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Dry conditions associated with the El Niño–Southern Oscillation (ENSO) and a positive Indian Ocean Dipole (IOD) are known to have caused major fire pollution events and intense carbon emissions over a vast spatial expanse of Indonesia in October 2006 and 2015. During these two events, a substantial increase in the carbon monoxide (CO) mixing ratio was detected by in situ measurements at Lulin Atmospheric Background Station (LABS; 23.47∘ N 120.87∘ E; 2862 ma.s.l.) in Taiwan, which is the only background station in the subtropical western North Pacific region. Compared to the long-term October mean (2006–2021), CO was elevated by ∼ 47.2 ppb (parts per billion; 37.2 %) and ∼ 36.7 ppb (28.9 %) in October 2006 and 2015, respectively. This study delineates plausible pathways for the CO transport from Indonesia to LABS using Measurement of Pollution in the Troposphere (MOPITT) CO observations and Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) reanalysis products (winds and geopotential height – GpH). Two simultaneously occurring transport pathways were identified, namely (i) horizontal transport in the free troposphere and (ii) vertical transport through the Hadley circulation (HC). The GpH analysis of both events revealed the presence of a high-pressure anticyclone over the northern part of the South China Sea (SCS), which played an important role in the free-tropospheric horizontal transport of CO. In this scenario, CO in the free troposphere is transported on the western edge of the high-pressure system and then driven by subtropical westerlies to LABS. Simultaneously, uplifted CO over Indonesia can enter the HC and be transferred to subtropical locations such as LABS. The vertical cross section of the MOPITT CO and MERRA-2 vertical pressure velocity supported the transport of CO through the HC. Furthermore, the results revealed a distinct HC strength in two events (higher in 2006 compared to 2015) due to the different ENSO conditions. Overall, the present findings can provide some insights into understanding the regional transport of pollution over Southeast Asia and the role of climate conditions on transport pathways.

Emission inventories are a critical basis for air quality and climate modeling, as well as policy decisions. Non-methane volatile organic compounds (NMVOCs) are key precursor compounds in ozone and secondary organic aerosol formation. Accurately representing NMVOCs in emission inventories is crucial for understanding atmospheric chemistry, the impact of policy measures, and climate projections. Improving NMVOC representation in emission inventories is fraught with challenges, ranging from the lack of (long-term) NMVOC measurements, limited efforts in updating emission factors, to the diversity of NMVOC species reactivity. Here we take an initial step to evaluate the representation of urban NMVOC speciation in an emission inventory (EDGARv4.3.2 and EDGARv6.1) at the global level. To compare the urban measurements of NMVOCs to the emission inventory estimates, ratios of individual NMVOCs to acetylene are used. Owing to limitations in measurement data and grouping of NMVOCs in emission inventories, the comparison includes only a limited number of alkanes, alkenes, and aromatics. Results show little to no agreement between the ratios in the observations and those in the global emission inventory for the species compared (r2 0.01–0.20). This could be related to incorrect speciation profiles and/or spatial allocation of NMVOCs to urban areas. Regional emission inventories show better agreement among the ratios (r2 0.43–0.70). The inclusion of oxygenated species in NMVOC measurements, as well as greater global coverage of measurements could improve representation of NMVOC species in emission inventories, and a mosaic of regional inventories may be a better approach.

Dry conditions associated with El Niño and a positive Indian Ocean Dipole (IOD) are known to have caused major fire pollution events and intense carbon emissions over a vast spatial expanse of Indonesia in October 2006 and 2015. During these two events, a substantial increase in carbon monoxide (CO) mixing ratio was detected by in-situ measurements at Lulin Atmospheric Background Station (LABS, 23.47° N 120.87° E, 2,862 m ASL) in Taiwan, the only background station in the subtropical western North Pacific region. Compared to the long-term October mean (2006–2021), CO was elevated by ~47.2 ppb (37.2 %) and ∼36.7 ppb (28.9 %) in October 2006 and 2015, respectively. In this study, plausible pathways for CO transport from Indonesia to LABS are delineated by using MOPITT CO observations and MERRA-2 reanalysis products (winds and geopotential height (GpH)). Two simultaneously occurring transport pathways were identified: (i) horizontal transport in the free troposphere and (ii) vertical transport through the Hadley circulation (HC). The GpH analysis of both events revealed the presence of a high-pressure anticyclone over the northern part of the South China Sea (SCS), which played an important role in the free tropospheric horizontal transport of CO. In this scenario, CO in the free troposphere is transported on the western edge of the high-pressure system and then driven by subtropical westerlies to LABS. Simultaneously, uplifted CO over Indonesia can enter the HC and transfer to subtropical locations such as LABS. The vertical cross-section of MOPITT CO and MERRA-2 vertical pressure velocity supported the transport of CO through the HC. Further, the results revealed a distinct HC strength in two events (higher in 2006 compared to 2015) due to the different El Niño conditions. Overall, the present findings can provide some insights into understanding the regional transport of pollution over Southeast Asia and the role of climate conditions on transport pathways.

