Journal of Environmental Radioactivity 109 (2012) 45e51

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Journal of Environmental Radioactivity

journal homepage: www.elsevier.com/locate/jenvrad

Lateral variation of 134Cs and 137Cs concentrations in surface seawater in and

around the Japan Sea after the Fukushima Dai-ichi Nuclear Power Plant accident
M. Inoue a, *, H. Kofuji b, S. Nagao a, M. Yamamoto a, Y. Hamajima a, K. Yoshida a,
K. Fujimoto c, T. Takada a, Y. Isoda d
a
Low Level Radioactivity Laboratory, Institute of Nature and Environmental Technology, Kanazawa University, Nomi, Ishikawa 923-1224, Japan
b
Japan Marine Science Foundation, Minato, Mutsu, Aomori 035-0064, Japan
c
Fisheries Research Agency, National Research Institute of Fisheries Science, Fukuura, Kanazawa, Yokohama 236-8648, Japan
d
Graduate School of Fisheries Sciences, Hokkaido University, Minato-cho, Hakodate 041-8611, Japan

a r t i c l e i n f o a b s t r a c t

Article history: A total of 82 surface seawater samples was collected in the Japan Sea and the southwestern Okhotsk Sea
Received 18 October 2011 before and after the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. Analysis of 134Cs and
Received in revised form 137
Cs concentrations using low-background g-spectrometry revealed that the 137Cs concentration of the
19 December 2011
samples collected in June 2011 was 1.5e2.8 mBq/L, which is approximately 1e2 times higher than the
Accepted 5 January 2012
pre-accident 137Cs level, while the 134Cs concentration was less than detectable to 1 mBq/L. In addition to
Available online 24 January 2012 134
Cs being clearly detected (w1 mBq/L), 137Cs concentration in water samples from the northeastern
Japan Sea (2e2.8 mBq/L) was also higher than that from the coast in the southwestern Japan Sea
Keywords:
134
Cs
(w1.5 mBq/L). These higher concentrations in the northeastern Japan Sea could be ascribed to the
137
Cs atmospheric transport of nuclides from the FDNPP as aerosols and subsequent transport and dilution
Surface seawater after delivery to the sea surface.
Fukushima Dai-ichi Nuclear Power Plant Ó 2012 Elsevier Ltd. All rights reserved.
accident
Japan Sea

1. Introduction these samples in May 2011 could be explained by the fallout of

The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident,
which occurred in northeastern Japan on March 11, 2011, resulted in
the widespread release of large amounts of the radioactive fission
products, 134Cs (half-life: 2.06 y) and 137Cs (half-life: 30.2 y) into the
atmosphere. These radioisotopes were subsequently deposited
over extensive ocean and land areas in eastern Japan. To under-
stand the mechanisms underlying the dissipation of these radio-
isotopes, their concentrations and distribution patterns have been
studied in aerosols, soil, and seawater samples from eastern Japan
(Momoshima et al., submitted for publication; Hirose, in press;
Tsumune et al., in press; Buesseler et al., in press). We previously
measured the concentrations of 134Cs and 137Cs in surface seawater
samples at various points along the coast, 250e450 km north of
Fukushima on the Pacific Ocean-side of the Japanese archipelago
after the FDNPP accident (Inoue et al., in press). The 134Cs
(2e3 mBq/L) and 137Cs (2.5e4 mBq/L) concentrations measured in
* Corresponding author. Tel.: þ81 761 51 4440; fax: þ81 761 51 5528.
E-mail address: mutsuo@llrl.ku-unet.ocn.ne.jp (M. Inoue).
these nuclides onto the ocean after atmospheric transport from the
FDNPP.
The Japan Sea, one of the largest marginal seas in the Western
Pacific Ocean, is surrounded by the Eurasian continent and the
Japanese archipelago (Gamo and Horibe, 1983). The Tsushima
Warm Current, which enters through the Tsushima Strait, is a major
oceanographic feature affecting the flow patterns of the Japan Sea.
After moving northeastward along Honshu Island, Japan, the
Tsushima Warm Current then flows into the Pacific Ocean and the
Okhotsk Sea through the Tsugaru and Soya Straits (Hase et al.,
1999). Despite being isolated from the water currents passing by
the FDNPP, 134Cs was clearly detected in coastal water samples from
the Tsugaru Strait, implying that radioactive aerosol particles from
the accident reached the surface of the Japan Sea (Inoue et al., in
press). In order to accurately clarify the contamination levels and
delivery mechanisms of the 134Cs and 137Cs derived from the
FDNPP, the lateral distribution and temporal changes of these
nuclides needed to be undertaken immediately in the Japan Sea,
Okhotsk Sea, and the Tsugaru Strait.
We therefore collected surface seawater samples from various
sites in the Japan Sea after the FDNPP accident, and examined the

