. Even at Antarctica, where the production rate of 35S is maximal [Lal and
3
Peters, 1967], 35SO24 varies from 120 to 1600 atoms/m
[Priyadarshi et al., 2011b]. Such a high concentration of
35
SO24 at AORI indicates the presence of another source of
35
S in the marine boundary layer. Priyadarshi et al. [2011b]
demonstrated that the partially damaged reactor core of the
Fukushima nuclear power plant produced radioactive 35S via
35
Cl(n,p)35S reaction during the rst few weeks following the
earthquake. The Hybrid Single Particle Lagrangian Integrated
Trajectory (HYSPLIT) model developed by NOAAs Air
Resources Laboratory (ARL) [Draxler and Rolph, 2011] was
used to calculate the air mass back-trajectories to determine
the origin and pathway of the air masses affecting the sampling
sites involved in this study. We considered the air mass mixing
and its transport within the boundary layer; the backward air
mass trajectories were calculated for 72 h at three different
altitudes (10, 500, and 1000 m) over each sampling station. As
shown in Figure 4, surface air masses at AORI arrived from the
north near Fukushima on 1 April 2011 and are thus responsible
4
3
for the observed spike in 35SO24 activity (6.1
10 atoms/m ).
The sampling site at Hokkaido lies north of Fukushima
and is thus not affected by the 35S emission at Fukushima.
A possible reason for lower 35SO24 activity at TUAT is its
geographical location and the prevailing air mass transport
vectors. TUAT is situated in Fuchu city, which has many
terraces and hills across it. The Fuchu and Kokobunji hills align
from west to east whereas the Sengen-Yama hill is located in
the northeastern side, which may affect the air mass trajectories
coming from Northeast Fukushima. Fine-scale air mass
trajectory analysis is not available, but future modeling efforts
could be instrumental in developing this.

1022

PRIYADARSHI ET AL.: 35S MEASUREMENT IN FUKUSHIMA DISASTER

Table 1. Measurement of radioactive

35

S in sulfate aerosol collected at different sampling sites near Fukushima

Collection Time (m/d/y)

Sample ID

Air Volume (m3)

Starting Date End Date

Tokyo Institute of Technology (Tokyo Tech), Yokohama

1
3/25/11, 3/26/11
2
3/26/11, 3/26/11
3
3/26/11, 3/27/11
4
3/27/11, 3/28/11
5
3/28/11, 3/30/11
6
3/30/11, 4/1/11
7
4/1/11, 4/3/11
8
4/3/11, 4/5/11
9
4/5/11, 4/7/11
10
4/7/11, 4/9/11
11
4/9/11, 4/11/11
12
4/11/11, 4/13/11
13
4/13/11, 4/15/11
14
4/15/11, 4/17/11
15
4/17/11, 4/19/11
16
4/19/11, 4/21/11
17
4/21/11, 4/23/11
18
4/23/11, 4/25/11
19
4/25/11, 4/28/11
20
4/28/11,
5/1/11
21
5/1/11,
5/4/11
22
5/4/11, 5/8/11
23
5/8/11, 5/10/11
24
5/10/11, 5/13/11
25
5/13/11, 5/17/11
26
5/17/11, 5/20/11
27
5/20/11, 5/24/11
28
5/24/11, 5/27/11
29
5/27/11, 5/30/11
30
5/30/11, 6/3/11
31
6/3/11, 6/7/11
32
6/7/11, 6/10/11
33
6/10/11, 6/14/11
34
6/14/11, 6/17/11
35
6/17/11, 6/21/11
36
6/21/11, 6/24/11
37
6/24/11, 6/28/11
38
6/28/11, 7/1/11
Atmosphere and Ocean Research Institute (AORI), Kashiwa, Chiba Pref.
39
3/23/11, 3/25/11
40
3/25/11, 3/28/11
41
3/28/11, 3/30/11
42
3/30/11, 4/1/11
43
4/1/11, 4/3/11
44
4/3/11,
4/5/11
45
4/5/11,
4/7/11
46
4/7/11,
4/9/11
47
4/9/11, 4/11/11
48
4/11/11, 4/13/11
49
4/13/11, 4/15/11
50
4/15/11, 4/17/11
51
4/17/11, 4/19/11
52
4/19/11, 4/21/11
Tokyo University of Agriculture and Technology, Fuchu, Tokyo
53
3/24/11, 3/26/11
54
3/26/11, 3/28/11
55
3/28/11, 3/30/11
56
3/30/11, 4/1/11
57
4/1/11, 4/3/11
58
4/3/11,
4/5/11
59
4/5/11,
4/7/11
60
4/7/11,
4/9/11
61
4/9/11,
4/11/11
62
4/11/11, 4/13/11
63
4/13/11, 4/15/11
64
4/15/11, 4/20/11
65
4/20/11, 4/22/11