A near-real-time (NRT) aerosol forecast and diagnostic approach is developed based on the system of Infusing satellite Data into Environmental Applications for East Asia, herein denoted as IDEA-EA. The design incorporates a 0.5-degree Global Forecast System (GFS) and Visible Infrared Imaging Radiometer Suite (VIIRS) aerosol and cloud retrievals for meteorological and remote sensing inputs. The primary output of IDEA-EA includes aerosol forward and backward air mass trajectory forecasts, migration visualization, and data synthesis purposed for NRT aerosol detection, monitoring, and source tracing in East Asia. Two aerosol episodes of Southeast Asia (SEA) biomass burning and Chinese haze infusion with Gobi dust are illustrated by IDEA-EA to demonstrate its forecast and source tracing capabilities. In the case of SEA biomass burning (late March 2021), forward trajectories of IDEA-EA forecasted air masses with high aerosol optical depth (AOD) from SEA affecting Taiwan. The IDEA-EA forecasts were verified by increased AOD and surface PM

Lulin Atmospheric Background Station (LABS, 23.47°N, 120.87°E; 2862 m above sea level) at the summit of Mount Lulin in central Taiwan was established in spring 2006 and is the only high-altitude background station over western Pacific region in East Asia to study the impact of various air pollutants through long-range transport. Continuous in-situ measurements of equivalent black carbon (EBC) and carbon monoxide (CO) concentrations were made at LABS from June 2012 to May 2014 and their association was investigated in this study. The highest monthly concentration of EBC (median; 840 ng m−3) and CO (212 ppbv) in March were primarily attributed to the westerly winds coupled with biomass-burning (BB) emissions from Southeast Asia (SEA) region. The association of EBC and CO was weak at LABS possibly due to the influence of dissimilar air masses from various sources, and scavenging or dilution of EBC during the long-range atmospheric transport to Mt. Lulin. The mean ΔEBC/ΔCO ratio (slope of least-squares regression line of ΔEBC-ΔCO scatterplot; where Δ indicates surplus amounts with respect to the background value) was found the most significant in March (5.3 ng m−3 ppbv−1 or 7.3 × 10−3 g of carbon as EBC per gram of carbon as CO). On the basis of episodic cases, the mean ΔEBC/ΔCO ratios at LABS were estimated to be 6.1, 8.0, and 2.4 ng m−3 ppbv−1 for SEA BB emissions, southern China mixed pollution, and northern China mixed pollution, respectively. A total of 32% loss in EBC aerosols (6.4% of EBC removal per day) was estimated for the atmospheric transport of BB emissions from SEA region to LABS. This study provides needful information to understand the ΔEBC/ΔCO ratios at a remote site and would be used in model simulations to evaluate BC aging and scavenging over western Pacific region in East Asia.

East Asian dust episodes have a multitude of impacts, including on human health, environment, and climate over near-source and receptor regions. However, the mechanistic understanding of the synoptic conditions of these outbreaks at different altitude layers, and their eventual environmental impacts are less studied. The present study analyzed the synoptic transport patterns of East Asian dust during multiple dust generation episodes that occurred over only a few days apart in northern China, and which eventually delivered high PM

In this study, we investigated the influences of stratospheric intrusion (SI) on the tropospheric ozone (O3) at Lulin Atmospheric Background Station (LABS, 2862 m MSL), a representative high-altitude site in East Asia. Thresholds for surface O3, carbon monoxide (CO), and relative humidity (RH) were set to identify SI events at LABS. Accordingly, 3.0% of the observation period was impacted by SI leading to a net O3 enhancement of 14.6 ± 9.6 ppb at LABS. Factors influencing the two most common SI event types affecting LABS, i.e. tropopause folds (major) and tropical cyclones (minor), were discussed. We utilized ERA5 reanalysis products (meteorology and O3) to trace and analyze the pathway and mechanism of these SI types over sub-tropical East Asia. With a conceptual model, we illustrate two driving circulations for SI air at ∼200 hPa that affect subtropical East Asia. SI air generated due to Rossby wave breaks are transported equatorward and downward into the troposphere. The southern westerlies passing south of the Tibetan Plateau can further push the SI air eastward. A SI event in 2007 with a significant O3 enhancement of 43.4 ppb caused by typhoon Nari was detected and discussed to depict the second SI type.

We exploited a novel sampling vehicle, a multi-rotor drone carrying a remote-controlled whole air sampling device, to collect aerial samples with high sample integrity and preservation conditions. An array of 106 volatile organic compounds (VOCs), CO, CH4, and CO2 were analyzed and compared between the aerial samples (300-m height) and the ground-level samples in pairs to inspect for vertical mixing of the trace gases at a coastal site under three different meteorological conditions of local circulation, frontal passage, and high-pressure peripheral circulation. A rather homogeneous composition was observed for the sample pairs immediately after the frontal passage, indicating a well-mixed condition below 300 m. In contrast, inhomogeneous mixing was observed for the sample pairs under the other two conditions (local circulation and high-pressure peripheral circulation), suggesting different layers of air masses. Furthermore, information of unique source markers, composition profiles, and lifetimes of compounds were used to differentiate the origins of the air masses aloft and at the surface to substantiate the observed inhomogeneity. The study demonstrates that, with the availability of the near-surface aerial sampling coupling with in-laboratory analysis, detailed compositions of trace gases can now be readily obtained with superior data quality. Based on the distinctive chemical compositions, the sources, transport, and atmospheric mixing of the airborne pollutants in the near-surface atmosphere can be better studied and understood.

An integrated sampling technique, dubbed trigger sampling, was developed to capture characteristic industrial emissions or plumes. In the field experiment, a hydrogen sulfide (H2S) analyzer was used as the triggering instrument at the boundary of a refinery plant due to frequent complaints of foul smell from local residents. Ten episodic samples were captured when the H2S level surpassed the prescribed trigger level of 8.5 ppbv over a three-day period. Three non-episodic (blank) samples and 23 road-side samples were also collected for comparison. All the 36 flask samples were analyzed by gas chromatography–mass spectrometry/flame ionization detection (GC–MS/FID) for 108 volatile organic compounds (VOCs). The total VOC abundance of the event samples was exceedingly higher than the non-episodic samples by over 80 times in the extreme case. Alkanes were found to be the dominant constituents in the event samples, amounting to over 90% of the total VOC concentrations vs. only 30–40% for the blank and metropolitan samples. In addition, light alkanes in the event samples were highly correlated with the trigger species H2S (R2 = 0.82), implying their common origin. The matrix of chemical composition vs. sample types permitted easy visualization of the dominance of light alkanes for the event samples compared to other types of samples. Principle component analysis (PCA) identified two major contributors to cover 93% of the total variance arising from the 36 samples, further quantifying the distinction of the triggered episodic samples from the contrast samples. The proposed trigger sampling is a coupling of fast-and-slow measurement techniques. In this example, the fast-response H2S analyzer served to “guide” sampling to capture industrial plumes which were then characterized by a relatively slow method of GC–MS/FID for detailed chemical composition representative of the prominent sources.

