Airborne estimation of SO2 emissions rates from a coal-fired power plant using two top-down methods: A mass balance model and Gaussian footprint approach.

In this study, two top-down methods-mass balance and Gaussian footprint-were used to determine SO2 emissions rates via three airborne sampling studies over Korea's largest coal power plant in October 2019 and 2020. During the first two flights in October 2019, mass balance approaches significantly underestimated the SO2 emissions rates by 75 % and 28 %, respectively, as obtained from the real-time stack monitoring system. Notably, this large discrepancy accounted for the insufficient number of transects altitudes and high levels of background SO2 along the upwind side. Alternatively, the estimated SO2 emissions rates of the third flight (October 2020) displayed a difference of <10 % from rea-time monitoring data (630 vs. 690 kg·hr-1), owing to the enhanced vertical resolution with increased transects and lower background SO2 levels. In contrast to the mass balance method, Gaussian footprints offered significantly improved accuracy (relative error: 41 %, 32 %, and 2 % for Flights 1, 2, and 3, respectively). This relatively good performance was attributed to prior emissions knowledge via the Clean Air Policy Support System (CAPSS) emissions inventory and its unique ability to accurately estimate stack-level SO2 emissions rates. Theoretically, the Gaussian footprint was less prone to sparse transects and upwind background levels. However, it can be substantially influenced by atmospheric stability and consequently by effective stack heights and dispersion parameters; basically, all factors with minimal-to-no influence on the mass balance approach. Conversely, the mass balance method was the only plausible approach to estimate unidentified source emissions rates when well-defined prior emission information was unknown. Here, the footprint approach supplemented the mass balance method when the emission inventories were known, and employing both strategies approaches greatly enhanced the integrity of top-down emissions inventories from the power plant sources, thus, supporting their potential for ensuring operational compliance with SO2 emissions regulation.

Atmospheric sulfate formation in the Seoul Metropolitan Area during spring/summer: Effect of trace metal ions.

Despite the effort to control SO2 emission, sulfate is still one of the major inorganic components of PM2.5 in urban area. Moreover, there is still a lack of understanding of the sulfate formation mechanism via SO2 oxidation under various ambient conditions. In this study, we focus on sulfate formation during a haze pollution episode in the spring/summertime of 2016 in Seoul Metropolitan Area (SMA). During the pollution episode, PM2.5 mass concentration exceeded over 60 µg m-3, and sulfate accounted for about 25% of the total PM2.5 mass concentration. A sharp increase of sulfur oxidation ratio (SOR) values along with aerosol liquid water content (AWC) under humid conditions could be ascribed to an apparent contribution of aqueous-phase oxidation of SO2 of sulfate formation during the pollution period. Comparisons of SOR values with four representative oxidants for the aqueous-phase oxidation (i.e., NO2, H2O2, O3, and TMIs) indicated that TMIs concentration, especially for Mn (II), showed the best positive correlation. Furthermore, for calculating the sulfate production rate, the contribution of TMIs concentration was found to be dominant within the pH range in SMA (2.1-3.0), which was determined by the chemical composition and derived AWC. These results imply that not only the SO2 emission but also other chemical components (e.g., TMI and nitrate) would play a critical combined role in sulfate formation under urban haze condition.

The Korea-United States Air Quality (KORUS-AQ) field study.

The Korea-United States Air Quality (KORUS-AQ) field study was conducted during May-June 2016. The effort was jointly sponsored by the National Institute of Environmental Research of South Korea and the National Aeronautics and Space Administration of the United States. KORUS-AQ offered an unprecedented, multi-perspective view of air quality conditions in South Korea by employing observations from three aircraft, an extensive ground-based network, and three ships along with an array of air quality forecast models. Information gathered during the study is contributing to an improved understanding of the factors controlling air quality in South Korea. The study also provided a valuable test bed for future air quality-observing strategies involving geostationary satellite instruments being launched by both countries to examine air quality throughout the day over Asia and North America. This article presents details on the KORUS-AQ observational assets, study execution, data products, and air quality conditions observed during the study. High-level findings from companion papers in this special issue are also summarized and discussed in relation to the factors controlling fine particle and ozone pollution, current emissions and source apportionment, and expectations for the role of satellite observations in the future. Resulting policy recommendations and advice regarding plans going forward are summarized. These results provide an important update to early feedback previously provided in a Rapid Science Synthesis Report produced for South Korean policy makers in 2017 and form the basis for the Final Science Synthesis Report delivered in 2020.

