LIDAR Measurements of the Vertical Aerosol Profile and Optical Depth during the ACE-Asia 2001 IOP, at Gosan, Jeju Island, Korea

In order to investigate the characteristic of optical properties of Asian dust particles, the atmospheric aerosol vertical profile was measured with the multi-wavelength LIDAR system, at the Gosan super site (33 degrees 17'N, 126 degrees 10'E) in Jeju Island, Korea, during the ACE-Asia intensive observation period, 11 March-4 May 2001. An air mass backward trajectory analysis, using Hysplit-4, was carried out to track the aerosol plume, with high mass loading, from the Chinese desert regions during the period of Asian dust storm events. Vertical atmospheric aerosol profiles on three major Asian dust storm event days, 22 March and 13 and 26 April 2001, have been analyzed. The LIDAR-derived aerosol optical depth values were compared with those measured by a collocated sunphotometer.     

Pool of Dust Particles over the Asian Continent: Balloon-borne Optical Particle Counter and Ground-based Lidar Measurements at Dunhuang, China

Measurements of aerosols were made in 2001 and 2002 at Dunhuang (40 degrees 00'N, 94 degrees 30'E), China to understand the nature of atmospheric particles over the desert areas in the Asian continent. Balloon-borne measurements with an optical particle counter suggested that particle size and concentration had noticeable peaks in super micron size range not only in the boundary mixing layer but also in the free troposphere. Super-micron particle concentration largely decreased in the mid tropopause (from 5 to 10 km; above sea level, a.s.l.). Lidar measurements made during August 2002 at Dunhuang suggested the possibility that mixing of dust particles occurred from near the ground to about 6 km even under calm weather conditions, and a large depolarization ratio of particulate matter was found in the aerosol layer. The top of the aerosol layer was found at heights of nearly 6 km (a.s.l.). It is strongly suggested that nonspherical dust particles (Kosa particles) frequently diffused in the free atmosphere over the Taklamakan desert through small-scale turbulences and are possible sources of dust particles of weak Kosa events that have been identified in the free troposphere not only in spring but also in summer over Japanese archipelago. Electron microscopic experiments of the particles collected in the free troposphere confirmed that coarse and nonspherical particles observed by the mineral particle were major components of coarse mode (diameter larger than 1 microm) below about 5 km over Dunhuang, China.     

Anthropogenic Calcium Particles Observed in Beijing and Qingdao, China

Analysis of individual particles collected at Beijing in northern China revealed that particles abundant in calcium (Ca) always constituted a large fraction of mineral particles in the urban atmosphere. The particles were characterized by cubic morphologies. The major mineral element in the particles was Ca and few or no other mineral elements were detected. A large number of the particles were in the range of diameter <1 μm, where common natural mineral particles were rarely detected. The contribution of the Ca particles to the volume of total mineral particles greatly exceeded that of other mineral particles during non-dust-storm periods and was comparable to that during dust-storm periods. Reagent film tests showed that particulate sulfate and nitrate formation on the Ca particles was similar to that on common mineral particles. These results indicate that a large portion of Ca in the atmospheric particulate matter in Beijing was from anthropogenic sources rather than from natural sources, and the anthropogenic Ca particles acted as a significant medium for the formation of sulfate and nitrate. Similar particles were also detected at Qingdao, a coastal city in northern China. Data of a dust storm event showed that Ca-abundant particles from East China arrived there and moved out of the continent, similarly to Asian dust storm particles, suggesting possible contributions of anthropogenic Ca even in Asian dust storm samples in the downstream areas. Therefore, Ca may not be a good indicator of Asian dust from natural sources. However, the Ca particles, due to their unique shapes and elemental compositions, may provide an indicator for the atmospheric dispersion of anthropogenic particulate matters in East Asia.     

