Atmospheric radioactivity over Tsukuba, Japan: a summary of three years of observations after the FDNPP accident

Abstract

A severe accident occurred in March 2011 at the Fukushima Dai-ichi nuclear power plant (FDNPP) operated by the Tokyo Electric Power Company (TEPCO), causing serious environmental pollution over a wide range covering eastern Japan and the northwestern Pacific. This accident created a large mark in the atmospheric radionuclide chronological record at the Meteorological Research Institute (MRI). This paper reports the impacts from the FDNPP accident over approximately 3 years in Tsukuba, Ibaraki (approximately 170 km southwest from the accident site), as a typical example of the atmospheric pollution from the accident. The monthly atmospheric ^sup 90^Sr and ^sup 137^Cs depositional fluxes in March 2011 reached approximately 5 Bq/m^sup 2^/month and 23 kBq/m^sup 2^/month, respectively. They are 3-4 and 6-7 orders of magnitude higher, respectively, than before the accident. Sr-90 pollution was relatively insignificant compared to that of ^sup 137^Cs. The ^sup 137^Cs atmospheric concentration reached a maximum of 38 Bq/m^sup 3^ during March 20-21, 2011. After that, the concentrations quickly decreased until fall 2011 when the decrease slowed. The pre-FDNPP accident ^sup 137^Cs concentration levels were, at most, approximately 1 [mu]Bq/m^sup 3^. The average level 3 years after the accident was approximately 12 [mu]Bq/m^sup 3^ during 2014. The atmospheric data for the 3 years since the accident form a basis for considering temporal changes in the decreasing trends and re-suspension (secondary emission), supporting our understanding of radioCs' atmospheric concentration and deposition. Information regarding our immediate monitoring, modeling, and data analysis approaches for pollution from the FDNPP accident is provided in the Appendices.

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44

DOI 10.1186/s40645-015-0066-1

RESEARCH ARTICLE Open Access

http://crossmark.crossref.org/dialog/?doi=10.1186/s40645-015-0066-1&domain=pdf

Web End = Atmospheric radioactivity over Tsukuba, Japan: a summary of three years of observations after the FDNPP accident

Yasuhito Igarashi1*, Mizuo Kajino1, Yuji Zaizen1, Kouji Adachi1 and Masao Mikami1,2

Abstract

A severe accident occurred in March 2011 at the Fukushima Dai-ichi nuclear power plant (FDNPP) operated by the Tokyo Electric Power Company (TEPCO), causing serious environmental pollution over a wide range covering eastern Japan and the northwestern Pacific. This accident created a large mark in the atmospheric radionuclide chronological record at the Meteorological Research Institute (MRI). This paper reports the impacts from the FDNPP accident over approximately 3 years in Tsukuba, Ibaraki (approximately 170 km southwest from the accident site), as a typical example of the atmospheric pollution from the accident. The monthly atmospheric 90Sr and 137Cs depositional

fluxes in March 2011 reached approximately 5 Bq/m2/month and 23 kBq/m2/month, respectively. They are 34 and 67 orders of magnitude higher, respectively, than before the accident. Sr-90 pollution was relatively insignificant compared to that of 137Cs. The 137Cs atmospheric concentration reached a maximum of 38 Bq/m3 during March 2021, 2011. After that, the concentrations quickly decreased until fall 2011 when the decrease slowed. The pre-FDNPP accident 137Cs concentration levels were, at most, approximately 1 Bq/m3. The average level 3 years after the accident was approximately 12 Bq/m3 during 2014. The atmospheric data for the 3 years since the accident form a basis for considering temporal changes in the decreasing trends and re-suspension (secondary emission), supporting our understanding of radioCs atmospheric concentration and deposition. Information regarding our immediate monitoring, modeling, and data analysis approaches for pollution from the FDNPP accident is provided in the Appendices.

Keywords: Temporal change, 90Sr, 137Cs, Atmospheric deposition, Atmospheric concentration, FDNPP accident

BackgroundWe have conducted observational research on radio-nuclides in the environment for almost 60 years at the Meteorological Research Institute (MRI) in Japan, ever since the 1950s when the USA, Soviet Union, and others performed vigorous nuclear tests in the atmosphere. The atmosphere is the major medium into which radioactive materials were directly injected by the nuclear tests and accidents, and within it, transport, diffusion, and wet and dry removal of these materials occur. During the nuclear testing era, the major purpose of our research was to clarify the radioactive pollution situation and its major controlling

factors in the atmosphere (Hirose et al. 1986; Katsuragi 1983; Miyake 1954; Miyake et al. 1963, 1975) and hydrosphere (Miyake et al. 1955, 1962, 1988). After the Chernobyl accident, the purpose of the research gradually shifted to obtaining more data about various processes in the atmosphere (Aoyama 1988; Aoyama et al. 1986, 1987, 1991, 2006; Hirose et al. 1993, 2001; Igarashi et al. 1996, 2003, 2009) and hydro-sphere (Aoyama 1995, Aoyama and Hirose 2004; Hirose et al. 1999, Hirose and Aoyama 2003; Miyao et al. 2000). Of particular interest in this study, observation of monthly radionuclide deposition (atmospheric total deposition/ radioactive fallout) for 90Sr (half-life, 28.8 years) and 137Cs (half-life, 30.2 years) had continued for 57 years as of April 2014, although the location of the observations moved from Koenji, Tokyo, to Tsukuba in 1980 when the science city was built (Katsuragi 1983). Both radionuclides are

* Correspondence: mailto:[email protected]

Web End [email protected]

1Meteorological Research Institute, 1-1 Nagamine, Tsukuba, Ibaraki 305-0052, JapanFull list of author information is available at the end of the article

2015 Igarashi et al. Open Access This article is distributed under the terms of the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/

Web End =http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made.

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 2 of 19

scientifically important because of their health and environmental impacts (e.g., see U.S. Department of Health and Human Services, Public Health Service, Agency for Toxic Substances and Disease Registry ATSDR2004Cs 2004; U.S. Department of Health and Human Services, Public Health Service, Agency for Toxic Substances and Disease Registry ATSDR2004Sr 2004). We continued collecting and analyzing atmospheric samples after the accident at Tokyo Electric Power Companys (TEPCO) Fukushima Dai-ichi Nuclear Power Plant (FDNPP) in Ohkuma-machi and Futabamachi, Fukushima prefecture (37.42 N, 140.97 E) in March 2011.

Many authors have attempted to determine the environmental impacts of the FDNPP accident, which have gradually come to light (e.g., Aoyama et al. 2012, 2013; Hirose 2012; Kusakabe et al. 2013; Masson et al. 2011; Masumoto et al. 2012; MEXT 2011a ; MEXT and USDOE 2011; Povinec et al. 2013a, b; Tsumune et al. 2013; Yamamoto et al. 2012; Yoshida and Kanda 2012; Yoshida and Takahashi 2012). We still need to study the following issues from an atmospheric science point of view (Igarashi 2009): (1) primary source terms including emissions inventory and temporal changes (e.g., Chino et al. 2011; Katata et al. 2012, b, 2014; Maki et al. 2013; Stohl et al. 2012; Terada et al. 2012; Winiarek et al. 2012), (2) transport and diffusion (e.g., Masson et al. 2011; Morino et al. 2011; Sekiyama et al. 2015; Stohl et al. 2012; Takemura et al. 2011; Tanaka 2013; Terada et al. 2012), and (3) dry and wet removal (e.g., Adachi et al. 2013; Hirose et al. 1993; Kristiansen et al. 2012), which governed radioactive surface contamination during the early phase of the accident. In addition, the physical and chemical properties of the radioactive materials (e.g., Adachi et al. 2013; Kaneyasu et al. 2012) are important factors that influence the second and third subjects to be investigated. Here, we summarize the observations, present a time series of the atmospheric impacts of the TEPCO FDNPP accident over approximately 3 years in Tsukuba, Ibaraki, Japan, and compare the levels to the situation before the accident as very basic scientific information (Igarashi, 2009). In addition, secondary emissions from contaminated surfaces to the atmosphere (re-suspension; Igarashi 2009) have become important during the later phases. Re-suspension comes from contaminated surfaces, terrestrial ecosystems, and open-field burning. These sources have undoubtedly supported atmospheric radionuclides but are not yet well understood and are thus considered briefly. Other information about the accident, related to our immediate monitoring and modeling endeavors and data analysis approaches to short-lived -emitters and 89Sr, is

summarized in the Appendices.

