As a part of ABC-EAREX 2005 (Atmospheric Brown Cloud–East Asia Regional Experiment 2005), trace gases and compositions of PM2.5 were measured at Gosan supersite in Jeju Island during 13–30 March 2005. Aerosol constituents were determined continuously on site at 1-a intervals. The mean concentrations of gases were 56 ppbv for O3, 297 ppbv for CO, 3.2 ppbv for SO2, and 2.2 ppbv for NOx. For PM2.5, the average mass concentration was 27.3 μg/m3, and mean concentrations of nss-SO42−, organic carbon (OC), and elemental carbon (EC) were 3.34 μg/m3, 4.22 μg/m3, and 1.00 μg/m3, respectively. The simultaneous measurements of gaseous and aerosol species revealed that the composition of PM2.5 was mainly determined by anthropogenic plumes from nearby lands. Most of pollution plumes were associated with the passage of cold frontal systems, when all major species were greatly enhanced. Of these, two episodes were followed by dust incidents. In general, EC and nss-SO42− were well correlated with CO while OC was in good agreement with O3. Particularly, the variations of OC/EC ratios exhibited a maximum in the afternoon corresponding to the peak of O3/CO ratios, suggesting OC/EC as a marker representing the degree of chemical processing of fine aerosol. The ratios of OC/CO for all measurements fell between emission ratios of China and South Korea. For pollution episodes, the correlations of CO with nss-SO42− and EC were significant and their relative enhancement was suggested as an indicator to distinguish different types of pollution plumes.
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 Fine aerosols and their precursor gases are produced from a wide variety of anthropogenic sources. Fossil fuel and biomass burning contribute to aerosol productions by emitting primary aerosol particles such as dust, fly ash, and black carbon [Andreae and Crutzen, 1997]. Aerosols are also formed from precursor gases through photochemical reactions in the atmosphere, which are called secondary aerosols. Anthropogenic or secondary aerosols are typically in the submicrometer- to micrometer-size range and composed of numerous inorganic and organic species such as sulfates, carbonaceous aerosols, dust, and sea salt [Ramanathan et al., 2001a].
 Atmospheric fine aerosols have several important environmental effects. They affect the Earth's climate directly by scattering and absorbing radiation and indirectly by serving as nuclei for cloud droplet activation. However, there are still large uncertainties involved in estimating both the direct and indirect effects of aerosols on the radiative forcing. One of the major limitations is the lack of comprehensive observational data documenting the temporal and spatial distributions of key species. Therefore there have been efforts to understand physical, chemical, and radiative properties of aerosols, which are critical factors determining climate forcing of aerosols. In this context, several multinational experiments have been conducted such as ACE-Asia (Aerosol Characterization Experiment–Asia) and INDOEX (Indian Ocean Experiment) [Huebert et al., 2003; Ramanathan et al., 2001b]. One of the new findings from these previous studies was the link between air pollution and regional climate change, that is, the large loading of aerosols mainly from anthropogenic sources impacted on radiative forcing through their direct and indirect effects. To elucidate this connection better, ABC (Atmospheric Brown Cloud) program has recently brought forth, particularly focused on Asian regions, where a rapid economic development has resulted in environmental problems such as air pollution (http://www-abc-asia.ucsd.edu).
 The northeast Asia has been lately under the heavy influence of greenhouse and pollution gases and aerosols from highly populated regions including fast industrializing China and India, which was clearly shown from TRACE-P (Transport and Chemical Evolution over the Pacific) mission [Crawford et al., 2003]. The TRACE-P observations confirmed that cold fronts sweeping across East Asia and the associated warm conveyor belts were the dominant pathway for Asian outflow to the Pacific in spring [Jacob et al., 2003]. From the results of ACE-Asia experiment deployed in the same period of TRACE-P, it was also evident that Asian aerosols had a wide range of physical and optical properties, depending on the mixture of mineral dust with pollutants such as black carbon, sulfates, nitrate, and organics [Huebert et al., 2003]. From these previous studies, much progress has been made in understanding on basic properties of aerosol. Nonetheless, the distributions and budgets of many important aerosol constituents as well as their precursor are poorly characterized yet.
