Radionuclides Behavior of Subsurface Water in Small Catchments, Covered by Different Vegetation in Kawamata Town, Fukushima Prefecture Ishwar PUN 201121329 January 2013 A Dissertation Submitted to The Graduate School of Life and Environmental Sciences, The University of Tsukuba in Partial Fulfillment of the Requirements for the Degree of Master of Environmental Sciences Abstracts The study was conducted after the catastrophic earthquake and tsunami triggered in 2011 March 11th and Fukushiam Dai-ichi Nuclear Power Plant (FDNPP) accident in Fukushima Prefecture. The accident results the huge number of radionuclides deposition in the environment. The study was performed in three different places covered by Grassland, Farmland and Forest (Matured and Young conifer trees). For the study, suction lysimeters in three different depths 10 cm, 30 cm and 50 cm were installed. The soil water was collected in a conical flask. At the same time, the soil moisture loggers were also installed in three places to know the soil water movement with different vegetation. The significant changes with rainfall event show in a Iboishi Yama Watershed (grassland) in every depth of 10, 30 and 50 cm depths. However, in a forest areas covered by conifer trees and some litter, the soil water movement are not so effective. The presence of litters in forest areas acts as the resistance of infiltration process, this results the overland flow. The soil water was analysed in Gamma ray detector. Gamma ray emissions at the energies of 604 keV (Cs 134) and 662 keV (Cs 137) were measured. The First samples were measured at Tsukuba Meteorological Institute and the University of Tsukuba. Rest of the sample was measured at Hiroshima University. The cesium (Cs-134 and Cs-137) concentration values varied during the study period is from 0.009 Bq/Kg ~ 2.38 Bq/kg and 0.021 Bq/Kg~2.48Bq/kg respectively. The study shows that Cesium is strong attached with soil in 2 cm depth of soil in Kawamata town (Kato et al., 2012). Only the few radiocesium goes to the soil water with preferential path of root channel or worm hole. The level of Cesium in soil water is very low concentration. i Contents Page Abstracts .................................................................................................................................................... i Contents.................................................................................................................................................... ii List of Table ............................................................................................................................................ iii List of Figures ......................................................................................................................................... iv Chapter 1 Introduction ............................................................................................................................. 1 1-1 Background ........................................................................................................................................ 1 1-2 Previous studies ................................................................................................................................. 1 1) The radionuclides fallout by Nuclear Weapon testing in mid-19th Century: ............................... 1 2) Radionuclides fallout from Chernobyl ......................................................................................... 1 3) Radionuclides fallout from Fukushima Dai-ichi Nuclear Power plant ........................................ 2 1-3 Research Objectives: .......................................................................................................................... 5 Chapter 2 Study Area and Method ........................................................................................................... 6 2-1 Study Area Description ...................................................................................................................... 6 2-2 Sample Collection .............................................................................................................................. 7 2-3 Measurement of Cesium .................................................................................................................... 7 2-5 Soil Texture Analysis ......................................................................................................................... 8 2-5. Soil Moisture Monitoring ................................................................................................................. 8 Chapter 3 Results ................................................................................................................................... 