Geochemical Journal, Vol. 47, pp. 683 to 692, 2013 doi:10.2343/geochemj.2.0291 NOTE Long-range transportation and deposition of chemical substances over the Northern Japan Alps mountainous area KAZUHIRO TOYAMA,1* JING ZHANG 2 and HIROSHI SATAKE2† 1 Center for Faculty Development, Okayama University, 2-1-1 Tsushima-naka, Kita-ku, Okayama-shi, Okayama 700-8530, Japan 2 Graduate School of Science and Engineering, University of Toyama, 3190 Gofuku, Toyama-shi, Toyama 930-8555, Japan (Received November 30, 2012; Accepted November 3, 2013) The chemical compositions in the snow layers of vertical snow samples collected from six sites in the central mountainous area, Japan, during early spring 2004 were analyzed to investigate the long-range transportation of chemical substances from the Asian continent to the high mountainous areas in Japan. These sites included Iou-zen, at 800 m above mean sea level (AMSL) and in closest proximity to the Sea of Japan: Kongoudou-zan, at 1300 m; Nishi-Hodaka-dake, the Northern Japan Alps at 2200 m; Hachimori-yama, at 2100 m; Kiriga-mine, at 2000 m; and Yatsuga-take, the most inlying site, at 2200 m. The concentration of anthropogenic components in the snow such as non-sea-salt (nss-) SO42– and NO3– range from nearly 0 to more than 100 µ eq/L. The nss-SO42–/NO 3– (S/N) ratio in snow typically ranges from 0.3 to 6.3. A considerable number of samples had higher S/N ratios than those found in Tokyo, Japan, at approximately 1.6, whereas some samples had a much higher ratio of approximately 4–6, which is more similar to values found in Beijing, China, at approximately 3.2. The vertical profile pattern variations of chemical components in the snow layers were found to correspond roughly. For example, the concentrations of nss-SO 42– in snow was found to reduce exponentially with increasing distance from the Sea of Japan to the Japan Alps, although the value decreased sharply at three sites located monsoon-leeward of the Japan Alps. This suggests that the anthropogenic components transported from the Asian continent with the monsoon were gradually removed from air and deposited in the snow cover as the air masses passed over the Northern Japan Alps. Keywords: mountain snow, chemical components, cross-border pollution, acid snow, anthropogenic contaminants tion, they are believed to cause acid rain and or acid snow. It is also well known that the snow in the Northern Japan Alps mountainous area contains these acidic substances, and previous snow surveys conducted in Mt. Tateyama, Toyama Prefecture, suggest that contaminants from the continent extend into the mountainous areas (Osada et al., 2000, 2009; Kido et al., 2001; Watanabe et al., 2005). Additionally, Toyama et al. (2007) has determined that these acidic substances have reached 100 km inland from the Sea of Japan and have been detected as far inland as Nishi-Hodaka-dake. Moreover, measurements of the sulfur isotope ratio (the value of δ34S) have revealed that the northeastern part of the Asian continent is the origin of much of the SO42–. The Northern Japan Alps mountainous area is located on the Sea of Japan side of the central Japanese island of Honshu, and is thus in closer proximity to the Asian continent than is the rest of the nation. Therefore, significant amounts of air pollutants transported from the continent over the Sea of Japan during the winter season are deposited in those areas; considerable research has been con- INTRODUCTION Economic developments in northeast Asia continue at a rapid pace, and the environmentally negative impact on neighboring countries such as Japan due to the increase in anthropogenic emissions, typically SO42–, is a major cause for concern. It is well known that during winter, various chemical substances including acidic components such as sulphate ions (SO42–), are transported in the atmosphere from the Asian continent to Japan’s coastal area along the Sea of Japan. These acidic substances have been identified primarily from observations in lowland areas (Satake and Yamane, 1992; Akata et al., 2002). Because such substances are responsible for acidifying precipita- *Corresponding author (e-mail: [email protected]) † Deceased in November 2009. Copyright © 2013 by The Geochemical Society of Japan. 