 Particularly, aerosols in northeast Asia have complicated structure: for example, mineral dust aerosols originating from the desert regions of China mixed with anthropogenic aerosols containing various carbonaceous compounds and inorganic ions, predominantly sulfate. Following ABC Maldives Monsoon Experiment (APMEX), therefore, the ABC East Asian Regional Experiment 2005 (EAREX 2005) was borne to investigate basic properties of fine aerosols over the East Asian region in spring (http://www-abc-asia.ucsd.edu/fieldcampaigns.htm). They are two regional experiments set for the first phase of the ABC project to delineate the regional aspects of the effects and to compare the results from instruments used by different groups.
 Major goals of ABC-EAREX are twofold: (1) to characterize differences and uncertainties of in situ aerosol measurements used for the ABC experiment by comparing simultaneous measurements and (2) to characterize properties of aerosols and precursor gases to identify key processes of aerosol formation and removal in the Asian outflow regime. In this context, major constituents of fine aerosols and precursor gases were determined at Gosan in Jeju Island during the ABC-EAREX 2005 intensive field experiment [e.g., Wong et al., 2007]. On the basis of measurement results, this paper described the compositions and distributions of fine aerosols and gaseous precursors, elucidated atmospheric processes controlling those chemical characteristics, and identified different source signatures.
 Experiment was conducted at Gosan in Jeju Island during March-April 2005 (Figure 1). Gosan station (33.17°N, 126.10°E, 70 m ASL) not only served as a base for ACE-Asia experiment in 2001, but also was designated as one of the ABC superstations. It has been considered as an ideal location to monitor Asian outflows and assess their impact on air quality over the northern Pacific [Carmichael et al., 1996, 1997; Chen et al., 1997]. Detailed description about ABC-EAREX 2005 and Gosan station will be found in this special issue.
 In this study, the concentrations of major gaseous and aerosol constituents were measured during 13–30 March 2005: O3, CO, NOx, and SO2 for gas species and soluble inorganic ions, organic carbon (OC), elemental carbon (EC), and mass concentrations of PM2.5 for aerosol. As soluble ions, 8 species were determined including SO42−, NO3−, Cl−, NH4+, K+, Na+, Ca2+, and Mg2+.
 The water-soluble inorganic ions were measured by URG-9000 Series Ambient Ion Monitor (URG, USA). Ambient air was collected through a PM2.5 sharp-cut cyclone and passed through a liquid diffusion denuder, where interfering acid gases were removed. Then, air stream entered saturation chamber for the growth of particles. Theses enlarged particles were collected by an inertial particle separator and stored in a sample collector before being injected into the ion detector. All ionic species were quantified every hour with detection limits of 0.02 μg/m3.
 Particulate OC and EC concentrations were automatically determined every hour using thermal-optical transmission (TOT) semicontinuous carbon analyzer (Sunset Laboratory, USA). For detailed procedure regarding temperatures and dwelling time, the National Institute of Occupational Safety and Health (NIOSH) method 5040 was followed (J. S. Han et al., Characteristics of fine carbonaceous aerosols at Gosan background site during ABC-EAREX 2005, submitted to Journal of Geophysical Research, 2007). The mass concentration of PM2.5 was measured every hour by Anderson FH-62 using β-ray absorption method.
 The concentrations of O3, NOx, SO2, and CO were measured by Themo Environmental Instrument 49C, 42C, 43C, and 48C, respectively (Thermo Inc., USA). One of the main purposes of ABC-EAREX 2005 was to intercompare and calibrate instruments used for long-term measurements by different groups. Hence ozone analyzer (TEI 49C) was calibrated against an Ozone Standard Reference Photometer of National Institute of Environmental Research (NIER) prior to field experiment. A special care was exercised for CO measurement to correct the drift of background. For this purpose, zero air was run for 10 min every hour alternatively with ambient samples. For O3 and CO, the ambient concentrations measured by several groups were compared on site. Detailed procedure and results about intercomparison is given by Tanimoto et al. [2007a, 2007b]. All instruments were remotely controlled and data were collected every 10 min using LabView.
 Meteorological parameters such as temperature, relative humidity, wind speed and direction, and precipitation, were measured at Gosan and shared by all participants in ABC-EAREX 2005.