MethodsAtmospheric deposition samplesThe monthly atmospheric total deposition/atmospheric fallout has been sampled using a weathering-resistant plastic tray (area = 4 m2) installed on a cottage roof in an open field of the MRI in Tsukuba, Ibaraki (36.1 N, 140.1 E; approximately 170 km southwest of the FDNPP) since the 1980s. After April 2011, the sample size was reduced to two trays, each 1 m2, which we considered sufficient for the levels present after the FDNPP accident. The collected samples were evaporated and concentrated into a gross quantity with a rotary evaporator (Eyela NE-12) or an evaporating dish, and the samples were saved in a polyethylene safekeeping container. Each evaporated sample, packed in a cylindrical plastic container, was measured for -ray emitting radionuclides (134Cs and 137Cs)

using a Ge semiconductor detector (coaxial-type from ORTEC EG&G or Eurisys) coupled with a computed spectrometric analyzer (Oxford-Tennelec Multiport or Seiko EG&G 92x). The precision, accuracy, and quality control of the measurements are described elsewhere (Otsuji-Hatori et al. 1996).

Part of the sample was then stored for future reanalysis. The remaining sample was added to concentrated nitric acid along with H2O2 and digested in a heating operation. Sr-90 was radiochemically recovered from the obtained sample solution, purified and finally fixed as Sr carbonate precipitate, an activity measurement source. After the source was left for several weeks to achieve

90Sr and 90Y radioequilibrium, its -activity was measured using a low-background 2 gas-flow detector (Tennelec LB5100) with P10 gas (Otsuji-Hatori et al. 1996). Within several months after the FDNPP accident,

89Sr (half-life, 50.5 days) from the accident coexisted with 90Sr and affected the -activity measurement. To remove the 89Sr influence, we occasionally repeated the Sr source measurement and evaluated the radioequilibrium between 90Sr and 90Y, as well as the decrease in

89Sr activity (see Appendix 2). When required, the influence of the 89Sr activity was subtracted from the -activity counts to obtain the 90Sr activity. The activity was always decay-corrected mid-sampling. The detection limit for 90Sr was approximately 7.0 mBq/sample, approximately 3.5 mBq/m2 using a total of 30,000 s of measurement. For 137Cs, the limit was approximately

16.0 mBq/sample, approximately 8.0 mBq/m2 for an average of 120,000 s of measurement.

Atmospheric radioactive aerosolsAerosol samples were collected weekly using a high-volume air sampler (HV; Sibata Scientific Technology Ltd., HV-1000 F) on a quartz fiber filter (Advantech QR100; 203 mm 254 mm) (Igarashi et al. 1999a). During March 2011, the sampling frequency was intensified.

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 3 of 19

The flow rate was set at 0.7 m3/min, and the daily sucked air volume was approximately 1000 m3. After collection, the filters were compressed into pellets using a hydraulic press device. They then underwent conventional -ray spectrometry with Ge detectors as described above. Current detection limits for 134Cs and

137Cs are approximately 9.0 mBq/sample (1.3 Bq/m3) and 10 mBq/sample (1.5 Bq/m3) for approximately 1,000,000 s measurements, respectively.

The filter samples collected before the radioactive plume arrived at Tsukuba were measured at the Kyoto University Research Reactor Institute to achieve lower detection limits and avoid contamination from the FDNPP accident. This was necessary because the Ge detectors, measurement environment, and experimental materials at the MRI were somehow contaminated by the radioactive plumes passage on March 1415 and 2023, 2011 (see Appendix 1). To date, radioSr analysis has been performed on only a limited number of aerosol samples collected during March 2011. The results are presented in Appendix 2.

Results and discussionFigures 1 and 2 depict the results of the atmospheric

90Sr and 137Cs deposition observations at the MRI for

different durations. The temporal changes in monthly radionuclide depositions shown in Fig. 1 include those from the late 1950s to more recently available data, i.e., after the FDNPP accident. Figure 2 compares the amounts of atmospheric deposition after the FDNPP accident and from the late 2000s. Analyses of 90Sr and

137Cs deposition samples taken 6 and 8 months before the accident are ongoing to control for possible sample contamination at the MRI caused by the accident. Thus, these data are missing in Figs. 1 and 2.

Figure 3 depicts the temporal change in atmospheric activity concentrations of radioCs since March 2011. Before the FDNPP accident, it was difficult to detect 137Cs

below about 1 Bq/m3 in the air (the global fallout background level).

Although there were small-scale Japanese nuclear accidents in the 1990s (Igarashi et al. 1999a, 2000; Komura et al. 2000), they did not cause significant marks in the present time series of monthly 90Sr and 137Cs deposi

tions. The effects of the Chernobyl accident that occurred in 1986 were more evident for 137Cs than 90Sr

(e.g., Aoyama et al. 1991) as illustrated in Fig. 1. However, the previous maximum 137Cs deposition was two orders of magnitude lower than those caused by the FDNPP accident. Thus, the impact of the FDNPP

Fig. 1 Sr-90 and 137Cs monthly deposition observed at the Meteorological Research Institute (MRI) from 1957 to 2014. Monthly deposition is

expressed in millibecquerel per square meter on a logarithmic scale. Sr-90 and 137Cs analyses from deposition samples taken 6 and 8 months before

the accident, respectively, are ongoing to avoid possible sample contamination at the MRI because of the accident. Thus, these data are missing not

only in Fig. 1 but also in Fig. 2. The measurement uncertainty (1) is shown only for the data obtained after the FDNPP accident and is reasonably small

compared to the analytical data. For comparison, uncertainty for the monthly data in 2010 is also given. The effects of atmospheric nuclear bomb tests

have been recorded since 1957. Until the Partial Test Ban Treaty (PTBT) became effective in 1963, the USA, Soviet Union, and UK conducted atmos

pheric tests. France and China continued atmospheric testing until 1974 and 1980, respectively. Since 1981, all the nuclear bomb tests have shifted

underground, so additional radioSr and Cs contamination should be negligible. However, the Chernobyl accident in 1986 also affected the time series.

The simple summation of the deposition from 1957 to the time before the FDNPP accident (mid-2010) and decay-corrected summations for 90Sr and

137Cs can be compared to the FDNPP-derived deposition

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 4 of 19

Fig. 2 Monthly 90Sr and 137Cs deposition levels in pre- and post-accident periods. Partial enlargement of Fig. 1. The monthly deposition is expressed in

millibecquerel per square meter on a logarithmic scale. The atmospheric depositions of 90Sr and 137Cs in 2013 observed at the MRI were a few orders

of magnitude higher than those from 2005 to 2011 before the FDNPP accident. For 90Sr and 137Cs, monthly depositions during 2005 to 2010 were

0.519 mBq/m2/month and 1.297 mBq/m2/month, whereas they were 133 mBq/m2/month and 239 Bq/m2/month in 2013, respectively

accident was more remarkable than any previous incident in our time series.

Temporal changes in monthly 137Cs atmospheric depositionThe monthly 137Cs deposition in March 2011, when the FDNPP accident occurred, was 23 0.9 kBq/m2/month, which is six to seven orders of magnitude higher than

the level before the Fukushima disaster (Figs. 1 and 2). Because the pollution source of the FDNPP accident is closer to the observation site (170 km) than it is to the weapons testing sites and Chernobyl (several thousand kilometers), the spatial representativeness of the MRI data (as an absolute value) is lower.

The cumulative 137Cs deposition at the MRI was25.5 kBq/m2/year for the year 2011. The sum of the

Fig. 3 Temporal change in atmospheric radioCs concentrations at the MRI before and after the FDNPP accident (Mar.-Aug. 2014). Activity

concentration is expressed in milli becquerel per cubic meter on a logarithmic scale. The measurement uncertainty (1) is shown. The maximum

concentration of 38 Bq/m3 of 137Cs was observed during March 2021, 2011. After that, the radioCs concentrations rapidly decreased until fall

2011 when the decrease slowed. The levels before (approximately 1 Bq/m3) and 3 years after the FDNPP accident (12 Bq/m3 from March to

August 2014) are also compared. A difference of at least one order of magnitude is observed between the concentration level from March to

August 2014 and the level before the FDNPP accident

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 5 of 19

simple monthly 137Cs depositions from 1957 to mid-2010, the time before the Fukushima disaster, is approximately 7.0 kBq/m2 (this figure is thought to contain some error since the pre-1970s data did show individual undefined errors), as shown in Fig. 1. Considering the radioactive decay of the individual monthly 137Cs deposi

tions, this past total contribution represents 2.3 kBq/m2.

