JOURNAL OF GEOPHYSICAL RESEARCH: ATMOSPHERES, VOL. 118, 3709–3722, doi:10.1002/jgrd.50317, 2013 Seasonal variations of black carbon observed at the remote mountain site Happo in Japan X. Liu,1,2 Y. Kondo,1 K. Ram,1,3 H. Matsui,1 K. Nakagomi,4 T. Ikeda,4 N. Oshima,5 R. L. Verma,1,6 N. Takegawa,7 M. Koike,1 and M. Kajino5 Received 6 December 2012; revised 26 February 2013; accepted 5 March 2013; published 13 May 2013. [1] The emission of black carbon (BC) from East Asia and its long-range transport strongly influence the mass concentration of BC (MBC) over the western Pacific. However, reliable and long-term BC data are still limited in this region, especially at elevated altitudes. In this study, we present accurate measurements of MBC using a continuous soot monitoring system at Happo, a remote mountain site at an altitude of about 1.8 km in Japan, from August 2007 to August 2009. The annual average MBC at Happo was about 0.26 0.18 (1s) mg m3. The monthly average MBC values exhibited similar seasonal variations during both years, with minimum values in winter. Around 40% of the air sampled at the site was of free tropospheric (FT) origin, with about 10% originating in North China (NC) origin, respectively. The MBC values for FT (0.24 mg m3) and NC (0.23 mg m3) air were representative of the MBC values (0.26 mg m3) at 1.8 km height in the western Pacific, which are strongly influenced by BC emissions in North China. The MBC values calculated using a regional-scale model reproduced well the MBC observed at Happo. The model predicted that BC transported from northern China alone contributed ~53% to the measured MBC, consistent with trajectory analysis. The comparison of model-calculated and observed MBC values indicates that the minimum values of MBC in winter were caused by the suppressed upward transport of BC over the Asian continent. Biomass burning in Siberia substantially increased MBC in the spring of 2008. Citation: Liu, X., Y. Kondo, K. Ram, H. Matsui, K. Nakagomi, T. Ikeda, N. Oshima, R. L. Verma, N. Takegawa, M. Koike, and M. Kajino (2013), Seasonal variations of black carbon observed at the remote mountain site Happo in Japan, J. Geophys. Res. Atmos., 118, 3709–3722, doi:10.1002/jgrd.50317. 1. Introduction [2] Black carbon (BC) is produced from the incomplete combustion of fossil fuels and biofuels and from biomass burning (BB) emissions [Horvath, 1993]. BC strongly absorbs solar radiation at visible wavelengths and significantly contributes to radiative forcing [e.g., Hansen and Sato, 2001]. 1 Department of Earth and Planetary Science, Graduate School of Science, The University of Tokyo, Bunkyo, Tokyo, Japan. 2 Now at the School of Mathematics and Physics, Changzhou University, Changzhou, China. 3 School of Earth, Ocean and Climate Sciences, Indian Institute of Technology, Bhubaneswar, India. 4 Nagano Environmental Conservation Research Institute, Nagano, Japan. 5 Meteorological Research Institute, Tsukuba, Japan. 6 Regional Resources Center for Asia and the Pacific, Asian Institute of Technology, Klong Luang, Thailand. 7 Research Center for Advanced Science and Technology, The University of Tokyo, Tokyo, Japan. Corresponding author: Y. Kondo, Department of Earth and Planetary Science, Graduate School of Science, The University of Tokyo, Hongo 7-3-1, Bunkyo-ku, Tokyo 113-0033, Japan. ([email protected]) ©2013. American Geophysical Union. All Rights Reserved. 2169-897X/13/10.1002/jgrd.50317 The Intergovernmental Panel on Climate Change (IPCC) has estimated that the global mean clear-sky radiative forcing of BC is 0.23 0.25 W m2 [IPCC, 2007]. However, the estimate of radiative forcing by BC is highly uncertain partly due to insufficient data on the spatial and vertical distributions of BC mass concentrations (MBC), which can be used to validate model calculations. [3] East Asia is a major source region of BC aerosols [Streets et al., 2003; Ohara et al., 2007; Zhang et al., 2009] and contributes about 30% of the estimated global BC emissions [Bond et al., 2004]. Long-term ground-based measurements of MBC over the western Pacific have been made at Hedo [26.87 N, 128.26 E, ~60 m above sea level (asl)] on the Japanese island of Okinawa [Kondo et al., 2011a; Verma et al., 2011]. Using this data set and model calculations, Kondo et al. [2011a] evaluated the BC emission rate from China and found it to be close to that estimated by Zhang et al. [2009]. The MBC measured at Hedo was found to be strongly influenced by BC transported from China throughout the year, except for summer [Kondo et al., 2011a; Verma et al., 2011]. [4] Measurements of MBC from remote and high-altitude sites in the western Pacific are crucial to improving our understanding of the long-range transport of BC from continental Asia. Kondo et al. [2011a] discussed the 3709 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO 2. Measurement 2.1. Observational Site [7] The BC measurements were made at the Happo observatory in Nagano prefecture in Japan, which is one of the national acid deposition monitoring stations of the Japanese Ministry of the Environment. The station is located in the Hakuba Mountains (northern Japanese Alps), in the center of the main island of Japan, about 200 km northwest of Tokyo and 25 km south of the Sea of Japan (Figure 1). No significant effects of BC emissions in the vicinity of the sampling site were detected. The nearest city to the observational site, Shinano-omachi, with a population of about 30,000, is about 25 km away toward the south. The site was often influenced by free tropospheric (FT) air parcels. 