Characteristics of HONO and its impact on O3 formation in the Seoul Metropolitan Area during the Korea-US Air Quality Study.

Photolysis of nitrous acid (HONO) is recognized as an early-morning source of OH radicals in the urban air. During the Korea-US air quality (KORUS-AQ) campaign, HONO was measured using quantum cascade - tunable infrared laser differential absorption spectrometer (QC-TILDAS) at Olympic Park in Seoul from 17 May, 2016 to 14 June, 2016. The HONO concentration was in the range of 0.07-3.46 ppbv, with an average of 0.93 ppbv. Moreover, it remained high from 00:00-05:00 LST. During this time, the mean concentration was higher during the high-O3 episodes (1.82 ppbv) than the non-episodes (1.20 ppbv). In the morning, the OH radicals that were produced from HONO photolysis were 50% higher (0.95 pptv) during the high-O3 episodes than the non-episodes. Diurnal variations in HOx and O3 concentrations were simulated by the F0AM model, which revealed a difference of ~20 ppbv in the daily maximum O3 concentrations between the high-O3 episodes and non-episodes. Furthermore, the HONO concentration increased with an increase in relative humidity (RH) up to 80%; the highest HONO was associated with the top 10% NO2 in each RH group, confirming that NO2 is one of the main precursors of HONO. At night, the conversion ratio of NO2 to HONO was estimated to be 0.88×10-2 h-1; this ratio was found to increase with an increase in RH. The Aitken mode particles (30-120 nm), which act as catalyst surfaces, exhibited a similar tendency with a conversion ratio that increased along with RH, indicating the coupling of surfaces with HONO conversion. Using an artificial neural network (ANN) model, HONO concentrations were successfully simulated with measured variables (r2 = 0.66 as an average of five models). Among these variables, NOx, aerosol surface area, and RH were found to be the main factors affecting the ambient HONO concentrations. The results reveal that RH facilitates the conversion of NO2 to HONO by constraining the availability of aerosol surfaces. This study demonstrates the coupling of HONO with the HOx-O3 cycle in the Seoul Metropolitan Area (SMA) and provides practical evidence of the heterogeneous formation of HONO by employing the ANN model.

Investigation of factors controlling PM2.5 variability across the South Korean Peninsula during KORUS-AQ.

The Korea - United States Air Quality Study (May - June 2016) deployed instrumented aircraft and ground-based measurements to elucidate causes of poor air quality related to high ozone and aerosol concentrations in South Korea. This work synthesizes data pertaining to aerosols (specifically, particulate matter with aerodynamic diameters <2.5 micrometers, PM2.5) and conditions leading to violations of South Korean air quality standards (24-hr mean PM2.5 < 35 µg m-3). PM2.5 variability from AirKorea monitors across South Korea is evaluated. Detailed data from the Seoul vicinity are used to interpret factors that contribute to elevated PM2.5. The interplay between meteorology and surface aerosols, contrasting synoptic-scale behavior vs. local influences, is presented. Transboundary transport from upwind sources, vertical mixing and containment of aerosols, and local production of secondary aerosols are discussed. Two meteorological periods are probed for drivers of elevated PM2.5. Clear, dry conditions, with limited transport (Stagnant period), promoted photochemical production of secondary organic aerosol from locally emitted precursors. Cloudy humid conditions fostered rapid heterogeneous secondary inorganic aerosol production from local and transported emissions (Transport/Haze period), likely driven by a positive feedback mechanism where water uptake by aerosols increased gas-to-particle partitioning that increased water uptake. Further, clouds reduced solar insolation, suppressing mixing, exacerbating PM2.5 accumulation in a shallow boundary layer. The combination of factors contributing to enhanced PM2.5 is challenging to model, complicating quantification of contributions to PM2.5 from local versus upwind precursors and production. We recommend co-locating additional continuous measurements at a few AirKorea sites across South Korea to help resolve this and other outstanding questions: carbon monoxide/carbon dioxide (transboundary transport tracer), boundary layer height (surface PM2.5 mixing depth), and aerosol composition with aerosol liquid water (meteorologically-dependent secondary production). These data would aid future research to refine emissions targets to further improve South Korean PM2.5 air quality.