0265-931X/$ e see front matter Ó 2012 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jenvrad.2012.01.004
46 M. Inoue et al. / Journal of Environmental Radioactivity 109 (2012) 45e51
lateral distributions of 134Cs and 137Cs concentrations using low-
background g-spectrometry. By comparing these data with pre-
accident 134Cs and 137Cs concentration data, we were able to infer
the level of contamination and the migration patterns of these
nuclides in the Japan Sea.
2. Samples and experimental procedures
The seawater sampling locations used in the present study are
shown in Fig. 1. We collected 45 surface seawater samples
(approximately 20 L) (OS11 water samples) along transects A
(A1eA8), B (B1eB8), C (C1eC5), D (D1eD6), E (E1eE7), F (F1eF7),
and at a coastal site ab in the Japan Sea, and along transect G
(G1eG3) in the southwestern Okhotsk Sea during the Oshoro Maru
expedition in June 2011 (Fig. 1b and c). In addition, 24 surface water
samples (SY09 and SY10) were collected during the Soyo Maru
expeditions in JulyeAugust 2009 and July 2010, and 13 coastal
water samples (OH) were collected in the Tsugaru Strait before and
after the FDNPP accident during MayeOctober 2011. The analytical
results of six OH water samples and eight SY09 samples (SY09C and
SY09s1-s7) were reported previously (Inoue et al., in press, 2012).
Detailed explanations of the g-spectrometry procedures are pre-
sented elsewhere (Inoue et al., in press). Briefly, 134Cs and 137Cs were
quantitatively separated by coprecipitation with ammonium phos-
phomolybdate (AMP)/Cs by adding 0.52 g of CsCl and 8.0 g of AMP to
a 18e21 L aliquot of water. Low-background g-spectrometry was
performed using Ge-detectors located at the Ogoya Underground
Laboratory, Japan (Hamajima and Komura, 2004). The precision of the
analyses, based on a standard deviation of counting statistics, was
5e25% for 134Cs and 3e13% for 137Cs. In this paper, 134Cs concentration
was corrected for cascade summing (21e27%) and 134Cs and 137Cs
concentrations were decay-corrected based on sampling date.
The blank radioactivity of 134Cs and 137Cs in the experimental
procedures was measured with three distilled water samples (15 L)
containing 100 g of dissolved NaCl at one-month intervals. The g-
ray peak intensities of 134Cs and 137Cs in these blank samples
(DW1106, 1107, and 1108) were taken as the background levels. The
salinity of water samples was measured using a salinometer
(AUTOSAL 8400B, Guildline Instruments, Ontario, Canada).
3. Results and discussion
3.1. Lateral distributions of 134
Cs and 137
Cs in the Japan Sea
The g-spectrometry results for the seawater samples are pre-
sented in Table 1 and the lateral profiles of the 134Cs and 137Cs
Fig. 1. a) Map showing the main ocean current systems around the Japanese archipelago, b) sample locations for seawater collection in the Japan Sea, and c) around Hokkaido
Island. Open and solid circles represent water samples collected before and after the FDNPP accident, respectively.
concentrations along each transect are presented in Fig. 2. The 137Cs
concentration in the water samples collected along transect A (sites
OS11-A1 to -A8) near the entrance of the Tsushima Strait is
w1.5 mBq/L (Fig. 2a), which is equivalent to pre-accident levels of
w1.5 mBq/L with no seasonal variation at the strait (Inoue et al.,
2007). The 134Cs concentration of these water samples is taken as
the detection limit.
While the 137Cs concentration in the surface waters on the
coastal side of transect B (OS11-B1 to -B3) and coastal water sample
OS11-ab is similar to pre-accident levels of w1.5 mBq/L in this area
(Inoue et al., 2007), the 137Cs concentration in water samples
collected further offshore (OS11-B4 to -B8) is relatively higher
(w2 mBq/L) than the pre-accident offshore level of SY09 and SY10
water samples. Similarly, the 134Cs concentration of water samples
collected along the coast was not detected, while that in the
offshore water samples was in the level of w0.2e0.3 mBq/L
(Fig. 2b). The 137Cs and 134Cs concentrations of water samples
collected along transect C are also generally higher than those
collected along transect B (Fig. 2c). The radiocesium concentrations
along transects D, E, and F are all similar and in the highest range in
all samples measured. The mean 137Cs and 134Cs concentrations
throughout transects D, E, and F were found as 0.9 mBq/L and
2.4 mBq/L, respectively (Fig. 2def).
The relations between 134Cs and 137Cs concentrations in our
surface water samples in the Japan Sea are presented in Fig. 3
together with the data for Pacific Ocean-side. The 137Cs concen-
trations in the surface seawater samples in the Japan Sea range
between 1.5 and 2.8 mBq/L. The 137Cs concentration in surface
seawater around Japan before the FDNPP accident, which peaked
during the years of atmospheric nuclear weapons testing and also
just after the Chernobyl disaster, had been gradually decreasing
(Ikeuchi, 2003). The 137Cs concentration of our water samples
collected in the Japan Sea during 2009e2010 (SY09 and SY10 water
samples) is 1.3e1.8 mBq/L with a mean of 1.6 mBq/L. The 137Cs
concentration in the OS11 water samples collected after the FDNPP
accident is 1e2 times higher than pre-accident levels.
The 134Cs concentration in the OS11 water samples ranges from
lower than detectable to 1.2 mBq/L, and shows a strong positive
correlation with 137Cs concentration (r2 ¼ 0.91, n ¼ 42). The inter-
cept 137Cs concentration on 134Cs axis with regression analysis is
1.5 mBq/L and the slope of the regression line is 1.0 (1.1 in case of
decay correction to March 11, 2011), implying the addition of 134Cs
and 137Cs with a fixed 134Cs/137Cs ratio to pre-accident levels. The
intercept and the slope agree well with observed 137Cs concentra-
tions in pre-accident SY09 and SY10 water samples from the Japan
Sea (1.6  0.1 mBq/L for 137Cs), and the 134Cs/137Cs ratio of
 M. Inoue et al. / Journal of Environmental Radioactivity 109 (2012) 45e51 47

