Reassessment of the radiocesium resuspension flux from contaminated ground surfaces in East Japan

. Resuspension of 137 Cs from the contaminated ground surface to the atmosphere is essential for understanding the environmental behaviors of 137 Cs and estimating external and inhalation exposure of residents. Kajino et al. (2016) assessed the 137 Cs resuspension flux from bare soil and forest ecosystems in East Japan in 2013 using a numerical simulation constrained by surface air concentration measurements. However, the simulation was found to underestimate the observed deposition amounts by two orders of magnitude. The reason for this underestimation is that the simulation assumed that resuspended 137 Cs is carried by submicron aerosols, which have low deposition rates. Based on the observational indications that soil dust and 40 bioaerosols are the major carriers of resuspended 137 Cs, a new simulation is performed with higher deposition rates constrained by both surface concentrations and deposition amounts. In the new estimation, the areal total annual resuspension of 137 Cs in 2013 is 25.7 TBq, which is equivalent to 0.96% of the initial deposition (2.68 PBq). Due to the rapid deposition rates, the annual redeposition amount is also large at 10.6 TBq, approximately 40% of the resuspended 137 Cs. The resuspension rate through the atmosphere (0.96% y -1 ) seems slow, but it (2.6×10 -5 d -1 ) may not be negligibly small compared to the actual 45 decreasing trend of the ambient gamma dose rate obtained in Fukushima Prefecture after the radioactive decay of 137 Cs plus 134 Cs in 2013 is subtracted (1.0–7.9×10 -4 d -1 ): Resuspension can account for 1–10% of the decreasing rate due to decontamination and natural decay through land surface processes. The current simulation underestimated the 137 Cs deposition in Fukushima city in winter by more than an order of magnitude, indicating the presence of additional resuspension sources. The site of Fukushima city is surrounded by major roads. Heavy traffic on wet and muddy roads after snow removal operations 50 could generate superlarge (approximately 100 µm in diameter) road dust or road salt particles, which is are not included in the model but might contribute to the observed 137 Cs at the site.


Introduction
More than ten years have passed since the Fukushima Daiichi Nuclear Power Plant (F1NPP) accident. Extensive studies have been performed thus far using field observations, laboratory experiments, and numerical simulations aiming at a full understanding of atmospheric dispersion and deposition of directly emitted radionuclides associated with the accident, which 60 occurred in March 2011 (i.e., primary emission). It is difficult to cite all relevant papers here, so one can refer to review papers such as Mathieu et al. (2018), but a few remarkable studies are introduced here with some updates. Aircraft monitoring studies (NRA, 2012;Torii et al., 2012;Sanada et al., 2014) have provided the spatial distributions of radio-Cs and radio-I that were deposited to the ground surface in March 2011 over all of Japan. Tsuruta et al. (2014) and Oura et al. (2015) measured the hourly surface air activity concentrations of 137 Cs at 99 stations in East Japan. These two powerful spatiotemporal 65 measurement datasets together with comprehensive emission scenarios provided by the Japan Atomic Energy Agency (e.g., Katata et al., 2015;Terada et al., 2020) enable us to identify transport and deposition events over the land surface in Japan (e.g., Tsuruta et al., 2014;Nakajima et al., 2017;Sekiyama and Iwasaki, 2018). These data were also useful to validate the numerical simulation results provided by various regional-scale atmospheric models Leadbetter et al., 2015;Kitayama et al., 2018;Sato et al., 2018;Kajino et al., 2019;Goto et al., 2020) and were applied for other advanced 70 numerical techniques, such as inverse modeling (Yumimoto et al., 2016;Li et al., 2019), ensemble forecasting (Sekiyama et al., 2021), and data assimilation (Sekiyama and Kajino, 2020).
In addition to spatial spatiotemporal observations, detailed measurements have been helpful to investigate the mechanisms of atmospheric deposition and emissions from reactors. Kaneyasu et al. (2012) used size distribution measurements of multiple chemical components obtained in April and May 2011 to indicate that submicron sulfate aerosols 75 can be a major carrier of radio-Cs, and in fact, numerical simulations assuming hydrophilic submicron carrier aerosols have been successful (all models mentioned above made this assumption). On the other hand, Adachi et al. (2013) isolated hydrophobic supermicron Cs-bearing particles (referred to as Cs-bearing microparticles; CsMPs) from aerosol filters collected in March 2011; the atmospheric behaviors of these CsMPs could be quite different from those of hydrophilic submicron particles. Detailed analyses of CsMPs are helpful for understanding emission events and mechanisms (Igarashi et al., 2019a;80 Kajino et al., 2021) and deposition processes (Dépée et al., 2019). Vertical Altitude-dependent measurements obtained on mountains (Hososhima and Kaneyasu, 2014;Sanada et al., 2018) have revealed the importance of cloud deposition over mountainous forests in East Japan. Even though the cloud deposition process is not included in other almost all models, its importance has been inferred from some numerical simulations (Katata et al., 2015;Kajino et al., 2019).
A great number of numerical studies have been conducted for primary emissions, but only one numerical study 85 (Kajino et al., 2016, hereinafter K16) has been performed on the atmospheric dispersion and deposition of radionuclides that have been resuspended from contaminated ground surfaces (secondary emissions). For primary emissions, the emission point is known, and many emission events can be identified, whereas for secondary emissions, the emission mechanisms are unknown, and the ground surfaces (as emission sources) are highly heterogeneous. It is impossible to measure radio-Cs resuspension fluxes from every ground surface, but knowledge has been accumulated from long-term atmospheric 90 measurements recorded at several locations. Ochiai et al. (2016) showed that the surface concentrations of 137 Cs were high in summer and low in winter in the contaminated forest area in the Abukuma Highlands. Ochiai et al. (2016) also showed that the temporal variations in fine-mode (< 1.1 µm in diameter) and coarse-mode (> 1.1 µm) 137 Cs behaved differently by season, indicating that the major emission sources could be different between winter and summer. Nakagawa et al. (2018) conducted size-resolved n-alkane and 137 Cs measurements in similar forest areas and concluded that among biogenic emission sources, 95 epicuticular wax is less likely and bioaerosols such as pollen and fungal spores are more likely. Based on long-term measurements taken in the same forest area, Kinase et al. (2018) indicated the association of mineral dust in late spring and bioaerosols in summer and autumn. Kinase et al. (2018) also found that the contribution of the forest fires that occurred in March 2013 to the surface 137 Cs concentrations was negligibly small. Kinase et al. (2018) reported that the surface concentration of 137 Cs was positively correlated with the surface wind speed in winter but not in summer. Igarashi et al. (2019b) 100 further investigated the possible sources of 137 Cs-rich bioaerosols in summer and suggested the substantial involvement of fungal spores. Atmospheric humidity plays a key role in the discharge of fungal spores, which is consistent with the findings of Kita et al. (2020), who stated that the surface concentration of 137 Cs in mountainous forests became higher in the presence of precipitation in summer. Cedar pollen particles could contain a considerable amount of 137 Cs in the forest areas of Abukuma Highlands, but they are emitted from late February to early May, not during summer (Igarashi et al., 2019b). In fact, the number 105 of pollen particles was 1/10 of the number of bacteria (including spores) or less in summer (Kinase et al., 2018;Igarashi, 2021).