Factors controlling surface ozone in the Seoul Metropolitan Area during the KORUS-AQ campaign.

To understand the characteristics of air quality in the Seoul Metropolitan Area, intensive measurements were conducted under the Korea-United States Air Quality (KORUS-AQ) campaign. Trace gases such as O3, NOx, NOy, SO2, CO, and volatile organic compounds (VOCs), photochemical byproducts such as H2O2 and HCHO, aerosol species, and meteorological variables including planetary boundary layer height were simultaneously measured at Olympic Park in Seoul. During the measurement period, high O3 episodes that exceeded the 90 ppbv hourly maximum occurred on 14 days under four distinct synoptic meteorological conditions. Furthermore, local circulation such as land-sea breeze and diurnal evolution of the boundary layer were crucial in determining the concentrations of precursor gases, including NOx and VOC as well as O3. During such episodes, the nighttime NOx and VOC and daytime UV levels were higher compared to non-episode days. The overall precursor levels and photochemical activity were represented fairly well by variations in the HCHO, which peaked in the morning during the high O3 episodes. This study revealed that toluene was the most abundant VOC in Seoul, and its concentration increased greatly with NOx due to the large local influence under stagnant conditions. When O3 was highly elevated concurrently with PM2.5 under dominant westerlies, NOx and VOCs were relatively lower and CO was noticeably higher than in other episodes. Additionally, the O3 production efficiency was the highest due to a low NOx with the highest NOz/NOy ratio among the four episodes. When westerlies were dominant in transport-south episode, the nighttime concentration of O 3 remained as high as 40~50 ppbv due to the minimum level of NOx titration. Overall, the Seoul Metropolitan Area is at NOx-saturated and VOC-limited conditions, which was diagnosed by indicator species and VOC/NOx ratios.

OH reactivity in urban and suburban regions in Seoul, South Korea - an East Asian megacity in a rapid transition.

South Korea has recently achieved developed country status with the second largest megacity in the world, the Seoul Metropolitan Area (SMA). This study provides insights into future changes in air quality for rapidly emerging megacities in the East Asian region. We present total OH reactivity observations in the SMA conducted at an urban Seoul site (May-June, 2015) and a suburban forest site (Sep, 2015). The total OH reactivity in an urban site during the daytime was observed at similar levels (∼15 s(-1)) to those previously reported from other East Asian megacity studies. Trace gas observations indicate that OH reactivity is largely accounted for by NOX (∼50%) followed by volatile organic compounds (VOCs) (∼35%). Isoprene accounts for a substantial fraction of OH reactivity among the comprehensive VOC observational dataset (25-47%). In general, observed total OH reactivity can be accounted for by the observed trace gas dataset. However, observed total OH reactivity in the suburban forest area cannot be largely accounted for (∼70%) by the trace gas measurements. The importance of biogenic VOC (BVOCs) emissions and oxidations used to evaluate the impacts of East Asian megacity outflows for the regional air quality and climate contexts are highlighted in this study.

Congener profiles and source-wise phase partitioning analysis of PCDDs/Fs and PCBs in Gyeonggi-do ambient air, South Korea.