The importance of Asian countries towards increase of atmospheric pollutants is being examined critically in recent times. In this context, we carried out analysis of nitrates separated from aerosol samples collected during 2010 from Mt. Lulin (NOAA code: LLN), Taiwan, located at an altitude of 2 862 m above sea level. Large temporal variations are seen in δ15N, δ18O and Δ17O values of the nitrate, with day-to-day variations comparable to the seasonal amplitude. The δ15N values of nitrate are found to be higher in spring months (March–April; −1±3‰) and lower in summer (June–September; −5±3‰). Similarly, the δ18O (69 ± 15‰ versus 32 ± 13‰) and Δ17O (23 ± 5‰ versus 12 ± 4‰) values are higher in spring and lower in summer. The lowest δ18O value observed was 10.8‰. The higher values of δ15N in spring could be attributed to enhanced contribution from fossil fuel combustions, especially burning of coal in nearby Asian countries like China, with the resultant pollutants being brought to the Lulin station by long-range transport. An alternative explanation is the isotopic exchange reaction between N2O5 and HNO3 that elevates the δ15N value in nitrate. The oxygen isotope variability is explained by changes in contribution from two major pathways of nitrate formation from its precursor NOx molecules. During spring time, nitrate formation via the N2O5 pathway is dominant, resulting in higher values of both δ18O and Δ17O. In contrast, during summer, formation involving HO2/RO2 radicals becomes important, producing lower values of δ18O and Δ17O. A chemistry box model was used to study the nitrate formation pathways through oxidation of NO and NO2 via formation of NO2 and NO3−/HNO3. Both the model results and observations suggest that for the formation of NO2 from NO, the pathway via O3 is more active in spring, whereas in summer the pathway via HO2/RO2 radicals predominates. For the subsequent formation of NO3− and HNO3, the OH pathway is more active in summer than in spring. These suggestions are supported by a wind rose diagram and back trajectory analysis of air masses bringing the precursor NOx to the sampling site.

Inter-annual variations of atmospheric isoprene in a major metropolis, Taipei, were reported based on a two-year continuous measurements of non-methane hydrocarbons (NMHCs) with an hourly resolution. It is by far the largest dataset ever collected in the urban subtropical environment with thriving vegetation and traffic flows. The dataset revealed the detailed interplay between the two major sources of biogenic and vehicular throughout the year. To separate the vehicular contribution from the biogenic one for the ambient isoprene, ethylene was used as an indicator of traffic emissions. While dramatic surge of isoprene was observed at noontime in hot months with the highest average peak mixing ratio of 1.6 ppbv in August, its abundance decreased to 0.2 ppbv on average in cold months. The vehicular contribution to ambient isoprene was largely masked over by the noontime surge of isoprene in hot seasons, but was still able to be vaguely observed on the slopes of the isoprene peaks mimicking the rush-hour features of ethylene. In winter, the diurnal variations of isoprene were very similar to those of ethylene, which suggests that ambient isoprene in cold months was almost of traffic origin. This study based on the continuous dataset could enhance the key findings in previous flask studies in the same metropolis. While canister sampling had a major advantage of area coverage, the highly time-resolved fixed-site monitoring could better reveal the evolution process from a biogenically overwhelmed condition in hot months to the condition where the biogenic source weakened to reveal the traffic source in cold months.

Air samples were collected at Mt. Fuji Research Station (FRS) for the measurements of volatile organic compounds (VOCs) in the summers of 2015 and 2016. In this study, 24 compounds were analyzed, of which only 12 halocarbons were quantified in 2015. The average total concentrations of target VOCs were 2.62 ± 1.38 and 2.99 ± 0.95 ppb in 2015 and 2016, respectively. The concentrations of individual VOCs ranged from a few ppt to a few ppb, indicating a highly inhomogeneous feature at the FRS. A cluster analysis of 3-day backward trajectories was performed for the sampling time. Except for the aromatic compounds, the VOCs showed relatively low concentrations in association with air masses originating from the coastal region in the low latitudes (15°N–35°N) of East Asia in 2015. By contrast, the clusters with elevated VOC concentrations mainly came from the high latitudes (35°N–60°N) of the Asian continent in 2016. No particular diurnal pattern was found for VOCs and CO, which might have resulted from suppressed mountain-valley winds at the FRS. Halocarbons regulated by the Montreal Protocol showed low variability and were in favorable agreement with background values at the Gosan station (GSN) and those reported in the literature. Other partially halogenated compounds with higher variability, such as CH3Cl and CHCl3, showed discrepancies at the FRS and GSN. 1,2-dichloroethane (R-150), 1,1-dichloroethane (R-150a), and 1,4-dichlorobenzene (p-DCB) were also measured at the FRS with concentrations of 24 ± 14, 38 ± 13, and 13 ± 10 ppt, respectively, in 2015. A close relationship between n-pentane and i-pentane with R2 more than 0.85 was found in both 2015 and 2016. Low ratios of n/i-pentane ranging from 0.25 to 0.67 were observed in the free troposphere at the FRS, comparable to most mountain stations.