3. Results and Discussion
 The measurement results for the whole experiment are shown in Figure 2, in which all measurements were hourly averaged. Most of gas and aerosol species were noticeably enhanced in several events. Throughout the campaign, two dust events accompanied by pollution plumes were observed during 17–18 and 28–29 March. There was another incident identified as an anthropogenic plume on the 22–23 March that was not affected by dust storm. These three episodes shaded in Figure 2, were all associated with frontal passages, during which both gas and aerosol concentrations were remarkably enhanced. In this study, it is noteworthy that dust plumes were clearly distinguished from pollution plumes by Ca2+ concentrations measured every hour. In addition to these major events, concentrations of major species were shown to be elevated by the influence of nearby continents on 15–16 and 21 March, even though these were not accompanied with frontal system. Thus the chemical characteristics of aerosols during the ABC-EAREX 2005 were mainly determined by these events. During the whole course of experiment from 13 to 30 March, the mean concentrations of major species were 56 ppbv for O3, 297 ppbv for CO, 3.2 ppbv for SO2 and 2.2 ppbv for NOx. The average mass concentration of PM2.5 was 27.3 μg/m3. Among PM2.5 constituents, OC and nss-SO42− were the most abundant, of which means were 4.22 μg/m3 and 3.34 μg/m3, respectively. Ammonium and nitrate concentrations were less than that of nss-SO42− and their mean concentrations were 1.38 μg/m3 and 1.14 μg/m3, respectively. In addition, the mean of EC concentrations was 1.00 μg/m3, which was about a factor of four lower than that of OC. Other soluble ions such as Na+, Cl−, Ca2+, Mg2+, sea-salt SO42−, and K+ were below 1.00 μg/m3 on average.
3.1. PM 2.5 Chemical Characteristics
 To examine the general characteristics of aerosol compositions during the ABC-EAREX 2005, aerosol constitutions were divided into four groups: soluble ions, organic matter (OM), EC, and the unidentified. Soluble ions include SO42−, NO3−, NH4+, Na+, Cl−, K+, Ca2+, and Mg2+. The OM content was estimated to be OC concentration times 2.1, which was a conversion factor for nonurban aerosols [Turpin and Lim, 2001]. The “unidentified” is the rest of PM2.5 that was not included in three categories. The concentrations of these four groups were daily averaged from 0 to 23 h and presented in Figure 3a with PM2.5 mass concentrations. The daily mean of PM2.5 varied from 12.56 to 56.50 μg/m3 and represented well episodic events associated with pollution and dust plumes. The amounts of OM and soluble ions were comparable and the unidentified varied greatly day by day. In general, the greater PM2.5 mass was, the greater amounts were left unidentified. To compare the relative importance of these constituents, the mass fractions of each subgroup against PM2.5 mass were calculated and shown in Figure 3b. The average mass fractions of soluble ions, OM, EC, and the unidentified were 31.3%, 39.7%, 3.9%, and 25.1%, respectively. The soluble ions and organic matters were about equal in contribution to PM2.5 mass concentrations. Since OM contents was driven from OC concentrations using the conversion factor, the fraction of OM to PM2.5 shown in Figure 3b had better be considered as an approximation.
 The variations of PM2.5 mass and their compositions were observed to be closely related to meteorological conditions. If averaged daily, meteorological parameters including temperature, relative humidity, wind speed, and the amount of precipitation exhibited a characteristic variation during the three weeks of experiment, reflecting the passage of cold fronts (Figure 3c). Details about meteorological setting during the campaign can be found in this issue. In Figure 3, PM2.5 and meteorological parameters show some similarity in daily variations, which exemplified the role of frontal system in altering chemical constituents of the atmosphere by carrying out continental outflows.
 PM2.5 mass reached the maximum on 24 March when wind speed was very high and its hourly mean went up to about 30 m/s. While concentrations of precursor gases or other major aerosol constituents stayed low, Cl− and Na+ concentrations were noticeably enhanced. Accordingly, the increase in unknown fraction was apparent, leaving about a half of PM2.5 unidentified. Other high concentrations of PM2.5 were mostly associated with either pollution or dust events with high unidentified fractions. The unknown portions were significantly reduced on 19, 20, 27, and 30 March with low PM2.5 concentrations and low wind speed. In contrast, OM fractions were sharply increased.