The atmospheric concentrations and gas-particle partitioning of polychlorinated dibenzo-p-dioxins and furans (PCDDs/Fs) and polychlorinated biphenyls (PCBs) were investigated at two sites (Suwon and Ansan) in Gyeonggi-do, a heavily industrialized area of Korea, during the year 2010. The sum level (Σ17) of PCDDs/Fs and dioxin-like PCBs (dl-PCBs) in the ambient air at Suwon and Ansan ranged from 0.04 to 0.30 pg-TEQ·m(-3) (geometric mean: 0.09 pg-TEQ·m(-3)) and 0.17 to 0.63 pg-TEQ·m(-3) (geometric mean: 0.36 pg-TEQ·m(-3)), respectively. Moreover, the geometric mean concentrations of Σ180 PCBs at Suwon and Ansan were 233.6 pg·m(-3) and 274.2 pg·m(-3), respectively, and di-chlorinated biphenyls and tri-chlorinated biphenyls were the predominant homologs. Among the PCB congeners, 3,3'-dichlorobiphenyl (PCB-11) was the dominant species at both sites during all sampling periods, comprising up to 15.1% of Σ180 PCBs at Ansan and 24.6% at Suwon. We evaluated their gas-to-particle equilibriums by conducting regression between the particle-gas partition coefficient Kp (m(3)·ug(-1)) and the corresponding subcooled liquid vapor pressure (PL°). The slope (m) values for log-log plots of Kp vs. PL° were steeper in industrial areas owing to local source proximity. Moreover, owing to enhanced emissions from combustion-related sources at low temperatures, PCDD/Fs exhibited the largest deviation from the regression line of the particle-gas partition coefficient. Incinerators were found to be the primary emission source of atmospheric PCDDs/Fs, whereas re-evaporation from pre-existing environmental loads (e.g., storage areas or spilled soil and water bodies) was the dominant source for PCBs.

Field-measured uptake rates of PCDDs/Fs and dl-PCBs using PUF-disk passive air samplers in Gyeonggi-do, South Korea.

The collection of 2,3,7,8-substituted polychlorinated dibenzo-ρ-dioxins and dibenzo furans (PCDDs/Fs) and dioxin-like polychlorinated biphenyls (dl-PCBs) using a polyurethane form (PUF)-disk passive air sampler (PAS) was investigated in urban-residential and industrial areas. This was performed to assess the feasibility of using this method as an alternative to an active air sampler (AAS). The PUF-disk PAS was exposed to ambient air over a period of 37-370 and 57-173 days in urban and industrial areas, respectively, together with AASs. The sum of total toxic equivalent quantity (TEQ) ΣPCDDs/Fs and Σdl-PCB was typically high in the industrial area, with values within the range 0.171-0.635 pg-TEQ/m(3), and 0.037-0.300 pg-TEQ/m(3) in the urban-residential area. To derive the time-weighted average (TWA) concentration from the PAS data accurately, it was estimated that the PAS deployed for less than 80 days was adequate to maintain linear accumulation conditions. PCDDs/Fs are mainly particle bound and showed low average uptake rates of 1.4m(3)d(-1), while dl-PCBs were slightly higher with 2.0m(3)d(-1) because of its high vapor pressure. Most of the congener concentrations measured using the PAS and AAS were within a factor of two, indicating that PASs can be used to monitor spatial and temporal variations in the concentrations of persistent organic pollutants (POPs) in the atmosphere.

Source identification and apportionment of halogenated compounds observed at a remote site in East Asia.

The sources of halogenated compounds in East Asia associated with stratospheric ozone depletion and climate change are relatively poorly understood. High-precision in situ measurements of 18 halogenated compounds and carbonyl sulfide (COS) made at Gosan, Jeju Island, Korea, from November 2007 to December 2011 were analyzed by a positive matrix factorization (PMF). Seven major industrial sources were identified from the enhanced concentrations of halogenated compounds observed at Gosan and corresponding concentration-based source contributions were also suggested: primary aluminum production explaining 37% of total concentration enhancements, solvent usage of which source apportionment is 25%, fugitive emissions from HCFC/HFC production with 11%, refrigerant replacements (9%), semiconductor/electronics industry (9%), foam blowing agents (6%), and fumigation (3%). Statistical trajectory analysis was applied to specify the potential emission regions for seven sources using back trajectories. Primary aluminum production, solvent usage and fugitive emission sources were mainly contributed by China. Semiconductor/electronics sources were dominantly located in Korea. Refrigerant replacement, fumigation and foam blowing agent sources were spread throughout East Asian countries. The specified potential source regions are consistent with country-based consumptions and emission patterns, verifying the PMF analysis results. The industry-based emission sources of halogenated compounds identified in this study help improve our understanding of the East Asian countries' industrial contributions to halogenated compound emissions.

Development of a pretreatment system for the analysis of atmospheric reduced sulfur compounds.