The FDNPP accidents influence was over ten times larger than that of any past event. Almost the same amount of 134Cs (half-life, 2.1 years) was simultaneously deposited with the 137Cs; thus, the total cesium deposition came to more than 50 kBq/m2. This value agrees quite well with figures for the area around Tsukuba in observation mapping provided by the Ministry of Education, Culture, Sports, Science and Technology (MEXT 2011a).

Later, the deposition decreased rapidly, but the monthly

137Cs deposition in 2012 and 2013 ranged from 836 and 239 Bq/m2/month, respectively, where deposition during 20052010 had been in the range of 1.2 97 mBq/m2/month, i.e., three to four orders of magnitude higher. The deposition level at the end of 2013 was still as high as values registered when atmospheric nuclear tests were conducted by China in the 1970s to the early 1980s. The deposition rate slowly decreased in the following years.

Atmospheric concentrations of radioCsFigure 3 displays the temporal change in the atmospheric radioCs activity concentrations at the MRI in Tsukuba since the FDNPP accident. The temporal trend shows an abrupt increase (peak) of several orders of magnitude, followed by a rather rapid concentration decrease over a short period (3 to 4 months after the FDNPP accident), with a smaller decreasing rate after. The highest 137Cs atmospheric concentrations (38 Bq/m3 in a 12 h sampling period) were registered on March 2021, 2011, which slightly exceeded the limit stipulated by Japanese regulations and ordinances (30 Bq/m3).

Although the pre-accident activity concentration level was not measured, it had been observed for a short period, from February to April 1997, which includes the time when the Power Reactor and Nuclear Fuel Development Corporation Tokai accident occurred (Igarashi et al. 1999a). The background level was approximately 1 Bq/m3 and did not decrease far below half that value (approximately 0.5 Bq/m3) until 2011. The decrease in monthly 137Cs deposition was small during the same period (Igarashi et al. 2003, 2009). Thus, the 137Cs ac

tivity concentration level registered during summer 2014 appears at least 10 times higher than that before the accident. During 2011 and 2012, small spikes were recorded from time to time (Fig. 4). In these cases, daily forward trajectory analysis suggested that the polluted

air masses were transported from the accident site during the corresponding observation period as shown in the figure. In addition, relatively high concentrations were registered in the winter (Fig. 3). This phenomenon was noted at other places in northern and eastern Japan (Hirose 2013), so there is most likely a common explanation, as described in the literature.

Temporal change in monthly 90Sr atmospheric deposition In contrast to 137Cs, the monthly 90Sr deposition in March 2011 was 5.2 0.1 Bq/m2/month. This was approximately 1/5000 the amount of 137Cs deposited in the same month. This deposition was 23 orders of magnitude larger than the level before the FDNPP disaster. The annual 90Sr deposition was 10.6 Bq/m2/year during 2011, approximately 1/2500 of the quantity of

137Cs deposited. The simple sum of the monthly 90Sr depositions from 1957 to mid-2010, before the Fukushima disaster, was approximately 2.7 kBq/m2, as shown in Fig. 1. Taking the radioactive decay of the individual monthly 90Sr depositions into account, the sum represents approximately 0.9 kBq/m2. The FDNPP accidents impact on 90Sr was very small. The most extreme monthly 90Sr deposition, recorded during the global fallout era of May 1963 in Tokyo, was 170 Bq/m2/month. The FDNPP accidents impact on the monthly 90Sr depos

ition was less than one-thirtieth of this maximum. Therefore, it is probable that 90Sr pollution over the Kanto Plain from the accident was relatively insignificant; the environmental and health impacts of 90Sr are relatively minor.

In addition, the 137Cs/90Sr activity ratio fluctuated between approximately 400 and 5000 (Fig. 5), except for some abnormal cases described below. This confirms that the degree of radioSr pollution is relatively insignificant compared to that of radioCs. However, it is still unknown why the 137Cs/90Sr activity ratio varied so widely despite the radionuclides having a common accident emission source, namely, the FDNPP accident. More discussion on the 137Cs/90Sr activity ratio is given in Appendix 2. The reason for the variability is worth studying in the future. The monthly 90Sr deposition recorded in 2012 was 1031 mBq/m2/month, whereas during 2005 2010, it was 0.519 mBq/m2/month, a difference of up to two orders of magnitude.

A 90Sr deposition anomaly in October 2012In October 2012, the monthly 90Sr deposition showed a peak of 145 2 mBq/m2/month (see the arrow in Figs. 5 and 6), which is 12 orders of magnitude higher than any monthly 90Sr deposition registered that year, and its influence lasted a few months (Fig. 6). This small 90Sr

event remains puzzling. By applying forward trajectory analysis and closely examining the precipitation over Tsukuba, we believe that the 90Sr may have come from

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 6 of 19

1x100

11/3/2 11/4/30 11/6/30 11/8/30 11/10/30 11/12/30 12/3/1 12/4/30 1 /30 13/3/2

Atmospheric activity concn. (mBq/m3 )

Fukushima Accident

8x10-1

6x10-1

134Cs

137Cs

4x10-1

2x10-1

0

ND level

Date (yy/m/d)

Fig. 4 Atmospheric concentration increases observed during 2011 and 2012 and their air mass trajectories. Note that the activity concentration

scale is linear. The forward air mass trajectory calculated by the NOAAs HYSPLIT model is depicted for the radioCs activity concentration peaks,

suggesting that the plume from the FDNPP site passed over the Tsukuba region. The shown trajectory cases are December 1, 2011 and April 5,

2012. The increases seem to be attributable to the transport of primary radioCs from the accident site

the FDNPP and encountered precipitation on October 7 and 1819, 2012. However, this increase was not accompanied by a radioCs deposition peak, and the major radionuclide emitted by the FDNPP accident is radioCs, which is inconsistent with FDNPP accident being the source of the October anomaly.

The Japanese Radioactivity Survey data on the Internet were checked, but no consistent data were evident for the corresponding period. In addition, no such anomaly

was reported in Europe (Masson 2014, personal communication). Based on the timescale of this contamination, however, the source should be neither very local nor very small. This episode shows some similarities to the case in fall 1995 in Tsukuba (Igarashi et al. 1999b). We also assume unidentified, unreported incidents of burning and/or melting of industrial 90Sr sources in the Far East region as a possible explanation, such as the Algeciras (Spain) incident in 1998 with its 137Cs source of

Fig. 5 Activity ratio of 137Cs/90Sr in monthly depositions since March 2011 at the MRI. The temporal changes do not show a clear decreasing or

increasing trend. The arrow shows the month during which an anomalous deposition of 90Sr was observed. Except for the anomaly, the 137Cs/

90Sr activity ratio fluctuated from approximately 150 to 6700

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Fig. 6 Exponential fitting of the decreasing monthly 137Cs deposition trend since March 2011 at the MRI. The curve is composed of three exponential

functions. These are attributable to the decreasing intensity of primary emission, tropospheric aerosol residence and re-suspension. The arrow shows

the month during which an anomalous 90Sr deposition was observed. Possible causes are mentioned in the text

3.7 TBq (Estevan 2003). Sr-90 is widely used in industrial applications, such as in thickness gauges, and its activity size ranges from 740 MBq to 3.7 GBq in Japan. Because 90Sr is a pure -emitter, it is more difficult to determine the sources of its environmental pollution than it is for 137Cs.

Decrease in monthly 137Cs deposition after the FDNPP accidentAlthough researchers do not agree precisely on the FDNPP radioactivity emission inventory (Chino et al. 2011; Katata et al. 2012, 2012b, 2014; Maki et al. 2013; Stohl et al. 2012; Terada et al. 2012; Winiarek et al. 2012), if the 137Cs emission in March 2011 is assumed to be 10 PBq/month, the deposition/emission ratio (the monthly deposition at the MRI divided by the monthly emissions from TEPCO (2012)) would be approximately 1012. If the MRI is included in the so-called hot spot area, the deposition could be approximately 100 kBq/m2 (five times larger). This would give a deposition/emission ratio of approximately 1011. After March 2011, the ratio is calculated to be in the range of 1010 to 109, which appears to be large, if the emission-deposition relation above is correct. We can presume that this excess deposition at the MRI, Tsukuba came from secondary emissions. Thus, Tsukuba can be regarded as representative of a typical suburban area in the Kanto Plain, and the relative trend of temporal changes there can be considered comparable to surface contamination levels for similar geographical domains. The temporal trends

(holding time constant) may also be spatially representative, although this potential is limited.