35

3
3
SO24 Atoms per m ( 10 )

991
735
724
2001
2945
2960
2931
2980
2969
2973
2962
2959
2980
2984
2993
2961
2980
2985
4479
4413
4495
2884
2980
4511
5949
4467
5959
4493
4138
6200
5900
4415
5969
4469
5887
4492
5961
4451

3.06  0.12
0.56  0.11
0.72  0.12
1.25  0.04
11.78  0.07
0.73  0.03
0.48  0.03
0.35  0.03
0.41  0.03
1.03  0.07
1.75  0.08
0.94  0.07
1.11  0.07
0.88  0.07
1.25  0.08
0.46  0.07
0.79  0.07
0.77  0.07
0.76  0.05
0.70  0.05
0.93  0.07
1.03  0.09
0.88  0.09
0.62  0.06
1.22  0.05
1.32  0.06
0.35  0.04
0.49  0.05
0.50  0.05
0.74  0.04
0.97  0.04
0.34  0.04
0.73  0.04
0.26  0.04
0.29  0.03
0.55  0.04
0.34  0.03
0.62  0.04

1303
2353
1597
1568
1553
1586
1584
1541
1584
1574
1558
1539
1566
1579

17.08  0.10
0.70  0.04
13.90  0.11
61.40  0.20
0.96  0.05
1.14  0.05
1.65  0.13
1.62  0.14
3.44  0.15
2.58  0.15
1.54  0.14
1.78  0.15
4.11  0.17
2.35  0.15

2837
2885
2855
2851
2939
2779
2869
2868
2885
2882
2743
2899
2911

0.65  0.03
0.52  0.03
1.22  0.04
1.16  0.03
0.52  0.03
1.00  0.08
0.97  0.08
1.05  0.08
1.42  0.08
0.81  0.08
0.93  0.08
0.87  0.07
0.70  0.07

(Continues)
1023

PRIYADARSHI ET AL.: 35S MEASUREMENT IN FUKUSHIMA DISASTER

Table 1. (continued)
Collection Time (m/d/y)
Sample ID

Air Volume (m3)

Starting Date End Date

66
4/22/11, 4/24/11
67
4/24/11, 4/26/11
68
4/26/11, 4/28/11
69
4/28/11, 5/13/11
National Institute of Environmental Studies (NIES), Tsukuba, Ibaraki Pref.
70
3/24/ 11, 3/29/11
71
3/29/11, 4/1/11
72
4/1/11, 4/4/11
73
4/4/11, 4/7/11
74
4/7/11, 4/11/11
Hokkaido Research Organization, Sapporo
75
3/25/11, 3/28/11
76
3/28/11, 3/30/11
77
3/30/11, 4/1/11
78
4/1/11, 4/3/11
79
4/3/11, 4/5/11
80
4/5/11, 4/7/11
81
4/7/11, 4/9/11
82
4/9/11, 4/11/11
83
4/11/11, 4/13/11
84
4/13/11, 4/15/11
85
4/15/11, 4/17/11
86
4/17/11, 4/19/11
87
4/19/11, 4/21/11
88
4/21/11, 4/23/11
89
4/23/11, 4/25/11