A new pretreatment system was used to evaluate a technology to analyze reduced sulfur compounds (RSCs). To conduct this research, a self-developed custom dryer (Desolvator) and a thermal desorber system (TDS) were installed in the front of GC/PFPD. The syringe pump inside the TDS was devised in such a way that it can be desorbed in a relatively low desorption temperature and low vacuum (730 Pa). When comparing water removal efficiency of the Desolvator and frequently used Nafion dryer, the removal efficiency of the Desolvator stood between 94.6 and 96.1%, considerably higher and more stable than the Nafion dryer (81.3-94.5%). Moreover, analyses were made under various conditions in order to minimize the loss of samples when analyzing sulfur compounds using the TDS, and it was determined that adsorption temperatures less than -25 °C and a flow rate of 50 mL/min were appropriate for the efficient analysis of these sulfur compounds. Moreover, the desorption flow rate and the degree of a vacuum were found to be significant variables for the RSCs desorption. Besides, it was observed that a peculiar peak was formed by thermal decomposition when some sulfur compounds were rapidly desorbed at high desorption temperatures.

Vertical variability of seawater DMS in the South Pacific Ocean and its implication for atmospheric and surface seawater DMS.

Shipboard measurements of atmospheric dimethylsulfide (DMS) and sea surface water DMS were performed aboard the R/V Onnuri across the South Pacific from Santiago, Chile to Fiji in February 2000. Hydrographic profiles of DMS, dissolved dimethylsulfoniopropionate (DMSP(d)), and particulate DMSP(p) in the upper 200m were obtained at 16 stations along the track. Atmospheric and sea surface water DMS concentrations ranged from 3 to 442pptv and from 0.1 to 19.9nM, respectively; the mean values of 61pptv and 2.1nM, respectively, were comparable to those from previous studies in the South Pacific. The South Pacific Gyre was distinguished by longitudinal-vertical distributions of DMS, DMSP(d), and DMSP(p), which was thought to be associated with the characteristic modification of biological activities that occurs mainly due to significant change in water temperature. The averaged DMS maximum appeared at 40m depth, whereas DMSP(p) and DMSP(d) maxima coincided with that of dissolved oxygen content at 60-80m. The sea-to-air fluxes of DMS were estimated to be 0.4-11.3micromold(-1)m(-2) (mean=2.8micromold(-1)m(-2)). A fairly good correlation between atmospheric DMS and sea-to-air DMS flux indicated that atmospheric DMS concentration was more sensitive to change in physical parameters than its photochemical removal process or surface seawater DMS concentrations.

Characteristic behavior of peroxyacetyl nitrate (PAN) in Seoul megacity, Korea.

We measured the concentrations of peroxyacetyl nitrate (PAN) and other photochemically reactive species, including O3, NO2, and non-methane hydrocarbons (NMHCs), in the Seoul Metropolitan area (SMA) during May through June in 2004 and 2005. PAN was determined using a fast chromatograph with luminol-based chemiluminescence detection. Mixing ratios of PAN ranged from below the detection limit (0.1ppbv) to 10.4ppbv with an average of 0.8ppbv. O3 concentrations ranged from 0 to 141ppbv. The average PAN/O3 ratio of 0.07 was higher than that observed in cities of Europe and North America (0.02) where control strategies have been enforced to reduce hydrocarbon emissions through extensively reformulated gasoline programs. Strong positive correlations between daily PAN and O3 maxima during the day demonstrate that similar photochemical factors controlled the production of these two chemicals. However, relationships between PAN and its precursors, NO2 and NMHCs, suggest that PAN production was more sensitive to NO2 than NMHCs levels whereas O3 production was limited by the overall availability of NMHCs. It is likely that the compositions of NMHCs in SMA were favorable for PAN production because of the low fractions of oxygenated compounds in automobile fuels. PAN maxima were observed around noon, which was 2-3h earlier than the much broader O3 maxima that occurred in the midafternoon. After reaching the maximum, PAN concentrations rapidly dropped within a few hours, which could be largely due to thermal destruction and to limited production under the typically low NO2 levels that occurred in the early afternoon. The heterogeneous destruction of particulate matter could be an additional sink for PAN in SMA.