683 Fig. 1. Sampling point locations. Site 1, Iou-zen (800 m above sea level); Site 2, Kongodo-zan (1300 m); Site 3, Nishi-Hodakadake (2200 m); Site 4, Hachimori-yama (2100 m); Site 5, Kiriga-mine (2000 m); and Site 6, Yatsuga-take (2200 m). Open circles indicate the locations of the Automated Meteorological Data Acquisition System (AMeDAS) stations nearest to each site. ducted on trans-boundary atmospheric pollution (Zhang and Liu, 2004; Yuan and Zhang, 2006; Mizoguchi et al., 2012). The Northern Japan Alps mountainous area is notable on a global scale for its heavy snowfall due to the winter monsoon; however, no large-scale sources of anthropogenic contaminants have been detected in the area. In contrast, the air parcel that causes heavy snow to fall on the Northern Japan Alps eventually moves to the Pacific side. However, the removal mechanisms of the chemical substances from the air over the mountainous area are unclear, and the negative impact to the environment of Pacific Ocean and Pacific side area in Japan has not been sufficiently investigated. For these reasons, we considered the snow of the Japan Alps mountainous area to be suitable for examination of the anthropogenic contaminants transported from the Asian continent to Japan by the winter monsoon. Because chemical substances of various origins such as sea salt and soil and anthropogenic contaminants such as SO42– may be carried by the winter seasonal winds above the Northern Japan Alps, they are also capable of reaching even farther inland. However, the transport range 684 K. Toyama et al. of these chemical substances beyond the mountain range of the Northern Japan Alps is unknown. Furthermore, the mechanism by which chemical substances suspended in clouds are deposited during this transport process is not understood, nor is the total quantity of these substances deposited in inland regions. Therefore, the authors conducted a snow survey during winter 2003–04 to investigate the transport conditions for chemical substances near the Northern Japan Alps. The survey followed the path of the seasonal wind from the Sea of Japan, running northwest–southeast and extending to a distance of more than 150 km inland. Snow was sampled at approximately the same time from six points located along the survey line, and the transport conditions for the contaminants landwards into the Japan archipelago were then investigated by comparing the vertical profiles of the chemical constituents at these points. OBSERVATIONS AND SAMPLING OF THE SNOW Snow sampling was conducted in February–March 2004 at the following six sites: Site 1, Iou-zen, February Fig. 2. Daily precipitation levels (December 2003 to April 2004) recorded at the Automated Meteorological Data Acquisition System (AMeDAS) stations nearest each sampling site. The locations of the stations are shown in Fig. 1. 19, 800 m above mean sea level (AMSL), close to the Sea of Japan; Site 2, Kongodo-zan, March 8, 1300 m; Site 3, Nishi-Hodaka-dake, located in the Northern Japan Alps mountain range, March 22, 2200 m; Site 4, Hachimori-yama, March 29, 2100 m; Site 5, Kiriga-mine, March 25, 2000 m; and Site 6, Yatsuga-take, located inland, March 15, 2200 m (Fig. 1). Site 1 is located in the most upwind location on the monsoon path, whereas Site 6 is the most downwind location. The amount of precipitation in the Northern Ja- pan Alps mountainous area is high on the monsoon upwind side at the Sea of Japan coastal area, where Sites 1– 3 are located, and the snow depth during the measurement period was between 2 m and 4 m. In contrast, precipitation amounts are less severe on the monsoon leeward side inland areas, which include Sites 4–6, and snow depths average approximately 1 m. Figure 2 shows the daily precipitation levels recorded during the period of December 1, 2003, to April 30, 2004, by the Japan