Table 1
134 137
Cs and Cs concentrations in seawater samples from in and around the Japan Sea.

Sampling site Location Depth Sampling date Salinity Concentration (mBq/L) Concentration ratio
(m) 134 137 134
N E Cs Cs Cs/137Cs
OS11 A1 33 380 130 130 0 Jun. 25, 2011 31.90 n.d. 1.45  0.07 e
A2 33 500 130 080 0 Jun. 24, 2011 34.09 n.d. 1.60  0.07 e
A3 34 000 130 020 0 Jun. 24, 2011 33.44 n.d. 1.53  0.07 e
A4 34 100 129 560 0 Jun. 24, 2011 33.30 n.d. 1.56  0.06 e
A5 34 200 129 490 0 Jun. 24, 2011 33.11 n.d. 1.44  0.09 e
A6 34 300 129 430 0 Jun. 24, 2011 34.00 n.d. 1.68  0.10 e
A7 34 400 129 360 0 Jun. 24, 2011 33.25 n.d. 1.68  0.12 e
A8 34 500 129 300 0 Jun. 24, 2011 33.14 n.d. 1.58  0.12 e
Mean of Transect A (A1eA8) n.d. 1.56  0.09 e
B1 36 030 135 480 0 Jun. 22, 2011 33.83 n.d. 1.43  0.09 e
B2 36 250 135 460 0 Jun. 22, 2011 34.27 n.d. 1.71  0.07 e
B3 36 460 135 430 0 Jun. 22, 2011 34.37 n.d. 1.52  0.13 e
B4 37 060 135 410 0 Jun. 22, 2011 34.32 0.18  0.03 1.72  0.07 0.11  0.02
B5 37 290 135 390 0 Jun. 22, 2011 34.07 0.27  0.08 1.88  0.09 0.14  0.05
B6 37 490 135 360 0 Jun. 22, 2011 33.95 0.26  0.06 1.83  0.05 0.14  0.03
B7 38 100 135 340 0 Jun. 21, 2011 34.02 0.35  0.07 1.84  0.07 0.19  0.04
B8 38 280 135 300 0 Jun. 21, 2011 34.39 0.16  0.07 1.72  0.10 0.10  0.04
Mean of Transect B (B1eB8) 0.14  0.14 1.70  0.15 0.08  0.08
C1 39 420 139 540 0 Jun. 19, 2011 30.61 0.86  0.12 2.12  0.11 0.41  0.06
C2 39 450 139 340 0 Jun. 19, 2011 34.15 0.43  0.08 2.20  0.09 0.19  0.04
C3 39 490 139 120 0 Jun. 19, 2011 34.25 0.41  0.11 1.82  0.11 0.22  0.06
C4 39 510 139 470 0 Jun. 19, 2011 34.04 0.33  0.10 2.04  0.10 0.16  0.05
C5 39 550 138 220 0 Jun. 20, 2011 33.97 0.57  0.10 2.10  0.09 0.27  0.05
Mean of Transect C (C1eC5) 0.52  0.21 2.05  0.14 0.25  0.10
D1 41 000 140 090 0 Jun. 16, 2011 32.65 1.20  0.13 2.41  0.11 0.50  0.06
D2 41 000 139 540 0 Jun. 16, 2011 32.15 1.07  0.14 2.61  0.12 0.41  0.06
D3 41 000 139 370 0 Jun. 16, 2011 32.66 0.90  0.11 2.40  0.10 0.37  0.05
D4 41 000 139 190 0 Jun. 16, 2011 33.49 0.68  0.12 2.13  0.11 0.32  0.06
D5 41 000 138 590 0 Jun. 15, 2011 33.96 0.99  0.10 2.59  0.09 0.38  0.04
D6 41 120 137 410 0 Jun. 15, 2011 33.91 0.93  0.11 2.50  0.11 0.37  0.05
Mean of Transect D (D1eD6) 0.96  0.18 2.44  0.18 0.39  0.06
E1 41 190 140 250 0 Jun. 8, 2011 33.28 0.98  0.13 2.78  0.13 0.35  0.05
E2 41 090 140 110 0 Jun. 8, 2011 32.82 1.02  0.12 2.59  0.11 0.39  0.05
E3 41 220 140 090 0 Jun. 8, 2011 33.36 1.21  0.18 2.48  0.14 0.49  0.08
E4 41 300 139 550 0 Jun. 8, 2011 33.44 1.09  0.09 2.79  0.08 0.39  0.04