The numerical simulations conducted by K16 were consistent with the findings described above: the surface concentrations in the mountainous forest area are low in winter and high in summer, the contributions of mineral dust are high in winter, and those of bioaerosols are high in summer. However, Watanabe et al. (2021) found that the simulations of K16 underestimated the observed deposition amounts by approximately two orders of magnitude. The major reason for this large 110 discrepancy in deposition is the incorrect assumption of the physical properties of resuspended 137 Cs by K16. K16 constrained the deposition efficiency of 137 Cs in their simulations to be consistent with the primary emission period (March 2011), which involved submicron carriers; however, based on the above-described measurements, the major carriers of resuspended 137 Cs should be much larger. In the current study, the deposition efficiency of 137 Cs in the simulation is constrained to be consistent with the measured concentration and deposition amounts in the resuspension period (i.e., 2013). The regional budgets of 137 Cs 115 are thoroughly reassessed using more realistic model configurations, and the differences between the old and current estimates are clearly compared in this study.

Observation data
To constrain the deposition rates and resuspension fluxes used in the simulations, activity measurement data containing surface concentrations and deposition amounts at three observation sites, one in a contaminated forest (Namie, Tsushima), one in an urban/rural area near the contaminated forest (Fukushima), and one in a downwind location (Tsukuba), are used (Fig. 1).
The Namie (Tsuhima) site is approximately 30 km northwest of the F1NPP, is located in the difficult-to-return zone 130 (DRZ; >50 mSv y -1 ), and is surrounded by forests in the Abukuma Highlands. The center of Namie town is located near the coast of the Pacific Ocean, but the observation site is surrounded by mountainous forests. Thus, to avoid confusion, the site is denoted as Namie (Tsushima) throughout the manuscript. The initial deposition amount indicated by the airborne measurements was 2300 kBq m -2 (Fig. 1b), and decontamination work was not conducted in 2013. The locations at which the surface concentration measurements and deposition measurements are taken are different but are very close to each other (the 135 direct distance is approximately 400 m). The concentration measurements are were conducted in the schoolyard of a high school (140.768°E, 37.562°N) (Ishizuka et al., 2017;Kinase et al., 2018), and the deposition measurements are were made by Fukushima Prefecture at Tsushima Screening Center (140.765°E, 37.561°N) (data available at https://www.pref.fukushima.lg.jp/site/portal/genan225.html, last access:ed 30 June 30, 2021). Aerosols are collected by highvolume air samplers at a height of 1.2 m from ground level and deposition samples are collected by a plastic tray. The gamma 140 rays from the samples are measured by high-purity germanium detectors. The sampling intervals of the concentration and deposition measurements at this site are 1-2 days and 1 month, respectively.
The Fukushima site is in Fukushima city, located approximately 60 km northwest of the F1NPP. The Fukushima site is located in the Fukushima Basin in the Nakadori Valley, surrounded by the Ou Mountains (the peaks of which are 1000 -2000 m in elevation) to the west and the Abukuma Highlands (the peaks of which are mostly lower than 1000 m in elevation) 145 to the east (Fig. 1). The concentration and deposition measurements are conducted at Fukushima University (140.45°E, 37.68°N) (Watanabe et al., 2021). Fukushima University is located on a small hill at the southern edge of the Fukushima Basin and is surrounded by major roads. The distances from Route 4 and national highway E4 to the university are shorter than 1 km. The land use type of the site is characterized as urban/rural. The initial deposition amount indicated by the airborne measurement was 190 kBq m -2 (Fig. 1b), one order of magnitude smaller than that at the Namie (Tsushima) site. 150 Decontamination was conducted in 2013 in Fukushima city, and almost 90% of decontamination was completed for agricultural fields and public facilities by March 2014 (Watanabe et al., 2021). The achievement ratios of decontamination for other land use types are 50%, 9%, and 5% for residential areas, roads, and forests (only living areas; onlythe removal of shrub and litter layers in areas within 20 meters from the forest edges), respectively (Watanabe et al., 2021). Aerosols are collected by high-volume air samplers and deposition samples are collected by a precipitation sampler, placed on the roof of a building 155 at Fukushima University at a height of 25 m from ground level. The gamma rays from the samples are measured by highpurity germanium detectors. The sampling intervals of the concentration and deposition measurements at this site are 3 days and 1 month, respectively.
The Tsukuba site is located in Tsukuba city, Ibaraki Prefecture, approximately 170 km southwest of the F1NPP. It is located in the eastern part of the Kanto Plain, the most populated area in Japan. The concentrations and deposition amounts 160 are were measured at the Meteorological Research Institute (MRI) (140.13°E, 36.06°N) (Igarashi et al., 2015). The initial deposition amount was 21 kBq m -2 (Fig. 1b), one order of magnitude smaller than that at the Fukushima site and two orders of magnitude smaller than that at the Namie (Tsushima) site. Decontamination was not conducted in most of the areas around this site due to the low ambient gamma dose rates. Aerosols are collected by high-volume air samplers at a height of 1.2 m from ground level and deposition samples are collected by a plastic tray placed on the roof of a six-story building at MRI. The 165 gamma rays from the samples are measured by high-purity germanium detectors. The sampling intervals of the concentration and deposition measurements at this site are 1 week and 1 month, respectively.
Note that the heights of the concentration measurements are different, 1.2 m for Namie (Tsushima) and Tsukuba, and 25 m for Fukushima. The heights of deposition measurements are also different, near the ground surface for Namie (Tsushima), but the roofs of buildings for Tsukuba and Fukushima. Concentration and deposition values can vary depending on the height 170 of the observation. It is difficult to quantify vertical differences due to the lack of vertical measurements. However, this difference should be considered to explain the data discrepancy between different sampling locations.
The locations, geographical features, and airborne-measured initial deposition amounts of these sites are visualized using Google Earth in the Supplement 1.

Numerical simulations 175
The Lagrangian model (LM) developed by K16 was used in this study. Thus far, a cumulus convection parameterization of Emanuel and Zivkovic-Rothman (1999) has been implemented to the model. The model description and simulation setup used in this study are identical to those of K16, except the cumulus convection parameterization, but are briefly repeated in this section. The differences of simulations with and without the cumulus convection are presented later in Fig. 10  GPV-MSM provides data on three hourly for meteorological variables with 3-hourly resolution on the surface and at 16 vertical layers from 1000 hPa to 100 hPa. No meteorological models are applied to simulate finer-scale phenomena or to obtain detailed meteorological variables such as turbulent diffusivities or mixing ratios of hydrometeor concentrations. The fundamental 190 variables such as the wind field, temperature, humidity, and geopotential height, and surface precipitation rate obtained from the meteorological analysis data are interpolated horizontally spatioand temporally and applied to simulate the locations and masses (or radioactivitiesactivity) of carried by Lagrangian particles. The output resolutions can be set independently of the meteorological input data. The model top level is set as 500 hPa but the grid box mean activity concentrations are obtained at heights above ground level up to 3000 m. The full simulation period is from December 1, 2012, to January 1, 20132014,195 including a spin-up period of 1 month: and tThe analysis period is the full year of 2013, from January 1, 2013, to January 1, 2014.