To study the decreasing trend in monthly 137Cs at

mospheric deposition caused by the FDNPP accident and to make future projections, a curve was fitted on the temporal trends using multiple components. A drawing software was employed, and the fitting operation was put through 100 iterations, each time changing the initial value so that the calculation results would converge, as shown in Fig. 6. A trinomial exponential function of the form a (ekt) was applied to fit the data (where a is a constant and k is an inverted time scale; Ln2/T1/2), and the individual half-times (T1, T2, and T3 in Fig. 6) were approximately 5.9 (11 %) days, 16 (18 %) days, and 1.1 (32 %) years, respectively. The relative uncertainty is shown in parentheses. These appear to correspond to the time scale of (1) the reduction in the original FDNPP accident surge (primary emission source), (2) the tropospheric transportation and diffusion of the radioactive plume (equivalent to the removal of radioactive aerosols from the atmosphere), and (3) the emission intensity of re-suspension (secondary emission sources). We posit that some primary radiological release to the atmosphere continues because the FDNPP is not isolated from the neighboring environment (Hirose 2013; TEPCO 2012). The results, then, cannot be assumed to be completely free of primary release. However, the first and second terms can be reasonable estimates corresponding to the primary emission and tropospheric aerosol residence, respectively.

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 8 of 19

The second term is almost identical to figures obtained by other recent studies (e.g., Hirose 2012, 2013; Kristiansen et al. 2012). Hirose (2013) analyzed radioCs deposition data obtained during 20112012 from several places over the Kanto Plain and Fukushima prefecture, Japan. According to his report, The apparent half-lives at Ichihara, Tokyo, Utsunomiya, Hitachinaka and Maebashi were 11.9, 10.6, 13.5, 11.5 and 12 d, respectively. Hirose (2012) states that the residence times of aerosols in the troposphere, which are in the range of 530 d, have been determined by natural and anthropogenic radionuclides, which depend on particle size and altitude (Ehhalt, 1973). Hirose (2012) also argues the temporal change of the Fukushima-derived 137Cs revealed that the apparent atmospheric residence time of the Fukushima-derived 137Cs

in sites within 300 km from the Fukushima Dai-ichi NPP is about 10 d. This long residence time might reflect the Fukushima radioactive plumes circulation over the Northern Hemisphere, which takes about 20 days (Hernndez-Ceballos et al. 2012). As shown in Fig. 8a in the Appendix 1, the third Fukushima plumes arrival over the Kanto Plain was observed from March 2831, 2011. It was well reconstructed by the aerosol transport model. Other observations over the Kanto Plain also revealed this transport event (e.g., Amano et al. 2012; Haba et al. 2012). However, we cannot clearly determine whether this concentration peak is due to delayed primary emission (e.g., Terada et al. 2012), hemispheric circulation, or a combination of both. This is because the current model simulation uses the emission inventory, which is also based on atmospheric monitoring results (e.g., Terada et al. 2012). Regarding this connection, Kristiansen et al. (2012) investigated the 131I and 137Cs removal times

from the atmosphere using global-scale monitoring data. Their estimated 137Cs removal times were in the range of 10.013.9 days, which is closer to our present result. They also noted the difference from the typical values of 37 days obtained by aerosol model simulations, suggesting that the aerosol transportation models need improvement. We would like to add that the deposition results should be interpreted to reflect not only the surface air but also the air column up to at least the mixed layer. Therefore, the deposition may be affected by large-scale transportation, in contrast to indications obtained from the surface concentration only. For further reference, based on the monthly emission of radioCs until the end of 2011 estimated by TEPCO 2012, the primary emission decrease can be fitted using two exponential laws with half-time constants of2.3 days (2 %) and 48 days (23 %).

The third terms half-time of 1.1 years for the MRI

data, despite its relatively large associated uncertainty, appears to reveal the total re-suspension of radioCs from contaminated surfaces. This value is too large to

correspond to any primary releases from the FDNPP in the early phases. In addition, it agrees with the value for the re-suspension descending trend due to the Chernobyl accident reported by Garger et al. (2012), which was 300 days. It was possible to fit a two-term exponential curve to the present 137Cs data by fixing the 1.1-year

half-time, obtaining a value of 7.8 days for the first term. When compared with the triple exponential (three-term) model, the fitting distance (defined by the ratio of the calculation to the observation) for the double exponential (two-term) model was larger for elapsed times of 2 12 months, although there were exceptions. The mean and standard deviation for the two- and three-term fit distances are 2.50 2.02 and 1.54 1.14, respectively. The medians are 1.82 and 1.09, respectively, suggesting that the three-term model fits better. Although we do not provide an illustration here, we found that fitting with three-term functions for the decrease in monthly

90Sr deposition after the disaster was also possible. Therefore, we preferred fitting with a trinomial exponential function to reproduce the deposition flux of radionuclides from the FDNPP accident. Again, the primary emissions of radioCs to the atmosphere are anticipated to continue at a non-negligible level (less than 7.2 GBq/ month is assumed in TEPCOs latest press release (in Japanese) at http://www.tepco.co.jp/life/custom/faq/images/d150129-j.pdf

Web End =http://www.tepco.co.jp/life/custom/faq/im http://www.tepco.co.jp/life/custom/faq/images/d150129-j.pdf

Web End =ages/d150129-j.pdf ) because the FDNPP is not isolated from the surrounding environment (Hirose 2013). These delayed primary emissions of approximately 7 GBq are 67 orders of magnitude lower than the emissions in March 2011 (e.g., 15 PBq for 137Cs; NISA 2011). If the

primary emission deposits were delayed in a fashion similar to those from March 2011, recent MRI records after the FDNPP accident would correspondingly be 67 orders of magnitude lower than the peak value caused by the accident (see Fig. 2). Therefore, we consider that the present decrease in the third term reflects secondary emission (re-suspension) trends over the Kanto Plain moderately well. In future, we plan to confirm this by applying different evaluation methods such as transport simulations or others.

Consideration of re-suspension and its persistence Currently, there may be interest and concern about how long it will take for the atmospheric radionuclide deposition fluxes to return to pre-FDNPP accident levels (cf. Garger et al. 2012; Hatano and Hatano 2003). Although it seems slightly arbitrary, the monthly 137Cs depositions can be estimated if the fitted curve described above is extrapolated. The result of this extrapolation is illustrated in Fig. 7. This simple estimation shows that more than a decade will likely be required for the activity levels to return to pre-accident levels. Thus, re-suspension (secondary emission to the atmosphere;

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 9 of 19

Fig. 7 Future projection for monthly 137Cs deposition level using a trinomial exponential function. The present simple estimation shows that

more than a decade would be necessary for the 137Cs atmospheric deposition level to return to pre-accident levels

e.g., Igarashi 2009) must be scrutinized with long-term monitoring. Because it seems natural that radionuclide emission flux would be proportional to surface pollution density, there could be radioCs fluxes several orders of magnitude higher than those measured in Tsukuba in areas nearer the FDNPP site whose Cs surface pollution is several orders of magnitude higher than in Tsukuba. Therefore, elucidating the secondary emission processes of the FDNPP radionuclides remains an imminent scientific challenge, especially for heavily polluted areas. Secondary sources can include soil dust suspension from polluted earth surfaces, emissions from polluted vegetation and forests, and volatilization and release from combustion of polluted garbage and open field burning (e.g., Igarashi 2009). Although the main emission sources are not yet well understood, this elucidation must be performed as soon as possible.

ConclusionsThe authors conducted atmospheric monitoring of airborne radioSr and Cs and their deposition at the MRI in Tsukuba, Japan. The monitoring period encompasses the FDNPP accident and the subsequent few years. The monthly 137Cs deposition at the MRI was (23 0.9) 103 Bq/m2/month in March 2011, which is 67 orders of magnitude higher than pre-accident levels. Almost equal amounts of 134Cs and 137Cs were deposited,

causing surface pollution of more than 50 kBq/m2 in

Tsukuba in 2011, in close agreement with the Ministry of Education, Culture, Sports, Science and Technology, Japan (MEXT)s airborne mapping. Deposition of 90Sr

was 5.2 0.1 Bq/m2/month in March 2011, which is less than 0.02 % of the total 137Cs deposition in that month. The level of 90Sr deposition was 34 orders of magnitude higher than pre-accident levels and did not reach the level registered during the 1960s after nuclear tests; the effects from 90Sr will not be as large as from

radioCs. During 2013, the Fukushima fallout decreased by 34 orders from its magnitude at the time of the accident, yet some becquerel per square meter of monthly deposition continues. This corresponds to the level in the 1970s and early 1980s when China performed atmospheric nuclear tests. During 2013, the 137Cs concentration remained at a level of tens of micro becquerel per cubic meter. Because re-suspension (secondary emission) will continue over a long time, it is necessary to monitor its future trends and variability. An apparent decrease in atmospheric radioCs deposition was fitted by trinomial exponentials, giving information regarding the reducing trend of airborne radionuclide persistence through re-suspension into the atmosphere. Extrapolation of the decreasing rate suggests that it would take at least a decade for the activity to return to pre-disaster period levels. Further monitoring efforts are essential.