3 NC 40 Happo 2 -1 KR JP 30 1 Hedo 20 BC (Gg year / grid) 50 Latitude (°N) measurements and the reliability of BC mass concentrations obtained during previous campaigns, including the Transport and Chemical Evolution over the Pacific (TRACE-P, 2001) mission [Jacob et al., 2003; Park et al., 2005] and the Asian-Pacific Regional Aerosol Characterization Experiment (ACE-Asia, 2001) [Uno et al., 2003]. The period of the measurement was too short for a quantitative understanding of the major sources and transport of BC in this region. In addition, the accuracy of the BC measured during ACE-Asia has not been fully quantified [e.g., Huebert and Charlson, 2000]. Aircraft measurements of BC, with improved accuracy, were recently made using a singleparticle soot photometer (SP2) instrument in spring 2009 during the Aerosol Radiative Forcing in East Asia (A-FORCE) campaign [Kondo et al., 2011a; Oshima et al., 2012]. Over the East China Sea, the average MBC values were about 0.5 mg m3 up to an altitude of 1.8 km and decreased sharply by about a factor of 10 at 3 km. The transport efficiency of BC (TEBC) from the East Asian region was also derived from the BC-carbon monoxide (CO) correlation, and it was found that TEBC in the free troposphere was strongly influenced by the precipitation amount that the sampled air masses experienced [Oshima et al., 2012]. [5] Considering the large spatiotemporal variability in MBC associated with emission and transport of BC from the East Asian region, long-term BC measurements at highaltitude sites are important. We made measurements of MBC at Happo (36.68 N and 137.80 E) in Japan at 1.8 km asl for two consecutive years (August 2007–August 2009). Earlier studies have suggested seasonal variability in the CO concentration at this site and downstream of the Asian continent. In fact, the site was strongly influenced by the transport of anthropogenic emissions in China and Korea and, occasionally, Siberian biomass burning events [Kato et al., 2002; Narita et al., 1999]. However, reliable longterm measurements of MBC are still limited at Happo and other locations in the western Pacific. [6] For the first time, we present accurate measurements of MBC for 2 years, i.e., 2007–2009, its seasonal and interannual variability, and the transport of BC aerosols from the Asian continent at this altitude in the western Pacific. The data on seasonal and interannual variability of MBC are interpreted using back trajectories. We quantify the influence of transport from source regions in East Asia and biomass burning on the MBC levels based on the model calculations. We also derive TEBC using the model. SC 0 10 100 120 140 Longitude (°E) Figure 1. Map of anthropogenic BC emissions over East Asia for the year 2006 with a spatial resolution of 0.5 0.5 [Zhang et al., 2009]. The regions of North China (NC), south China (SC), Korea (KR), and Japan (JP) defined in this study are shown with white boxes. The white circles are the locations of the measurement sites at Happo (137.80 E, 36.68 N) and Hedo (26.87 N, 128.26 E) in the western Pacific region. The gray lines show the flight tracks of the Aerosol Radiative Forcing in East Asia (A-FORCE) aircraft campaign [Oshima et al., 2012], conducted over the East China Sea in spring 2009. The air masses arriving at the site, including FT air, were under the influence of anthropogenic emissions in China and Korea throughout the year and, occasionally, Siberian biomass burning events in spring. Continuous measurements of MBC were made from August 2007 to August 2009. We analyzed the data for two springs (March–May), summers (June–August), falls (September–November), and winters (December–February). 2.2. Instrumentation [8] MBC in the fine mode (PM2.5, i.e., particles with aerodynamic diameter smaller than 2.5 mm) were measured using a filter-based absorption photometer, namely, a continuous soot monitoring system (COSMOS) [Miyazaki et al., 2008; Kondo et al., 2009, 2011b, 2012]. The instrument measures changes in the transmittance at 565 nm wavelength (l) across an automatically advancing quartz fiber filter tape. The changes in the transmittance are converted to MBC using the mass absorption cross section (MAC) by the following equation. MBC ¼ b0 ½ ffill =MAC (1) [9] Here b0 is the absorption coefficient directly measured by COSMOS, and ffill is the correction of the magnification of absorption by multiple scattering in the filter media. Therefore, the ffill/MAC ratio is of upmost importance, not the absolute value of MAC in determining MBC, because the MAC value depends on the scheme used for ffill [Kondo et al., 2011b]. We determined the ffill/MAC ratio and MAC (by specifying ffill as a function of filter transmittance) by comparison with a single-particle soot photometer (SP2) 3710 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO [12] Figure 2a shows the trajectories of the air masses arriving at Happo for each day during the spring and summer of 2008. The majority of the air masses passed over the Asian continent, mostly over Mongolia and northwestern China in spring, winter, and fall, driven by the Siberian high, persistent during the winter monsoon period. In summer, the North Pacific high-pressure system was much stronger, and the Siberian high