Deposition schemes 200
The key parameters used in this study are introduced below using equations. The LM does not include comprehensive deposition schemes; deposition processes are simply parameterized. The wet scavenging rate Λ wet (s -1 ) is expressed as a function of the surface precipitation rate P (mm s -1 ) as follows: where E c is the collection efficiency of aerosols by the hydrometeor and a m and r m are the mean radii of the hydrometeor and aerosols, respectively. Empirically, a m is characterized by P as a m = 0.35 P 0.25 . E c is a function of a m and r m , but, practically, a 205 single constant value is used for each simulation. Eq. 1 is applied for all types of wet deposition. The differences among rain, snow, and graupel precipitation and the differences between in-cloud and below-cloud scavenging are not considered.
The dry scavenging rate Λ wet (s -1 ) is expressed as follows: where z is the height of Lagrangian particles, z srf is the surface layer height set as 100 m in this study, and v d is the dry deposition velocity. v d depends on aerosol sizes and surface conditions such as wind speed, roughness, and land use types, but a single 210 constant value is applied in this study. We only consider the difference in v d over the land and the ocean; v d over the ocean is 0.1 times smaller than that over the land (K16).
Fog or cloud deposition plays a key role in the deposition of 137 Cs over the mountains in East Japan (Hososhima and Kaneyasu, 2015;Katata et al., 2015;Sanada et al., 2018;Kajino et al., 2019;Imamura et al., 2020) but is not considered in the study because the GPV-MSM product does not provide fog data (or cloud water in the bottom layers of the model grid boxes). 215 100 nm in diameter, e.g., Kaneyasu et al., 2012); thus, the optimized deposition parameters are the orders ofvalid for these 220 submicron particles. However, the major carriers of 137 Cs resuspended from the ground surface could be supermicron particles such as soil dust and bioaerosols (from 1-several 10 μm in diameter, e.g., Ishizuka et al., 2017;Kinase et al., 2018); thus, the deposition parameters should be much larger. In this study, E c and v d are significantly substantially improved from compared to those used in K16, as is extensively described later in Sect. 2.3.

Resuspension schemes 225
K16 considered three emission sources during the analysis period of 2013: resuspension from bare soil, resuspension from forest ecosystems, and additional emissions from the reactor buildings of the F1NPP. K16 simulated the contributions from these additional emissions and resulting activity concentrations as beingwere two to three orders of magnitude smaller than the observed surface activity concentrations, and these contributions were thus neglected in this study. The emission flux of 137 Cs carried by dust aerosols from a bare soil surface, F dust (Bq m -2 s -1 ), is formulated by Ishizuka et al. (2017) as follows: 230 where p 20μm is the surface area fraction of dust particles smaller than 20 μm in diameter against soil containing a maximum particle size of 2 mm and varies depending on the soil texture (1.3×10 -8 for sand, 0.19 for loamy sand, 0.45 for sandy loam, and 0.80 for silt loam), F M is the total dust mass flux (kg m -1 2 s -1 ) as a function of the friction velocity * ( 3.6 10 * , Loosmore and Hunt, 2002), f forest is the forest areal fraction, and B 5mm (t) is the specific radioactivity of the surface soil (from the surface to a depth of 5 mm; Bq kg -1 ) as a function of time considering radioactive decay. Changes in the vertical profiles 235 of 137 Cs due to land surface processes or decontamination are not considered in the study. The f forest value is obtained from the Weather Research and Forecasting model version 3 database (WRFV3; Skamarock et al., 2018). Eq. 3 was developed based on measurements taken in a schoolyard, so it may not be applicable for every soil surface type. For simplicity, we introduce the constant correction factor C const to adjust the simulated 137 Cs in dust aerosols to the observed value. C const was set to five in K16. This adjustment factor differs in this study because a larger adjustment factor is required to sustain the observed surface 240 concentration levels for faster deposition rates, as shown later in Sect. 2.3.
The resuspension flux of 137 Cs from forest ecosystems (regarded as forest aerosols), F forest (Bq m -2 s -1 ), is formulated by K16 as follows: , where f green is the monthly mean green area fraction, r const is the constant resuspension coefficient (s -1 ), B obs is the observed initial deposition amount (Bq m -2 , Fig. 1b), and R decay (t) is the radioactive decay. f green is obtained from the WRFV3 database 245 and was originally derived from Advanced Very High Resolution Radiometer (AVHRR) normalized difference vegetation index (NDVI) data (https://www.usgs.gov/core-science-systems/eros/phenology/science/ndvi-avhrr, last access: 11 November 2021). r const is the adjustment parameter and was set as 10 -7 h -1 in K16 for adjustment to the observed surface concentrations in the forests in summer. Similar to the dust aerosol case, a larger adjustment factor is required due to the faster deposition rates to sustain the simulated surface concentrations close to the observed values, as is shown later in Sect. 2.3. Similar to the 250 dust aerosol case, no 137 Cs migration within the local forest ecosystems due to land surface processes is considered in the formulation.
For both the dust and forest aerosol cases, only emissions from the grid boxes in which the mean initial deposition amounts exceed 10 kBq m -2 , the detection limit of the airborne measurements, are considered (NRA, 2012). However, horizontal interpolation from the original grid boxes to the LM grid boxes can convert values slightly above the detection limit 255 to less than 10 kBq m -2 . However, excluding regions in which the deposition amount is 9.9 kBq m -2 , for example, may not be appropriate. Thus, a sensitivity test is performed to additionally consider areas with deposition amounts of 1-10 kBq m -2 as emission sources, as is presented in Sect. 3.4.
Other sources, such as the unexpected releases associated with the debris removal operations at the F1NPP site that occurred in August 2013 (NRA, 2014;Steinhauser et al., 2015;K16), forest fires, and resuspension due to decontamination 260 work, are not considered in the study. The debris removal operations caused a sporadic peak in the surface concentrations (60.4 mBq m -3 from 13:00 LT on August 14 to 13:00 LT on August 15 at Namie (Tsushima), Figs. 4a and 4b), but these elevated values may not affect the background (or steady state) concentrations for the full year, which are the target of this study. Forest fires may not be a major source of 137 Cs resuspension in Fuskuhima because the temporal variations in levoglucosan concentrations were not found to be associated with those of 137 Cs (Kinase et al., 2018). Resuspension due to 265 decontamination work should be considered, but it was hard to estimate because the emission factor and the precise location and time of decontamination are unknown. It should be noted here that, as described in Sect. 2.1, decontamination was not performed around the Namie (Tsushima) or Tsukuba sites, and but decontamination might have been performed around the Fukushima site in 2013.