Meteorological Agency’s (JMA) Automated Meteorological Data Acquisition System (AMeDAS) stations located nearest to each observation site. The locations of these AMeDAS stations are shown in Fig. 1. AMeDAS 1 (Kanazawa, nearest to Site 1), AMeDAS 2 (Tonami, Site 2), and AMeDAS 3 (Tochio, Site 3) are located in the upwind monsoon area, whereas AMeDAS 4 (Nagawa, Site 4), AMeDAS 5 (Matsumoto, Site 5), and AMeDAS 6 (Suwa, Site 6) are located on the leeward side. Precipitation amounts gradually decreased from the upwind side including the coastal area of the Sea of Japan to the leeward side inland; when the leeward side (Sites 4–6) experienced precipitation, the upwind side (1– 3) also received precipitation almost simultaneously. When selecting snow observation sites, care was taken to choose locations that were typical in terms of snow depth for that area, level, and unaffected by contamination from surrounding trees, buildings, or the local population. At each site, a snow pit was dug from the snow surface to the ground level. The wall surfaces of the pit were shaped such to prevent the order of the snow layers from being disturbed and to allow the conditions of the snow layers to be studied. Snow samples 5.8 cm wide, 5.8 cm deep, and 3 cm high were then collected from the surface of the wall by using a snow sampler. These samples were then sealed into contaminant-free plastic bags, stored at temperatures below 0°C to avoid microorganism breeding due to rising temperatures, and transported to the University of Toyama. The chemical composition concentrations of the samples were then measured by using ion chromatography (anions: Metrohm Compact IC 761, cations: TOSO IC-8010) by melting the snow immediately before measurement. The accuracy of the measured values was approximately ±5%. Because negligible snow melting was observed at the sample collection sites, it can be reasonably assumed that the complete record of the chemical constituents present in the snow at the time of its precipitation was preserved. VERTICAL PROFILES OF CHEMICAL COMPOSITION Figure 3 shows the vertical profiles of the typical chemical constituents (Na+, Ca 2+, SO42–, NO3–) contained in the samples, and the maximum, minimum, and average values at each site are given in Table 1. Because the Long-range transportation and deposition of chemicals in the Northern Japan Alps 685 Fig. 3. Vertical profiles of typical chemical constituents including Na+, Ca2+, SO42–, and NO3– contained in the snow samples obtained at each site. snow cover nearest to the ground is subject to geothermal heat-induced melting, the chemical constituents in that layer were likely contaminated by plants and soil. Therefore, samples up to 10 cm above the ground surface were excluded from the values shown in Table 1. Depending on the snow layer, concentration differ- 686 K. Toyama et al. ences in the vertical profiles of the chemical constituents can be up to 10- to 100-fold, and in a single winter, conspicuous peaks resembling spikes have been noted where such concentrations increased. In our study, such a tendency was most remarkable for Sites 1–3, with snow depth increasing at sites closer to the Sea of Japan. For example, 139 cm, 115 cm, and 70 cm were measured at Sites 1, 2, and 3, respectively. However, at inland locations such as Sites 5 and 6, the concentrations were not remarkably high even if a peak was observed; approximately 28 cm and 30 cm were measured at Sites 5 and 6, respectively. Additionally, we determined that the concentrations of most components were higher at sites in coastal areas and lower in inland areas. For example, Table 1 shows average Na+ values of 164 µeq/L at Site 1 (closest to the Sea of Japan), 12 µeq/L at Site 3 (inland), and 7 µeq/L at Site 6 (farthest inland). These figures show a difference in concentration of approximately 20-fold. In contrast, components that did not show such large differences in concentration showed only high values at specific sites, such as NO3–, with 19 µeq/L at Site 1, 10 µeq/L at Site 3, and 8 µ eq/L at