was reversed to a low-pressure system, typical of the summer monsoon in East Asia. Associated with the summer monsoon, cleaner Pacific air was transported to Happo more frequently near the surface. [13] We classified the air mass types based on the residence time (RT) of an air mass in a given region as predicted by the trajectories. These regions are defined as North China (NC) (40 N–50 N, 100 E–130 E and 33 N–40 N, 100 E–123 E), south China (SC) (20 N–33 N, 100 E–123 E), Korea (KR) (33.5 N–40 N, 123 E–129.5 E), Japan (JP) (30 N–46 N, 130 E–147 E), marine (MA), and FT. We have used the same classifications as were used for the analysis of the BC data at Hedo [Verma et al., 2011]. The air masses were defined as NC, KR, SC, or JP if their back trajectories originated in the boundary layer (BL) of NC, KR, SC, or JP, respectively. In this study, we defined the top level of the BL over the Asian continent as the 700 hPa atmospheric pressure level (about 3.0 km). The air masses were classified as MA if their back trajectories did not pass over the domain areas of NC, KR, SC, or JP. Similarly, the air masses were categorized as FT if their back trajectories traveled above the BL over the domain areas of NC, KR, and SC. The residence time has been calculated as the time spent by individual air based on the laser-induced incandescence technique and the thermal-optical transmittance (TOT) technique [Kondo et al., 2009, 2011b]. The stability of MAC (or, more correctly, the ffill/MAC ratio) is achieved by removing volatile aerosol components with the use of an inlet heated at 400 C, prior to the collection of BC particles on filters. The MBC values are given in units of mass per unit volume of air (mg m3) at standard temperature and pressure (273.15 K and 1013 hPa). [10] The accuracy of the MBC measured by COSMOS has been fully estimated to be about 10%, by comparison with that measured by SP2 and TOT instruments [Kondo et al., 2009, 2011a; Kanaya et al., 2013]. We used 1 h average BC data for the present analysis. In addition to the BC data at Happo, we used the ground-based MBC data obtained at Hedo [Verma et al., 2011] and those obtained by the A-FORCE aircraft campaign conducted over the East China Sea in spring 2009 [Kondo et al., 2011a; Oshima et al., 2012]. The location of Hedo and the flight tracks of the A-FORCE campaign are also shown in Figure 1. 3. Origin of Air Masses [11] We calculated 5 day backward trajectories using the trajectory model of the National Institute of Polar Research [Tomikawa and Sato, 2005] driven by the pressure and wind field data from the National Center for Environmental Prediction-Final Analyses to study the transport patterns of air masses arriving at the observation site. Each trajectory started from 800 hPa at 12:00 local time (LT). (a) (b) FT 1000 900 50 800 40 700 Pressure(hPa) Latitude(°N) 60 600 30 500 20 80 100 120 140 160 Longitude(°E) Figure 2. Five day back trajectories of air masses for (a) spring and summer seasons of the year 2008 and (b) free tropospheric (FT) air masses during April 2008. Back trajectories were calculated starting at 800 hPa pressure altitude and 12:00 local time. The regions of North China (NC), south China (SC), Korea (KR), and Japan (JP) defined in this study are shown with red boxes (same as in Figure 1). 3711 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO masses in the respective regions. To ensure robustness in the analysis, we have used only data with RT > 24 h in the specified regions. Based on the criteria of RT (>24 h), SC air rarely reached Happo. [14] As can be seen in Figure 2a, air masses originating from NC often passed over the Korean region before reaching Happo. We calculated the Rf(NC) ratio of the residence time in NC to the total residence time in NC + KR. We defined KR for air masses with Rf(NC) < 0.2, Mixed (NC + KR) for 0.2 < Rf(NC) < 0.8, and NC for Rf(NC) 0.8. We follow this classification for NC, KR, and mixed (MX) type of air masses throughout this paper. The trajectories for FT air masses for April 2008 (Figure 2b), a typical example, show that FT air passed predominantly over the Asian continent, especially China. [15] Figure 3 shows the percentage (%) contribution of different air mass types during the observation period. Generally, the FT air masses dominated the total air masses reaching Happo, except for summer. The contribution of NC air was 9%–14% during the study period and was a minimum during summer and fall 2008 (Figure 3). If the air masses from KR and MX are considered to have been influenced by BC emissions in NC, the total fractions of air masses of NC origin increase to 35%–55%. The fractions of the Chinese air (NC + SC + MX + KR) are similar to the values of 47%–55% observed at Hedo [Verma et al., 2011]. 