Characteristics of atmospheric hydrogen peroxide variations in Seoul megacity during 2002-2004.

Atmospheric hydrogen peroxides (H(2)O(2)) and methyl hydroperoxide (CH(3)OOH) were measured in Seoul, the capital of South Korea. Experiments were performed for several days almost every month from January 2002 to April 2004. Gaseous hydroperoxide was collected in aqueous solution and determined by HPLC-fluorescence method. In general, the higher levels of H(2)O(2) were found in warm and humid air with high ozone concentrations, but lower concentrations of SO(2), NO(2), CO and PM(10). For two-year measurements, seasonal factor was the most dominant and the concentrations of H(2)O(2) were highest in summer, for which the median, mean, and upper 90% values were 0.53 ppbv, 0.81 ppbv, and 1.61 ppbv, respectively. In highly polluted metropolitan Seoul, the photochemical activity controlling H(2)O(2) variations was seemingly more sensitive to meteorological conditions than the level of chemical pollutants. It was mainly due to high emissions of pollutants, particularly NOx, which was demonstrated by the occasional occurrence of CH(3)OOH.

Atmospheric peroxides over the North Pacific during IOC 2002 shipboard experiment.

Atmospheric hydrogen peroxide and methyl hydroperoxide were determined onboard the Melville over the North Pacific from Osaka to Honolulu during May-June 2002. The concentrations of H(2)O(2) and CH(3)OOH increased from 0.64+/-0.57 ppbv and 0.27+/-0.59 ppbv in subpolar region (30-50 degrees N) to 1.96+/-0.95 ppbv and 1.56+/-1.3 ppbv in subtropical region (24-30 degrees N). The increase in concentrations towards the Equator was more pronounced for CH(3)OOH than H(2)O(2). In contrast, the levels of O(3) and CO were decreased at lower latitudes as air mass was more aged, denoted by the ratios of C(2)H(2)/CO and C(3)H(8)/C(2)H(6). CH(3)OOH concentrations showed a clear diurnal variation with a maximum around noon and minimum before sunrise. Frequently, the concentrations of peroxides remained over 1 ppbv in the dark and even gradually increased after sunset. In addition, the ratios of C(2)H(4)/C(2)H(6) and C(3)H(6)/C(3)H(8) were increased in aged subtropical air, which implies that these alkenes were emitted from the ocean surface. As a result, the reaction of these biogenic alkenes with O(3) was suggested to be a potential source for peroxides in aged marine air at lower latitudes.

DMS photochemistry during the Asian dust-storm period in the Spring of 2001: model simulations vs. field observations.

This study examines the local/regional DMS oxidation chemistry on Jeju Island (33.17 degrees N, 126.10 degrees E) during the Asian dust-storm (ADS) period of April 2001. Three ADS events were observed during the periods of April 10-12, 13-14, and 25-26, respectively. For comparative purposes, a non-Asian-dust-storm (NADS) period was also considered in this study, which represents the entire measurement periods in April except the ADS events. The atmospheric concentrations of DMS and SO2 were measured at a ground station on Jeju Island, Korea, as part of the ACE-Asia intensive operation. DMS (means of 34-52 pptv) and SO2 (means of 0.96-1.14 ppbv) levels measured during the ADS period were higher than those (mean of 0.45 ppbv) during the NADS period. The enhanced DMS levels during the ADS period were likely due to the increase in DMS flux under reduced oxidant levels (OH and NO3). SO2 levels between the two contrasting periods were affected sensitively by some factors such as air mass origins. The diurnal variation patterns of DMS observed during the two periods were largely different from those seen in the background environment (e.g., the marine boundary layer (MBL)). In contrast to the MBL, the maximum DMS value during the ADS period was seen in the late afternoon at about sunset; this reversed pattern appears to be regulated by certain factors (e.g., enhanced NO3 oxidation). The sea-to-air fluxes of DMS between the ADS and NADS periods were calculated based on the mass-balance photochemical-modeling approach; their results were clearly distinguished with the values of 4.4 and 2.4 micromole m(-2) day(-1), respectively. This study confirmed that the contribution of DMS oxidation to observed SO2 levels on Jeju Island was not significant during our study period regardless of ADS or NADS periods.