 Since trace metal and silicate contents were not measured in this study, a considerable fraction of the unidentified constituents was possibly to be metals and silica. The major source of trace elements is the Earth's crust and accordingly, their concentrations in aerosols used to be highly elevated during dust events [e.g., Choi et al., 2001]. In their study, metal content was as high as 17% of the PM10 mass for heavy dust incident, even though Si, the most abundant crustal material, was not counted. As the median size of dust particles are about 2–3 μm [Chun et al., 2001], mineral aerosols are thought to have less significant influence on mass concentrations of PM2.5 than PM10. During this experiment, the increase in PM2.5 mass was more pronounced in pollution plumes, whereas PM10 concentrations were much higher in association with dust plumes [this issue]. In recent study conducted in Hong Kong area [Ho et al., 2006], the contribution of crustal elements to PM2.5 was not negligible, even though their relative amount were higher in PM10 than in PM2.5. Taking unmeasured trace metals into account, the unidentified fraction are in reasonable agreement with other studies [Ho et al., 2006; Rees et al., 2004]. It is also worthy to mention that the fraction of soluble ions were remarkably decreased on 18, 24, and 29 March, when the wind speeds were very high or Asian dust events were observed. These results illustrated that the chemical composition of fine aerosols were tightly couple with meteorological conditions.
 Since aerosol compositions were determined hourly, their diurnal variations were available to investigate characteristic changes of aerosol composition by time, particularly between day and night. Daily variations of major species and meteorological parameters are shown in Figure 4. While PM2.5 mass reached the maximum in the afternoon, its major constituents showed slightly different patterns in diurnal variations (Figure 4a). The variation of OC was in phase with that of PM2.5. On the other hand, both sulfate ion and EC were enhanced at night. These results highlight the role of OC in determining PM2.5 mass concentrations as the most abundant constituent. It is also interesting to compare diurnal patterns of gases with those of aerosol species (Figure 4b). While variations of both SO42− and EC were similar to that of CO with maximum concentrations at night, variations of O3 and OC looked alike with afternoon peaks. It is noteworthy that the enhancement of SO42− and OC was found in different times, which could have significance in the generation of fine aerosols of the research region. In addition, SO2 and CO showed higher concentrations at night. For NOx, concentrations were increased in the morning that was typical for vehicle source, along with evening peak. Particularly, the concentrations of gases except O3 were enhanced at night, which was concomitant with the shift of wind direction (Figure 4c) and increase in PM2.5 mass and all aerosol species including SO42− and EC. It signifies the importance of transport to controlling PM2.5 mass concentrations.
3.2. PM2.5 Chemical Tracers
Figure 4 illuminated the relationship among precursor gases and aerosol species. For example, nss-sulfate and OC track the variations of CO and O3, respectively. Hence the correlations between compounds including aerosol and gas were investigated. Any good correlation could be useful to identify source or to trace transport path, on which chemical compositions of fine aerosols were largely dependent. CO has been most widely used as a tracer for ozone production in pollution plumes owing to its role as a precursor and relatively long lifetime in the atmosphere. In this study, CO was well correlated with EC for all measurements (Figure 5), which was understood in terms of common source of combustion processes [de Laat et al., 2001]. EC and CO were often found to covary [Chen et al., 2002; Lim and Turpin, 2002]. One of the striking results of this study is a good correlation of a major secondary aerosol such as nss-SO42− with CO, which was comparable to that of EC with CO. It implies that CO can be used to trace the formation of secondary aerosols in anthropogenic plumes.
 In previous study, the ratio of OC to CO was suggested as a useful tracer to identify different sources for fine aerosols [Maria et al., 2003]. The relationship between OC and CO from this study was illustrated in Figure 6, where OC was plotted against CO. Since the lifetime of OC is much shorter than CO, the ratio of CO/OC would decrease as the formation of secondary aerosols, while increasing with being transported away from the source. Although these two processes affect the ratio in opposite directions, the CO/OC ratios were useful to distinguish different sources of fine aerosols over the northeast Asia [Maria et al., 2003]. In this study the average ratio of CO (ppbv) to OC (μg/m3) was estimated to be 35 from the linear regression. Although the correlation of OC with CO was not as good as those of EC or nss-SO42− with CO, the emission ratios of OC to CO are better distinguished among adjacent countries. On the basis of emission inventories of Asia in the year of 2000 [Streets et al., 2003], the ratio of CO to OC is 27 for China and 81 for South Korea, which are presented as dotted lines in Figure 6. All data are within the envelope of these two lines, while the majority of data are scattered along the line of CO/OC ratio for China. Accordingly, the high OC associated with relatively low CO shown in the lower right of Figure 6 were obtained in air transported from the southern part of China. However, the extremely high CO values shown in the upper right near the line representing Korean emission were observed in pollution plumes carried by cold front system from the northwest. These facts address the limitation of applying averaged ratios to single out specific source, even though overall, the measured ratios of CO/OC conveyed the signatures from possible sources of fine aerosols. In addition, it is worthy to mention that the background concentration of surface CO during the ABC-EAREX2005 was about 144 ppbv, estimated from the linear fit shown in Figure 6, which was higher than ∼100 ppbv of the estimated from airborne measurements during the ACE-Asia [Maria et al., 2003].