17 3-1 Temporal and Spatial Variation of Cesium Concentration of Soil Water........................................ 17 3-2 Soil Texture...................................................................................................................................... 23 3-3 Soil Moisture Change ...................................................................................................................... 26 Chapter 4 General Discussion ................................................................................................................ 30 Chapter 5 Conclusion ............................................................................................................................. 34 Acknowledgements ................................................................................................................................ 36 References: ............................................................................................................................................. 37 ii List of Table Table 1 Field Survey .............................................................................................................................. 13 iii List of Figures Figure 1 Radiocesium Deposition in Regional......................................................................................... 3 Figure 2 Regional Dispersion of Radionuclides from Chernobyl Accident ............................................. 4 Figure 3 Study Area ................................................................................................................................. 9 Figure 4 Overview of Grassland Site and Suction Lysimeters Sampling Devices of Soil Water .......... 10 Figure 5 Overview of Young Conifer Forest and Suction Lysimeters Sampling Devices of Soil Water ................................................................................................................................................................ 11 Figure 6 Overview of Matured Conifer Forest and Suction Lysimeters Sampling Devices of Soil Water ................................................................................................................................................................ 11 Figure 7 Outline of Suction Lysimeters Devices for Soil Water Sampling and Hand Pump ................. 12 Figure 8 Soil Core Sampling in winter ................................................................................................... 14 Figure 9 Soil Core Sampling in Winter .................................................................................................. 14 Figure 10 Soil Water Extraction by Centrifugal Process ....................................................................... 14 Figure 11 Soil Core Sample Shipped and Sieving ................................................................................. 15 Figure 12 Particle Size Separation ......................................................................................................... 15 Figure 13 Soil Moisture Monitoring Sensors installed at Multiple Depth (Left) and Data Logging System (Right) ....................................................................................................................................... 16 Figure 14 Temporal Variation of Cesium Concentration in Iboishi Yama Watershed (Grassland) ...... 18 Figure 15 Vertical Profile of Cesium Concentration in Soil Water ....................................................... 19 Figure 16 Vertical Profile of Cesium Concentration in Kotaishi Watershed (Farmland) ...................... 20 Figure 17 Temporal Variation of Cesium Concentration in Young Conifer Forest ............................... 21 Figure 18 Temporal Variation of Cesium Concentration in Matured Conifer Forest ............................ 22 Figure 19 Vertical Profile of Cesium Concentration in Matured Forest ................................................ 22 Figure 20 Iboishi Yama Watershed (Soil Texture) ................................................................................ 24 Figure 21 Kotaishi Watershed (Soil Texture) ........................................................................................ 24 Figure 22 Young Conifer Forest (Soil Texture) ..................................................................................... 25 Figure 23 Matured Conifer Forest (Soil Texture) .................................................................................. 25 Figure 24 Temporal Variation of Soil Water Movement in Iboishi Yama Watershed .......................... 27 Figure 25 Temporal Variation of Soil Water Movement in Young Conifer Forest ............................... 28 Figure 26 Temporal Variation of Soil Water Movement in Matured Conifer Forest ............................ 