E5 41 400 139 410 0 Jun. 8, 2011 33.29 1.00  0.16 2.63  0.14 0.38  0.06
E6 41 510 139 290 0 Jun. 9, 2011 33.95 0.57  0.11 2.31  0.13 0.25  0.05
E7 41 590 139 160 0 Jun. 9, 2011 34.11 0.70  0.11 2.19  0.10 0.32  0.05
Mean of Transect E (E1eE7) 0.94  0.22 2.54  0.23 0.37  0.07
F1 43 390 141 140 0 Jun. 13, 2011 33.07 0.86  0.11 2.15  0.09 0.40  0.05
F2 43 380 140 500 0 Jun. 13, 2011 33.76 1.12  0.13 2.64  0.11 0.42  0.05
F3 43 380 140 240 0 Jun. 13, 2011 33.19 0.99  0.16 2.43  0.14 0.41  0.07
F4 43 380 139 550 0 Jun. 13, 2011 33.83 0.76  0.11 2.17  0.10 0.35  0.05
F5 43 380 139 290 0 Jun. 13, 2011 33.89 1.31  0.19 2.59  0.16 0.51  0.08
F6 43 380 138 570 0 Jun. 14, 2011 33.90 1.49  0.17 2.86  0.13 0.52  0.06
F7 43 380 138 280 0 Jun. 14, 2011 33.90 0.82  0.11 2.51  0.10 0.33  0.05
Mean of Transect F (F1eF7) 1.05  0.27 2.48  0.25 0.42  0.07
G1 45 190 142 290 0 Jun. 10, 2011 33.80 0.44  0.08 2.08  0.09 0.21  0.04
G2 45 280 142 480 0 Jun. 10, 2011 32.30 0.73  0.10 1.51  0.08 0.48  0.07
G3 45 230 145 020 0 Jun. 11, 2011 32.58 0.57  0.09 1.58  0.08 0.36  0.06
Mean of Transect G (G1eG7) 0.58  0.14 1.72  0.31 0.35  0.13
ab 35 430 132 450 0 Jun. 23, 2011 34.04 n.d. 1.63  0.10 e
OHa 1105-1 41 320 140 540 0 May 11, 2011 33.27 1.45  0.26 3.39  0.18 0.43  0.08
1105-2 0 May 22, 2011 33.06 1.38  0.19 3.02  0.14 0.46  0.07
1106-1 0 Jun. 3, 2011 33.54 0.87  0.15 2.60  0.13 0.33  0.06
1106-2 0 Jun. 11, 2011 33.33 0.99  0.15 2.24  0.14 0.44  0.07
1106-3 0 Jun. 17, 2011 33.71 0.48  0.11 2.17  0.11 0.22  0.05
1106-4 0 Jun. 25, 2011 33.33 0.51  0.07 1.96  0.13 0.26  0.04
1107-1 0 Jul. 10, 2011 32.80 0.41  0.10 1.95  0.12 0.21  0.05
1107-2 0 Jul. 19, 2011 33.26 0.30  0.06 1.66  0.07 0.18  0.04
1108-1 0 Aug. 4, 2011 33.59 0.25  0.05 1.71  0.07 0.15  0.03
1108-2 0 Aug. 21, 2011 33.32 0.36  0.07 1.93  0.09 0.19  0.04
1109-1 0 Sep. 4, 2011 33.65 0.16  0.04 1.66  0.07 0.10  0.02
1109-2 0 Sep. 23, 2011 33.02 0.20  0.03 1.80  0.07 0.11  0.02
1110-1 0 Oct. 8, 2011 32.74 0.12  0.04 1.51  0.07 0.08  0.03
SY09b C 45 010 145 010 5 Aug. 2, 2009 32.15 n.d. 1.09  0.06 e
s1 44 330 144 410 5 Aug. 2, 2009 32.12 n.d. 0.93  0.11 e
s2 44 530 143 220 5 Aug. 1, 2009 32.00 n.d. 0.96  0.12 e
s3 45 240 142 290 5 Aug. 3, 2009 33.90 n.d. 1.58  0.15 e
s4 45 350 141 560 5 Aug. 1, 2009 33.43 n.d. 1.65  0.11 e
s5 45 170 140 470 5 Aug. 4, 2009 33.66 n.d. 1.47  0.17 e
s6 44 500 141 210 5 Jul. 31, 2009 33.35 n.d. 1.54  0.14 e
(continued on next page)
48 M. Inoue et al. / Journal of Environmental Radioactivity 109 (2012) 45e51