Constraint of modeled deposition parameters
Since K16 was published, several emission sources of resuspended 137 Cs have been indicated, such as soil dust (Ishizuka et al., 2017;Kinase et al., 2018) and bioaerosols (Kinase et al., 2018;Nakagawa et al., 2018;Igarashi et al., 2019b;Kita et al., 2020;Minami et al., 2020;Igarashi, 2021), but the relative contributions of these sources, the spatiotemporal variations in the associated emission fluxes, and their size distributions are still not well understood. Kita et al. (2020) indicated 275 the associations of rain with fungal spore emissions, and Minami et al. (2020) estimated the emission flux of 137 Cs associated with bioaerosols; however, the emission flux has not yet been formulated as a function of meteorological or land surface variables. Therefore, the same formulations as those applied in K16 (Eqs. 3 and 4) are used in this study. It is also noted here that the same deposition rates are applied for both dust and forest aerosols, even though the size distributions of these two aerosol types should be different. 280 K16 had two major drawbacks: (1) K16 constrained the deposition parameters (i.e., E c and v d ) by using the primary 137 Cs emission and initial 137 Cs deposition amounts measured in March 2011, and (2) K16 did not compare their simulation results against the deposition amounts. Recently, Watanabe et al. (2021) evaluated the performance of the K16 model using concentrations and deposition amounts measured at the Fukushima sites and found that the seasonal variations in simulated concentrations were opposite to those observed and that the simulated deposition amounts were underestimated by one to two 285 orders of magnitude. The reason for this underestimation of the deposition amounts is obvious; the typical deposition rates of major carrier aerosols (submicron aerosols) of K16 are much smaller than those the resuspension ratesof soil dust and bioaerosols (supermicron aerosols). For example, the dry deposition velocities of aerosols with diameters of approximately 10 µm are two to three orders of magnitude larger than those of aerosols with diameters of approximately 0.1-1 µm (e.g., Petroff and Zhang, 2010). The difference between these two size ranges for below-cloud scavenging due to rain is also two to 290 three orders of magnitude (e.g., Wang et al., 2010). To constrain the deposition parameters suitable for 137 Cs resuspension, we performed a climatological deposition velocity analysis similar to that conducted by Watanabe et al. (2021).
Suppose there is a simple nonlinear relationship between the periodic mean deposition flux (D) (Bq m -2 s -1 , for example) and periodic mean surface concentration (C) (Bq m -3 ): , where a represents the removal rate and b represents nonlinear features such as spatial and temporal variabilities. If b = 1, the 295 unit of a is m/s, which is on of the dimension of the deposition velocity. If long-term averaging is conducted, Eq. 5 may hold.
(6) 2. The purple, orange, and green symbols indicate the observations, simulations by K16 (E c = 0.04 and v d = 0.1 cm s -1 ) and simulations conducted in this study (E c = 0.4 and v d = 10 cm s -1 ). This analysis is novel because emission flux adjustments 300 (C const in Eq. 3 and r const in Eq. 4) do not change the slope of the regressions, so the deposition parameters can be adjusted independently from the emission flux adjustment. The intercept of the y-axis indicates the deposition velocity. Among the several sensitivity tests with the combinations of E c = 0.04 and 0.4 and v d = 0.1, 1, and 10 cm s -1 , the y-axis intercept of the simulation with E c = 0.4 and v d = 10 cm s -1 matched best with that of the observations. This analysis is novel because emission flux adjustments do not change the slope of the regressions, so the deposition 305 parameters can be adjusted independently from the emission flux adjustment. In this study, we need to constrain both emission and deposition parameters. If emission and deposition parameters both affect the slope, the adjustment should be tough.
However, in this analysis we constrain the deposition parameters first to fix the slope (or the intercept of y-axis) with whatever emission parameters, and then constrain the emission parameters using observed concentration and deposition values as presented in the next subsection (2.3.2). 310 The slope of the observed regression line, b, is 0.92, so the relationship between the concentrations and depositions of resuspended 137 Cs in East Japan is almost linear, but the relationship itself is not very solid (coefficient of determination (R 2 ) = 0.018). However, by excluding two exceptional data points, the observations obtained in January at Fukushima (maximum deposition) and August at Namie (Tsushima) (maximum concentration), the R 2 increases to 0.65, and b becomes 0.98 (not shown in the figure). In January at Fukushima, the measured deposition is extremely high compared to the surface 315 concentration. Watanabe et al. (2021) hypothesized the existence of superlarge particles (~100 µm in diameter) whose gravitational deposition velocities are too fast (as fast as drizzle) to enter the high-volume air samplers used for the concentration measurements but are efficiently collected deposition samplers., as tThe traveling distance of such superlarge particles is estimated as approximately 1 km (e.g., Kajino et al., 2012;Kajino et al., 2021). January is the month with the highest snow cover in Fukushima city and the highest snow removal operations (using snowblowers and deicing agents), and 320 heavy traffic on the major roads within 1 km of the Fukushima site produce substantial amounts of superlarge particles from wet and muddy road surfaces. The August data at Namie (Tsushima) are also exceptional because the surface concentrations are biased due to the sporadic peak associated with the debris removal operation in the F1NPP (K16). Because the aerosols associated with the debris removal operation traveled a sufficiently long distance (i.e., 30 km), the deposition velocity was not significantly substantially large and did not affect the monthly mean deposition, although it did affect the monthly mean 325 concentration. Therefore, the data obtained in August at Namie (Tsushima) are exceptional when compared to the trends shown by other datasets. The slopes of the simulated regression lines are b =1.17 for K16 (orange line) and b =1.16 for this study (green line). R 2 values of 0.71 and 0.97 were obtained by K16 and this study, respectively. The difference in the magnitude of R 2 can be explained by the differences in the deposition rates. Because the deposition rates obtained in this study are much faster higher than those applied by K16, the deposition amounts are more strongly associated with the concentrations in this 330 study. In other words, this climatological deposition velocity analysis was successful (by excluding the two exceptional datapoints) because the sizes of the major carrier aerosols of resuspended 137

Adjustment of emission fluxes 350
In K16, the emission fluxes of 137 Cs associated with dust and forest aerosols were adjusted to match the surface concentrations at Namie (Tsushima). In K16, first, C const in Eq. 3 was set to five so that the simulated dust 137 Cs concentrations matched the observations in winter, when the temporal variation in the observed 137 Cs concentration at Namie (Tsuhima) correlated well with that of the wind speed (Kinase et al., 2018) and when the vegetation activity was supposed to be low. The adjusted dust 137 Cs concentrations could not reproduce the enhanced concentrations measured at Namie (Tsushima) in summer 355 (Fig. 4a). Thus, r const in Eq. 4 was set to 10 -7 h -1 so that the simulated forest 137 Cs concentrations matched the observations in summer. The temporal variation of 137 Cs was not correlated with that of the wind speed in summer (Kinase et al., 2018).