 As a major light absorbing component of the atmospheric aerosols, EC is known to be formed during the combustion of hydrocarbons [Jones and Harrison, 2005; Mader et al., 2002]. OC may derive from a wide variety of sources; combustion processes including fossil fuel combustion and biomass burning, and natural sources such as ocean and terrestrial vegetation [Duce et al., 1983; Matsumoto et al., 2003]. Several studies have used measurements of the OC to EC slope as an indicator of aerosol source types and evidence of secondary organic aerosol formation [Kadowaki, 1990; Kim et al., 2000; Lim and Turpin, 2002]. These analyses utilize the fact that EC is produced only in combustion processes as a primary pollutant while OC is both emitted from sources and produced by atmospheric reactions from gaseous precursors.
 As the first data set obtained at Gosan station, the average OC and EC concentrations of PM2.5 were 4.22 μg/m3 and 1.00 μg/m3, respectively. During ACE-Asia program conducted in March-April 2001, OC and EC contents were measured for TSP (total suspended particles) at Gosan station and for PM1.0 on the ship, which are available for comparison. For TSP collected at Gosan, the mean OC and EC concentrations were 7.00 μg/m3 and 1.29 μg/m3, respectively [Simoneit et al., 2004]. In shipboard measurement, 4.00 μg/m3 of OC and 1.32 μg/m3 of EC were observed near Korea in the East Sea [Lim et al., 2003]. All existing measurements resulted in higher OC/EC ratios than the assessed from emission inventories, which are 1.27 for South Korea and 3.23 for China [Streets et al., 2003].
 It was already shown in Figure 4 that there was similarity found between distributions of OC and O3. If daily averaged, the ratios of OC to EC were in good agreement with O3/CO ratios for both daily and diurnal variations (Figure 7). As the latter represents the extent of atmospheric oxidation in gaseous composition, the former could be the one for aerosol composition. Although the diurnal trend of OC/EC was not as smooth as that of O3/CO, their maximum values were found in the afternoon. These findings imply the formation of organic carbons from chemical transformation, as reported from previous studies [Lim and Turpin, 2002; Simoneit et al., 2004]. The OC/EC ratio was very high on 27 March, which was mostly caused by very low EC concentrations with the minimum PM2.5 mass concentration.
3.3. High PM2.5 Episodes
 During the ABC-EAREX 2005, several cold fronts passed by Gosan station, which not only was clearly depicted in the variations of meteorological parameters (Figure 3c), but also had a great influence on the compositions of major chemical constituents (Figure 3a). This frontal passage is a common meteorological feature over the northeast Asia in spring and effective in exporting Asian pollutants as well as mineral dust to the north Pacific. In this section, the high-concentration episodes associated with frontal system were examined in detail. The first case is a pollution plume coupled with Asian dust observed during 17–18 March. In about 10 d, a similar but rather weak pollution plus dust incident took place on 28–29 March. Between these two, another pollution plume that was not accompanied by dust storm was detected during 22–23 March. For three pollution and two dust plumes during the high-concentration episodes, the daily means of key species were summarized in Table 1. It shows that the relative enhancement of major species varied among plumes, which could have resulted from different source, transport path, and chemical processing of air masses.
Table 1. Measurement Summary for High Concentration Episodesa
Aerosol species are given in μg/m3, and gas species are given in ppbv.
Slope of the linear regression fittings for three episodes (see Figure 9).
Ratios of mean concentrations for each event.