4. Model Calculations [16] We calculated MBC using the Community Multiscale Air Quality (CMAQ) three-dimensional model (version 4.7) [Byun and Ching, 1999; Binkowski and Roselle, 2003], combined with the source and process apportionment method (process, age, and source region chasing algorithm; PASCAL) [Matsui and Koike, 2012]. The meteorological inputs were calculated using the Weather Research and Forecasting model (version 3.1.1) [Skamarock et al., 2008]. The model calculations and emission inventories used in this study are the same as those described in detail by Matsui et al. (submitted). [17] The CMAQ-PASCAL calculation domain covers the entire North and East Asian region (60 – 180 E, 5 – 70 N) with a horizontal grid spacing of 81 km (140 90 grids) and 20 vertical layers from the surface to 100 hPa [Matsui and Koike, 2012; Matsui et al. (submitted)]. In this study, PASCAL is used to trace source regions and types of emissions in Asia to understand the observed variability of MBC at Happo. Source regions and types are defined in this study as anthropogenic sources in East Asia (5 N–50 N and 60 E–150 E), North China (>32 N), south China (<32 N), Korea, and Japan and biomass burning sources in Siberia and Kazakhstan (50 N–70 N and 60 E–180 E). However, the latitudinal division between North China and south China (32 N) was slightly different from that used for the trajectory analysis (33 N). [18] The CMAQ-PASCAL model was also used to calculate TEBC at Happo. TEBC values are defined in this study as the fraction of BC concentrations in the base simulation relative to those assuming no removal processes (i.e., sum of the base simulation and DDEP and WDEP tags: DDEP and WDEP are the loss amounts by dry and wet deposition processes, respectively, traced in PASCAL). TEBC values can be also calculated using derived MBC-CO correlations. These two definitions of TEBC are identical provided the MBC-CO correlation that is not influenced by wet deposition of BC is appropriately chosen. [19] We used the Asian anthropogenic emission inventory with a grid resolution of 0.5 0.5 in latitude and longitude Figure 3. Fractions of the air masses of different categories arriving at Happo in different seasons for the entire measurement period. For statistics, we included only air masses that spent at least 24 h (i.e., RT > 24 h) in a specified region. NC: North China, SC: south China, KR: Korea, MA: marine, FT: free troposphere. 3712 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO developed by Zhang et al. [2009] for the year 2006. We have also incorporated daily biomass burning (BB) emissions from fire counts (MOD14A1 and MYD14A1) and land use (MCD12Q1) data measured by Moderate Resolution Imaging Spectroradiometer (MODIS) satellites with predetermined values of combustion and emission factors [Reid et al., 2009; Chang and Song, 2010]. These BB emissions were evaluated in Matsui et al. (submitted) through comparison with other inventories of biomass burning emissions. [20] Figure 1 shows a map of the BC emission rate (Gg/yr/ grid) in East Asia using the emission estimates of Zhang et al. [2009] for the year 2006. BC emissions in East Asia (comprising China, Japan, and Korea) for the year 2006 were estimated to be about 1.90 Tg/yr, with most of the contribution (~95% or 1.81 Tg) coming from China alone [Zhang et al., 2009], as can be seen from Figure 1. The relative contributions from Japan and Korea to the total BC emissions over East Asia were about 3% and 2%, respectively. Most of the BC emissions in China are derived from industrial, vehicular, and coal-based emissions [Zhang et al., 2009]. However, a recent study has suggested that biomass burning (BB) emissions contribute ~13% of total BC aerosols in China [Kondo et al., 2011a]. 5. Results and Discussion 5.1. Temporal Variations of MBC [21] Figure 4 shows the variations of the daily average MBC at Happo during 2007–2009. On average, MBC was generally stable throughout the year, with an annual mean of 0.26 0.18 (1s; one standard deviation; SD) mg m3. There were large variations, however, especially in spring. The lower envelope of MBC underwent some seasonal variation, reaching a minimum in summer. Before further analysis of this data set, we assessed the possible effects of local BC emission sources on the observed MBC. [22] Figure 5 shows the diurnal variation of the average MBC values at Happo for July 2008 and January 2009. Unlike the prominent diurnal variability observed in MBC within the source regions of BC emissions [Kondo et al., 2006, 2012; Han et al., 2009; Verma et al., 2010], MBC values showed small diurnal variations at Happo. The MBC is anticipated to increase during the daytime after sunrise Figure 4. Time series plot of daily averaged MBC during the measurement period (August 2007–August 2009). The vertical dashed line is used to distinguish different seasons as defined in the text. Figure 5. Diurnal variations of MBC observed at Happo in (a) July 2008 and (b) January 2009. The vertical bars represent 1s of the measured MBC. associated with the upslope wind from the foothills of the mountains, transporting lower-latitude air with presumably higher MBC. During the nighttime, radiative cooling of the surface of the mountains acts to bring down FT air with lower MBC, most prominently in the early morning prior to sunrise. Thus, the MBC is anticipated to be lowest during this period. [23] The amplitude of the diurnal variation in MBC seems to be larger in July 2008 than in January 2009 (Figure 5). To be more quantitative, the MBC values were averaged for daytime (extended to early evening) (07:00–20:00 local time, LT) and nighttime (20:00–6:00 LT). The daytime/ nighttime ratios of MBC were 1.21 for July 2008 and 1.11 for January 2009. The ratios for other months were generally in this range (not shown). The seasonal variation of the ratio is mainly due to the variation of the heating rate of the mountain slopes. The diurnal variation of MBC is not necessarily due to BC emitted locally. As discussed later in this section, MBC generally