Because the deposition rates are significantly substantially increased in this study, we require much larger emission fluxes to sustain the simulated surface concentrations at the observed levels. The same adjustment procedure as that used in K16 could be applied to the simulations in this study; however, for example, adjusting the values at Namie causes the values 360 to be underestimated at Tsukuba, so it is hard to find a combination of C const and r const that is best for all aspects (i.e., concentrations and depositions of the three sites). Thus, for simplicity, we simply multiplied both fluxes used in K16 by 20 so that number fractions of data within a factor of five exceeded 0.5 for both concentrations and depositions at the three sites: C const was 100 and r const was 2×10 -6 h -1 . The discrepancies between the simulated and observed concentrations and depositions at the three sites are summarized later in Sect. 3.1. 365 Figure 3 shows the observed and simulated (dust and forest) activity deposition amounts of 137 Cs at Namie (Tsushima), Fukushima, and Tsukuba for the submicron (K16) and supermicron (this study) cases. Statistical measures such as the correlation coefficient (R), simulation-to-observation median ratio (Sim/Obs), numerical number fraction of data within a factor 370 of two (FA2), and numerical number fraction of data within a factor of five (FA5) are embedded in the panels. Note that the simulated temporal variation lines show the dust and forest amounts separately, but the statistical measures are derived using the summation of the two aerosol sources. As discussed in the previous sections and presented in Fig. 2, the underestimation of simulations assuming submicron particles is remarkable, with simulated values approximately two orders of magnitude lower than the observations at all sites. On the other hand, the simulations assuming supermicron particles are significantly 375 remarkably improved. Positive correlations are found at Namie (Tsushima) and Tsukuba (R ~ 0.6-0.7), and the same order of median ratios are found at Fukushima and Tsukuba (Sim/Obs = 1.2-1.3, FA5 = 0.9-1.0). In terms of the seasonal variations, the monthly trend (high in winter and spring and low in summer) at Tsukuba is explained well by the simulated dust aerosols.

Seasonality and quantity of surface air concentrations and depositions
Due to the land use types around the site (over of the plain), the 137 Cs of dust aerosols is larger than that of forest aerosols throughout the year. In summer, the contributions of forest aerosols are larger than those of dust aerosols at Namie (Tsushima)  380 and Fukushima, which are surrounded by mountainous forest and close to the forest area, respectively. Despite the overestimation at Namie (Tsushima) (Sim/Obs = 4.89), the monthly trend is reproduced well by the model: both the observations and simulations show double peaks in winter and summer. Most likely, the same emission factors of mineral dust should not be applied to the whole area. Nevertheless, we regard this a uniform application as acceptable in the current study, as this study aims to grasp a rough outline of the atmospheric behaviors of resuspended 137 Cs. The monthly variations output 385 by the simulations do not match those of the observations at Fukushima due to the exceptionally high deposition amounts in Fukushima city is highest in January, but there are certain areas periods of snow coverage in December and February as well. However, the R value of deposition at Fukushima is not greatly improved if the winter datasets are excluded.
The initial 137 Cs depositions at the three sites are 2300, 190, and 21 kBq m -2 , and the differences are approximately 390 on one order of magnitude. The orders of the monthly depositions in 2013 at the three sites are 0.1% of the initial deposition, at 10 2 -10 3 , approximately 10 2 , and approximately 10 1 Bq m -2 , which are similar to the order differences obtained for the initial depositions. A value of 0.1% per month is 1% per year. K16 reported an annual resuspension ratio of 0.048% y -1 , but this simple order estimation readily shows that this value is excessively underestimated. As shown later in Fig. 8, the improved annual resuspension ratio is 0.96%, which is consistent with the deposition measurements at the three sites. From this 395 estimation, one can assume that the observed deposition amounts at Fukushima in January (3100 Bq m -2 ) are exceptionally high.  unified to the sampling intervals to obtain the statistical measures. The measurements of the three sites are not directly comparable because their temporal resolutions are different (1 d for Namie (Tsushima), 2-3 d for Fukushima and 1 w for Tsukuba), but those of the two aerosol cases (submicron and supermicron) are comparable. Although R is low for the submicron case at Namie (Tsushima), good consistency Sim/Obs (0.99) and FA5 (0.94) values are obtained because the emission factors C const and r const are adjusted to this case. However, the unrealistic assumption of aerosol sizes results in the opposite simulated 420 seasonal trend at Fukushima: the simulations are too high in summer due to forest aerosols for the submicron case. The Fukushima site is located downwind of the contaminated forest in the Abukuma Highlands in summer (Fig. S1), so the transport of 137 Cs from the forest area is dominant. However, as the particle sizes are larger and the traveling distances are shorter, the summer enhancement due to forest aerosols is less dominant for the supermicron case (Fig. 4d). The observed surface concentrations are high at Fukushima in winter, and the observed short-term peaks correspond to the simulated dust aerosols, 425 indicating that the emission of resuspended 137 Cs at Fukushima in winter is driven by wind. The simulated forest aerosols are approximately one order of magnitude smaller than the dust aerosols in winter. The simulated dust peaks also correspond to the observed peaks in later spring and early summer. The simulated contribution of forest aerosols is as great as dust aerosols, but there may also be an association of wind-induced dust aerosols during the season. The Sim/Obs, FA2, and FA5 values of submicrons and supermicrons at Fukushima are similar, but R is substantially improved. At Tsukuba, like the Fukushima site, 430 the contribution of forest aerosols is less in the supermicron case than in the submicron case due to less transport from the forest area. The contribution of dust particles is dominant in winter, but the simulated dust aerosols are underestimated compared to the observations in winter in both cases. Nevertheless, Sim/Obs is not very low (0.80), and tThe R value obtained for supermicrons is improved from the submicron case (from 0.18 to 0.45).
The orders of the surface concentrations at the three sites are 10 0 , 10 -1 , and 10 -2 -10 -1 mBq m -3 . These order differences 435 are similar to those of the initial depositions. One can assume that the resuspension and redeposition of 137 Cs occurs within a limited areal scale (e.g., several tens of km) and that long-range transport (i.e., hundreds to a thousand km) from the emission source is not very dominant.
In the following subsections (Sects. 3.2 and 3.3), the source-receptor relationship and annual resuspension ratios are discussed, although the simulation is associated with the discrepancies presentedbut it should be noted that the numbers 440 presented in these sections are associated with the discrepancies in the simulations described in the currentis section.
Nevertheless, we can safely conclude here that the supermicron simulations are more (or maybe much more) consistent with the observations than the submicron simulations are.  Figure 5 shows the simulated seasonal mean concentrations and the horizontal distributions of the source-receptor relationship. 455

Source-receptor relationship and its seasonality
The resuspension source area is defined as gridsdomain in which the grid box -mean initial deposition exceeds 300 kBq m -2 (Fig. 1b). Thus, Namie (Tsushima) (2300 kBq m -2 ) is located within the source area, but Fukushima (190 kBq m -2 ) and Tsukuba (21 kBq m -2 ) are outside the source area (or are regarded as being in downwind area). The source-receptor relationship maps (or source contribution maps) (Figs. 5e-5h) are derived using the seasonal mean activity concentrations resulting from 300-kBq m -2 areas divided by those from whole the overall areas (i.e., > 10 kBq m -2 ). Because of the shorter atmospheric lifetime 460 of supermicron 137 Cs-bearing particles, the concentration maps of the supermicron cases are patchy due to insufficient amounts of Lagrangian particles (Figs. 5b and 5d) compared to the submicron cases (Figs. 5a and 5c), especially in areas where the seasonal mean surface concentrations are below 0.01 mBq m -3 . There are substantial numerical errors in these areas, so the source contribution shades (Figs. 5e-5h) depict only areas in which the seasonal mean concentrations exceed 0.01 mBq m -3 (Figs. 5a-5d). We select two three-monthly means, covering January, February, and March for winter to early spring (or simply 465 winter hereinafter) when the simulated dust aerosols are dominant and June, July, and August for summer when the simulated forest aerosols are dominant.