Perfluorocarbons (PFCs) are potent greenhouse gases with Global Warming Potentials up to several thousand times greater than CO2 on a 100-year time horizon. The lack of any significant sinks for PFCs means that they have long atmospheric lifetimes on the order of thousands of years. Anthropogenic production is thought to be the only source for most PFCs. Here we report an update on the global atmospheric abundances of the following PFCs, most of which have for the first time been separated according to their isomers: c-octafluorobutane (c-C4F8), n-decafluorobutane (n-C4F10), n-dodecafluoropentane (n-C5F12), n-tetradecafluorohexane (n-C6F14), and n-hexadecafluoroheptane (n-C7F16). Additionally, we report the first data set on the atmospheric mixing ratios of perfluoro(2-methylpentane) (i-C6F14). The existence and significance of PFC isomers has not been reported before, due to the analytical challenges of separating them. The time series spans a period from 1978 to the present. Several datasets are used to investigate temporal and spatial trends of these PFCs: time series of air samples collected at Cape Grim, Australia, from 1978 to the start of 2018; a time series of air samples collected between July 2015 and April 2017 at Tacolneston, UK; and intensive campaign-based sampling collections from Taiwan. Although the remote background Southern Hemispheric Cape Grim time series indicates that recent growth rates of most of these PFCs are lower than in the 1990s, we continue to see significantly increasing mixing ratios that are between 6 % to 27 % higher by the end of 2017 compared to abundances measured in 2010. Air samples from Tacolneston show a positive offset in PFC mixing ratios compared to the Southern Hemisphere baseline. The highest mixing ratios and variability are seen in air samples from Taiwan, which is therefore likely situated much closer to PFC sources, confirming predominantly Northern Hemispheric emissions for most PFCs. Even though these PFCs occur in the atmosphere at levels of parts per trillion molar or less, their total cumulative global emissions translate into 833 million metric tonnes of CO2 equivalent by the end of 2017, 23 % of which has been emitted in the last eight years. Almost two-thirds of the CO2 equivalent emissions are attributable to c-C4F8, which currently also has the highest emission rates that continue to grow. Despite this, the sources of all PFCs covered in this work remain poorly constrained and reported emissions in global databases do not account for the abundances found in the atmosphere.

Instead of manual sampling in a random way near a source area, this study used trigger sampling guided by an analyzer at a fixed site near a refinery plant to obtain the chemical composition of volatile organic compounds (VOCs) representative of the source. The analyzer was built in-house to measure total VOC (TVOC) levels by subtracting methane from total combustible organic compounds (TOC) with flame ionization detection. The analyzer with minute resolution provided instantaneous measurements of TVOCs to trigger canister sampling at the moments of VOC plumes in a source area. The chemical composition of the 13 trigger samples were compared with the other non-trigger samples randomly collected either within the refinery or on an urban street. All samples were analyzed by gas chromatography-mass spectrometry/flame ionization detection (GC-MS/FID) for detailed speciation. High agreement in total VOC abundance between the analyzer and GC-MS/FID indicates internal consistency of the two techniques and the robustness of the TVOC analyzer to guide sampling of VOC plumes. The trigger samples showing very high consistency in the overall composition imply that sampling at the right moments of plume arrivals can facilitate characterization of the source profiles, which can hardly be achieved by random sampling. The coupling of the fast-and-slow analytical techniques to guide sampling is proven to be an effective means to probe source characteristics.

Springtime biomass burning (BB) in peninsular Southeast Asia (PSEA) has a large impact on the downwind air quality as has been frequently observed at the Lulin Atmospheric Background Station (LABS). Numerous PSEA BB long-range transport events have been observed at LABS in the past decade, of which the biggest event (based on the carbon monoxide (CO) mixing ratio and particulate matter (PM) loading) occurred on March 18, 2009. In this study, for the first time, in-situ observations from LABS, MERRA-2 reanalysis data, and satellite data were combined to elucidate this remarkable event. This event lasted over 29 h and seriously impacted the air quality at LABS. Average concentrations (±S.D.) of CO, ozone (O3), and PM10 were 586.2 ± 164.5 ppb, 105.2 ± 23.4 ppb, and 90.4 ± 24.4 μg m−3, respectively, which were enhanced ranging from 98% to 280% over the March 2009 average. Furthermore, significant increases in toxic air pollutants (e.g., gaseous elemental mercury (GEM) and dibenzo-p-dioxin/furan) concentrations were also observed, implying a severe impact from BB smoke on ecosystems and human health. The transport pathway and BB smoke layer height were investigated with backward trajectories, daily satellite aerosol products, and lidar observations. The mean SSA440 value of 0.87 suggested that the plume contained highly adsorbing aerosols, and the high char-EC/soot-EC ratio (low-temperature elemental carbon/high-temperature elemental carbon) of 29.4 suggested predominance of BB aerosols. In addition, plume aging indicators (e.g., ΔGEM/ΔCO, ΔO3/ΔCO, char-EC/soot-EC) suggest the BB plume was only weakly aged (i.e. low air mass intermixing, low chemical transformation, low cloud interaction) and in a nearly pristine state during the whole of the long-range transport. This event study can serve as a valuable benchmark when identifying unaged BB plumes that have been transported from PSEA to LABS (>2000 km) and will be useful for characterizing PSEA BB and its impact on greater Asia environment.

An automated gas chromatographic system aimed at performing unattended measurements of ambient volatile organic compounds was configured and tested. By exploiting various off-the-shelf components, the thermal desorption unit was easily assembled and can be connected with any existing commercial gas chromatograph in the laboratory to minimize cost. The performance of the complete thermal desorption gas chromatographic system was assessed by analyzing a standard mixture containing 56 target nonmethane hydrocarbons from C2 -C12 at sub-ppb levels. Particular attention was given to the enrichment efficiency of the C2 compounds, such as ethane (b.p. = -88.6°C) and ethylene (b.p. = -104.2°C), due to their extremely high volatilities. Quality assurance was performed in terms of the linearity, precision and limits of detection of the target compounds. To further validate the system, field measurements of target compounds in ambient air were compared with those of a commercial total hydrocarbon analyzer and a carbon monoxide analyzer. Highly coherent results from the three instruments were observed during a two-month period of synchronized measurements. Moreover, the phenomenon of opposite diurnal variations between the biogenic isoprene and anthropogenic species was exploited to help support the field applicability of the thermal desorption gas chromatographic method.