decreased with the increase in altitude from the BL to the FT over the western Pacific. The vertical gradient in MBC can cause small diurnal variations in MBC at Happo, coupled with diurnal variations of the upward and downward transport of ambient air. Because of this, we used diurnally averaged values of MBC for the quantitative analysis in this paper without discarding the daytime data. The uncertainty in the interpretation of the 3713 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO [26] We calculated monthly averaged MBC values for NC, FT, and MX air masses, as shown in Figure 7a. The mean MBC values in FT air masses are close to those of NC air masses, for which trajectories were located below 700 hPa. The mean pressure level of FT air near the eastern boundaries 0.8 Happo NC (Obs) Happo FT (Obs) Happo MX (Obs) (a) 0.6 BC (µg m-3) MBC data associated with the 24 h averaging is estimated to be about 5% for winter and 10% for summer. [24] Figure 6 shows time series plots for monthly mean values of MBC separately for 2007–2008 and 2008–2009 at Happo. The statistics of the measured MBC (mean 1s) values for each season are also summarized in Table 1. The mean MBC was 0.26 0.18 mg m3 for the entire measurement period. The comparison of monthly mean and median values of MBC shows that MBC underwent similar seasonal variations in both years (Figure 6) with the mean MBC highest in spring (~0.35 mg m3) for the 2 years. [25] The important features of the seasonal variations of MBC are better understood by extracting the seasonal variations of the different types of air. The observational site was under the influence of continental outflow from China and Korea during the study period (Figure 3). In addition, FT air masses constituted about 35%–59% of the total air masses measured at Happo, except for summer (Figure 3). By definition, these air masses were located above 700 hPa (~3 km altitude) when they passed over the eastern borders of the NC or SC regions. NC air constituted about 9%–14% of the sample air masses throughout the seasons. 0.4 0.2 0.0 Mar May Jul Sep Nov Jan 2008 Mar May 2009 1.6 (b) Hedo NC Hedo FT BC (µg m-3) 1.2 0.8 0.4 0.0 Figure 6. Interannual variability of the monthly average MBC during the 2 year measurement period (August 2007– August 2009). Spring 08 Summer 08 Fall 08 Winter 08 Spring 09 Figure 7. (a) Monthly mean ( 1s) of the observed MBC values at Happo in FT, NC, and MX air masses during 2008–2009. (b) Seasonally averaged MBC values observed at Hedo in NC and FT air masses. The 1s values are those of the hourly MBC values. Table 1. Seasonal Statistics of Observed and Model-Calculated (CMAQ-PASCAL) MBC at Happoa CMAQ-PASCAL for East Asia Observation WWD WWOD (Base) (Without Deposition) Season Av. SD Median Av. SD Median Av. SD Median Summer 07 Fall 07 Winter 07 Spring 08 Summer 08 Fall 08 Winter 08 Spring 09 Summer 09 All data 0.25 0.20 0.22 0.15 0.24 0.16 0.37 0.29 0.22 0.15 0.24 0.15 0.24 0.12 0.33 0.18 0.24 0.16 0.26 0.18 0.18 0.19 0.21 0.28 0.18 0.21 0.22 0.28 0.19 0.22 NA NA NA 0.36 0.29 0.16 0.13 0.20 0.17 0.17 0.20 0.32 0.26 0.18 0.17 0.23 0.23 NA NA NA 0.28 0.14 0.14 0.10 0.24 0.13 0.15 NA NA NA 0.61 0.37 0.57 0.28 0.39 0.27 0.37 0.40 0.52 0.32 0.56 0.30 0.49 0.35 NA NA NA 0.57 0.52 0.34 0.24 0.49 0.57 0.43 WWD: MBC calculated by CMAQ-PASCAL considering the effects of wet deposition. WOWD: MBC calculated by CMAQ-PASCAL without considering the effects of wet deposition. NA: Not available. a The average (Av.) standard deviation (SD) and median are given in units of mg m3. 3714 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO was about 570 hPa (about 4.5 km). This suggests that BL air was well mixed up to at least about 700 hPa. It is also possible that FT air was mixed with NC air before reaching Happo at 1.8 km (~750 hPa). In this regard, the MBC values in NC and FT air are interpreted to be the most representative MBC values at 1.8 km height in the western Pacific, strongly influenced by BC emissions in North China. [27] The MBC values in FT and NC air were the lowest in the November–March period, and they were similar for the other months. The MBC values showed rather sharp increases from March to April. The lower MBC values in late fall/early spring were also seen for MX air, although less pronounced, suggesting some differences in the characteristics of MX air. [28] Figure 7b shows seasonally averaged MBC values for NC and FT air masses at Hedo. The observed MBC values for NC and FT air masses at Hedo are very different from those at Happo. In contrast to the relatively similar MBC values for NC and FT air masses at Happo, MBC values were a factor of 2–3 higher for NC air mass at Hedo. However, the level of MBC in FT air masses at Hedo is more or less similar to that at Happo. This suggests that the mixing and transport pathways of the NC air masses were somewhat different between Happo and Hedo. The measurements of MBC at Hedo represent values near the surface, whereas those at Happo were at an altitude of ~1.8 km. In the case of Hedo, the NC air masses were transported at lower altitude, well within the BL. The high MBC in winter at Hedo, is consistent with the low MBC at Happo in the same season. The higher BL/FT MBC ratio in winter is interpreted to be due to the weakened upward transport of BC from the mixed layer. [29] The MBC values for MX air in April and May 2008 were considerably higher than those