In winter, northwesterly monsoon winds prevail over Fukushima Prefecture (Figs. 5a and 5b). In particular, fall and gap winds from the Ou Mountains caused strong winds in the Nakadori Valley, which in turn cause high dust aerosol surface concentrations in these areas in winter. Even though the surface concentrations of supermicron particles (Fig. 5b) over 470 Fukushima Prefecture are larger than those of submicron particles (Fig. 5ab), the supermicron concentrations over the downwind regions are smaller (e.g., concentrations > 0.01 mBq m -3 over Saitama (#6 in Fig. 1) for the submicron case but of < 0.01 mBqg m -3 for the supermicron case) due to the shorter lifetime of supermicron particles. This feature is also significant evident for the source contribution maps (Figs. 5e and 5f). Due to the northwesterlies, most of the resuspended 137 Cs is transported toward the southeast over the ocean, the values are 40-90%, and the source contributions of the downwind regions 475 over the land are lower than 10%, except the coastal regions in Ibaraki (#3 in Fig. 1) and Chiba (#7 in Fig. 1) Prefectures for the submicron case (20-30%) due to the longer lifetimes of these particles in air (Fig. 5e).
In summer, southerly winds prevail over East Japan due to the marginal flows of the Pacific High. The wind speeds are generally lower in summer than in winter (please see that the lengths of the arrows are different in Figs. 5a-5b and 5c-5d).
The seasonal mean wind patterns are complex over land (Figs. 5c-5d), but the seasonal mean source contribution maps reflect 480 the seasonal mean transport patterns from the source areas (Figs. 5g-5h). Even though tThe seasonal mean wind fields over the ocean close to land are directed toward the land, indicating that ocean-to-land wind blows are more frequent (and/or stronger) than land-to-ocean wind blows. Thus, less frequent and/or weaker land-to-ocean wind transported substantial proportions of 137 Cs in forest aerosols are transported toward the ocean in summer (the source contributions are > 60% for submicron and >70% for supermicron cases). Then, the 137 Cs transported toward the ocean are is transported toward the land 485 again to Ibaraki and Miyagi (#1 in Fig. 1) prefectures. The source contributions over Ibaraki and Miyagi are substantial for the submicron case (30-70%). For the supermicron case, the source contributions over Ibaraki and Miyagi exceeded 30% at a limited number of grid boxes, but the mean concentrations were are much lower (Fig. 5d) than those in the submicron case ( Fig. 5c) over these prefectures. Due to the lower wind speeds in summer and the short lifetime of the supermicron particles, the horizontal spread of the mean concentrations (e.g., areas > 0.01 mBq m -3 ) of supermicron forest aerosols in summer (Fig.  490 5d) is obviously smaller than that of any other case (Fig. 5a-5c). sizes of 137 Cs-bearing particles at Namie (Tsushima), Fukushima, and Tsukuba. Figure 6 shows the simulated monthly mean source contributions for the concentrations and depositions at the three sites and compares these contributions between the submicron and supermicron cases. At Namie (Tsushima), more than 90% of the surface concentrations originate from the source area. The annual mean values are 90% for the submicron case (Fig. 6a) 500 and 94% for the supermicron case (Fig. 6b). It is natural that the source contributions are larger in the source area (Namie (Tsushima)) for the supermicron case, as the lifetime of these particles is shorter than that of submicron particles. As previously discussed, the submicron source contributions at Fukushima are larger in summer and autumn (approximately 40% in June, September, and October and 20% in July and August) (Fig. 6a). The source contributions of supermicrons in summer and autumn are approximately 50% smaller than those of submicrons in July and August (10%) and are slightly smaller in June, 505 September, and October (20-30%) (Fig. 6b). The annual mean concentration values at Fukushima are 16% for submicrons ( Fig. 6a) and 9% for supermicrons (Fig. 6b). As observed in Figs. 4e-4f and Figs. 5e-5h, the source contributions of submicrons and supermicrons at Tsukuba are remarkably different. The source contributions of submicrons are larger in summer and autumn at approximately 30%, with an annual mean value of 21% (Fig. 6a). On the other hand, those of supermicrons are smaller than 20% for all months, and the annual mean value is 5% (Fig. 6b). 510 In terms of deposition, the source contributions of submicrons (Fig. 6c) are similar to those for the concentrations (Fig. 6a), but the source contributions of supermicrons (Fig. 6d) are remarkably different from those for the concentrations (Fig. 6b). Removal rates of submicron particles are small so that they do not affect surface concentrations (D = aC, recall Eq. 5) and thus Figs. 6a and 6c are similar. However, the large removal rates of supermicron particles can substantially alter the surface concentrations (D = aC(D)). For the supermicron case, both emissions and depositions are substantially enhanced with 515 compared to the submicron case. The enhanced depositions (by almost two orders of magnitude, see Fig. 3) directly alter the source contributions for depositions (Fig. 6d). However, changes in concentration due to enhanced emissions (set as 20 times) are compensated by enhanced depositions, and thus the source contributions for concentrations of supermicrons (Fig. 6b) are slightly but not drastically different from the submicron cases (Fig. 6a). As presented later in Fig. 7, approximately 40% of supermicron emissions were deposited in the same grid. Thus, the local deposition contributions become much larger than the 520 concentration contributions. Consequently, as shown in Fig. 6c, the annual mean source contributions are 95%, 13%, and 19% for Namie (Tsushima), Fukushima, and Tsukuba, respectively, which are equivalent to those of the concentrations (90%, 16%, and 21% in Fig. 6a), whereas in Fig. 6d, the annual mean source contributions of supermicron depositions are shown to be 99.5%, 2.2%, and 1.0% for Namie (Tsushima), Fukushima, and Tsukuba, respectively. Figure 7 presents the simulated annual resuspension and redeposition amounts for the submicron and supermicron cases. The areal summation values are embedded in the panels. Figure 8 shows the annual resuspension ratio, which is the annual total resuspension amount divided by the initial deposition (Fig. 1b), and the annual redistribution amount, which is the deviation between the annual total redeposition amount and the resuspension amount. Negative redistribution values indicate a decrease in deposition due to resuspension, and positive values indicate an increase in deposition due to resuspension. The annual total 530 amounts embedded in Figs. 8b and 8d (-1.06 TBq and -15.1 TBq) indicate the amount of 137 Cs transported outside the model domain.

Annual total resuspension amounts 525
As previously discussed, due to the faster deposition rates and thus larger emission fluxes necessary to sustain the surface concentrations at the observed levels, the annual resuspension and redeposition amounts are both larger for the supermicron case than for the submicron case (Figs. 7c7a-7d). In K16, the total areal resuspension amount was 1.28 TBq (Fig.  535 7a), equivalent to only 0.048% of the initial deposition (2.68 PBq), and the redeposition amount (0.22 TBq) (Fig. 7b) was approximately 20% of the resuspension amount. On the other hand, based on the new estimations, the annual resuspension amount (25.7 TBq) (Fig. 7c) is approximately 20 times the previous estimate, and the redeposition amount is even larger (10.6 TBq) (Fig. 7d), at 50 times the previous estimate (0.22 TBq).