Heterogeneous Sulfate Formation on Dust Surface and Its Dependence on Mineralogy: Balloon-Borne Observations from Balloon-Borne Measurements in The Surface Atmosphere of Beijing, China

This study focuses on providing a direct insight into the process by which sulfate is formed on mineral dust surface in the actual atmosphere. Six sets of aerosol measurements were conducted in the outskirts of Beijing, China, in 2002–2003 using a tethered balloon. The mineralogy of individual dust particles, as well as its influence on the S (sulfur) loadings was investigated by SEM-EDX analysis of the directly collected particles. The mixed layer in the urban atmosphere was found to be quite low (500–600m), often appearing as a particle dense stagnant layer above the surface. It is suggested that mineral dust is a common and important fraction of the coarse particles in Beijing (35–68%), and that it is relatively enriched with Calcite (>28%). An exceptional amount of S was detected in the mineral particles, which can be explained neither by their original composition, nor by coagulation processes between the submicron sulfates and the dust. Heterogeneous uptake of gaseous SO₂, and its subsequent oxidation on dust was suggested as the main pathway that has actually taken place in the ambient environment. The mineral class found with the largest number of particles containing S was Calcite, followed by Dolomite, Clay, Amphibole etc., Feldspar, and Quartz. Among them, Calcite and Dolomite showed distinctly higher efficiency in collecting sulfate than the other types. A positive correlation was found with the number of S containing particles and the relative humidity. Calcite in particular, since almost all of its particles was found to contain S above 60% r.h. On the other hand, the active uptake of SO₂ by the carbonates was not suggested in the free troposphere downwind, and all the mineral classes exhibited similar S content. Relative humidity in the free troposphere was suggested as the key factor controlling the SO₂ uptake among the mineral types. In terms of sulfate loadings, the relationship was not linear, but rather increased exponentially as a function of relative humidity. The humidity-dependent uptake capacity of mineral types altogether showed an intermediate value of 0.07 gSO₄ ²⁻ g⁻¹ mineral at 30% r.h. and 0.40 gSO₄ ²⁻ g⁻¹ mineral at 80%, which is fairly consistent with laboratory experiments.     

Comparison of the Chemical Composition of Mineral Particles Collected in Dunhuang,China and those Collected in the Free Troposphere over Japan: Possible Chemical Modification during Long-Range Transport

The Asian continent is recognized as one of the most important sources of mineral (or soil) particles. These particles have a large potential to effect global changes through the biogeochemical cycle of particulates and through radiative balance (IPCC Third Assessment Report, 2001). Therefore, comparison of particle compositions near the source region and those after long-range transport is important in understanding the long-range particle transport phenomenon. Individual aerosolparticles were collected in Dunhuang (40°09N; 94°41E), China. Particles were collected at the campus of the Meteorological Bureau of Dunhuang City (17 August 2001) and near the Mogao Grots, located approximately 30 km from Dunhuang (18 August 2001, 18 October 2001 and 13 January 2002) using a two-stage low-volume impactor. The morphology of individual aerosol particles and their elemental compositions were examined via a scanning electron microscope (Hitachi, S-3000N) equipped with an energy dispersive X-ray (EDX) analyzer (Horiba, EMAX-500). The particles collected at these locations were comprised primarily of minerals, with the exception of sulphateparticles in the submicron range that were contained in thesample collected on 18 October 2001 (likely, ammonium sulphate). The most abundant elements were found to be Si and Al. Approximately 46–77% of the collected particles were Si-richparticles (composed primarily of quartz and aluminosilicate),and 13–41% of the collected particles were Ca-rich particles,such as calcite (CaCO₃), dolomite (CaMg(CO₃)₂),and gypsum (CaSO₄2H₂O). The fractions of Fe-rich, Mg-rich, Ti-rich, K-rich, and Cl-rich were 3–10, 0–7, 0–3, 0–1, and 0–1%, respectively. Similar types of mineral particles were found in the free troposphere over Japan(Trochkine et al., 2002). A number of differences were found to exist between the particles collected in China and thosecollected in Japan, and these differences can be explained bychemical modification of the particles during transport fromChina to Japan.     