Appendix

Appendix 1 Temporal changes in radioactive aerosol concentrations and plume transport from the FDNPP accident over Tsukuba in March 2011 IntroductionThe heat and blast at the FDNPP accident resulted in the leakage of a huge amount of anthropogenic radionuclides, near the levels of the Chernobyl accident in 1986, into the environment (IAEA 2006; Janekovi and Kriman 2011; NISA 2011), as seen on both the domestic and Northern Hemispheric scale (Hernndez-Ceballos et al. 2012; Masson et al. 2011; Takemura et al. 2011; Tanaka 2013). The transport of the radioactive plume and its deposition over the Pacific Ocean (Aoyama et al. 2013; Honda et al. 2012), North America (e.g., Schwantes et al. 2012; Zhang et al. 2011), and Europe (e.g., Masson et al. 2011) as well as within the Japanese

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 10 of 19

territories (Hirose 2012; Kinoshita et al. 2011; Morino et al. 2011; Terada et al. 2012; Tsuruta et al. 2014) has been well depicted by many researchers. The pattern of domestic pollution of the land by local fallout was made fairly clear by the creation of a contamination map based on many university investigations (Kinoshita et al. 2011; Tanihata 2013) and airborne surveys by Japans MEXT and the USAs NASA/DOE (MEXT and USDOE 2011; Sanada et al. 2014; Torii et al. 2013; USDOE 2013). The transport of the radioactive plume and its subsequent deposition over the capital area (the Kanto Plain; Amano et al. 2012; Haba et al. 2012; Tsuruta et al. 2014) has been reported and monitored in Tsukuba (Doi et al. 2013; Kanai 2012). The MRI in Tsukuba suffered almost no electricity outage soon after the earthquake. Thus, aerosol sampling at the observation field continued from before the FDNPP accident through its aftermath. Here, we add our independent observations of the temporal changes in atmospheric radionuclide concentrations over Tsukuba covering all of March 2011, with our specific transport model simulation for reference.

ExperimentIntensified aerosol samplingAerosol samples were collected onto quartz fiber filters using a high-volume sampler, as described in the body of the paper; the only change was the duration of sampling, from 1 day to 6 hwhich was altered as soon as the accident was made public. The total sucked air volume was thus between 250 and 1000 m3.

Activity measurementAfter collection, the filters were treated in the same manner as usual and measured with Ge detectors, as described previously. The filter samples collected before the radioactive plumes arrival at Tsukuba were measured at the Kyoto University Research Reactor Institute (KURRI) to lower the detection limits. This was necessary because the Ge detector and the laboratory environment at the MRI building were contaminated by the radioactive plume on March 1415 and 2022, increasing the background levels. Before the compression procedure, portions of the filter were punched out (33 mm 4 pieces), of which one piece was selected for radioSr analysis, as noted in Appendix 2.

Transport modelingThe Eulerian chemical transport model RAQM2 (Kajino et al. 2012; Adachi et al. 2013; Sekiyama et al. 2015) was used to simulate radioactive plume transport from the FDNPP accident over the Kanto Plain. The JMA/MRI non-hydrostatic meteorological model (NHM; Saito et al. 2007) was used to simulate the meteorological

field to calculate the transport and deposition processes of radionuclides using RAQM2. The horizontal domain and its grid resolution (3 km) were common to both NHM and RAQM2, with 50 vertical layers from the surface up to 22 km for NHM and 20 layers to 10 km for RAQM2. The JMAs Meso-Regional Objective Analysis (MANAL), which has a horizontal resolution of 5 km, was used to define the boundary conditions for NHM. The calculated domains cover southern Tohoku and the central part of Honshu. Details of the transport (advection, diffusion, and convective transport) and deposition schemes (dry and wet (in cloud and below cloud, grid-scale and sub-grid-scale)) are described in Kajino et al. (2012) and Sekiyama et al. (2015).

We simulated five species of particulate radionuclides (volatile and reactive 131I (I2), volatile and non-reactive 131I (CH3I), non-volatile

131I, 134Cs, and

137Cs). We conducted dispersion and deposition simulation of radioCs in two very different formshygroscopic submicrons vs. hydrophobic supermicronsin a previous study (Adachi et al. 2013) and showed that the deposition regions were significantly different. However, because the proportions of hygroscopic and hydrophobic radioCs in emissions have never been estimated, we assumed the hygroscopic submicron aerosols to be the carriers of radionuclides and used dimensions equivalent to the geometric mean of the dry diameter Dg,n,dry = 102 nm, geometric standard de

viation g = 1.6, particle density p = 1.83 g/cm3, and hygroscopicity = 0.4 (Petters and Kreidenweis 2007; Adachi et al. 2013). The emission inventories of 131I

and 137Cs were taken from Katata et al. (2014). RAQM2 incorporates aerosol dynamic processes, such as nucleation, condensation/volatilization, and coagulation, within and among different aerosol categories, but the size distribution of the aerosols was assumed to remain unchanged in this simulation.

Results and discussionParticulate fission products and radioCsThe detected -emitting radionuclides were 99Mo-99mTc (half-life, 65.96 hours), 129mTe (33.6 days), 131I (8.02 days),

132Te-132I (3.20 days2.3 hours), 133I (20.8 hours), 134Cs(2.07 years), 136Cs (13.2 days), and 137Cs (30.0 years) as shown in Fig. 8a in the Appendix 1. Note that gaseous iodine was not captured by the present sampling. The 90Sr results are also plotted in the figure (for analytical details, please refer to Appendix 2). There were two significant transport events that brought the radioactive plume toward the Kanto Plain in March 2011. One was during March 1415 and the other occurred during March 2022. Plume transport is determined by temporal changes in emission

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intensity and the wind field near the ground surface, which have been addressed by many authors (e.g., Katata et al. 2012, 2014; Morino et al. 2011; Terada et al. 2012). The releasing sources are attributed to a venting operation at an individual reactor vessel, reactor core damage, buildings damaged by a hydrogen explosion, and continuous release through a reactor building (see, e.g., TEPCO 2012; Katata et al. 2014). The activity concentrations of these radionuclides were consistent with those described in previous reports regarding Tsukuba (e.g., Doi et al. 2013; Kanai 2012). The March 712, 1213, 13, and 1314 samples exhibited detectable levels of radioCs and 131I, for which

we cannot totally rule out the possibility of sample contamination despite their measurement at KURRI. The two events exhibited different radionuclide compositions, reflecting different source at the accident site. Although the 134Cs/137Cs ratio was unity for

both transport events, the activity ratios were 131I/

137Cs 5 and 132Te/137Cs 8 during the first event

and 131I/137Cs 2.5 and 132Te/137Cs 1 during the

second event. Te-132 was significant during the first transport event. Because the melting point of metallic Te is 450 C, whereas that of Cs is only 28 C, the finding may suggest a higher temperature for the source in the earlier phase. For comparison, 90Sr data

are included in Fig. 8a in the Appendix 1; the details of the measurements are given in Appendix 2.

After the FDNPP accident, unlike in Chernobyl, no radioRu was found (Aoyama et al. 1986, 1987). This may be because of the different accident scenarios; the melting temperature of metallic Ru is very high (approximately 2500 C).

Another notable point is the magnitude of the concentration drop between the first and second plume events. RadioCs and 132Te concentrations were 45 orders of magnitude lower for the second plume than the concentration peaks, and those for 131I were 23 orders of magnitude lower. This difference appeared to be caused by either the re-suspension of radioI or the contamination of our materials and instruments. The latter seems unlikely, however, because the filter samples were treated identically and the maximum contamination levels would be those found for the March 714 samples (measured at the KURRI). We gave sufficient attention to reducing contamination during sampling and sample handling. Nevertheless, the entire environment was contaminated, and therefore, it was difficult to avoid entirely. In any case, the volatile nature of iodine (the boiling point of CH3I is 42 C, while the melting point of I2 is 113 C) is likely part of the cause. Therefore, immediate re-suspension of radioI should be given more attention. This is briefly addressed below.