35

3
3
SO24 Atoms per m ( 10 )

2857
2857
2849
2825

0.97  0.10
1.26  0.10
1.05  0.10
0.78  0.09

7065
4230
4224
4284
5686

5.02  0.03
18.05  0.14
4.39  0.08
1.41  0.06
1.94  0.05

3953
2933
2933
2918
2919
2857
2919
2923
2922
2924
2929
2930
2932
2931
2937

1.26  0.10
1.20  0.08
0.96  0.08
0.78  0.07
0.76  0.07
0.95  0.08
1.08  0.08
1.05  0.08
0.96  0.08
1.04  0.07
2.63  0.10
0.56  0.07
0.83  0.10
0.75  0.10
0.62  0.09

The standard error associated with individual measurement.

[6] Based on 35S activity measurements in California and a

moving box model, the surface air concentration of 35SO24 at
Fukushima was predicted to be 2
105 atoms/m3 in the week
following the earthquake [Priyadarshi et al., 2011a]. The
present data show a maximum activity of 6.1
104 atoms/
m3 at AORI on 1 April 2011, which is about three times lower
than the model estimated value. Because the AORI site is
nearly 250 km away from the Fukushima nuclear plant, a
dilution of the radiation plume in the boundary layer and loss
of 35SO24 aerosol particles by dry and wet deposition during
the transport are expected to decrease the 35SO24 concentration
signicantly before reaching the AORI site. Morino et al.
[2011] used a 3D chemical transport model to simulate the
distribution of radioactive 131I and 137Cs over Japan (both
inland and the surrounding nearby oceanic surface) during
10-30 March 2011. The model considered the emission of
radionuclides (131I and 137Cs) at the Fukushima nuclear power
plant, horizontal and vertical advection, diffusion affecting the
radiation plume during transport, dry and wet deposition of
gas and aerosols, and radioactive decay to determine the
percentage loss of radioactive 131I and 137Cs over Fukushima
and nearby prefectures. Since 137Cs behaves as an aerosol particle due to its attachment to ne aerosols [Sportisse, 2007], we
compare its distribution with 35SO24 aerosols. According to
Morino et al. [2011], nearly 15% of 137Cs emitted from the
Fukushima nuclear power plant were deposited over the
Fukushima prefecture, whereas on average, 22% of emitted
137
Cs was deposited over land in Japan during March. The
percentage loss was greater (8-41%) during a transient cyclone
that passed over Japan during 15-17 March and 19-23 March
[Morino et al., 2011].
[7] Based on the observed 35SO24 concentration peak at
AORI on 1 April 2011 (Figure 2) and the model estimation

of Morino et al. [2011], the surface air concentration of

35
5
SO24 at Fukushima was estimated to be between 1.1
10
5
3
and 2.8
10 atoms/m during March, whereas the predicted
concentration was 2
105 atoms/m3 [Priyadarshi et al.,
2011a]. This difference may be due partially to uncertainties
related to the calculation of depositional rates of radionuclides,
because the collection efciency of dry-deposited aerosols is
difcult to quantify precisely [Morino et al., 2011]. In addition,
the model used by Priyadarshi et al. [2011a] to calculate the
5
3
concentration of 35SO24 (2
10 atoms/m ) at Fukushima
contains unavoidable uncertainty. The model is particularly
sensitive to the dilution rate of the radiation plume during the
long-range transport from Fukushima to La Jolla, California.
A 10% change in dilution rate in the model would change the
model output (surface air concentration of 35SO24 , i.e.,
2
105 atoms/m3) by 20%.
[8] At Fukushima, 35SO24 activity measured in ne sulfate
aerosols are higher than in the coarse fraction during August
through September 2011 (Figure 3 and Table 3). This is
because 35S produced at the reactor was oxidized to 35SO2
and subsequently oxidized to 35SO24 in the ne fraction by
gas-phase oxidation of 35SO2. We note that, even after
6 months, 35S activity was very high in the marine boundary
layer in the Fukushima region, which implies that the reactor
core was still active and releasing neutrons. However, the presence of a viable chlorine source is not known. The neutrons
might be reacting either with residual evaporated salt deposits
or with sea water coming in and out across a crack developed
in the containment vessel. The reason for the higher 35S activity
observed during September compared with July-August is not
yet clear and warrants extended future sampling.
[9] The 35SO24 concentration in rain water collected
during March-May 2011 at Tokyo Tech Yokohama varies