29 Figure 27 Vertical Soil Profile of Cesium Concentration in Kawamata Town ...................................... 32 Figure 28 Cesium Concentration in Through Fall Water in Kawamata Riko ........................................ 33 iv Chapter 1 Introduction 1-1 Background Soil water movement is one of the hydrological processes of hydrological cycle. In the hydrological process, water comes in the surface through precipitation. Some portions of the water run in the surface of the earth. Some portion of the water enters in the soil surface by the process of infiltration, percolation and in the shallow and deep groundwater. The soil water is one of the important factors in agriculture activity. It shows the availability of water for the plant and how much rainfall can affect the groundwater recharge. It is also important to know the spatiotemporal variation of soil water for the water availability. There are many studies about the soil water movement by using isotopes of stable and unstable elements. There are very few studies using the radioisotopes as a tracer to study the soil water movement. The previous studies using stable isotopic ratio shows that soil water movement is active between the soil surface and a depth of 100 cm (Tsujimura et al., 1998). 1-2 Previous studies Radionuclides in the environment occurs either by natural cosmic ray reaction in the atmosphere or human activities like nuclear weapon testing in 19th century and the development of nuclear power plant. For the study of radionuclides in the environment, the three phases of radionuclides fallout in the environment will be studied. First, radionuclides fallout by nuclear testing in mid of 19th century, Second is radionuclides fallout by Chernobyl accident in 1986 in Ukraine and third one is Fukushima dai- ichi nuclear power plant accident in 2011. 1) The radionuclides fallout by Nuclear Weapon testing in mid-19th Century: There are several practices of nuclear weapon testing. First it was tested in atmosphere and underground testing. The first atmospheric nuclear weapon test occurred in USA on 16th July 1945. The most powerful countries at that time USA, UK and USSR continued the testing of Nuclear weapon untill 1962. After, there was a treaty between these countries to ban the testing in 1963. After the treaty in 1963, there were few number of nuclear testing by France and China. The last explosion of nuclear weapon testing occurred in 1980. The fallout of radionuclides in the 19th century was typical as shown in figure 1. 2) Radionuclides fallout from Chernobyl After the Nuclear weapon testing, another catastrophic Nuclear power plant accident occurred in Ukraine in 1986.According to UNSCEAR report (2000), from 1945 to 2000, the number of atmospheric test was 543 and underground test was 1876. Comparing to Chernobyl nuclear accident and Nuclear weapon test, almost the radiocesium deposition in Russia and Finland was half. The contaminated area by radiation is higher in the region of Chernobyl nuclear 1 power plant and lower in far regional part of the world as shown in figure 2. From the Chernobyl Nuclear accident total amount of radiation was releases approximately 5.2×1018 Bq. 3) Radionuclides fallout from Fukushima Dai-ichi Nuclear Power plant After the Chernobyl Nuclear accident, another catastrophic nuclear accident was occurred in Japan ion March 11, 2011. The total amount of radiation was released from the Fukushima Dai-ichi nuclear power plant was estimated approximately 1.5×1017 Bq (Chino et al., 2011). Which is the just 7% radiation released from Chernobyl Nuclear accident in 1986. The atmospheric released radiation dose settled on the ground either through dry or wet deposition. The primarily deposition of Cesium in the ground surface is associated with precipitation (Tamura, 1964). The total amount of the cesium concentration is strongly attached with surface soil particle. It is seems to be moved in the subsurface by heavy rainfall input causing the infiltration and percolation. So, hypothetically, the movement of radiocesium will not be uniform because it is considered that infiltration and percolation process depend on compact of soil, soil texture, litters and vegetation types. After the rainfall, with the movement of soil water, cesium seems to be undergo subsurface water. Very few studies have been done on subsurface water contamination by radiocesium. 