Table 1 (continued )

Sampling site Location Depth Sampling date Salinity Concentration (mBq/L) Concentration ratio
(m) 134 137 134
N E Cs Cs Cs/137Cs
 0  0
s7 44 42 139 48 5 Aug. 5, 2009 33.85 n.d. 1.61  0.13 e
s8 43 420 139 450 5 Aug. 5, 2009 33.80 n.d. 1.49  0.10 e
s9 42 580 139 380 5 Jul. 27, 2009 33.72 n.d. 1.50  0.10 e
s10 41 580 139 460 5 Aug. 6, 2009 33.18 n.d. 1.49  0.11 e
s11 41 180 139 470 5 Jul. 21, 2009 33.90 n.d. 1.83  0.15 e
s12 41 350 140 520 5 Jul. 20, 2009 33.71 n.d. 1.59  0.13 e
s13 41 200 140 190 5 Jul. 21, 2009 33.51 n.d. 1.69  0.14 e
s14 41 210 141 490 5 Jul. 20, 2009 33.85 n.d. 1.84  0.11 e
s15 40 530 141 490 5 Aug. 6, 2009 32.79 n.d. 1.43  0.10 e
s16 41 000 138 000 5 Jul. 21, 2009 e n.d. 1.69  0.15 e
s17 40 560 136 380 5 Jul. 25, 2009 33.50 n.d. 1.49  0.12 e
s18 39 500 135 530 5 Jul. 23, 2009 e n.d. 1.64  0.09 e
s19 39 050 135 320 5 Jul. 24, 2009 e n.d. 1.51  0.10 e
SY10 s20 37 410 134 030 5 Jul. 21, 2010 33.99 n.d. 1.61  0.08 e
s22 35 210 131 350 5 Jul. 21, 2010 33.09 n.d. 1.31  0.08 e
s23 34 350 130 540 5 Jul. 22, 2010 32.19 n.d. 1.46  0.09 e
s24 34 240 130 440 5 Jul. 22, 2010 32.25 n.d. 1.33  0.13 e