17 Mar (24 h)
18 Mar (24 h)
22–23 Mar (48 h)
28 Mar (24 h)
29 Mar (24 h)
 First, to get a hint of the origin and transport path of plumes, the trajectory analysis was performed using HYSPLIT-4 model that was developed by the National Oceanic and Atmospheric Administration (http://www.arl.noaa.gov/ready/hysplit4.html). For five plumes during three episodes, backward trajectories arriving at 1000 m above sea level were calculated for 5 d, assuming that air moved along the isentropic surface. The results are presented in Figure 8. For the first and third episodes, pollution (1 and 4) and subsequent dust (2 and 5) plumes were distinguished in trajectories. The air carrying large amount of pollutants came from the northwest, whereas Asian dust was delivered directly from the north.
 In this study, the dust-containing plume was unambiguously identified by high Ca2+ concentrations (Figure 2 and Table 1). All the other major species were raised ahead of Ca2+ only in pollution plumes. Particularly on 17 March, the enhancement of both gas and aerosol species were the most pronounced (Table 1). For the pollution event detected on 23 March, the air originated from the northern part of China but arrived at Gosan after passing by the Korean Peninsular. Hence Korean influence was likely superimposed on preexisting plume from China. Particularly, this episode was characterized by high EC and OC concentrations in daily mean (Table 1).
 These plumes were also distinguished by relative enhancement of nss-SO42− and EC to CO. Their correlations were much improved for individual pollution episode (Figure 9). The enhancement ratio of ΔSO42−/ΔCO and ΔEC/ΔCO was obtained from linear regression and given on the plot. In dust plumes, on the other hand, no significant relationship was found between nss-SO42− and CO or EC and CO. Moreover, the concentrations of other species than Ca2+ were lower than mean values of the whole measurements (Table 1). Hence the effect of dust was thought to be relatively less important in determining chemical compositions of PM2.5. Among three pollution episodes, both Δnss-SO42−/ΔCO and ΔEC/ΔCO were greatest on 28 March but least on 17 March. During 22–23 March, ΔEC/ΔCO was comparable to that of 28 March. Considering the trajectories and the nature of chemicals, it is likely that ΔEC/ΔCO tended to be modified by sources, while Δnss-SO42−/ΔCO reflected the extent of chemical processing during the transport. In addition, the ratios of mean concentrations for key species, including NO3−/NOx, nss-SO42−/SO2, and OC/EC were particularly high on 28 March (Table 1), when the fraction of soluble ions was the highest (Figure 3b). These results demonstrate that the chemical characters of fine aerosols were well distinguished by relative enhancement of major species including precursor gases and aerosol constituents. Thus these ratios can be useful indicators to identify sources and processes determining the chemical properties of fine aerosols.
4. Summary and Conclusions
 Concentrations of trace gases and compositions of fine aerosol less than 2.5 μm were determined at Gosan ABC superstation during 13–30 March 2005. All major species were greatly increased during several pollution episodes, which were driven by cold front systems. Of these, two episodes were followed by dust plumes, which were clearly differentiated by sharp increase in Ca2+ concentrations. Other than Ca2+, no significant enhancement was observed in major chemical constituents including PM2.5 mass concentrations during dust events. The chemical compositions of PM2.5 were, therefore, mainly determined by anthropogenic plumes. In PM2.5, OC was the most abundant and concomitantly elevated with PM2.5 mass in the afternoon. Other major aerosol species such as nss-SO42− and EC were raised at night. Overall, the distributions of EC and nss-SO42− were compatible with that of CO, but OC tended to vary in accordance with O3. It was likely due to the common source for the former, but for the latter it resulted from common process experienced in the atmosphere. Thus nss-SO42− and OC showed different behavior as secondary aerosols. The ratio of OC to EC was in good agreement with the ratio of O3/CO, particularly for diurnal variations, suggesting OC/EC ratio as an indicator representing the degree of atmospheric oxidation. Although the correlation of OC with CO was not great, the ratio of CO/OC was useful to compare sources of fine aerosols as a whole. The all measurements fell between emission ratios of China and South Korea. In individual pollution plume, both nss-SO42− and EC were enhanced almost linearly with CO. Hence their enhancement ratios can be a useful tracer to distinguish the type of pollution plumes according to their sources and history.
 This paper was published by the support of the Center for Atmospheric Sciences and Earthquake Research (CATER 2007-3204).