Site 6. In the case of Ca2+, which does not originate from sea salt (non-sea-salt, nss-), the value was 35 µeq/L at Site 4 but only approximately 10 µ eq/L at the other sites. The pattern variations of each component’s vertical profile were roughly similar at each site. Toyama et al. (2005) compared the vertical profiles of the oxygen isotope ratio (δ 18O) in coetaneous snow layers at three distant locations near Mt. Tateyama in the Northern Japan Alps and showed that snow layers maintained their original isotopic compositions at the time of precipitation and that the pattern of δ 18O vertical profiles between each location tended to correspond. The present study also observed precipitation during approximately the same time periods; thus, the vertical profiles of the chemical components can be considered as comparable. Figure 4 shows the corresponding peaks (groups) between each of the sites. The correspondence in the patterns for the vertical profiles is high in the three sites close to the Sea of Japan (Sites 1–3) and the three inland sites (Sites 4–6). The undulating profile of the peaks shows significant variations on the Sea of Japan side (upwind of the monsoon), with very significant peaks occurring. In contrast, only small variations are evident on the inland side (downwind of the monsoon) with no tendency of outstanding peaks. This result caused by the comparatively low precipitation levels at the sites on the downwind side in which precipitation is created only by clouds that begin precipitating on the upwind side and finish the process on the inland side. In contrast, precipitation frequently occurs at sites on the upwind side where changes in the concentrations of Table 1. Maximum, minimum, and average concentrations of typical chemical components such as Na +, Ca2+, SO 42–, and NO 3– contained in the snow samples obtained at each site Elevation Distance from the Sea of Japan (m) (km) Site 1 800 21 Site 2 1300 48 Site 3 2200 100 Site 4 2100 118 Site 5 2000 143 Site 6 2200 162 chemical components included in the precipitation are more frequently recorded. Therefore, although the pattern itself may not necessarily match over a single winter season, the peaks (groups) associated with the possible events such as periods of increasing or decreasing concentration are recorded and are believed to reflect cases in which chemical substances are advected 150 km inland from the coastline of the Sea of Japan by masses of air. TRANSPORT CONDITIONS FOR ACIDIC CONTAMINANTS Anthropogenic contaminants such as nss-SO 42– and NO 3– cause precipitation acidification. In our study, the concentration of nss-SO42– was determined to be highest, at an average of 47 µeq/L, at Site 1 (closest to the Sea of Japan coast) with a notable tendency to decrease inland. However, past Site 4, where the lowest concentration of 11 µ eq/L was recorded, the concentration increased slightly at Site 6 at 16 µ eq/L. Toyama et al. (2007) analyzed δ34S and other chemical components extracted from the snow of Nishi-Hodakadake during the winter months of February 2001 and April 2003 and reported that considerable amounts of the nssSO42– deposited in the Northern Japan Alps originated in China and the Russian Far East. Accordingly, in this study it was also assumed that the nss-SO42– component had been transported from the Asian continent. Although the reason for the slight increase in concentration at Site 6 farthest inland (2200 m) remains unclear, it is, however, an interesting result. Na + nss-Ca 2 + NO3 – nss-SO4 2 – ( µ eq/L) Max. Min. Ave. Max. Min. Ave. Max. Min. Ave. Max. Min. Ave. Max. Min. Ave. Max. Min. Ave. 868 14 164 410 1 70 80 0 12 46 1 17 31 1 13 17 0 7 41 1 10 112 0 9 66 0 7 90 3 35 48 4 13 97 1 8 87 2 19 114 1 11 42 1 10 58 3 18 43 4 15 19 2 8 146 3 47 140 0 25 97 1 19 57 3 19 31 2 11 72 1 16 For NO3–, the highest concentration value, at an average of 19 µeq/L, was recorded at Site 1. The value decreased to 10 µ eq/L at Site 3, increased again to 18 µ eq/ L at Site 4 and 15 µeq/L at Site 5, then dropped to 8 µ eq/ L at Site 6. This contaminant can be considered to originate from the nitrogen oxide included in the exhaust gas from automobiles and machinery. However, the concentration increase at Sites 4 and 5, after crossing the Northern Japan Alps mountain range (Site 3), can be attributed to NO 3 – originating from local sources such as the Matsumoto Basin, where a significant amount of industrial activity occurs. Figure 5 shows the relationship among nss-SO 42– , NO3–, and nss-SO 42–/NO3– ratios (S/N ratios) in Beijing, China (approximately 3.2, in 2003; Tang et al., 2005), and Tokyo, Japan (approximately 1.6, in 1990–2002; Okuda et al., 2005), respectively. The S/N ratio is used as an index for the conditions of substance transport from the Asian continent (Tsuruta, 1989; Takahashi and Fujita, 2000; Toyama et al., 2007). As indicated in the figure, for Sites 1–3 (close to the Sea of Japan coast), the samples are distributed between the lines showing S/N ratios in Tokyo (1.6) and Beijing (3.2), which shows that the transport of substances from the Asian continent to these areas is particularly prominent. Figure 6 shows the relationship between the S/N ratio and the distance from the coast of the Sea of Japan. The ratio of the NO3– concentration gradually increases from the coastal area to inland, and at Sites 4 and 5, most of samples are distributed at approximately 1.0–1.5, which is lower than the Tokyo value. The S/N ratio based on Long-range transportation and deposition of chemicals in the Northern Japan Alps 687 Fig. 4. Estimated corresponding peaks (groups) between each of the sites. 688 K. Toyama et al. Fig. 6. Relationship between the ratio of non-sea-salt (nss-) SO42– and NO3– (the S/N ratio) and the distance from the coast of the Sea of Japan. Fig. 5. Non-sea-salt (nss-) SO 42– versus NO3– plot of the snow samples. The lines showing the SO 42–/NO3– ratios in precipitation recordings taken at Beijing, China (Tang et al., 2005), and Tokyo, Japan (Okuda et al., 2005), are also shown. observations of wet deposited chemical components between 1997 and 2000 in Matsumoto City was 1.0–2.0 with an average of 1.6 (Suzuki and Shirohada, 2006). These values correspond to the S/N ratios detected at Sites 4 and 5, which are close to Matsumoto. However, at Site 6, which is farthest from the coast, many samples showed levels distributed between the Tokyo and Beijing observations. Additionally, whereas the average S/N ratio values at Site 1 (2.8)–Site 3 (2.3) lie between those for Tokyo (1.6) and Beijing (3.2), those at Site 4 (1.1) and Site 5 (0.8) are lower than those in Tokyo, and that at Site 6 (1.8) is slightly higher, thus suggesting transport from the Asian continent. Therefore, Figs. 5 and 6 reveal that even for inland sites exceeding elevations of 2100–2200 m, substance transport is indicated from the Asian continent. DEPOSITION CONDITIONS FOR THE C HEMICAL COMPONENTS Figure 7 shows the deposition amount of each component along with distances from the coast of the Sea of Japan, and Table 2 shows the total deposition amounts at each of the sites. Overall, deposition amounts tended to decline at the sites farther inland in a noticeable trend. More specifically, the acidic contaminant nss-SO 4 2– , which is carried from the Asian continent, declined exponentially from the vicinity of the coast (Site 1, 2.24 g/m2) to the Northern Japan Alps mountain range (Site 3, 1.07 g/m2), with a deposition amount inland (Site 6, 0.33 g/m2) on the order of one-seventh that observed on the coast. It is known that SO42– concentrations in snow decrease exponentially with increasing distance from seaside to inland areas (Inoue et al., 1985; Ueno, 1993; Suzuki et al., 2012). However, most previous studies were based on observations of new surface snow caused by precipitation in a single period. Honoki et al. (2007) compared SO42– concentration in snow at 10 locations in the Hokuriku district of central Japan by using snow core boring and bulk sampling collection methods. They recorded the same tendency of decreasing SO42– concentrations