The analytical error is based on 1s of counting statistics.

“n.d.” denotes “not detected”(<w0.1 mBq/L under present analytical conditions).
Concentrations are decay-corrected based on sampling date.
a 134
Cs and 137Cs concentrations of OH1105 and 1106 water samples are from Inoue et al. (in press).
b 137
Cs concentration data for SY09C and SY09s1-s7 water samples are from Inoue et al. (2012).

134 137
Cs Cs
3 3
a Transect A d
2 2 Transect D

A8 A7 A6 A4 A3 A2 D6 D5
A5 A1
1 1 D4
D1
D2
D3
0 0
150 100 50 0 150 100 50 0

3 3
b e
Concentration (mBq/L)

Transect B
2 2 Transect E
E3
B8 B7 B6 B5 E5 E4 E2
B4 B2 E1
1
B3 B1 1 E7 E6

Japan Sea Tsugaru Str.

0 0
350 300 250 200 150 100 50 0 100 50 0 50

3 3
c Transect C f
F6
2 2
F7 F5 F2
F3
C2 F4 F1
C5 C4 C1
C3
1 1

Transect F
0 0
150 100 50 0 250 200 150 100 50 0

Distance from Japan coast (km)

134 137
Fig. 2. Lateral fluctuations in Cs and Cs concentrations in the surface waters of the Japan Sea along transects AeF, respectively.
 M. Inoue et al. / Journal of Environmental Radioactivity 109 (2012) 45e51 49

approximately 1 was found in emissions from the FDNPP 200 1.5

(Emergency Operations Center, 2011), respectively. Although this
Deposition
correlation was also typical for the coastal waters with salinity of

Cs deposition (MBq/(km month))

Mar. 2011

134
>32 in the Pacific Ocean-side area of northeastern Honshu during Apr. 2011

Cs concentration (mBq/L)
MayeJune 2011 (Inoue et al., in press), the 134Cs and 137Cs 150 May 2011 F
concentrations in the Japan Sea-side area of Japan are relatively Jun. 2011 D E

2
1
Cumulative (Mar.-Jun.)
lower than those in the Pacific Ocean-side. Interestingly, the 134Cs
Surface water
and 137Cs concentrations in the OS11 water samples gradually transect (mean)
100
increase from transects A to D, and appear to be similar in magni-
tude to the concentrations measured at transects D, E, and F.
C
Since the Japan Sea is isolated from the ocean currents that pass 0.5
the FDNPP, the increase in 134Cs and 137Cs concentrations within the
50
Japan Sea is likely due to the input of radioactive aerosol particles
derived from the FDNPP, and not due to the transport of contami-

134
nated water as we discussed previously (Inoue et al., in press). ab B
A
Cesium-134 and 137Cs were spread over a wide area, and were 0 0

Niigata
Dazaifu

Sapporo
Akita
Tottori
Matsue
even found on the Japan Sea-side of Honshu Island through the