This study aimed to investigate aerosol chemical characteristics and to obtain the chemical profile of near-source biomass burning (BB) aerosols at a site (675 m a.s.l.) in Sonla, Northern Vietnam. Particulate matter (PM) with an aerodynamic diameter less than or equal to 2.5 μm (PM_(2.5)) was collected over a 24 h sampling period as part of the Seven South East Asian Studies (7-SEAS) campaign. The studies were conducted when BB was highly active - that is, in the spring of 2012 and 2013. The collected particles were analyzed for carbonaceous fractions and water-soluble components, in addition to the mass concentration. Data obtained were further analyzed to determine the stable species profile by classifying the 5-day air-mass backward trajectories. The average PM_(2.5) mass concentrations were 51 ± 19 μg m^(-3) and 57 ± 27 μg m^(-3) in 2012 and 2013, respectively. Carbonaceous contents dominated BB aerosol, with 59% ± 9% and 58% ± 9% in organic carbon (OC) and 9% ± 3% and 10% ± 3% in elemental carbon (EC) of PM_(2.5) in 2012 and 2013, respectively. Of the 8 carbonaceous fractions analyzed thermo-optically for PM_(2.5), OC3 (evolution temperature at 280°C-480°C) was most abundant in OC fractions, and EC1-OP (elemental carbon evolved at 580°C minus the pyrolized OC fractions) was predominant in EC fractions in most occasions. Among the measured water-soluble inorganic ions, NH_4^+ and SO_4^(2-) widely varied, indicating the influence of different trajectory origins. This finding was confirmed by trajectory classification of aerosol data. The trajectories were also distinguished with respect to char-EC to soot-EC ratio, and water-soluble OC. These characteristics were highest in the trajectory from the BB source area.

This study presents measurements of aerosol chemical properties at Sonla, northern Vietnam (675 m a.s.l.) during spring time, when biomass burning (BB) was very active in the northern Indochina Peninsula, as part of the 7-SEAS (Seven South East Asian Studies) campaign in 2013. The gas chromatography-mass spectrometry (GC-MS) analysis of BB markers in 14 selected samples indicated that mixed softwood, hardwood, grass, and non-woody vegetation were burned. More than 50 organic compounds including levoglucosan, lignin and resin products, sugar and sugar alcohol compounds, fatty acids, phthalate esters, aromatic acids, poly-acids, and biogenic oxidation products (e.g., 2-methyltetrols, alkene triols, 3-hydroxyglutaric acid) were measured in PM_(2.5). Levoglucosan, a BB tracer, was the predominant species among aerosol sugars, with an average concentration of 1.62 ± 0.89 μg m^(-3), comprising 2.23 ± 0.5% of PM_(2.5) mass. For the collection period of the selected samples, backward air mass trajectories were classified into the source regions of Indochina (BBIC), southern China (BBSC), and the South China Sea (BBSS). All resolved molecular compounds show their dominance on the trajectory from BBIC, verifying the BB smoke origin of that region. Trajectory classification provides additional information, such as higher level of diethyl phthalate associated with BBSC trajectory, revealing urban or industrial influence, and more low-molecular-weight than high-molecular-weight fatty acids, indicating distributions with more microbial and lesser plant wax/vegetation burning contributions along the BBSC trajectory. In addition, we report, for the first time, stable carbon isotopic data (δ^(13)C) for PM_(2.5) aerosols in northern Vietnam, which ranged from -26.6 to -25.4 per mille in PM_(2.5), indicating contributions from burning of C_3 plants and fossil fuel combustion.

The spring 2015 deployment of a suite of instrumentation at Doi Ang Khang (DAK) in northwestern Thailand enabled the characterization of air masses containing smoke aerosols from burning predominantly in Myanmar. Aerosol Robotic Network (AERONET) Sun photometer data were used to validate Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 6 "Deep Blue" aerosol optical depth (AOD) retrievals; MODIS Terra and Aqua provided results of similar quality, with correlation coefficients of 0.93-0.94 and similar agreement within expected uncertainties to global-average performance. Scattering and absorption measurements were used to compare surface and total column aerosol single scatter albedo (SSA); while the two were well-correlated, and showed consistent positive relationships with moisture (increasing SSA through the season as surface relative humidity and total columnar water vapor increased), in situ surface-level SSA was nevertheless significantly lower by 0.12-0.17. This could be related to vertical heterogeneity and/or instrumental issues. DAK is at approximately 1,500 meters above sea level in heterogeneous terrain, and the resulting strong diurnal variability in planetary boundary layer depth above the site leads to high temporal variability in both surface and column measurements, and acts as a controlling factor to the ratio between surface particulate matter (PM) levels and column AOD. In contrast, while some hygroscopic effects were observed relating to aerosol particle size and Angstrom exponent, relative humidity variations appear to be less important for this ratio here. As part of the Seven South-East Asian Studies (7-SEAS) project, the Biomass-burning Aerosols & Stratocumulus Environment: Lifecycles and Interactions Experiment (BASELInE) was intended to probe physicochemical processes, interactions, and feedbacks related to biomass burning aerosols and clouds during the spring burning season (February-April) in southeast Asia (SEA).