as that observed in results based on new snow samples. In the present study, the exponential decrease of SO42– in snow was observed during the entire winter season and in large-scale spatial distributions from the Sea of Japan coast to the Pacific side of central Japan. Although NO3– was also reduced from the coastal area (Site 1, 1.14 g/m2) to inland (Site 6, 0.21 g/m2), the rate of reduction was fairly mild. However, the total values were likely affected by contributions from within the country that were absorbed into the air parcel as it was being transported. This observation is consistent with the decreasing trend of the S/N ratio toward inland, as was discussed in Section “Transport Conditions for Acidic Contaminants”. Because the addition of Na+, which originates in sea salt, during the transportation process was insignificant, the coastal area (Site 1, 3.72 g/m2) and the inland (Site 6, 0.07 g/m2) showed differences in Na+ distribution amounts of nearly 50-fold. The exponential decrease of sea salt component concentrations in precipitation with increasing distance from seaside to inland has also been reported in other studies (Tsunogai, 1975; Inoue et al., 1985; Long-range transportation and deposition of chemicals in the Northern Japan Alps 689 Fig. 7. Deposition amounts of typical chemical components such as Na+, Ca 2+, SO42–, and NO3– with distance from the coast of the Sea of Japan. Suzuki et al., 2012). However, Ueno (1993) determined that in some cases, sea salt components do not decrease exponentially as the air travels inland. Tsunogai (1975) reported that concentration levels decreased at a rate of approximately half per 20 km, which is nearly consistent with the results of this study. Essentially, nss-Ca 2+ levels declined somewhat while moving inland from the coast; however, deposition amounts still hovered at approximately 0.1–0.4 g/m2, and no significant site-based differences were observed. Inoue et al. (1985) and Ueno (1993) also reported that the decreasing trend of Ca 2+ did not parallel SO42– and Na+ values, which was attributed by Inoue et al. (1985) to the contribution from substances originating from the Asian continent. nss-Ca2+, it should be noted, is the primary component of yellow sand known as KOSA, which always exists as background KOSA in the atmosphere (Iwasaka et al., 1988), and is considered as the nuclei of snow crystals (Kumai, 1951; Ishizaka, 1973). Because nss-Ca 2+ is supplied on a regular basis at all of the sites, deposition amounts should not significantly differ. CONCLUSIONS In this study, the snow cover at six sites was continuously sampled over roughly the same period of time during a single winter season. Sample sites ranged from a 690 K. Toyama et al. Table 2. Deposition amounts of typical chemical components such as Na+, Ca2+, SO 42–, and NO3– contained in the snow samples obtained at each site Distance from the Sea of Japan Na + nss-Ca 2 + 1 2 3 4 5 6 21 48 100 118 143 162 nss-SO4 2 – (g/m2 ) (km) Site Site Site Site Site Site NO3 – 3.72 2.21 0.33 0.23 0.14 0.07 0.20 0.26 0.16 0.40 0.13 0.07 1.14 0.98 0.72 0.65 0.43 0.21 2.24 1.63 1.07 0.52 0.24 0.33 location close to Iou-zen near the coast of the Sea of Japan to Yatsuga-take, which is farther inland. Samples were obtained from snow deposits at the ground level up to the snow surface, and the chemical components contained therein were analyzed. After making comparisons between the various sites, the following findings related to the transport of substances were noted: i. We showed that the spatial distribution of chemical component concentrations in the snow cover was high at the sites on the upwind side of the wind, which is northwest relative to the Northern Japan Alps, and low on the downwind side. Additionally, we revealed that chemical substances suspended in the air precipitate out with the falling snow and thus decrease in concentration as air masses move downwind. ii. Chemical components concentrations vary at each of the sites. Chemical substances that are brought in with