Aomori
Fukui

Kanazawa
atmospheric transport of radioactive aerosols. In Fig. 4, the atmo-
spheric deposition rates of 134Cs measured in fallout samples along
the Japan Sea-side of Kyushu-Honshu (Ministry of Education,
Culture, Sports, Science and Technology in Japan, 2011) are pre- Fig. 4. Comparison of amount of 134Cs in radioactive fallout of aerosol particles along the
sented together with the 134Cs concentrations of OS11 water Japan Sea-side of Japan (Ministry of Education, Culture, Sports, Science and Technology in
Japan, 2011) and 134Cs concentration of OS11 water samples from the Japan Sea.
samples. As shown in the figure, the cumulative deposition during
MarcheJune 2011 of 134Cs increased markedly from Dazaifu
(1 mBq/km2) to Akita (170 mBq/km2) along the Japan Sea-side of
and 137Cs from Akita (transect C) to Aomori and Hokkaido (tran-
Kyushu-Honshu and decreased markedly from Akita to Sapporo
sects D, E, and F) is considered to partly reflect the involvement of
(9 mBq/km2). The depositions of 134Cs from the FDNPP to the Japan
water transport of 134Cs and 137Cs by the Tsushima Warm Current.
Sea-side of Japan were highest in April. The distribution of 134Cs in
surface water samples is not considered to be consistent with levels
that could be delivered using only radioactive aerosol particles. The 3.2. Tsugaru strait
coastal waters of the Japan Sea are constantly being influenced by
the Tsushima Warm Current, and the mean speed of this current Temporal changes in the 134Cs and 137Cs concentrations of OH
during the summer season was estimated to be 25e50 cm/s (Lee water samples are shown in Fig. 5. At site OH in the Tsugaru Strait,
et al., 1997; Katoh, 1994). Although the distribution of 134Cs in the 134Cs and 137Cs concentrations exhibit only small variations
offshore surface seawaters in the Japan Sea (Yasunari et al., 2011) from July to September 2011 (w10%/month) compared to a steep
and the riverine input of re-mobilized 134Cs in coastal areas are not decrease in May and June 2011 (w20%/month). The surface waters
well clarified, the northward shift of high concentrations of 134Cs in the Tsugaru Strait originate from the strong Tsushima Warm
Current in the Japan Sea (1e2  106 m3/s) (Nishida et al., 2003) and
concentration levels of 134Cs and 137Cs at the OH site in June 2011
3 are similar to those observed along transects D, E, and F, reflecting
the large contribution of water from the Japan Sea at this site
OS11 (2011)
SY09 and SY10 (2009-2010)
Pacific Ocean-side (2011)

Transect D
Cs concentration (mBq/L)

OH (2011)
Transect E
2 OH (2009)
3 137Cs Transect F
Concentration (mBq/L)