2 Figure 1 Radiocesium Deposition in Regional Source: (S.M. Wright et al., 1999) 3 Figure 2 Regional Dispersion of Radionuclides from Chernobyl Accident Source: UNSCEAR Report, 1998 4 1-3 Research Objectives: There are many studies about the radiocesium in soil but very few studies have been conducted about the radiocesium in the water. Specially, there is rare study about the subsurface water contaminated with radiocesium. Only soil erosion and vertical profile of soil study was done by using cesium as a tracer (Takenaka et al., 1998, Kato el at., 2011). The main objective of the study is how the radionuclides move with the water environment. The objectives of the investigation are as follows. 1) To make clear of the soil water movement comparing with the input of rainfall event in different layer of the soil surfaces with the temporal changes of soil moisture 2) To explain the behavior of Radionuclides (Cs-137 and Cs-134) in a soil surface of different layer and it movement in different vegetation. 5 Chapter 2 Study Area and Method 2-1 Study Area Description To make the clear movement of radionuclides (137 Cs and 134 Cs) in Soil water in the four places of Kawamata town of Fukushima covered by grassland, Farmland and Forest (cedar). The Field study area is located 35 km north-west from the Fukushima Daichi Nuclear Power plant. An observation points in three vertical depth of soil surface. Soil water was collected from 10 cm, 30 cm and 50 cm depth in Grassland and Matured and Young Forest. In the case of Farmland, the soil texture is dominated by granite and it became necessary to bore the holes only 10 cm, 20 cm and 30 cm depths of soil surface, to enable water collection. The study site is located in Kawamata Town, Yamakiya District, Fukushima Prefecture. The mean annual precipitation is 1249 mm from the year of 2003-2009 (Yamakiya weather station, JMA) and the mean annual temperature 12degree centigrade (Nihonmatsu weather station) as referred to the Kato et al., 2012. For the study, four places were selected with different vegetation types. Iboishi Yama Watershed (Grassland): The grassland was dominated by small vegetations shrubs and herbs rather than the trees. The upper part of the grassland was dominated by Trees and down part of the grassland is covered by small vegetation as shown in figure 3. Kotaishi Watershed (Farmland): The farmland was mostly covered by small weeds. The surface of soil layer was presence of gravel. When it was boring, the area of farmland was quite hard because of presence of stone. The upper part of farmland landscape was also dominated by trees. The landscape of grassland and farmland are different in vegetation types as shown in fig 4. Young Conifer Forest: The landscape of Young forest is steeper. The forest area is dominated by cedar trees. The small vegetation is not present. Only the litter of the cedar leafs were present in all the season. Inside the field area, the densities of the trees are more as shown in figure 5. Matured Conifer Forest: The landscape of Matured Forest is more flat comparing to Young conifer forest. The area is dominated by cedar trees. In the surface of area, large volume of litters is present. Comparing to Young forest, the density of tree is rare as shown in figure 6. 6 2-2 Sample Collection To collect the soil water, every four place were chosen covered by different vegetation covered by grass, forest. The soil water sampling was performed from the beginning of the June 2011 to end of December 2011. The soil water was sampled at the depths of 10cm, 30cm and 50 cm in grassland and Forest areas. In the Farmland, 10 cm, 20 cm and 30 cm depths were chosen. The soil water was collected by suing suction lysimeter consisting of a ceramic cup with a diameter of 18mm. The water was collected by using the flasks of 500 ml volume. To make the low pressure into the flask, hand pump (DK-8390, Daiki Rika Kogyo Co., Ltd) were used until -70 to -80 kPa as shown in Fig 11. In comparison of four sites, larger volumes of water were collected in Grassland than farmland. In the forest area, the larger volumes of soil water were extracted in Matured forest than Young Forest as shown in Table 1. In the winter season, from mid-December to end of the March, soil water sampling by suction lysimeter and flask, were not possible. In the winter, most of the glass were broken and frozen of low temperature. So, during that period, soil core sample were collected. The collected soil core samples were process in Centrifugal and extracted the soil water as shown in the Fig 8 and 9. The volume of water collected by centrifugal is very low. The average volume of soil water was 10 ml. 2-3 Measurement of Cesium The soil water was filtered by using 0.45 m membrane, and the Cesium 134 and 137 concentrations were determined by a gamma ray spectrometry using a germanium semiconductor detector counting for 30,000 seconds per sample in Meteorological Research Institute, Japan Meteorological Agency. The sample taken in end of June and July, 2011 were measured in Tsukuba Meteorological institute. The soil core samples taken in winter were measured at Onda laboratory in the University of Tsukuba. The method used in Hiroshima University for the cesium measurement was “cesium enrichment method by Ammonium phosphomolybdate”. For this process, HNO3 adjusted to pH1, Cs-133 carrier solution, ammonium phosphomolybdate were mixed. Then agitating for one hour and then left for 12 hours. After that the solution was filtered using 0.45 µm membrane filter. Hence, filtrate residue (sediment) was dried under the temperature (90ºC for 12 hours). After weighing, the residue sample was measured in in Gamma Ge semiconductor detector. 