for FT and NC air. They were also higher than those for MX air in 2009. This suggests additional sources of BC aerosols in Asia, especially in spring 2008. The possible cause of the high MBC in MX air in spring is discussed in detail in section 5.4. [30] We have also compared MBC values of ground-based observations at Hedo and Happo to understand the observed vertical distribution of MBC over the western Pacific Ocean. The vertical profile of MBC (between altitudes of 0.5 and 8 km) was obtained during the A-FORCE aircraft campaign [Kondo et al., 2011a; Oshima et al., 2012]. The mean MBC values were between 0.3 and 0.5 mg m3 at altitudes below 2 km, strongly influenced by the transport of BC from China and decreasing sharply above 2 km altitude (Figure 8). The mean MBC values at Happo are similar to the MBC values obtained during the A-FORCE campaign, within the variability of MBC shown as horizontal bars in Figure 8. The small vertical gradient of MBC from the surface up to 1.8 km is consistent with the similarity in the MBC for FT and NC air at Happo, as discussed above. were used for quantitative interpretation of the observed MBC data. [32] Figure 10a shows the time series of comparison of the monthly mean MBC (1s) observed (MBC-obs) and modeled (MBC-model) during the 2 year measurement period. The model calculations for anthropogenic + biomass burning (AN + BN) and anthropogenic alone (AN) are shown separately. Table 1 summarizes the seasonal average MBC-model (AN + BB) for a quantitative comparison. The average MBC-model/MBC-obs ratio was 0.96 for all the data, indicating that the CMAQ-PASCAL model (base case data) reproduced well the yearly averaged MBC at Happo. The model generally reproduced the seasonal variations of MBC, although it overestimated MBC by 11%–15% for spring 2008 and 2009. [33] The MBC-model calculation for anthropogenic only (AN) showed a small spring maximum, and the inclusion of BB emissions further increased MBC-model values (Figure 10a). Therefore, it is likely that the spring maximum of MBC was due to increased efficiency of transport of anthropogenic BC from the Asian continent and BB emissions in Siberia. These effects are discussed more quantitatively using statistical data of FT, NC, and MX air in section 5.4. 5.2. Comparison of Observed and Model-Calculated MBC [31] Figures 9a and 9b show the horizontal distributions of MBC at about 990 hPa (0.2 km), 810 hPa (1.8 km), and 720 hPa (2.8 km) calculated by CMAQ-PASCAL (MBC-model) for April 2008 and January 2009, respectively. The calculations were made including anthropogenic and BB emissions (AN + BB), and excluding BB sources (i.e., AN only). The model calculations were made with and without wet deposition (base) using AN + BB emissions. These model results 5.3. Transport from the Asian Continent and Its Efficiency [34] The relative contributions of anthropogenic BC emissions from different countries in Asia (China, Japan, Korea, Southeast Asia (SEA), and others) to the MBC values observed at Happo were calculated by the CMAQ-PASCAL model and are shown in Figure 10b (source regions are defined in section 4). Table 2 summarizes the relative contributions of BC emitted from China (fChina), NC (fN-China), SC (fS-China), and the other countries (e.g., Japan and Korea; fOthers) to the observed Aircraft (Latitude: 26-33°N) Observation 8 Ground-based at Happo Mean and SD Altitude (km) 6 Ground-based at Hedo Mean Median 4 2 0 0 500 1000 BC (ng 1500 m-3) Figure 8. Comparison of MBC values from ground-based observations at Hedo (~60 m asl) and Happo (~1800 m asl) in the western Pacific. The vertical profile of MBC obtained during the Aerosol Radiative Forcing in East Asia (A-FORCE) [Oshima et al., 2012] aircraft campaign over the western Pacific is also shown for comparison. 3715 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO Figure 9. (a) Distributions of the model-calculated (CMAQ-PASCAL) MBC at about 2.8 km (720 hPa), 1.8 km (810 hPa), and 0.2 km (990 hPa) for April 2008. The calculations were made including anthropogenic and BB emissions (AN + BB) and excluding BB sources (i.e., AN only). (b) Same as Figure 9 (a) but for January 2009. The locations of Happo and Hedo are marked as circles. MBC. The model estimate indicates that China was the largest contributor to the total MBC at Happo, with an fChina of about 67% for the entire period. It was also observed that, on average, northern China alone contributed ~61% of the MBC at Happo, whereas only 6% was from south China. According to this model, the average contributions of BC emitted from 3716 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO Figure 9. (Continued) Japan and Korea are estimated to be about 14% and 6%, respectively, during the whole period. [35] The transport efficiencies of BC (TEBC) calculated by the CMAQ-PASCAL model for different seasons are shown in Figure 11, together with fChina. The TEBC was relatively stable throughout the year except for summer, when it fell to 0.27. We have also calculated TEBC values for different types of air masses reaching Happo (not shown). The TEBC values for the MX type of air masses were similar to those of NC air masses. TEBC values were lowest in summer when the fraction of MA air was as high as ~35% (Figure 3). 