2
F
1
D E
134

C
134Cs Transect D
1 OH (2011)
Transect E
B OH (2009)
A Transect F
0
1 2 3 4
137
Cs concentration (mBq/L) 0
134 137
Fig. 3. Relationship between Cs and Cs concentrations in OS11 water samples May Jun. Jul. Aug. Sep. Oct. Nov.
collected in the Japan Sea. Solid circles indicate mean concentrations of water samples
137 134
along transects AeF. Concentration data from collection sites on the Pacific Ocean-side Fig. 5. Temporal variations in Cs and Cs concentrations in OH water samples and
of northeastern Honshu are from Inoue et al. (in press). mean values of samples collected along transects DeF.
50 M. Inoue et al. / Journal of Environmental Radioactivity 109 (2012) 45e51
3 1.5
a b
E
Cs concentration (mBq/L)
2.5 D F
G1
2
G2 G3
s4-s7
1.5
C
1 s2 s1
137
0.5
32 32.5 33 33.5
Salinity
Fig. 6. Plot of a) 137Cs and b) 134Cs concentrations vs. salinity in OS11 (G1eG3) and SY09 water samples (C and s1es3) and mean values of samples collected along transects DeF to
show their lateral variations in the southwestern Okhotsk Sea. The SY09 water samples were collected in August 2009 (Inoue et al., 2012). Shaded area represents the pre-accident
levels in surface waters around the Soya Strait of the Japan Sea (SY09s4-s7).
(Fig. 5). Thus, the marked decreases in 134Cs and 137Cs concentra-
tions in the OH water samples in May and June 2011 are likely due
to the outflows of surface waters, which received radioactive
aerosol particles from the FDNPP (e.g., coastal to offshore areas in
Akita; Fig. 4). Further, the relatively small decreases in radiocesium
concentrations during JuneeSeptember could be ascribed to
surface waters only being slightly, but widely, affected by the input
of aerosol particles on the Japan Sea-side of the Japanese archi-
pelago (e.g., coastal waters from Tottori to Niigata area).
3.3. Southwestern Okhotsk Sea
Fig. 6 shows 137Cs and 134Cs concentrations in the surface waters
of the southwestern Okhotsk Sea plotted against salinity. These
samples were taken at the confluence of the low-salinity (<32) East
Sakhalin Current Water (ESCW) with poor 137Cs, which flows along
the eastern coast of Sakhalin, and the highly saline (33.6e34.3)
Soya Warm Current Water (SWCW) with rich 137Cs from the
Japan Sea (Takizawa, 1982; Inoue et al., 2012). Therefore, the 137Cs
concentration in the surface waters of the southwestern Okhotsk
Sea showed marked lateral fluctuations (Fig. 6a), clearly reflecting
the considerable mixing between the SWCW and ESCW. The 134Cs
and 137Cs concentrations in the OS11-G1, -G2, and -G3 water
samples along transect G are higher than those in pre-accident SY09
water samples (C and s1es3). Conversely, the 134Cs and 137Cs
concentrations in these water samples are lower relative to those
collected along transects D, E, and F on the Japan Sea-side of the
archipelago. The 134Cs concentration in the G2 and G3 water
samples (salinities of 32.30 and 32.58) is similar to that in the G1
water sample, which has a high salinity (33.80) (Fig. 6b). As
observed in the OH water samples (Fig. 5), the 134Cs and 137Cs
concentrations in the SWCW are also considered to have changed
over time, and the magnitude of direct aerosol input from the
FDNPP at these sites has not been clarified. However, based on the
large contribution of the SWCW to the sea area in summer (Itoh and
Ohshima, 2000), the SWCW is considered to have effected the
radionuclide concentrations in samples G1, G2, and G3 from the
southwestern Okhotsk Sea.
Further clarification of the fallout patterns of 134Cs and 137Cs in
and around the Japan Sea could be undertaken by characterizing
OS11 Transect D
SY09 Transect E
Transect F
Cs concentration (mBq/L)
F
1 D E
G2
s3
G3
0.5 G1
134
s2 s1 C s4-s7 s3
0
34 32 32.5 33 33.5 34
Salinity
the temporal changes in 134Cs and 137Cs concentrations in the sea
and combining these data with simulation model data that
consider the transport patterns of aerosol particles and surface
waters from the FDNPP.
4. Conclusions
A total of 82 surface seawater samples was collected in the Japan
Sea, the Tsugaru Strait, and the southwestern Okhotsk Sea
before and after the FDNPP accident and analyzed for 134Cs and 137Cs
concentrations. The following interesting findings were obtained:
(1) The 137Cs concentration of water samples collected in June 2011
ranged from 1.5 to 2.8 mBq/L, which was 1e2 times higher than
pre-accident levels. The 134Cs average concentration was
approximately 0.5e1 mBq/L in the northeastern Japan Sea and
the southwestern Okhotsk Sea, and was found as under the
detection limit along coastal areas in the southwestern Japan
Sea. The observed distributions could be explained by fallout of
134
Cs and 137Cs into the sea after atmospheric transport from
the FDNPP and transport of surface waters during/after the
deposition.
(2) The marked decreases in 134Cs and 137Cs concentrations
(w20%/month) in the Tsugaru Strait during MayeJune 2011
were related to a steep decrease in their concentrations in the
Japan Sea. The relatively small decreases (w10%/month) during
JulyeSeptember 2011 reflect the marked diffusion of these
isotopes on the Japan Sea-side of the Japanese archipelago.
(3) Significant concentrations of 134Cs and 137Cs were also observed
in surface waters of the southwestern Okhotsk Sea, although
these 134Cs and 137Cs concentrations were lower relative to
those in the northeastern Japan Sea. The lower levels of these
nuclides are likely due to the SWCW transport after fallout of the
radioactive aerosol particles over the northeastern Japan Sea
(and/or atmospheric input after the FDNPP accident).
Acknowledgments
We thank the researchers, captain, and crew of the T/V Oshoro
Maru and R/V Soyo Maru for their assistance during sampling. We
 M. Inoue et al. / Journal of Environmental Radioactivity 109 (2012) 45e51
would like to thank Dr. S. Hisamatsu and two anonymous reviewers
for constructive comments on this manuscript. This study was
supported partly by a Grant-in-Aid for Scientific Research No.
21510011 (M. Inoue) from the Ministry of Education, Culture,
Sports, Science and Technology of Japan and Cooperative-study (Y.
Isoda) by Institute of Low Temperature Science, Hokkaido
University.
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