precipitation due to advection in the same clouds are transported from the Sea of Japan coastal area to inland. iii. In the Northern Japan Alps in winter, beginning with SO42–, acidic contaminants are deposited together with the snowfall. Much of these contaminants originate from the northeastern part of the Asian continent, such as northern China. iv. The concentration of SO42–, much of which originates from the Asian continent, reduces exponentially as the air mass moves inland; however, such reduction is not as remarkable for NO3–. Portions of this contaminant originate domestically and presumable supplement those already present in air masses as they travel. Therefore, much of the acidic substances deposited in the mountainous areas close to the Sea of Japan are transported from the Asian continent, whereas the contribution from acidic substances originating domestically is somewhat more pronounced in inland regions. This paper has introduced a chemical study, carried out by the authors, of the snow cover in the mountainous regions of the Northern Japan Alps and has clarified the previously little-known processes of extensive transport and deposition of chemical substances that occur throughout mountainous areas. However, the full nature of the burden imposed on the environment of mountainous regions by acidic contaminants such as SO42– and NO3–, for example, has yet to be understood. Additionally, the combination of detailed dating of the snow layers (such as the ratio of oxygen and hydrogen isotope; Toyama et al., 2005) with the corresponding chemical analyses of snow may remarkably contribute to investigations into the long-range transportation of anthropogenic contaminants from the Asian continent. In the East Asia region across from the Sea of Japan, as the source origin of such contaminants as SO42–, rapid economic development that continues unabated; therefore, the increasingly important phenomenon of cross-border pollution from such regions will need to be scrutinized in more detail in the future. Concerning the snow cover in mountainous regions, various studies reporting that chemical substances are transported in the winter air include the data required to solve several issues introduced in the present study. Examining the types of substances being transported across the Sea of Japan from the Asian continent, for example, and not limiting our discussion to simply explaining the environment in these mountainous regions, will provide extremely important basic data for use in elucidating the environment encircling the Sea of Japan. Acknowledgments—The authors wish to thank to the members of Laboratory of Environmental Geochemistry and the Laboratory of Glaciology of the University of Toyama for their assistance with the snow observations and collections under the severe weather conditions in the Northern Japan Alps mountain area. We also thank two anonymous reviewers, whose suggestions helped to improve our presentation of the data and the manuscript. This research was partially supported by the 4000 m environmental research project in the University of Toyama, and the water circulation study of Uozu City, Toyama Prefecture. One of the authors, Prof. Satake of the University of Toyama, passed away on November 22, 2009. We would like to offer our deepest condolences. REFERENCES Akata, N., Yanagisawa, F., Motoyama, R., Kawabata, A. and Ueda, A. (2002) Sulfur Isotope Ratios of Non-Sea Salt Sulfate in Wet Deposits in Japan. Seppyo, 64, 173–184 (in Japanese with English abstract). Honoki, H., Watanabe, K., Iida, H., Kawada, K. and Hayakawa, K. (2007) Deposition analysis of non-sea-salt sulfate and nitrate along to the northwest winter monsoon in Hokuriku district by a snow boring core and bulk samples. Bull. Glaciological Res. 24, 23–28. Inoue, J., Okuyama, K., Watanabe, O. and Fusimi, H. (1985) The mountain snowfall in Chugoku district, west Japan. Seppyo, 47, 97–104 (in Japanese with English abstract). Ishizaka, Y. (1973) On materials of solid particles contained in snow and rain water: Part 