Trace gases and aerosols (particularly biomass-burning aerosols) have important implications for air quality and climate studies in Southeast Asia (SEA). This paper describes the purpose, operation, and datasets collected from NASA Goddard Space Flight Center’s (NASA/GSFC) Chemical, Optical, and Microphysical Measurements of In-situ Troposphere (COMMIT) laboratory, a mobile platform designed to measure trace gases and optical/microphysical properties of naturally occurring and anthropogenic aerosols. More importantly, the laboratory houses a specialized humidification system to characterize hygroscopic growth/enhancement, a behavior that affects aerosol properties and cloud-aerosol interactions and is generally underrepresented in the current literature. A summary of the trace gas and optical/microphysical measurements is provided, along with additional detail and analysis of data collected from the hygroscopic system during the 2015 Seven South-East Asian Studies (7-SEAS) field campaign. The results suggest that data from the platform are reliable and will complement future studies of aerosols and air quality in SEA and other regions of interest.

Dioxin and dioxin-like compounds such as polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs) are persistent organic pollutants (POPs) generated through human activities. In recent times, extreme weather events such as wild fires have significantly affected the remobilization and successive bioavailability of PCDD/Fs. In Seven South East Asian Studies (7-SEAS), a Southeast Asia biomass burning event that influenced the environmental outcome and transport of PCDD/Fs in Taiwan was investigated on the basis of a climate change situation. During the 7-SEAS campaign on 20-28 March, 2011, significantly high levels of atmospheric PCDD/Fs were observed at Lulin mountain in central Taiwan and in the source region of Northern Vietnam (Son La). Measurements indicated that the patterns of variation of atmospheric PCDD/Fs at both locations were similar, but with a time lag of approximately 2 to 3 days. At Mt. Lulin, there was a significant increase of PCDD/F concentrations from 3.69 to 11.1 fg I-TEQ m^(-3) and 3.32 to 19.1 fg I-TEQ m^(-3) to reach their peaks on 23 March and 26 March. In this study, a tracer simulation using the Weather Research and Forecasting model coupled with chemistry was conducted to investigate the effects of the Southeast Asia biomass burning. The combined results of air mass paths simulation and satellite data can be used as evidence supporting the hypothesis that the source of the increasing PCDD/F level is originated from biomass-burning regions in Indochina, particularly Northern Vietnam and Northern Thailand.

Hydrochlorofluorocarbon HCFC-133a (CF3CH2Cl) is an anthropogenic compound whose consumption for emissive use is restricted under the Montreal Protocol. A recent study showed rapidly increasing atmospheric abundances and emissions. We report that, following this rise, the at- mospheric abundance and emissions have declined sharply in the past three years. We find a Northern Hemisphere HCFC-133a increase from 0.13 ppt (dry air mole fraction in parts-per-trillion) in 2000 to 0.50 ppt in 2012–mid-2013 followed by an abrupt reversal to 0.44 ppt by early 2015. Global emissions derived from these observations peaked at 3.1 kt in 2011, followed by a rapid decline of 0.5 kt yr−2 to 1.5 kt yr−1 in 2014. Sporadic HCFC-133a pollution events are detected in Europe from our high-resolution HCFC-133a records at three European stations, and in Asia from sam- ples collected in Taiwan. European emissions are estimated to be

Speciated hydrocarbons (NMHCs) and CO were simultaneously measured by evenly distributed samples along the entire length (12.9 km) of the tunnel in different traffic conditions. Four passes (two round-trips) were made at four different fleet speeds (i.e., 45, 65, 75 and 85 km h−1). Individual NMHC and CO mixing ratios were observed to be sensitive to the fleet speed, which is compounded by driving conditions and traffic volumes. We propose using ratios of NMHCs to CO to cancel out the factor of traffic volumes to determine CO-normalized NMHC emissions, such that a less biased comparison can be made between different fleet speeds in this study and even between different studies. Moreover, to obtain robust CO-normalized NMHC emissions which are sufficiently representative of the fleet speeds, only samples collected deep inside the long-tunnels between 8 and 12 km were used. Of the 61 target NMHCs, isomers of butane, pentane, ethylene, acetylene and toluene were the most abundant species regardless of the driving conditions. We observed that different driving conditions not only affected the emission strengths but also altered the compositions of the NMHCs. To simplify the data analysis, the target NMHCs were classified into four chemical groups, i.e., alkanes, alkenes, aromatics and alkynes. For the slower and more congested driving condition (fleet speed = 45 km h−1), the CO-normalized NMHC emissions were the highest, with alkanes contributing to approximately 60% of the total NMHC levels, suggesting poorer fuel utilization at slower driving conditions. In terms of the CO-normalized ozone forming potentials (OFPs), the contribution of the alkanes diminished dramatically to approximately 9–22% despite their high weight percentage, whereas the contribution of the alkenes was enhanced significantly to 50–60% from their weight percent of only approximately 26%. Our total NMHC to CO ratios of 0.06–0.20 for the four fleet speeds generally fall within the range constrained by many other tunnel or chassis dynamometer studies; however, the sensitivity to the driving conditions and the robustness with the long-tunnel data are better demonstrated in this study.

Atmospheric CO were monitored at the Lulin Atmospheric Background Station (LABS) with an elevation of 2862 m AMSL from April 2006 to April 2011 by the in-situ non-dispersive infrared (NDIR) spectrometer and weekly flask sample collections via collaboration with NOAA/ESRL/GMD. In general very coherent results were observed between the two datasets, despite a slight difference between the two. A distinct seasonal pattern of CO was noticed at the LABS with a springtime maximum and a summertime minimum, which was predominately shaped by the long-range transport of biomass burning air masses from Southeast Asia and oceanic influences from the Pacific, respectively. Diurnal cycles were also observed at the LABS, with a maximum in late afternoon and a minimum in early morning. The daytime CO maximum was most likely caused by the up-slope transport of lower elevation air. After filtering out the possibly polluted data points from the entire dataset with a mathematic procedure, the mean background CO level at the LABS was assessed as 129.3 ± 46.6 ppb, compared to 149.0 ± 72.2 ppb prior to the filtering. The cluster analysis of the backward trajectories revealed six possible source regions, which shows that air masses originating from the Westerly Wind Zone were dominated in spring and winter resulting in higher CO concentrations. As a contrast, the oceanic influences from the Pacific were found mostly in summer, contributing a lower seasonal CO concentration throughout a year.