Transport model simulationThe aerosol simulation model captures the events that transported the radioactive plume to the Kanto Plain very well (see Fig. 8b and 9 in the Appendix 1). The transport of the plume from the southern Tohoku district is not considered very exceptional (the MRI is approximately 170 km southwest from the accident site). Aoyama et al. (1999) and Igarashi et al. (1999a) analyzed the radioactive plume over the Kanto Plain from the earlier PNC accident in Tokai, Ibaraki, in 1997. Igarashi et al. (2000a,b) conducted continuous observations at the MRI of 85Kr, of which the local source was the Tokai nuclear fuel reprocessing plant approximately 60 km northeast of Tsukuba. They noted the incidence of plume transport from a point source in northern Ibaraki over the Kanto Plain with a northeasterly wind, a prevalent weekly wind pattern occurring during the spring in Japan. Similar meteorological situations appeared to occur on March 1415 and March 2022, 2011 over the Kanto Plain. Notably, the drop in activity concentration between the plume advections is evident in the simulation results ( Fig. 8b and c in the Appendix 1) despite only primary emissions coming from the FDNPP accident. The reality of the observations differed from the simulations (Fig. 8a in the Appendix 1). As described above, contamination in the observation procedures cannot be totally ruled out, but by coupling the model and observations, it is possible to evaluate the immediate re-suspension of the atmospheric Fukushima radionuclides (see section below).

Finally, we argue that aerosol transport modeling is an indispensable tool for the assessment of accident effects. However, many uncertainties remain, especially concerning the emission inventory, wet and dry deposition, and cloud processes. Data and information are collected to improve the transport model schemes, and comparison of different models has been performed to contribute to an accurate evaluation of the source term and transport and deposition processes (SCJ 2014).

Estimation of immediate re-suspension factorThe quantity of the deposited radionuclides that could return again to the air (re-suspension) is notable. Maximum re-suspension is known to occur just after radioactive plume passage (hereafter, we call this immediate re-suspension). Thus, as a primary approach, immediate re-suspension factors were roughly estimated with modeled amounts deposited in the Kanto Plain by the first plume and the observed minimum activity concentration between the two plume events, i.e., March 17 09JST to March 20 09JST. We assumed mass closure between re-suspension from the contaminated surface and outflow by horizontal advection and turbulence vertical mixing as below.

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 12 of 19

Fig. 8 Atmospheric activity concentrations of radionuclides from the FDNPP accident in March 2011. a Observed data from filter samples collected at

the MRI, Tsukuba, Japan; b comparison of observed (black) and simulated results (red) for 137Cs; and c similar to b but for particulate 131I. The abscissa is

expressed in dates in March 2011 and is labeled at the start of the day in a and the middle of the day in b and c. Contamination of the filter samples

cannot be totally ruled out for the period before March 14 in a, which is depicted by the left-right pointing double arrow

The continuity equation is expressed as

C=t K

dif C

UC

C ;

in which C is concentration, Kdif indicates three-dimensional diffusion terms, U denotes the wind field, is

the decay constant, and is a re-suspension term for individual radionuclides. On the other hand, the concentration increase in one unit of time from re-suspension is expressed as

C=t ki Di xy=xyz;

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 13 of 19

a b

Fig. 9 Radioactive plume transport from the FDNPP accident in the Kanto Plain in March 2011. a On March 15 07JST and b on March 20 12JST.

The figures show the simulated surface 137Cs concentration in shaded colors with the model topography in grayscale

in which ki and Di are a re-suspension factor (/s) and surface contamination (Bq/m2) for individual radionuclides, respectively. Also, x, y, and z are the horizontal and vertical lengths of the space where the mass closure is obtained.

We can disregard radioactive decay, horizontal diffusion, and convective wind. Balancing the mass between inflow and outflow, we finally obtain the following relationship:

kiDi=z K z=z C=z u=x

v=y Ci;

in which i indicates the radionuclides, namely, 137Cs

and 131I; Di indicates the modeled total (gas + aerosol) cumulative deposition (Bq/m2) by March 17 09JST; ki is the re-suspension factor (s1); U and Kz are the modeled space- and time-averaged horizontal wind speed (m/s) and vertical turbulent diffusivity (m2/s), respectively; Ci indicates the time-averaged observed concentrations of the radionuclides (9.75 104 and 3.14 101 Bq/m3 for

137Cs and 131I, respectively); and x, y, and z are the horizontal and vertical distances in space over which the above mass closure is obtained. To obtain the horizontal and vertical gradient terms on the right-hand side of the equation, the concentrations outside the space are assumed to be zero (no inflow into the space).

The re-suspension factors for 137Cs and 131I are 7.0

106 /s and 5.3 104 /s, respectively, for the smallest volume of the RAQM2 model grid (x = 3 km, y = 3 km, and z = 100 m). Those for 137Cs and 131I varied

from 1.6 106 /s to 1.5 105 /s (6.1 106 /s on average) and from 5.3 104 /s to 1.3 103 /s (4.6 104 /s on average), respectively, for the various horizontal spaces plus neighboring zero, one, or two RAQM2 grids from the grid where the MRI is located (i.e., x, y = 3,

9, or 15 km) and vertical spaces plus zero, one, or two RAQM2 grids from the bottom (z = 100, 200, or 400 m).

In summary, the immediate re-suspension factors ki of

137Cs and 131I are estimated to be on the order of 106 105 /s and 104103 /s, respectively, and that of 131I is approximately two orders of magnitude larger than that of 137Cs. These values are converted correspondingly, often quoting the concentration ratio over the contaminated surface as follows: 5.8 106 1.7 105and 4.4 104 1.3 103 /m) for 137Cs and 131I, respectively. The present data do not display the large deviation hitherto reported (e.g., 106104 /m; Maxwell and Anspaugh 2011). Because those values are based on rough assumptions, further studies based on surface flux measurements need to be conducted to more accurately estimate the re-suspension factors.

Appendix 2 RadioSr in the aerosol samples collected during March 2011IntroductionThere are several reports containing estimates of the radioactive contamination from the FDNPP accident, presented in the form of mapped images produced from the results of investigations of radionuclides in the soil (e.g., MEXT 2011a ; Sanada et al. 2014; Torii et al. 2013) and in the form of air dose rate figures produced from aircraft observations. Among the radionuclides, radioSr is an important indicator of contamination. The former Nuclear and Industrial Safety Agency (NISA) in Japan reported the following emission estimates within the atmosphere: 89Sr (half-life, 50.5 days) as 2.0 1015 Bq and

90Sr (half-life, 28.8 years) as 1.4 1014 Bq (NISA 2011). Nevertheless, there have been no reports on 89Sr and

90Sr in air samples because of analytical difficulty. The detection of nine different -emitting radionuclides, including 99Mo, is described in Appendix 1. However, 89Sr

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and 90Sr emit no -rays with their radioactive decay, making it impossible to determine their presence by -spectrometry. To evaluate their radioactive pollution levels, the aerosol components were radiochemically extracted from the HV filter sample to analyze the radioSr and assess the emission ratios of 137Cs, 89Sr, and 90Sr.

ExperimentSub-HV filter sample for Sr analysisHV filter samples from the -spectrometry measurements noted earlier were used for the radioSr analysis. Approximately 2 % of the filter area was punched out (as circles) and provided for this analysis, which was performed on sub-filter samples collected during March 2011 (Table 1 in the Appendix 2).

Analysis of radioSrTo dissolve the aerosols on the filter, 100200 ml of concentrated nitric acid was added and heated on a 200 C hotplate, then 15 ml of hydrogen peroxide solution was added to accelerate the decomposition of any organic matter. This was followed by further thermolysis for more than an hour. The obtained solution was subjected to separation, which was conducted through radiochemical analysis comprising several precipitation separations, such as oxalate, fuming nitric acid, hydroxide, carbonate, and barium chromate precipitations. The last separation was repeated twice, which allowed the Sr fraction to be freed from radioBa and Ra isotopes. The final strontium carbonate deposit was -counted with the low-background 2 gas-flow counter described earlier (Tennelec LB5100).