7 2-5 Soil Texture Analysis In order to study the soil physical property, soil core sample were taken from every sites; Iboishi Yama Watershed (grassland) , Kotaishi Watershed (Farmland) and Forest sites (Young and Matured Conifer). Each core sample was extracted from 10 cm, 30 cm and 50 cm in Iboishi Yama Watershed and Conifer Forest sites and 10cm, 20 cm and 30 cm depth in Kotaishi Watershed (Farmland). In order to avoid the falling of soil from the vessel, the lower part of vessel was fixed with cloth by using rubber band. The sample soil was then shipped in laboratory by keeping it in a plastic container. The soil core samples were dried for 12 hours at 105 degree centigrade. The sample was then crushed to pass through a 2mm sieve (gravel) , 2mm>> 850µm(Sand), 850 µm>>425µm (Silt) and 425µm< (Clay). Then the weight of soil percentage and water content were calculated. Also the particle sizes of soil distribution were analyzed using sieve method as shown in figure 10 and 11. 2-5. Soil Moisture Monitoring To measure the soil water movement in every sites covered by different vegetation, soil moisture logger and sensors (HOBO micro station, ONSET Computer Corporation) were installed. The soil moisture loggers were installed in Iboishi Yama Watershed (Grassland) and Conifer Forest sites (Young and Matured) in each depth of 10cm, 30 cm and 50 cm depths as shown in figure 12. However in Kotaishi Watershed (Farmland), the presence of gravel made it difficult to install the soil moisture sensors. 8 Figure 3 Study Area 9 Figure 4 Overview of Grassland Site and Suction Lysimeters Sampling Devices of Soil Water 10 Figure 5 Overview of Young Conifer Forest and Suction Lysimeters Sampling Devices of Soil Water Figure 6 Overview of Matured Conifer Forest and Suction Lysimeters Sampling Devices of Soil Water 11 Figure 7 Outline of Suction Lysimeters Devices for Soil Water Sampling and Hand Pump 12 Table 1 List of soil water samples and soil cores for moisture extraction Site Iboishi Yama Watershed Grassland Kotaishi Watershed Young Conifer Forest Cedar Trees Matured Conifer Forest Cedar Trees Land Grassland domination water cycle Recharge area Discharge area Recharge area Recharge area condition Depth 10cm 30cm 50cm 10cm 20cm 30cm 10cm 30cm 50cm 10cm 30cm 50cm 2011 8/29 800 1000 200 300 200 150 100 150 50 50 200 450 9/7 1100 800 1000 300 300 450 100 200 50 100 230 450 9/23 1100 800 1000 500 1000 500 200 450 80 200 350 500 10/8 500 1100 1200 1400 900 500 300 400 150 180 300 550 10/22 600 1100 1100 300 50 80 200 450 80 200 200 500 11/5 250 1000 700 280 250 210 50 200 0 200 210 500 11/19 600 1000 500 50 100 150 100 150 50 150 150 460 12/5 1000 550 500 530 1010 300 130 130 50 150 110 700 2012 1/12 C C C C C C C C C C C C 2/17 C C C C C C C C C C C C 3/9 C C C C C C C C C C C C 4/14 C C C C C C C C C C C C C: Soil core sample 13 Figure 8 Soil Core Sampling in winter Figure 9 Soil Core Sampling in Winter Figure 10 Soil Water Extraction by Centrifugal Process 14 Figure 11 Soil Core Sample Shipped and Sieving Figure 12 Particle Size Separation 15 Figure 13 Soil Moisture Monitoring Sensors installed at Multiple Depth (Left) and Data Logging System (Right) 16 Chapter 3 Results 3-1 Temporal and Spatial Variation of Cesium Concentration of Soil Water Iboishi Yama Watershed (grassland): The vertical profiles of soil water with concentration of radiocesium are plotted against the depth from the soil surface as shown in figure 13 and 14. The temporal variation of Cesium was found in the surface soil water at 10 cm depth and then exponentially decreasing with depth. Both the Cs-137 and Cs-134 had found higher concentration in the beginning of July 2011. Because of its decaying in the nature, the concentration of Cs-134 is found to be lower in the beginning of September 2011. The vertical profile of Cesium in soil water shows that Cesium has reached in all the depth of 10 cm, 30 cm and 50 cm depths with the rainfall input. In the Iboishi Yama Watershed, Cesium concentration varies from 0.009 Bq/Kg~2.5 Bq/Kg. Kotaishi Watershed (Farmland): The Cesium concentration (Cs 134 and Cs 137) varies in Kotaishi Watershed is 0.026 