The areal mean annual resuspension ratio obtained by K16 (Fig. 8a) was 0.048%, with high values above 0.1% in 540 Nakadori Valley and the mountainous areas of Tochigi (#4 in Fig. 1) and Gunma (#5 in Fig. 1) Prefectures. The new estimate of the annual mean areal resuspension ratio is 0.96%, with high-value areas showing values of 1-3% (Fig. 8c). Iwagami et al. (2017) evaluated that the annual discharge rate from the local environment through rivers was 0.02-0.3% y -1 . The new estimate of the resuspension rate through air (0.96% y -1 ) is much larger than the discharge rate through rivers but is still not very large (i.e., only 1% per year of surface contamination). We can conclude here that the ground surface 137 Cs stays or circulates within 545 the local terrestrial ecosystems and is hardly discharged through the air or rivers.
However, when these values are compared with the actual decreasing trends in the ambient gamma dose rate in Fukushima Prefecture, we can reach a different conclusion. The first-order decrease rate of the dose rate in Fukushima Prefecture ranged from 1.0 to 7.9×10 -4 d -1 in 2013 after the radioactive decay of 137 Cs plus 134 Cs (3.0-4.2×10 -4 d -1 in 2013) (K16) was subtracted. The previous and current resuspension rate estimates, 0.048% y -1 and 0.96% y -1 , are equivalent to 550 1.3×10 -6 d -1 and 2.6×10 -5 d -1 , respectively. K16 concluded that the impact of resuspension to the atmosphere was negligibly (two to three orders of magnitude) small in the gross decreasing rate of ground surface contamination, such as by land surface processes or decontamination. However, the difference between the current estimate (2.6×10 -5 d -1 ) and the decreasing trend without radioactive decay (1.0-7.9×10 -4 d -1 ) is only one to two orders of magnitude. The annual resuspension ratio in 2013 was only 0.96% of the initial deposition amount, but the amount of 137 Cs discharged due to resuspension through the air could 555 contribute approximately 1-10% of the gross decreasing rate, which may not be negligibly small.
For the submicron case (Fig. 8b), the positive redistribution area (area with enhanced deposition due to resuspension) is limited, and the amounts are up to 10 Bq m -2 per year. On the other hand, for the supermicron case (Fig. 8a8d), even though the transport distance is shorter than that for submicrons, the positive redistribution area for 1-10 Bq m -2 is much larger, and the maximum values are up to 100 Bq m -2 for the downwind regions close to the emission sources, especially over the ocean 560 close to the land of Fukushima Prefecture. Nevertheless, these values are much smaller than those obtained for the initial deposition amounts (the lowest limit value is 10 kBq m -2 , which is two to three orders of magnitude larger than the annual enhanced deposition amounts of 10-100 Bq m -2 ). supermicron (this study; E c and v d are 0.4 and 10 cm s -1 , respectively) sizes of 137 Cs-bearing particles. The areal total amounts ratios (a,c) and the areal total amounts (b,d) are embedded at the bottom right of the panels.

Sensitivities
Several sensitivity tests are performed, as shown in the current section. Since the cumulus convection parameterization scheme 580 is installed, a comparison is made between the simulations performed with (in the current study) and without (in K16) this scheme. The current study assumes that resuspension occurred from the grid boxes in which the grid box -mean initial deposition amount exceeded 10 kBq m -2 , the reliable limit of the aircraft measurement. On the other hand, horizontal interpolation from the measurement grid boxes to the LM grid boxes can convert values slightly above the detection limit to less than 10 kBq m -2 it is inappropriate to exclude grids in which, for example, the deposition amount was 9.9 kBq m -2 , so 585 additional sensitivity tests include resuspension from grid boxes with 1-10 kBq m -2 . As was discussed in part in the previous sections, the snow cover effect is also tested. In summary, for each aerosol size case, we conduct four sensitivity tests: (1) (Riggs et al., 2016). In the presence of snow cover, the simulated dust emission is suppressed by the snow cover fraction (Eq. 3 is multiplied by one minus snow cover). No impact of snow cover on forest emissions is assumed in the simulation. December, January, and February are the months with the widest snow coverage in East Japan. In November, only small snow cover fractions are observed in the high-mountain areas (i.e., > 1000 m in Fig. 1a). In March, the snow cover in the low-elevation areas (i.e., < 1000 m in Fig. 1a and over all prefectures numbered in Fig. 1b except the western part (Ou 600 Mountains) of Fukushima Prefecture) is mostly melted. The snow cover in the Nakadori valley, including at the Fukushima site, is highest in January. Some areas over the Kanto Plain are also covered with snow in January. Extensive snow cover is in addition also observed in the Abukuma Highlands, including in Namie (Tsushima), in February. Removed contaminated areas [1-10 kBq m -2 ] do not cause any substantial differences changes in the performances of simulating the concentrations and depositions, but the difference induced by including the snow cover effect [Snow cover] is significantevident. The supermicron simulations indicate that including snow cover improves the performance at Namie (Tsushima) (indicated by the Sim/Obs and FA5 values of the deposition) but deteriorates the performance at Fukushima (as 645 indicated by the R value of the concentrations and the FA5 value of the deposition). Fig. 11 compares the simulated dust between these two settings, [1-10 kBq m -2 ] and [Snow cover], to analyze the concentrations and depositions of the supermicron case at the three sites. Apparently, [Snow cover] improves both the concentration and deposition simulations at Namie (Tsushima) in January, February, and December, but deteriorates both the concentration and deposition simulations at Fukushima. This result is consistent with the fact that no decontamination work occurred in the DRZ around Namie (Tsushima) 650 in 2013, so snow cover suppressed resuspension from the bare soil. On the other hand, people lived in Fukushima city and the surrounding municipalities, so snow removal operations (deicing agents and snowblowers) are applied after each snowfall. In fact, substantial amounts of road salts are observed in road-side PM 10 measurements in Nordic countries in winter (Denby et al., 2016), indicating the presence of road dust emissions after snow removal operations. In Fukushima city in 2013, most public facilities and agricultural fields were already decontaminated, but the achievement ratios of decontamination on roads 655 and forests were lower than 10% (Watanabe et al., 2021). Thus, snowfall did not suppress the dust emissions around Fukushima city, which may be the reason why [Snow cover] deterioratesd the model performance at the Fukushima site. In addition, as previously discussed, we hypothesize that the deposition amount in January 2013 at Fukushima was much higher than that at Namie due to the opposing impacts of snow cover on dust emissions over the two different locations: the suppression around the Namie site and the production of very large road dust particles around the Fukushima site. 660

Conclusions
The regional budget of resuspended 137 Cs originating from the Fukushima nuclear accident assessed by Kajino et al. (2016) (K16) for 2013 is reassessed in this study. K16 assumed resuspension aerosol sizes similar to those of primary emissions (the direct emissions from the F1NPP associated with the accident), which are submicron-sized. However, Watanabe et al. (2021) determined that the deposition amounts simulated by K16 were significantly substantially underestimated. Based on recent 665 cumulative knowledge, major resuspension aerosols could be supermicron-sized, such as soil dust (Ishizuka et al., 2017;Kinase et al., 2018) and bioaerosols (Kinase et al., 2018;Igarashi et al., 2019b;Kita et al., 2020;Minami et al., 2020;Igarashi, 2021). Lower possibilities of submicron particle involvement, such as that resulting from forest fires (Kinase et al., 2018) and epicuticular wax (Nakagawa et al., 2018), have been reported. Thus, the regional budget considering supermicron aerosols is significantly remarakably different from that considering submicron aerosols: faster supermicron deposition rates necessitated 670 higher emission fluxes to sustain the simulated surface concentrations at the observed levels.