Estimating the activity ratio of 89Sr and 90Sr

The atmospheric aerosol sample contained 89Sr and 90Sr,

indicating that the total -activity must be deconvoluted. The measurement sensitivity of the gas-flow counter was confirmed for possible energy independence; therefore, the temporal change in the -counting rate of a purified 90Sr (maximum -ray energy 0.546 MeV) source and 90Y (maximum -ray energy 2.24 MeV) growth from the parent nuclide was observed in five specimens of the MRI reference fallout samples (Otsuji-Hatori et al. 1996) that contained no 89Sr. The following equation was then applied to find the counting efficiency of 90Sr and 90Y:

Ntotal ASr90 m1 AY90 1et m2:

Ntotal is the total counting rate (cpm); A stands for

each nuclides -activity (dpm); is the decay constant of 90Y; t is the elapsed time; and m1 and m2 are the counting efficiencies of 90Sr and 90Y, respectively. The -ray energy emitted by 90Y is approximately 4 times that of 90Sr, and the average values of m1 and m2 from the five specimens were 27.3 1.8 % and 24.8 3.7 %, respectively.

There were no statistically significant differences. Thus, the -activities of radioSr were interpreted to have the same counting efficiency regardless of the -energy. The activity ratio of 89Sr and 90Sr was elucidated from the value traced back to the date of sample collection as well as the fixed date when the strontium carbonate precipitated. The activity was always decay corrected in the middle of the sampling time. The current detection limit for radioSr in air at that time was approximately 230 Bq/m3.

Results and discussionEstimation of 90Sr in the aerosol sampleWe will now quantify and describe the radioSr found in the air over Tsukuba. The radioactivity in Tsukuba indicated a two-fold concentration increase in March 2011, as shown in Fig. 8 in the Appendix 1. The amount of radioSr in the sample was smaller than what was anticipated based on past experience (e.g., Aoyama et al. 1991). 90Sr was unable

to be detected except when plume transport occurred. From March 14 9 pm (JST) to March 15 9 am, from March 15 9 am to 3 pm, and March 20 9 pm to March 21 9 am, the results were 1.5 0.13, 1.0 0.10, and 1.3 0.13 mBq/ m3, respectively. For the other samples, the radioSr was

Table 1 Temporal variation of 90Sr activity concentration in the air over Tsukuba

Sampling start date

and time (JST)

End date and

time (JST)

90Sr activity concentration

(mBq/m3)

March 12 21 pm March 13 9 am ndMarch 13 21 pm March 14 9 am ndMarch 14 9 am March 14 21 pm ndMarch 14 21 pm March 15 9 am 1.50 0.13 March 15 9 am March 15 15 pm 1.04 0.095 March 15 15 pm March 15 21 pm ndMarch 15 21 pm March 16 9 am ndMarch 16 9 am March 17 8 am ndMarch 17 9 am March 18 8 am ndMarch 18 8 am March 19 9 am ndMarch 19 9 am March 20 8 am ndMarch 20 9 am March 20 21 pm ndMarch 20 21 pm March 21 9 am 1.32 0.13 March 21 9 am March 22 9 am ndMarch 22 9 am March 23 8 am ndMarch 23 9 am March 24 9 am ndMarch 24 9 am March 25 9 am ndMarch 25 9 am March 28 9 am ndMarch 28 9 am March 29 9 am ndMarch 29 9 am March 30 9 am nd

Although the nd measurements change, depending mainly on the sample volume, the average level was approximately 0.2 mBq/m3nd not detected

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lower than the detection limits (Table 1 in the Appendix 2). The 90Sr activity results shown here were calculated based on -counts made long enough after the events that the contribution of 89Sr could be negligible (less than 5 % of

90Sr activity). For example, we waited at least 200 days after chemical separation (separation was performed after December 2011). The accompanying uncertainty was estimated from the average of the relative -count uncertainties in the five latest individual measurements.

The activity ratio of 137Cs/90Sr in the aerosol samples,

which was in the range of 470023,000, is very large compared with the activity ratio of radioactive fallout, which was 1.63 during the 19601970s; this indicates a clear difference in the data before and after the FDNPP accident. Furthermore, the MRIs estimated 137Cs/90Sr ratio for the

Chernobyl radionuclides in May 1986 in Japan was 96 (Aoyama et al. 1991), which indicates that the Fukushima radionuclide composition was dominated by radioCs. In the activity peak on March 1415, the ratio was 4700 6000, and the peak on March 2021 was 23,000 times higher with 137Cs, which also shows that the composition of the radioactive plume differed between the earlier and later dates during the course of the FDNPP accident.

The measured 137Cs/90Sr activity ratio in Tsukuba was more than 40 times higher than the emission assessment by NISA 2011 for the FDNPP accident (137Cs: 90Sr = 15:

0.14). The IAEA (2006) had estimated that the amount of

90Sr emitted (approximately 10 PBq) for the Chernobyl accident was only 12 % that of 137Cs (approximately85 PBq), yet in reality, the atmosphere/precipitation observations in Japan showed approximately the amount of 90Sr

to be only 1/100 that of 137Cs (Aoyama et al. 1991), indicating that less than 1/10 of the emitted 90Sr was trans

ported. Thus, the 8000 km long-range transportation from Chernobyl produced the radionuclide separation. With that in mind, it could be possible that fractionation

caused by particle size deviation (Hirose et al. 1993) occurred in the FDNPP plume. The plume was transported less than a few hundred kilometers in the present case, but fractionation could be very effective.

89Sr/90Sr activity ratioThe emissions estimated by NISA 2011 showed that the

89Sr proportion was 14 times higher than that of 90Sr after the nuclear accident, which indicated that the radioactivity estimate would be 1/3 that of 90Sr after a year. The results from the aerosol sample observations suggest the presence of 89Sr; therefore, the temporal change in the -counts was fitted based on emission estimates by the former NISA (89Sr:90Sr = 2:0.14). Figure 10 in the Appendix 2 shows the fitted results of the aerosol sample measurements for March 1415. As shown in the figure, the sample counting values exhibited a large decay after 40 days of fixation as strontium carbonate, which indicates that the amount of coexisting 89Sr was relatively large. Therefore, appropriately different ratios were examined instead of the 2:0.14 ratio, which could not be fitted. Therefore, the emitted ratio for the sample collected on March 14 15 was 10:0.14 for 89Sr:90Sr. The peak data for March 20 21 indicated that a ratio of 9:0.14 fit perfectly. Table 2 in

Table 2 Curve fitting results with assumed 89Sr over 90Sr activity ratio

March 1415, 2011 March 2021, 2011

89Sr:90Sr 89Sr:90Sr 9:0.14 0.3356 8:0.14 0.4550 10:0.14 0.3340 9:0.14 0.4165 11:0.14 0.3493 10:0.14 0.5432 12:0.14. 0.3795 11:0.14 0.5869

The results for two air filter samples collected in March 2011. The minimum standard deviation suggests the best estimate

Fig. 10 Deconvolution of the 89Sr, 90Sr and 90Y activities. It is possible to deconvolute radionuclides by measuring the temporal change in the

total -activity (cpm) of the purified radioSr source (March 1415, 2011 sample). Elapsed days means the time after the radiochemical separation.

An initial activity ratio of 89Sr/90Sr was assumed and applied to the curve fit as 2/0.14 and 10/0.14.

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Table 3 Efficiency of 137Cs extracted from air filter samples by heated concentrated nitric acidSampling date and time (JST) Before ext. 137Cs (Bq) After ext. 137Cs (Bq) Extraction efficiency (%) March 14 21 pmMarch15 9 am 243 0.7 72 0.4 70.4

March 15 9 amMarch 15 15 pm 41 0.3 7.4 0.12 82.0 March 15 15 pmMarch 15 21 pm 20 0.2 6.1 0.11 69.5 March 15 21 pmMarch 16 9 am 19 0.2 0.51 0.04 97.3 March 16 9 amMarch 17 9 am 9.2 0.19 0.52 0.04 94.3 March 19 9 amMarch 20 21 pm 94.2 0.6 0.20 0.03 99.8 March 20 21 pmMarch 21 9 am 423 0.9 1.2 0.05 99.7 March 21 9 amMarch 22 9 pm 30.8 0.24 0.15 0.03 99.5

Air filter samples were subjected to heated conc. nitric acid extraction for Sr analysis. Cs-137 was measured to confirm the extraction efficiency. Samples shown as nd before extraction were excluded from the table. Some samples exhibited significantly lower extraction efficiencies of 7080 %. Insoluble and refractory radioactive particles must have been incorporated in these samples

the Appendix 2 shows these fitting results. Therefore, the emission ratio of 89Sr/90Sr for both March 1415 and 2021 was approximately 70 (10:0.14), which was five times bigger than what NISA 2011 had estimated.