Bq/Kg~ 0.111 Bq/Kg respectively. From the result shown in Figure 16, cesium does not move until the 30 cm depth. The soil texture result in figure 21 shows that the in every depth of 10cm, 20 cm and 30 cm, high percentage of clay content and trap the Cesium. Young Conifer Forest: In the case of Young Forest, higher value of cesium concentration shows in 10 cm depth. The cesium value ranging from 0.141 Bq/Kg~0.466 Bq/kg. The figure 17 shows the temporal variation of Cesium in Young Conifer Forest. The vertical profile of Cesium in Young Conifer forest shows that in every depth, cesium has been reached and in 50 cm high concentration of Cs-137 has been detected. The forest sites contents high volume of litters and roots. Matured Conifer Forest: In the case of Matured Forest, the cesium concentration in 10 cm is higher than 30cm and 50 cm depths. The cesium value is ranging from 0.036Bq/Kg~0.682 Bq/kg. The profile of vertical distribution and rainfall input is shown in the figure 18. 17 Figure 14 Temporal Variation of Cesium Concentration in Iboishi Yama Watershed (Grassland) 18 Rainfall 7/1 7/8 7/15 7/22 7/29 8/5 8/12 8/19 8/26 9/2 9/9 Day mm/hr 0 10 Rainfall 20 30 Figure 15 Vertical Profile of Cesium Concentration in Soil Water 19 Rainfall Day 7/1 7/31 8/30 9/2910/2911/2812/28 mm 0 10 Rainfall 20 30 Figure 16 Vertical Profile of Cesium Concentration in Kotaishi Watershed (Farmland) 20 Bq/Kg Figure 17 Temporal Variation of Cesium Concentration in Young Conifer Forest 21 Bq/Kg Figure 18 Temporal Variation of Cesium Concentration in Matured Conifer Forest Day Rainfall 7/1 7/31 8/30 9/29 10/2911/2812/28 mm 0 10 Rainfall 20 30 Figure 19 Vertical Profile of Cesium Concentration in Matured Forest 22 3-2 Soil Texture Iboishi Yama Watershed (Grassland) In the Iboishi Yama Watershed, the presence of root is dominated in the 10 cm depth to 30 cm depth. In the case of 30 cm depth, the presence of sand and silt is higher than clay. In 50 cm depth, the presence of gravel and clay is higher as shown in Figure 20. Kotaishi Watershed (Farmland) Soil core sample was analyzed particle distribution by sieving method as shown in figure 12. Each component of soil texture root, gravel, sand, silt and clay was separated. In every depth of 10cm, 30 cm and 50 cm were separately analyzed. As shown in figure 21, in 10 cm depth, soil is dominated by gravel and silt. Similarly in 30 cm and 50 cm depth, soil are dominated by clay, silt and sand respectively. Young Conifer Forest (Kawamata Riko) In the Young Conifer Forest, root was present in all the depth of 10 cm, 30 cm and 50 cm depth. It means presence of root channel upto 50 cm depths. In the 50 cm depth, soil is dominated by high clay but 30 cm depth, very few percentage of clay as shown in figure 22. Matured Conifer Forest (Kawamata Riko) In case of Matured Conifer forest, equal proportion of root is present in all depths. Except in 10 cm depth, high clay content in the 30 and 50 cm depths of matured conifer forest as shown in figure 23. 23 Figure 20 Iboishi Yama Watershed (Soil Texture) Figure 21 Kotaishi Watershed (Soil Texture) 24 Figure 22 Young Conifer Forest (Soil Texture) Figure 23 Matured Conifer Forest (Soil Texture) 25 3-3 Soil Moisture Change Iboishi Yama Watershed (Grassland) The temporal variation of soil water movement in grassland shows the direct effect of rainfall input until 50 cm depth. The higher the rainfall input, higher the movement of water in soil surface. From starting of August 5th to end of October 2011, soil water movement is highly affected by rainfall input as shown in figure 24. In the winter, the change of soil water movement is not effected as there is no rainfall event. Kotaishi Watershed (Farmland) The farmland is highly dominated by gravel. It became difficult to installed suction lysimeter until 50 cm depth. So, for the soil water extraction, only the 10cm, 20 cm and 30cm depth were chosen. The soil moisture logger and sensor were not installed because of difficulties in digging the hole. Young Matured Forest The temporal variation of soil water movement in the Young forest with the rainfall input, is highly affected in 10cm and 30 cm depth whereas in the 50 cm depth, the soil water movement is comparatively lower. From July 1st to end of Sept 2011, the soil water movement is affective in all three depths. In the winter season, there is only small movement. But in 10 cm depth, soil water movement is changing than 30 cm and 50 cm depths as shown in figure 25. Matured Conifer Forest The temporal variation of soil moisture in Matured forest shows that only the little amount of rainfall input reached to the 50 cm depth. In the case of 10 cm and 30 cm depth, the movement of soil water is similar. Even in winter season when there is no rainfall input, the soil water movement is differently in 50 cm depth as shown in figure 26. 