3717 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO (a) (b) (c) Figure 10. (a) Time series plots of the monthly mean ( 1s) values of the observed and modelcalculated (CMAQ-PASCAL) MBC at Happo. The calculations including anthropogenic and BB emissions (AN + BB) and excluding BB sources (AN) are shown separately. The 1s values represent the hourly MBC values. (b) Fraction of MBC at Happo originating from anthropogenic sources (AN) in Asian countries (China, Japan, Korea, Southeast Asia (SEA), and others). (c) Fractions of MBC at Happo originating from biomass burning (BB) in Asian countries and Siberia. Table 2. Fractions of MBC ( f ) Originating From China, North China, and Others (Korea and Japan), Along With the Transport Efficiency of BC (TEBC) for Different Seasons Season fChina fN-China fS-China fOthers fN-China/fChina TEBC Spring 2008 Summer 2008 Fall 2008 Winter 2009 Spring 2009 All data 0.59 0.57 0.66 0.82 0.66 0.67 0.53 0.48 0.64 0.70 0.60 0.61 0.06 0.09 0.02 0.11 0.06 0.06 0.41 0.43 0.34 0.18 0.35 0.33 0.90 0.85 0.97 0.86 0.91 0.91 0.58 0.27 0.50 0.46 0.61 0.49 5.4. Upward Transport and Biomass Burning [36] It is estimated that BC emissions and surface BC concentrations in China are relatively higher during winter compared to those during spring months [Streets et al., 2003; Zhang et al., 2009]. However, the MBC levels were significantly higher during the spring of both years than those in winter at Happo (Figure 6). The MBC at Happo increased to 0.37 mg m3 from an average value of 0.22 mg m3, in particular during the month of April of both years. There could be two reasons for the enhancement in Figure 11. Fractional contribution of China to MBC ( fChina) and TEBC for different seasons. the levels of MBC at Happo during spring. First, the ambient temperature over North China is usually lower during winter than that in the spring season, resulting in shallower mixing layer heights over North China during winter as compared to that in spring. Therefore, upward transport of BC enriched air masses from the surface to the regions above the mixed 3718 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO layer could be lower during winter than those in spring. Second, BC emissions from biomass burning during the spring season could be the cause of the winter-spring difference. [37] For quantitative investigations of the dynamical effect, we extracted the MBC values for FT, NC, and MX air, separately. MBC-model (AN) values for these air masses are compared with the observed MBC values in Figure 12. The model calculations reproduced well the winter minimum for FT and NC air. Excellent agreement was obtained for FT air, which was least impacted by BB. This agreement indicates that the changes in the upward transport mainly caused the seasonal variations of the MBC in FT air. [38] The MBC-model (AN) values at 1.8 and 2.8 km at 130 – 140 E were higher in April than in January (Figures 9a and 9b). In contrast, the MBC-model (AN) in the BL (~0.2 km) over the Asian continent was much higher in January than in April. These results also support that the increase in the upward transport followed by northeastward horizontal transport was the main cause of the rapid increase in the MBC values in April. Figure 12. Comparison of the model calculated monthly mean MBC (AN + BB) values with those observed for (a) FT, (b) NC, and (c) MX air masses. [39] Second, there could be additional BC emissions other than AN, such as those from biomass or agricultural waste burning in the Asian continent during the spring season. Earlier studies have suggested that the spring maximum of CO concentration at Happo results from biomass burning events in East Asia, particularly from Siberia [Kato et al., 2002; Narita et al., 1999]. Because BC and CO are produced simultaneously, as indicated by a strong correlation between their mass concentrations near source regions [Kondo et al., 2006; Limon–Sanchez et al., 2011; Pan et al., 2011], it is likely that Siberian biomass burning events had a strong influence on the MBC at Happo during spring as well. [40] The distribution of active fire detections during 2008 and 2009 was produced by the MODIS rapid response system and is shown in Figure 13a. The map of fire counts was plotted online using the NASA-Northern Eurasia Earth Science Partnership Initiative (NASA-NEESPI). The time series plot of fire counts (Overpass-Corrected Fire Pixel Counts) for the period of 2007–2009 is shown in Figure 13b. A number of biomass burning events were detected in northeast China, Mongolia, and Siberia during spring of the years 2008 (peaking in April) and 2009 (peaking in April–May). However, the fire counts of the Siberian biomass burning were relatively lower during April 2009 (Figure 13b). [41] We also investigated the effect of BB over Eurasia and East Asia in April 2008 on measured MBC based on the trajectories shown in Figure 2b. About 18% of the trajectories of the FT air passed over the BB region in Siberia (40 N–60 N, 60 E–80 E) and 49% over Northeast China (40 N–60 N, 100 E–135 E) in April 2008. The same analysis was also applied to the spring of 2009. [42] The observed MBC for FT and NC air in April and May in 2008 were similar to those in 2009, despite large differences in the BB activities in Siberia during those 2 years. The substantial difference is seen for MX air, and thus, it is possible that the BB in Siberia influenced the MBC in this air in the spring of 2008. [43] For more quantitative estimates of the effect of the BB, we calculated horizontal distribution of MBC at about 