Hourly observations of 56 non-methane hydrocarbons (NMHCs) performed by a network of photochemical assessment monitoring stations (PAMS) at 11 locations across Taiwan were used to evaluate 56 speciated emissions and the resulting simulations of an air quality model. Based on the PAMS observations at two urban sites, emission modification was made for the 56 PAMS species in the model. To further test the applicability of this emission correction approach, the same modified emissions were subject to seven different meteorological conditions and comparison with observations of all the 11 PAMS sites. Originally there was a minimum of only 8 of 56 species showed agreement with observations for the worst of the 11 PAMS sites and 28 of 56 species for the best site. With modified emissions, the number increased to 13–52 species across the 11 PAMS sites, demonstrating that the simple urban based correction procedure has broad applicability. When applying this modification of PAMS emissions to the simulations of other air quality gases, SO2 and NOx showed small changes compared with observations (−0.27% and −2.51%, respectively), while total VOC concentrations showed significant changes (+15.28%) as a result of the adjustment in VOC emissions (+26.7%). Although VOCs are the precursor of ozone, the relatively large changes in VOC did not seem to affect ozone formation to the similar extent, only resulting in the changes of average O3 by 2.9 ppb (+9.41%). It shows that although the emission modification improves individual VOC simulations, the performance in oxidant simulation is still largely unaltered. Although the original U.S. VOC emission profiles can capture the general features of ambient VOCs, further optimization of emissions may still be needed by referencing extensive observations, so that emissions can better fit domestic conditions and accuracy in model simulations can be improved.

Polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) are persistent organic pollutants (POPs) that are formed and released unintentionally from anthropogenic sources. The high persistence of PCDD/Fs results in the concentrations of these contaminants in environment decreasing only very slowly. Two transport pathways, air and water, carry PCDD/Fs into all regions of the world. Recently, more frequent extreme weather events, such as storms and floods, have been projected to occur as a result of global warming. Extreme weather events have a documented impact on the remobilization and subsequent bioavailability of POPs. In this study, three specific episodes, namely winter monsoon, southeast biomass burning and tropical cyclone (typhoon) events, which influence the environmental fate and transport of PCDD/Fs in Taiwan, were evaluated based on a climate change scenario. During the winter (northeast) monsoon period, the temperature and relative humidity observed in northern Taiwan decreases sharply. During this time, the quantity of PCDD/Fs adsorbed onto suspended particles, as observed at background sites, was found to increase from 300 ± 127 to 630 ± 115 pg I-TEQ g-TSP −1 , which is even higher than that measured in Taipei City (438 ± 80 pg I-TEQ g-TSP −1 ). Hence, the winter monsoon not only brings cold air but also transports air pollutants and dust over long distances from mainland China to Taiwan. During the 2010 Southeast Asia biomass burning events (2010/3/22–3/28), the level of atmospheric PCDD/Fs were measured in central Taiwan (Mt. Lulin) and in the source region of northern Thailand (Chiang Mai); this revealed that the variations in atmospheric PCDD/F concentrations at these two sites followed a similar pattern. On 25 March 2010, the atmospheric PCDD/F concentration increased dramatically from 1.43 to 6.09 fg I-TEQ m −3 at Mt. Lulin and from 7.64 to 12.1 fg I-TEQ m −3 in northern Thailand. However, the atmospheric PCDD/F concentration decreased dramatically 1 day after the biomass burning event. Based on the measurements from a dated sediment core collected at a reservoir in northern Taiwan, the sharp increases in input fluxes of PCDD/Fs and mineral-derived elements levels in 1990 (20 ng I-TEQ m −2 year −1 ), 2001 (17 ng I-TEQ m −2 year −1 ), 2004 (16 ng I-TEQ m −2 year −1 ) and 2005 (15 ng I-TEQ m −2 year −1 ) seem to be a result of a deep turbid layer formed upstream due to landslides and/or mud flows during the typhoon season. This finding demonstrates the effect of typhoon events on the long-term remobilization of PCDD/Fs as well as supporting the hypothesis that such events would have the potential to remobilize pollutants that have been deposited previously.

By modulating the Earth-atmosphere energy, hydrological and biogeochemical cycles, and affecting regional-to-global weather and climate, biomass burning is recognized as one of the major factors affecting the global carbon cycle. However, few comprehensive and wide-ranging experiments have been conducted to characterize biomass-burning pollutants in Southeast Asia (SEA) or assess their regional impact on meteorology, the hydrological cycle, the radiative budget, or climate change. Recently, BASE-ASIA (Biomass-burning Aerosols in South-East Asia: Smoke Impact Assessment) and the 7-SEAS (7-South-East Asian Studies)/Dongsha Experiment were conducted during the spring seasons of 2006 and 2010 in northern SEA, respectively, to characterize the chemical, physical, and radiative properties of biomass-burning emissions near the source regions, and assess their effects. This paper provides an overview of results from these two campaigns and related studies collected in this special issue, entitled “Observation, modeling and impact studies of biomass burning and pollution in the SE Asian Environment”. This volume includes 28 papers, which provide a synopsis of the experiments, regional weather/climate, chemical characterization of biomass-burning aerosols and related pollutants in source and sink regions, the spatial distribution of air toxics (atmospheric mercury and dioxins) in source and remote areas, a characterization of aerosol physical, optical, and radiative properties, as well as modeling and impact studies. These studies, taken together, provide the first relatively complete dataset of aerosol chemistry and physical observations conducted in the source/sink region in the northern SEA, with particular emphasis on the marine boundary layer and lower free troposphere (LFT). The data, analysis and modeling included in these papers advance our present knowledge of source characterization of biomass-burning pollutants near the source regions as well as the physical and chemical processes along transport pathways. In addition, we raise key questions to be addressed by a coming deployment during springtime 2013 in northern SEA, named 7-SEAS/BASELInE (Biomass-burning Aerosols & Stratocumulus Environment: Lifecycles and Interactions Experiment). This campaign will include a synergistic approach for further exploring many key atmospheric processes (e.g., complex aerosol–cloud interactions) and impacts of biomass burning on the surface–atmosphere energy budgets during the lifecycles of biomass-burning emissions.