26 Figure 24 Temporal Variation of Soil Water Movement in Iboishi Yama Watershed 27 Figure 25 Temporal Variation of Soil Water Movement in Young Conifer Forest 28 Figure 26 Temporal Variation of Soil Water Movement in Matured Conifer Forest 29 Chapter 4 General Discussion The concentration of radiocesium in the surface soil is not uniform. It is well known that Cesium-137 is supplied through deposition like rain or dry fallout and absorbed into the surface soil (McCallan et al., 1980). The radiocesium behavior is highly attached with soil particle and 80% of radiocesium attached in top soil (Tamura, 1964, Kato et al., 2012). Only the small portion of radiocesium will undergo into the soil surface with the rainfall input in a preferential path i.e root channel and worms hole and then by the process of infiltration and percolation. It is also proved that the depth distribution of radiocesium in soil also very clear with decreasing order of concentration with depth. 4-1. Iboishi Yama Watershed The depth distribution of radiocesium in soil water shows that the contamination of soil water in 10 cm depth is higher than the 30 cm and 50 cm depth. When comparing with soil depth distribution of radiocesium in soil and water, very few amount of radiocesium will move through the preferential path like root channel and worm holes proceeding the infiltration and percolation. If it is compared with the soil moisture data, the movement of water is very effective during rainfall input. In grassland, the water is reached until 50 cm very clearly but the cesium concentration is very low in 50 cm depths. It proves that the cesium is strongly attached in soil particle rather than water drops. 4-2. Kotaishi Watershed (Farmland) In Kotaishi Watershed, very low level of cesium is reached upto 30 cm depth. The soil is largely dominated by clay silt sand. The vertical profile of Cesium (figure 16) shows that Cs137 is higher concentration in 20 cm depth. The equal proportion of soil particle is present as shown in figure 21 i.e. sand, silt and clay. The presence of sand, silt and clay dominated sites; soil water does not go clearly in deeper depth. 4-3. Conifer Forest (Young and Matured) The soil water movement in Matured forest and Young forest are similar. With the rainfall input, it is clear that soil water reached until 50 cm depth. It means there is a chance to reach the radiocesium in 50 cm depth. In case of forest areas, the highest concentration of Cs 137 0.466 Bq/ Kg at 50 cm depth at young conifer forest. It is observed that near the trunk of the tree, soil water was able to collect plenty than other places. So, it is easy to move the soil water near the rhizoids and tree roots zones. It means the rainfall input through stem flow and through fall (which is highly contaminated by cesium, Kawamori 2012, Figure 28) to the subsurface water is easy to undergo. The highly contaminated water is moved to soil water of every depth in Forest sites. Which made the high cesium concentration is soil water in Conifer forest areas. 30 In the matured conifer forest, every 10 cm depth, high concentration of Cesium have been detected. The cesium value of 10 cm depth is Matured conifer forest is about 0.682 Bq/Kg. When the rainfall event occurs, the water moves in the ground surface through stem flow, through fall and interception, the thick litter of Forest (shown in figure 7) is soaked with contaminated water in upper surface level of 10 cm depth. So, high concentrations have been found in 10 cm depth in Matured Conifer forest. Hypothetically, the cesium should move in subsurface by rainfall input, process of infiltration and percolation. Rainfall event in mountain area like Yamakiya is uneven. The rain fall data from one place to another place can be differ (P.C. et al., 2012). Also during the Field study sampling, it was clearly observed that precipitation pattern was differed from every 1000 meters. It could be clear either the movement of Cesium in Soil water is in vertical profile condition or not. If the rain gauge were installed in the study sites, it will make the clear idea of soil water movement with cesium. 