Features in Number Concentration-Size Distributions of Aerosols in the Free Atmosphere over the Desert Areas in the Asian Continent: Balloon-Borne Measurements at Dunhuang,China

Vertical changes of aerosol concentration and size in the freetroposphere over the Asian desert areas were firstly observed using a balloon-borne optical particle counter at DunHuang, China (40°00N, 94°30E) (17 August and 17 October 2001, and 11 January 2002). In the free troposphere highly concentrated aerosol layers were frequentlyobserved, suggesting the importance of regional scale particletransportation over the Asian continent. Concentration ofparticles with a diameter larger than 0.15 m was about 5–10particles cm^-3 in the free troposphere.Particle number-size distribution in the free troposphereshows important contribution of super micron particles. Regionalscale transportation, in addition to diffusion of soil particlesfrom the lower atmosphere to the free troposphere through localand small scale air motions, is suggested by backward trajectoryanalysis of air masses containing super micron particles. The importance of horizontal transport of coarse size particles in the free troposphere was strongly suggested.Thickness of the boundary mixing layer, from distributions ofparticle concentration, was about 4 km in summer (17 August 2001)and apparently higher than the height of layers in fall (17 October2001) and in winter (11 January 2002), which suggest an active mixingof particles near the boundary in summer. In winter measurement(11 January 2002), strong inversion was found in the vertical profile of temperature, suggesting cold ground surface and vertically stable atmosphere near the ground.     

Feature of Dust Particles in the Spring Free Troposphere over Dunhuang in Northwestern China: Electron Microscopic Experiments on Individual Particles Collected with a Balloon-borne Impactor

Free tropospheric aerosol particles were collected using a balloon-borne particle impactor in August of 2002 and March of 2003 at Dunhuang in northwestern China (40°00′N, 94°30′E), and the morphology and elemental composition of the aerosol particles were analyzed in order to understand the mixing state of coarse dust particles (diameter >1 μm) over the desert areas in the Asian continent in spring. Electron microscopic experiments on the particles revealed that dust particles were major constituents of coarse mode particles in the free troposphere over the Taklamakan Desert in spring and summer. Si-rich or Ca-rich particles are major components of dust particles collected in the free troposphere over dunhuang and the values of [number of Ca-rich particles]/[number of Si-rich particles] differs markedly between spring and summer, being about 0.3 in the spring of 2003 and about 1.0 in the summer of 2002 at heights 3–5 km above sea level. It is likely that the condition of the ground surface and the strength of vertical mixing in source areas of Asian dust are potential factors causing the difference in the chemical types of dust particles. Comparison of the elemental compositions of these particles with those of particles collected over Japan strongly suggests that these particles were chemically modified during their long-range transport in the free troposphere. Analysis of wind systems shows that both the predominating westerly wind in the free troposphere and the surface wind strongly controlled by the geographical structure of the Tarim Basin are important in the long-range transport of KOSA particles originating in the Taklamakan Desert.     

Nature of Atmospheric Aerosols over the Desert Areas in the Asian Continent: Chemical State and Number Concentration of Particles Measured at Dunhuang,China

Measurements of aerosol were made in August and October 2001, and January 2002, at Dunhuang, China (40°00N, 94°30E), to understand the nature of atmosphericparticles over the desert areas in the Asian continent. Balloon-borne measurements with an optical particle counter suggested that particle size and concentration had a noticeable peak in size range of super micron in not only the boundary mixing layer but also the free troposphere. Thickness of the boundary mixing layer, from distributions of particle concentration, was about 4 km in summer (17 August 2001), about2.5 km in fall (17 October 2001), and about 3 km in winter (11 January 2002), which suggest active mixing of particles near the boundary in summer. Number-size distribution of particleshowed a noticeable peak in the super micron particles size range inthe mixing boundary layer: 0.4–2 particles cm^-3 at diameter>1.2 m in summer, 0.05–4 particles cm^-3 at diameter >1.2 m in fall, and 0.1–5 particles cm^-3 at diameter>1.2 m in winter. In winter strong inversion of atmospherictemperature was found in the height range from the boundary to about 3 km and vertical distribution of particle concentration well corresponded with the temperature distribution. Chemical elements of individual aerosols, which were collectedin the boundary layer atmosphere at Dunhuang (18 October 2001) were analyzed with an electron microscope equipped with EDX. Thosesingle particle analysis suggested that most of the particles with supermicron size were soil particles, and those particles had littlesulfate on its surface. This is a very important different point,comparing with the chemical state of soil particles, which weretransported from the desert area of China to Japan, and showed frequentlythe existence of sulfate on the particle surface. Therefore, it isstrongly suggested that dust particles can be chemically modifiedduring their long-range transport from desert areas to Japan.