The MEXT has reported 89,90Sr in approximately 50 soil samples within 80 km of the FDNPP (MEXT 2011b). The decay data are corrected as of June 2011, and the activity ratio was reported to be in the range of1.96.5 (average: 4). Another decay correction as of March 11, 2011 gives 89Sr/90Sr ratios of 724 with an average of 15. The ratio is not consistent with our results, and the fluctuation was large. The cause of the discrepancy and fluctuation is still unknown. The most likely explanation is that stable Sr, already present in reactor materials or seawater components, absorbed neutrons and formed 89Sr. The extent of and fluctuation in mixing (inhomogeneity) might produce the discrepancy.

Efficiency of acid extraction of 137Cs from filter specimens

The rates at which 137Cs could be extracted from the filter and aerosol samples using acid are shown in Table 3 in the Appendix 2. The samples collected on March 1415 and 2021 have different extraction rates, indicating that the 137Cs in the sample from

the March 1415 was refractory to some extent (20 30 %), even in a heated solution of nitric acid. This is possibly because of the difference in the physical and chemical nature of the radioactive aerosol. Thus, it is possible that the current radioSr concentration has been slightly underestimated (2030 %) because of the low water dissolution rate of the radioactive material, especially for the March 1415 sample.

As shown here, observations of the radioactive plume over Tsukuba at different times demonstrated that the

89Sr/90Sr ratio was almost constant, but the 137Cs/90Sr ratio and the extraction efficiency of 137Cs with nitric acid

differed. Moreover, it was shown earlier that the activity ratios among other -emitters differed (see Appendix 1).

These findings confirm that the characteristics of the aerosol particles that carried major radionuclides from the first plume differed from later advected radioactive plumes. Adachi et al. (2013) addressed this sort of contrast in the characteristics of the two plumes radioactive aerosols in detail, and Abe et al. (2014) added more information. They documented the discovery of insoluble, glassy spherules containing radioCs and assumed that the major fraction came from the first event. Indeed, no such particles were detected in the later event. This should also affect the ratio of 137Cs/90Sr

in the air, and evidence regarding this will be obtained in future work. In conclusion, the present results support the previous findings of less 90Sr contamination than radioCs contamination from the FDNPP accident and indicate the necessity of further investigations of radioSr in the atmospheric environment.

AbbreviationsATSDR: US Department of Health and Human Services, Public Health Service, Agency for Toxic Substances and Disease Registry; DOE: US Department of Energy; FDNPP: Fukushima Dai-ichi nuclear power plant; HYSPLIT: Hybrid Single Particle Lagrangian Integrated Trajectory Model; IAEA: International Atomic Energy Agency; JMA: Japan Meteorological Agency; KURRI: Kyoto University Research Reactor Institute; MANAL: Meso-regional objective analysis; MEXT: Ministry of Education, Culture, Sports, Science and Technology, Japan; MRI: Meteorological Research Institute, Japan;

NASA: National Aeronautics and Space Administration, USA; NHM: The JMA/MRI non-hydrostatic meteorological model; NISA: The former Nuclear and Industrial Safety Agency, Japan Carriage Return; RAQM2: Regional Air Quality Model 2; SCJ: Science Council of Japan Carriage Return; TEPCO: Tokyo Electric Power Company.

Competing interestsThe authors declare that they have no competing interests.

Authors contributionsYI designed and supervised the study and summarized the manuscript. MK conducted the transport simulation and wrote that part of the manuscript. Both YI and MK analyzed the data and helped in their interpretation. YZ helped conduct the sampling. KA and MM provided important suggestions for summarizing the work. They collaborated with the corresponding author in the preparation of the manuscript. All the authors read and approved the final manuscript.

Igarashi et al. Progress in Earth and Planetary Science (2015) 2:44 Page 17 of 19

Authors informationYI received his PhD degree in chemistry from the University of Tsukuba in 1987. From 1987 to 1991, he was at the National Institute of Radiological Sciences and studied radiochemical analysis and radioecology. He moved to the MRI in 1991 because of his scientific ambition to be involved in more global issues. His current interests are atmospheric aerosols and their precursors, including Asian dust and PM2.5, and their possible influences on climate, general environmental change, and other phenomena. He is working enthusiastically and is a member of several organizations, including the Japan Association of Aerosol Science and Technology, the Geochemical Society of Japan, the Japan Society of Nuclear and Radiochemical Sciences, the Meteorological Society of Japan, the Japan Radioisotope Association, the Japan Society of Analytical Chemistry, and the Japan Geoscience Union. He considers collaboration between observational researchers and modelers asa basic requisite in pursuing the geo- and environmental sciences.

MK received his PhD from the Graduate School of Science at Kyoto University in 2005. Since then, he has been engaged in the development of chemical transport models coupled with regional-scale meteorological models at the Disaster Prevention Research Institute, Kyoto University, Research Center for Advanced Science and Technology, University of Tokyo, and currently, the MRI. His main research interest is elemental processes of chemistry and microphysics of airborne particles and its impacts on air quality, ecosystem, and climate.

YZ graduated Meteorological College in 1984 and worked at the Nagasaki Marine Observatory, Japan Meteorological Agency from 1984 to 1989. He has been studying atmospheric aerosols at the MRI since 1989 and received his PhD from Nagoya University in 2005.

KA received his PhD from Kobe University in 2005, worked at Arizona State University between 2005 and 2011 as a postdoctoral/faculty research associate, and is currently studying atmospheric aerosols at the MRI.

MM received his PhD from Tohoku University in 1996, has worked at the MRI from 1985 to 2015, and finally holds the position of Senior Researcher for Research Affairs at the institute. Currently, he is working at Japan Meteorological Business Support Center.

AcknowledgementsThe authors are deeply indebted to the following part-time and temporary staff members at the MRI: Chitsuko Takeda, Tokyo Nuclear Service Co. Ltd., and Kazue Inukai and Keiko Kamioka, currently at ATOX Co. Ltd. for the difficult work of analyzing samples and preparing samples measurements under an unusually severe accident situation; Hiroshi Sakou, Toru Kimura, and Sakae Mayama, ATOX Co. Ltd. for sampling, sample preparation, and general analysis; Wakari Iwai and Kazuma Nabeshima for radiochemical analysis of Sr isotopes and sample preparation, respectively; and Yuriko Kamiya, Kayo Yanagida, and Rina Mori for sampling, logistical support, figure preparation, and manuscript editing. Takeshi Ito helped with the trajectory analysis in the revised manuscript. The authors are also grateful to the following MRI academic colleagues: Hiroaki Naoe, Michio Aoyama (currently at Fukushima University), and Hiroshi Takahashi (currently at the Japan Meteorological Agency) for their help with sampling. Additionally, they acknowledge the assistance of Naoyuki Osada (currently at Okayama University) and Yuichi Oki (Kyoto University Research Reactor Institute) with low-background -ray measurements. The authors benefitted from discussions with Kazuyuki Kita (Ibaraki University) and Yuko Hatano (University of Tsukuba) regarding the re-suspension issue. Olivier Masson, IRSN, France, kindly gave critical comments on an early version of the manuscript, for which the authors are grateful. This study was financially supported by the former MEXT and current Nuclear Regulation Authority Japanese Radioactivity Survey fund and partially by the MEXT Kakenhi (a Grant-in-Aid for Scientific Research on Innovative Areas under the A01-1 and A01-2 research teams in the Interdisciplinary Study on Environmental Transfer of Radionuclides from the Fukushima Daiichi NPP Accident (ISET-R; leader: Professor Yuichi Onda, University of Tsukuba); grant nos. 24110002 and 24110003) and the JSPS Kakenhi (leader Dr. Tsuyoshi T Sekiyama, MRI; grant no. 24340115). We gratefully acknowledge NOAAs ARL for providing the HYSPLIT transport and dispersion model and the READY website used in this study. The present paper was written and organized based on previous proceedings (Iwai et al. 2012; Igarashi et al. 2013a) and presentations at the ICAS, AMS, EGU, domestic meetings, and other settings (Igarashi et al. 2011, 2013b , 2013c) and the MRI home page (MRI 2011).

Author details

1Meteorological Research Institute, 1-1 Nagamine, Tsukuba, Ibaraki 305-0052, Japan. 2Present address: Japan Meteorological Business Support Center, Chiyoda-ku, Tokyo 101-0054, Japan.

Received: 16 March 2015 Accepted: 22 October 2015

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