1024

PRIYADARSHI ET AL.: 35S MEASUREMENT IN FUKUSHIMA DISASTER

Table 2. 35S Measurement in Aerosol Particles of different Size Fraction Collected From Fukushima Prefecture, ~100 km From the
a
Fukushima Nuclear Power Plant
Sample ID

Collection Time (m/d/y) Start Time End Time

Cedar forest, Kawamata-cho, Fukushima prefecture

0718-Q1
7/9/11,
0718-Q2
0718-Q3
0718-Q4
0718-Q5
0718-Q6
0718-Q7
0725-Q1
7/18/11,
0725-Q2
0725-Q3
0725-Q4
0725-Q5
0725-Q6
0725-Q7
0801-Q1
7/25/11,
0801-Q2
0801-Q3
0801-Q4
0801-Q5
0801-Q6
0801-Q7
0815-Q1
8/8/11,
0815-Q2
0815-Q3
0815-Q4
0815-Q5
0815-Q6
0815-Q7
0824-Q1
8/15/11,
0824-Q2
0824-Q3
0824-Q4
0824-Q5
0824-Q6
0824-Q7
0830-Q1
8/24/11,
0830-Q2
0830-Q3
0830-Q4
0830-Q5
0830-Q6
0830-Q7
0916-Q1
8/30/11,
0916-Q2
0916-Q3
0916-Q4
0916-Q5
0916-Q6
0916-Q7
School ground, Kawamata-cho, Fukushima prefecture
0715-Q1
7/9/11,
0715-Q2
0715-Q3
0715-Q4
0715-Q5
0715-Q6
0715-Q7
Agriculture eld, Kawamata-cho, Fukushima prefecture
0722-Q1
7/9/11,
0722-Q2
0722-Q3
0722-Q4
0722-Q5
0722-Q6
0722-Q7
0819-Q1
8/17/11,
0819-Q2
0819-Q3

Air volume (m3)

35

3
3
SO24 atoms/m (
10 )

0.34  0.04
0.65  0.05
0.52  0.04
1.41  0.06
1.34  0.06
30.41  0.18
57.53  0.24
0.20  0.05
0.15  0.05
0.13  0.05
0.56  0.06
8.12  0.12
10.31  0.14
6.02  0.11
0.27  0.05
0.43  0.05
0.46  0.05
2.06  0.08
14.56  0.15
17.97  0.17
50.38  0.26
0.20  0.05
0.48  0.050
0.50  0.05
4.55  0.10
28.39  0.20
56.0  0.27
34.12  0.22
0.16  0.04
0.19  0.04
0.25  0.04
1.64  0.06
10.72  0.12
0.52  0.05
28.03  0.19
0.21  0.05
0.18  0.05
0.22  0.05
1.60  0.08
11.95  0.15
16.74  0.17
14.75  0.16
0.05  0.02
0.04  0.02
0.05  0.02
0.43  0.03
4.59  0.06
8.58  0.08
8.14  0.07