31 Figure 27 Vertical Soil Profile of Cesium Concentration in Kawamata Town (Source: Kato el al., 2012) 32 Activity(Bq/L) Through fall in Young Conifer Forest 1200 1000 800 600 400 200 0 Cs-134 Cs-137 Figure 28 Cesium Concentration in Through Fall Water in Kawamata Riko (Source: Kawamori et al 2011) 33 Chapter 5 Conclusion In this study, radionuclides (radiocesium) behavior of subsurface water in different vegetation types were studied. The fallout of radiocesium in first time in surface depends upon the wind pattern, velocity and rainfall events. Based on experienced of field visit to Fukushima, rainfall event was also uneven in different location of sites. When we measured the radiation air dose, Kotaishi Watershed (Farmland) was quite higher than other sites. It shows that trap of radiocesium and radiation dose in the air depends on the topography, landscape, trees, and small vegetation. The previous study by Kato et al. 2012 in the same sites shows that 80% of radiocesium strongly deposit in the top soil of upper 2 cm soil surface. That shows that upper surface level of soil is highly contaminated with radiocesium. It means hypothetically, with the typhoon and heavy rainfall pattern, infiltration and percolation, the radiocesium presence in the upper surface level should be moved to the deep groundwater. However, in soil water, the cesium concentration was found very low comparing to the surface soil. From the initial result of radiocesium in soil water, the concentration value is ranging from (Cs-134 and Cs-137) 0.009 Bq/Kg ~ 2.38 Bq/kg and 0.021 Bq/Kg~2.48Bq/kg respectively. It means the concentration of cesium is very low in soil water. After the Fukushima Dai Ichi Accident, in the initial monitoring of radionuclides both Cs 134 and Cs 137 have been found higher. Only from the heavy rainfall input, radiocesium should be forced to move in the deep surface but the presence of soil particle, the movement of Soil water is different from place to place as shown in figures 24, 25, 26. The soil water movements are different in different vegetation types. In Iboishi Yama Watershed (grassland), movement of soil water is more effective in every depth because of small types of vegetation shown in figure 3 and 17. Also, the vertical profile of cesium in soil water in grassland shows the cesium concentration in every depth and decreasing the every value with time period. From the study, it is also clear that an isotope of cesium decaying in the environment because of its half-life. The cesium concentration in forest sites are comparatively higher than other sites like grassland. This shows that when the fallout of cesium in ground surface, the vegetations differs the cesium deposition. From the result, it is known that small grass does not trap the cesium but large canopy of tree trap the cesium and moves to the ground surface with forest hydrological cycle. Similarly, in forest site, soil water movement is different from Iboishi Yama Watershed (grassland). Because of presence of trees, inception occurs and presence of litter in ground surface, the movement of soil water reach until the 50 cm depth even the rainfall input is small. Because of thick layer of litter in forest areas, in every depth, soil water movement is effective. From the soil water movement phenomena, chance of reaching of radiocesium upto 50 cm is highly possible. The result obtained in Young conifer forest of 50 cm depth is higher value of Cesium proves that the possibility of Cesium movement by preferential path of root 34 channel and also it proves the presence of roots in every depth of Forest sites as shown in figure 22 and 23. 35 Acknowledgements This study was carried under financial assistance of FMWSE project funded by (MEXT Special Coordination Funds for Promoting Science and Technology 2011), Japan. I am extremely thankful to my supervisors Prof Maki Tsujimura, who provided me chance to study hydrology and EDL program in the University of Tsukuba. I am also thankful to Professor Yuichi Onda, Professor Keisuke Sueki, Department of Life and Environmental Science, The University of Tsukuba, for their noble guidance, support with full encouragement and enthusiasm. I am grateful to Assistant Professor Atsushi Kawachi and Dr. Yutaka Abe for his valuable suggestions, ever encouraging and motivating guidance. Very special thanks to team mate Ms. Manami Hada, who was always there with me during sampling in the field as well as sorting and identification of the samples in the lab. I would also like to thank all the laboratory members of watershed and hydrology for their kind assistance in helping and encouragement. Last but not the least I would also like to thank all of my friends, EDL members, family members for encouraging and supporting me whenever I needed them. 36 References: Chino, M., Nakayama, H., Nagai, H., Terada, H., Katata, G., Yamazawa, H., 2011. Preliminary Estimation of release amounts of 131I and 137Cs accidentally discharged from the Fukushima Dai-ichi nuclear power plant into the atmosphere. Journal of Nuclear Science and Technology 48 (7), 1129-1134. Cremers A, Elsen A, Peter PD, Maes A. Quantitative analysis of radiocaesium retention in soils. Nature 1988; 335:247-249. Kato, H., Onda, Y., and Teramage, M., 2012. 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