2.8 km (720 hPa), 1.8 km (810 hPa), and 0.2 km (990 hPa), originating from anthropogenic and BB emissions (AN + BB), and excluding BB sources using the CMAQ-PASCAL model. Figures 9a and 9b present the horizontal distribution of the effect of BB emissions for April 2008 and January 2009, respectively. The calculations were made separately for anthropogenic and BB emissions (AN + BB) and excluding BB sources. The average MBC values with AN + BB emissions for April 2008 and 2009 were 0.44 and 0.45 mg m3, respectively. In contrast, MBC values for AN emission were significantly lower: 0.21 and 0.27 mg m3, respectively. The observed MBC values at Happo during April 2008 also were much higher than the average nonspring MBC values (about 0.25 mg m3), and Figure 9a suggests that MBC values were highly influenced by the Siberian biomass burning in spring. The average contribution of the BB in Siberia to the MBC is estimated to be as high as 50% for April 2008 (Figure 10c). [44] The effect of BB on MBC is more clearly seen in the comparison of the model and observed MBC with higher time resolution. The MBC calculated by CMAQ-PASCAL incorporating these BB events in April are compared with the measured MBC in Figure 14. It can be seen that the timing and magnitudes of MBC calculated, including anthropogenic 3719 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO (a) Fire Counts/ Month 70000 60000 Eurasia (40-60 °N, 60-140 °E) East Eurasia (45-55 °N, 100-135 °E) (b) 50000 40000 30000 20000 10000 0 09/07 12/07 03/08 06/08 09/08 12/08 03/09 06/09 Time Figure 13. (a) Maps of fire counts (Overpass-Corrected Fire Pixel Counts) in the months of April 2008 and 2009, plotted online using the Northern Eurasia Earth Science Partnership Initiative (NASA-NEESPI; website (http://gdata1.sci.gsfc.nasa.gov/daac-bin/G3/gui.cgi?instance_id=neespi). The distribution of active fire detections is during a 5 day period from April 20 to April 24, 2008, produced by the MODIS rapid response system, where red dots represent single 1 km MODIS active fire pixels (developed by the University of Maryland with funds from NASA; website (http://maps.geog.umd.edu). (b) Time series plots of monthly averaged fire counts over Eurasia and East Eurasia during the measurement period (August 2007–August 2009). Figure 14. Time series plots of the observed MBC and that calculated separately including emissions from Siberian biomass burning (BB), all BB emissions, and total emissions (anthropogenic (AN) + BB) during April 2008. and all BB sources (AN + all BB), agree reasonably well with the observations. More detailed studies of the effect of BB are given in Matsui et al. (submitted). [45] These results suggest that BB events in Siberia substantially contributed to the spring maximum of MBC at Happo. However, the estimates of BC emissions from BB are still highly uncertain. The model overestimated MBC in MX and NC air for May in 2008. In addition, an even larger overestimate is seen for May in 2009, when the Siberian BB was much less active. It is likely that the emissions of BC from BB in China and Siberia were overestimated. Quantifying the effect of the BB on MBC in spring requires further 3720 LIU ET AL.: SEASONAL VARIATIONS OF BC AT HAPPO improvements in the estimates of the BC emissions from BB and simultaneous measurements of MBC at this site for a longer time period. 6. Conclusions [46] We made accurate and long-term measurements of MBC using a COSMOS at Happo, a remote mountain site at about 1.8 km altitude in Japan, from August 2007 to August 2009. The annual average MBC at Happo was about 0.26 mg m3. The MBC values exhibited similar seasonal variations in both years, with a maximum value of ~0.35 mg m3 in spring. About 40% and 10% the air masses sampled were classified as free tropospheric (FT) and North China (NC) air. The MBC values in these air masses represent the values most strongly influenced by BC emitted from China. The MBC values calculated using the CMAQ-PASCAL model reproduced well the MBC for these air masses. The best agreement was obtained for FT air. [47] The MBC values in FT and NC air reached minimum values from late fall to early spring. The comparisons with the CMAQ-PASCAL model results indicate that the lowest values in winter were caused by the suppressed upward transport over China. In the other seasons, the more active convective activities increased the levels of MBC values. [48] The model predicted that BC transported from China contributed ~67% to the measured MBC, consistent with the trajectory analysis. The contribution of MBC from NC was much higher (~61%) than that from SC (only 6%), reflecting the transport pathways. The average transport efficiency of BC (TEBC) for all the source regions was about 0.50 for the spring, winter, and fall seasons and 0.27 for summer. [49] In addition to the anthropogenic emissions in East Asia, it is likely that BB also contributed to MBC values at Happo, particularly in the spring season. An increase in observed MBC values in April and May in 2008, especially in MX air, suggest the substantial effects of very active BB in Siberia. These observations are supported by the MODIS fire counts maps of BB emissions over Siberian regions. More quantitative analyses of the effect of the BB are required to improve the estimates of BC emissions from BB in East Asia. [50] Acknowledgments. 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