7/18/11

6616

7/25/11

5783

8/1/11

5746

8/15/11

5870

8/24/11

7444

8/30/11

4975

9/16/11

12,762

7/13/11

3105

0.63  0.09
0.48  0.09
0.77  0.10
3.96  0.14
7.24  0.17
20.74  0.26
62.32  0.41

7/22/11

9909

8/19/11

1460

0.12  0.03
0.15  0.03
0.21  0.03
0.68  0.03
16.52  0.13
1.14  0.04
50.64  0.20
0.56  0.16
0.44  0.16
0.41  0.16

(Continues)
1025

PRIYADARSHI ET AL.: 35S MEASUREMENT IN FUKUSHIMA DISASTER

Table 2. (continued)
Sample ID
0819-Q4
0819-Q5
0819-Q6
0819-Q7
0908-Q1
0908-Q2
0908-Q3
0908-Q4
0908-Q5
0908-Q6
0908-Q7

Air volume (m3)

Collection Time (m/d/y) Start Time End Time

8/27/11,

9/7/11

35

3
3
SO24 atoms/m (
10 )

1.35  0.18
7.74  0.27
12.39  0.31
8.84  0.28
0.56  0.17
0.50  0.17
0.49  0.18
1.21  0.20
17.02  0.38
1.17  0.19
99.98  0.77

1460

Higher 35S activity is associated with ne sulfate particles, which are produced mainly from gas-phase oxidation of 35SO2. Q1, Q2, Q3, Q4, Q5, Q6, and
Q7 represent aerosol size fraction of >10.2 mm, 4.2-10.2 mm, 2.1-4.2 mm, 1.3-2.1 mm, 0.69-1.3 mm, 0.39-0.69 mm, and <0.39 mm, respectively.

from 1.1
105 to 9.8
105 atoms/liter, whereas stream water collected near Fukushima was found to have 1.2
105
atoms/liter during April (Table 3). The concentration in rain
water is nearly 10 times higher than the 35SO24 concentration
(6.2
104 atoms/liter) contained in rain water collected at
La Jolla, California, during January 2010. Atmospheric
processes such as rainout or washout cleanse the atmosphere
by removing aerosol particles and gases. Model simulation
dealing with long-range transport of dust and aerosols and
deposition on the surface/ocean depends sensitively on the
adapted aerosol-scavenging coefcient. We utilized 35S
measurements in aerosols and rainwater to calculate the
aerosol-scavenging coefcient. The scavenging coefcient
(k) is dened as [Okita et al., 1996]:
h
i
k Cw =Ca 106 P=h

Figure 4. HYSPLIT-3 days air masses back-trajectories were

calculated over the AORI sampling site at three different altitudes
(10, 50, and 1000 m). The surface air masses arrive from northwestern regions of Japan near Fukushima and are mainly responsible for the spike in 35SO24 activity observed on 1 April 2011.

[10] where Cw and Ca are the 35S concentration in rain water

(mg/liter) and air (mg/m3), respectively; P is the precipitation
rate (cm/s); and h is the height of the cloud top (cm). We do
not have measurements of the rate of precipitation of each individual event. The average precipitation rate (varying between
1.4 and 2.6 mm/h) was taken from the Japan Meteorological
Agency and is given in Table 3. The height of the cloud top
was assumed to be 2 km based on the fact that rainfall rate is
more signicant below the melting height (2-3 km), where
the main wet removal occurs in cloud [Mittermaier and
Illingworth, 2003]. After this height, the precipitation rate
decreases and becomes less intense [Scott, 1982]. A recent
measurement also shows that the mean cloud top height in
the Hawaiian region is 2.1 km [Zhang et al., 2012]. For our

Table 3. 35S measured in rain water samples collected in tokyo and Fukushima during March-May 2011 shows that 35S/liter of rain water
a
was 10 times higher than that in background rain water, as observed at La Jolla, (California) rain
Rain Samples
Tokyo Tech #1
#2
#3
#4
#5
Fukushima stream waterc
La Jolla rain

Sampling date

Average Rainfall Rate (mm/h)