To evaluate the simulations, measured concentration and deposition data obtained at three stations, Namie (Tsushima), Fukushima, and Tsukuba, are used. In this study, the resuspension source area is defined as areas in whichwhere the initial deposition amounts exceed 300 kBq m -2 . The Namie (Tsushima) site (2300 kBq m -2 ) is in the resuspension source area and is surrounded by mountainous forests in the Abukuma Highlands. The Fukushima site (190 kBq m -2 ) is characterized as an 675 urban/rural region located outside but nearby the source area. The Tsukuba site (21 kBq m -2 ) is characterized as a downwind region. A source-receptor relationship analysis is performed, and resuspension ratios and redistribution amounts are derived.
The effects of snow cover on resuspension and the contributions of resuspension to the actual decreasing trends in the ambient gamma dose rates are discussed.
The major findings in the context of contrasting the two different particle sizes are summarized as follows. 680 ・ Regarding the submicron particles, the surface concentrations of 137 Cs at Namie (Tsushima) in winter are quantitatively explained by multiplying the dust emission scheme of Ishizuka et al. (2017) by five, but these values are significantly substantially underestimated in the summer. Additional forest emissions with applying a constant factor of 10 -7 h -1 explain the enhancement of the observed 137 Cs surface concentrations in summer at Namie (Tsushima). However, this effect causes opposite seasonal variations at the Fukushima site: the simulated concentrations are high in summer, but the observations 685 are low in summer. In addition, this factor causes deposition underestimations by two orders of magnitude at all sites, Namie (Tsushima), Fukushima, and Tsukuba. The annual mean source contributions of the re-suspension source area for the concentrations are 90%, 16%, and 21%, and those for the depositions are 95%, 13%, and 20% for Namie (Tsushima), Fukushima, and Tsukuba, respectively. The total areal annual resuspension of 137 Cs is 1.28 TBq, which is equivalent to only 0.048% of the initial deposition in March 2011, i.e., 2.68 TBq. The decreasing trend of the observed gamma dose 690 rate in Fukushima Prefecture was 1.0-7.9×10 -4 d -1 in 2013 after the radioactive decay of 134 Cs and 137 Cs was excluded.
The decreasing trend is due to decontamination and natural decay, such as that occurring due to land surface processes.
The resuspension rate through the atmosphere is 0.048% y -1 (1.3×10 -6 d -1 ), which is negligibly small compared to the decreasing trend. Together with the discharge rate through rivers estimated as 0.02-0.3% y -1 (Iwagami et al., 2017), K16 concluded that ground-surface 137 Cs stays or circulates within local terrestrial ecosystems and is hardly discharged through 695 the atmosphere or rivers.
・ Regarding the supermicron particles, by using the climatological deposition velocity analysis proposed by Watanabe et al. (2021), the dry and wet deposition parameters are successfully constrained by the concentrations and depositions measured at the three sites. The constrained dry and wet scavenging rates of supermicrons are 100 times and 10 times those of 700 submicrons, respectively, resulting in the emission fluxes of both dust and forest aerosols to be enhanced twenty-fold.
Compared to the submicron case, the source contributions of supermicrons are higher in the source areas and lower in the receptor regions. The annual mean source contributions of the re-suspension source area for the concentrations are 94.0%, 9.1%, and 5.4%, and those for the depositions are 99.5%, 2.2%, and 1.0% at Namie (Tsushima), Fukushima, and Tsukuba, respectively. The areal total annual resuspension of 137 Cs is 25.7 TBq, which is equivalent to 0.96% of the initial deposition. 705 Due to the rapid deposition rates, the annual redeposition amount is also large, at 10.6 TBq; thus, approximately 40% of emissions are redistributed over East Japan. However, the traveling distance should not be large because the source contributions of the depositions at Fukushima and Tsukuba are only 2.2% and 1.0%, respectively. The resuspension rate through the atmosphere is 0.96% y -1 (2.6×10 -5 d -1 ), which may not be negligibly small, as it can account for 1-10% of the decreasing rate due to decontamination and natural decay except radioactive decay (1.0-7.9×10 -4 d -1 ). The areas with 710 positive redistribution amounts (enhanced deposition due to resuspension) of 1-10 Bq m -2 are much larger for the supermicron case than those for the submicron case, and the maximum values are up to 100 Bq m -2 for the submicron case, especially over the ocean close to the coast of Fukushima Prefecture.
From the current analysis, it is likely that snow cover in winter (January, February, and December) suppressed the dust emissions in the source areas around the Namie (Tsushima) site but did not suppress emissions around the Fukushima 715 site. This is because Namie (Tsushima) is located in the DRZ and human activities in this region were very limited in 2013, whereas snow removal operations involving deicing agents and snow blowers were performed in Fukushima city and the surrounding municipalities at this time. In addition, heavy traffic on the major roads close to the Fukushima site (< 1 km) may produce substantial numbers of superlarge road dust (or road salt) particles (~100 µm, which can travel only 1 km) from wet and muddy surfaces, which may in turn cause exceptionally large deposition amounts in Fukushima in January. The completion 720 of decontamination in 2013 was lower than 10% for roads and forests in Fukushima city.
More than ten years have passed since the accident but the issues to be resolved in the future are still the same as those listed in K16. The current study represents an order estimation of the regional budget for only one year using a simple model and schemes. In addition to the utilized model and schemes, the current horizontal grid resolution is too coarse to reflect the heterogeneous distributions of various land use types. Soil dust and road dust emissions are relatively well-formulated, but 725 bioaerosols are not. Substantial efforts have been made to understand the emission mechanisms and quantifications of bioaerosol emission fluxes (Igarashi et al., 2019b;Kita et al., 2020;Minami et al., 2020), but it is still difficult to establish a set of formulas that is applicable for various vegetation surfaces. Our hypothesis of the existence of superlarge particles is not proven at allyet. The decreasing trends in atmospheric 137 Cs differ between the periods before and after approximately 2015 (Watanabe et al., 2021), but the reason for this distinction is not clear. A long-term (i.e., 10-year) assessment using long-term 730 measurements and numerical simulations is required. The quantification and formulation of size-resolved 137 Cs emission fluxes from various sources should directly connect to the comprehensive understanding of the regional budget of resuspended 137 Cs.