Assessment of the photochemistry of OH and NO3 on Jeju Island during the Asian-dust-storm period in the spring of 2001.

In this study, we examined the influence of the long-range transport of dust particles and air pollutants on the photochemistry of OH and NO3 on Jeju Island, Korea (33.17 degrees N, 126.10 degrees E) during the Asian-dust-storm (ADS) period of April 2001. Three ADS events were observed during the periods of April 10-12, 13-14, and 25-26. Average concentration levels of daytime OH and nighttime NO3 on Jeju Island during the ADS period were estimated to be about 1x10(6) and 2x10(8) moleculescm(-3) ( approximately 9 pptv), respectively. OH levels during the ADS period were lower than those during the non-Asian-dust-storm (NADS) period by a factor of 1.5. This was likely to result from higher CO levels and the significant loading of dust particles, reducing the photolysis frequencies of ozone. Decreases in NO3 levels during the ADS period was likely to be determined mainly by the enhancement of the N2O5 heterogeneous reaction on dust aerosol surfaces. Averaged over 24 h, the reaction between HO2 and NO was the most important source of OH during the study period, followed by ozone photolysis, which contributed more than 95% of the total source. The reactions with CO, NO2, and non-methane hydrocarbons (NMHCs) during the study period were major sinks for OH. The reaction of N2O5 on aerosol surfaces was a more important sink for nighttime NO3 during the ADS due to the significant loading of dust particles. The reaction of NO3 with NMHCs and the gas-phase reaction of N2O5 with water vapor were both significant loss mechanisms during the study period, especially during the NADS. However, dry deposition of these oxidized nitrogen species and a heterogeneous reaction of NO3 were of no importance.

Monitoring of reduced sulfur compounds in the atmosphere of Gosan, Jeju Island during the Spring of 2001.

The atmospheric concentrations of dimethylsulfide (DMS) and carbon disulfide (CS2) were measured concurrently with relevant environmental parameters at Gosan, Jeju Island, Korea during 5-26 April 2001. The mean concentrations for these two compounds were 18.7+/-17.9 and 6.4+/-9.9 pptv, respectively. Results of our analysis indicated that relative temporal variations between DMS and CS2 can be best described by dividing the whole data set into three different periods which reflect the variable transport patterns of air masses into the study area. (Periods I, II, and III denote: 5-10, 10-18, and 19-26 April.) The environmental conditions during those three periods varied greatly. The effects of continental and/or oceanic processes were evident for certain periods, yielding diverse relationships between DMS and CS2 in both absolute and relative terms. Most observed variations were best explained in terms of an interplay between source/sink processes and air mass transport patterns. The sea-to-air flux of DMS, when estimated using our measurement data during this study period, was approximately 4 micromole m(-2)d(-1).

Observations of aerosol-bound ionic compositions at Cheju Island, Korea.

To investigate the regional cycle of aerosols and their ionic constituents, three field intensive campaigns were conducted during fall and winter of 1997 and spring of 1998. The concentrations of most ionic species were found to decrease significantly across fall, winter, and spring such that the sum for all cation (and anion) species of each season is computed as: 193 > 96 > 73.7 nequiv m(-3) (and 240 > 104 > 51.5 nequiv m(-3)). To examine the fundamental characteristics of aerosol compositions in the study area, we conducted correlation analysis in various manners. The results indicated that the concentrations of major ionic species were strongly affected by some meteorological parameters including wind speed. It was also seen that relative strengths of correlations between important parameters (e.g., between wind speed and most of major inorganic species) maintain close relationships with the factors associated with the air mass origin. In addition, the results of factor analysis indicated the existence of at least three major sources in the study area which include: sea-salt aerosol, secondary aerosol, and organic aerosol component. The springtime occurrence of unexpectedly low concentrations of most ionic constituents is found to sensitively reflect the influence of the inflow of southeasterly winds that prevailed during spring, while it is not common for that season of the year. Because most of those changes are closely tied with the variabilities in the regional circulation patterns for each measurement period, assessment of the ionic composition in concert with the temporal variations of meteorological conditions provided valuable insights into the source signals of different air masses that passed by the study area.