3/24/11
4/25/11
5/11/11
5/13/11
5/24/11
4/28/11
1/26/10

1.4
2
2
2.6
1.7

35

SO24 (Atoms/Liter)
9.8E + 05
2.1E + 05
1.9E + 05
1.1E + 05
2.2E + 05
1.2E + 05
6.2E + 04

Ca (Atoms/m3)
-770
616
616
344

The rain-scavenging coefcient (k) was calculated based on the 35SO2

4 concentration measured in rainwater and air.
35
2The
concentration
of
SO
in
air
collected
at
Tokyo
Tech,
Yokohama.
4
c
Water sample collected from a stream situated in Fukushima prefecture, 50 km away from Fukushima nuclear power plant.
b

1026

K (s-1)
-- b
7.6 b
8.7 b
6.5 b
1.5

103
103
103
102

PRIYADARSHI ET AL.: 35S MEASUREMENT IN FUKUSHIMA DISASTER

sample, the value of k varies from 6.5
10-3/s to 1.5
10-2/s,

which agrees with other measurements [Andronache, 2004;
Chate et al., 2011; Laakso et al., 2003; Maria and Russell,
2005; Okita et al., 1996; Schumann, 1989]. The calculated
values from Andronache [2004] vary from 2.1
10-3/s to
4.3
10-4/s, for corresponding precipitation rates of 1.5 mm/h
and 4.7 mm/h.
[11] It has been demonstrated that 35S is a unique tracer in
understanding air mass mixing and quantifying aerosol dry
and wet deposition [Cho et al., 2011; Priyadarshi et al.,
2011b, 2012; Tanaka and Turekian, 1991; Turekian and
Tanaka, 1992]. Approximately 2
1011 atoms of 35S were
produced from Fukushima within the rst 6 months following
the earthquake, which is lower by a factor of 1011 compared
with the total global production of 2
1022 atoms of 35SO24
by cosmic rays, of which 5
1020 atoms of 35S are contained
in boundary layer itself. However, because Fukushima is a very
localized point source, the released 35SO24 was detected several
thousand miles away from the source.
[12] The presence of excess 35SO24 (two orders of magnitude higher than the natural background) provides a unique
opportunity to understand the chemical transformation, the
air mass transport, and potentially the fate of 35SO24 in soil
on short time scales. A yearlong sampling of aerosol, soil,
and rain water collected at several sampling sites in Japan
for 35S analysis along with a regional transport model
will further resolve and quantify the distribution rate of
regional radiogenic (and by proxy stable) sulfur in the
natural environment.

4. Conclusions
[13] We report the rst measurement of radioactive 35S in
sulfate aerosol collected at six different sampling sites close to
the Fukushima nuclear power plant during March-September
2011. A very high 35SO24 activity was observed at Fukushima,
AORI, NIES, Tsukuba, and Tokyo Tech Yokohama that is
nearly 100 times higher than the natural background 35S. Based
on 35SO24 concentrations measured at AORI in April, the
surface air concentration of 35S was estimated to be 2.8
105
atoms/m3 at Fukushima during March. Even after 6 months,
35
S activity was very high in the marine boundary layer in the
Fukushima region, which implies that the reactor core was still
active. The reason for higher 35SO24 during September compared with July-August is probably the periodic use of seawater
as a coolant. 35SO24 concentration in rainwater collected at
Tokyo Tech Yokohama varies from 1.1
105 to 9.8
105
atoms/liter. The 35SO24 concentration measured in air and
rainwater was employed to determine the rain-scavenging
coefcient, which varies from 6.5
10-3 to 1.5
10-2 s-1.
[14] Acknowledgments. We thank the reviewers of the manuscript
for their insightful comments that improved this manuscript. We also thank
K. Kita for aerosol sampling at Kawamata town. This work was supported
by KAKENHI (23224013 and 24110003) of the Ministry of Education,
Culture, Sports, Science and Technology, Japan.

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