2. J. Meteorol. Soc. Japan 51, 325–336. Iwasaka, Y., Yamato, M., Imasu, R. and Ono, A. (1988) Transport of Asian dust (KOSA) particles: importance of weak Kosa events on the geochemical cycle of soil particles. Tellus 40B, 494–503. Japan Meteorological Agency (2013) Weather statistics information. Available at http://www.jma.go.jp/jma/menu/ report.html (in Japanese). Kido, M., Osada, K., Matsunaga, K. and Iwasaka, Y. (2001) Temporal change in ammonium/sulfate ratios for free tropospheric aerosols from early winter to spring at high elevation site in the Japanese Alps. J. Environ. Chem. 11, 33–41. Kumai, M. (1951) Electron-microscope study of snow-crystal nuclei. Journal of Atmospheric Sciences 8, 151–156. Mizoguchi, T., Zhang, J., Satake, H., Mukai, H., Murano, K. and Kawasaki, K. (2012) Lead and sulfur isotopic ratios in precipitation and their relations to trans-boundary atmospheric pollution. Atmos. Res. 104, 237–244. Okuda, T., Iwase, T., Ueda, H., Suda, Y., Tanaka, S., Dokiya, Y., Fushimi, K. and Hosoe, M. (2005) Long-term trend of chemical constituents in precipitation in Tokyo metropolitan area, Japan, from 1990 to 2002. Sci. Total Environ. 339, 127–141. Osada, K., Kido, M., Iida, H., Yabuki, H., Kohshima, S., Kawada, K. and Nakawo, M. (2000) Chemical stratigraphy of water soluble constituents in spring snow cover at Murododaira, Tateyama Mts., Japan. Seppyo, 62, 3–14 (in Japanese with English abstract). Long-range transportation and deposition of chemicals in the Northern Japan Alps 691 Osada, K., Ohara, T., Uno, I., Kido, M. and Iida, H. (2009) Impact of Chinese anthropogenic emissions on submicrometer aerosol concentration at Mt. Tateyama, Japan. Atmos. Chem. Phys. 9, 9111–9120. Satake, H. and Yamane, T. (1992) Deposition of non-sea salt sulfate observed at Toyama facing the Sea of Japan for the period of 1981–1991. Geochem. J. 26, 299–305. Suzuki, K. and Shirohada, M. (2006) Seasonal and temporal changes in the fluxes of major inorganic ions via wet and dry depositions, observed in Matsumoto, central Japan. Geochem. J. 40, 609–623. Suzuki, K., Yokoyama, K. and Ichiyanagi, H. (2012) Chemical survey of the snowpack in central Japan. Bull. Glaciological Res. 30, 25–32. Takahashi, A. and Fujita, S. (2000) Long-term trends in nitrate to non-seasalt sulfate ratio in precipitation collected in western Japan. Atmos. Environ. 34, 4551–4555. Tang, A., Zhuang, G., Wang, T., Yuan, H. and Sun, Y. (2005) The chemistry of precipitation and its relation to aerosol in Beijing. Atmos. Environ. 39, 3397–3406. Toyama, K., Suzuki, G., Satake, H., Kawada, K. and Iida, H. (2005) Dating of snow layers in the mountain area based on the variation of oxygen isotope ratio. Seppyo, 67, 319– 330 (in Japanese with English abstract). 692 K. Toyama et al. Toyama, K., Satake, H., Takashima, S., Matsuda, T., Tsuruta, M. and Kawada, K. (2007) Long-range transportation of contaminants from the Asian Continent to the Northern Japan Alps, recorded in snow cover on Mt. Nishi-Hodakadake. Bull. Glaciological Res. 24, 37–47. Tsunogai, S. (1975) Sea salt particles transported to the land. Tellus 27, 51–58. Tsuruta, H. (1989) Acid rain in East Asia. Kagaku 59(5), 305– 315 (in Japanese). Ueno, K. (1993) Spatial distribution of chemical constituents of the new snow cover from the coastal area to the mountain ranges of central Japan. Geographical Review of Japan 66A, 401–415 (in Japanese with English abstract). Watanabe, K., Iwai, A., Takeda, N. and Takebe, Y. (2005) Measurements of peroxide concentrations in precipitation in Toyama and in the snow pit at Murododaira, near the summit of Mt. Tateyama. Bull. Glaciological Res. 22, 51–55. Yuan, W. and Zhang, J. (2006) High correlations between Asian dust events and biological productivity in the western North Pacific. Geophys. Res. Lett. 33, L07603, doi:10.1029/ 2005GL025174. Zhang, J. and Liu, C.-Q. (2004) Major and rare earth elements in rainwaters from Japan and East China sea Natural and anthropogenic sources. Chem. Geol. 209, 315–326.
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