Asian continental outflow is known to have very pronounced seasonality, which in turn can alter the trace gas contents of the Northern Hemisphere. In this study, field measurements were conducted during the spring of 2010, Dongsha, a small island situated between Taiwan and the Philippines, served as a remote site for monitoring surface ozone. Ozone was used as an effective indicator to distinguish between continental and marine air masses. Our measurements suggested that strong northeasterly winds arising from the winter Asian monsoon may have transported polluted air masses from the northern continent to locations as far south as Dongsha (latitude 20.70°N), as indicated by elevated ozone levels of approximately 60 ppbv. In contrast, during periodic calm periods when the monsoon subsided low ozone levels of about 30 ppb were detected, which is typical for marine air masses. This outflow of polluted air masses from the Asian continent and Taiwan facilitated by the winter monsoon was also successfully simulated using the Pennsylvania State University/National Center for Atmospheric Research Mesoscale Model, version 5 (PSU/NCAR MM5) and the Taiwan Air Quality Model (TAQM).

Northern South China Sea (SCS) is adjacent to major atmospheric mercury (Hg) emission source regions; however, studies concerning regional atmospheric Hg distribution and cycling are very limited. Accordingly, measurements of atmospheric Hg were conducted in March and April during the 2010 Dongsha Experiment to study its spatial and temporal distribution. Atmospheric Hg was measured at Hengchun and Dongsha Island (Taiwan), Da Nang (Vietnam), Chiang Mai (Thailand) and over the northern SCS. Atmospheric Hg concentrations ranged between 1.54 and 6.83 ng m −3 , mostly higher than the Northern Hemisphere background value. Regional wind fields and backward trajectories indicated that the atmospheric Hg concentrations over northern SCS should principally reflect the export of the East Asian Hg emissions by northeast monsoon. However, significantly elevated Hg concentrations were always observed at Da Nang, possibly due to the influence of local Hg emissions. Chiang Mai is located in the intense biomass burning region in northern Thailand. Therefore, atmospheric Hg concentrations at Chiang Mai reflected the influence of regional biomass burning Hg emissions. Two dust storms were encountered at Dongsha Island, one on March 16 and the other on March 21, with atmospheric Hg enhancements. Compared with the 2008 summer values, elevated Hg levels were observed at Dongsha Island in the spring of 2010. Summer air masses were mainly from the deep SCS, representing relatively clean marine air. On the other hand, air masses were from the north in spring, passing eastern China or Taiwan prior to reaching Dongsha Island. Results of this research thus demonstrated the transport of atmospheric Hg from the East Asian continent to northern SCS by regional monsoon activity in spring, but special events, such as biomass burning and dust storms, can also cause enhancements of ambient Hg levels.

This study is conducted to identify the synoptic weather patterns that are prone to cause high carbon monoxide (CO) concentrations observed at a mountain site, Lulin atmospheric background station (LABS), in Taiwan due to the biomass-burning activity in Southeast (SE) Asia. LABS is recognized as a clean background station. The study period targets the biomass-burning season (February to May) from 2007 to 2010. The synoptic weather patterns were classified using a two-stage clustering method with inputs from the Weather Research and Forecasting (WRF) meteorological model simulation result in a 27-km spatial grid. A 9-km resolution WRF modeling was performed additionally for 13 to 26 March 2007, when a high CO concentration reaching 500 ppb was observed at LABS. The simulation result indicates that not only the existence of the thermal forcing induced low pressure system formed in Indochina, but also the presence of the high terrain located in the northern part of SE Asia that further forced the uplift of the biomass-burning emissions. On the other hand, when the northeasterly monsoonal flow is strong enough and intruding into Indochina, this would hinder the development of the thermal low and weaken the upward movements, in turn preventing the transport of biomass-burning emissions from Indochina to the area of Taiwan. The simulation results also demonstrate that the location of the SE Asia high pressure system has a moderate effect on the particle dispersion path in the upper level.

This study is to develop a GC×GC method with electron capture detection (ECD) to analyze atmospheric halocarbons in the concentration range of parts per trillion by volume (pptv). To enrich atmospheric halocarbons a home-built thermal desorption (TD) device was coupled to the GC×GC-ECD. The technique of flow modulation was adopted using a Deans switch for GC×GC. Several column combinations of first and second dimensions were tested and the column set of DB-5×TG-1301 was found to show the best orthogonality for halocarbons. A series of modulation parameters were tested for their optimal settings. The modulation period (PM) was found to have minimal wrap-around when set at 3s. The modulation ratio (MR) was determined to be 7.82 to ensure reproducible results and maximum sensitivity. The modulation duty cycle (DC) was calculated to be approximately 0.17. Nine halocarbons were separated successfully and seven were calibrated with the use of a certified standard gas mixture. The correlation coefficients (R2) were greater than 0.9972. The reproducibility was better than 1.90% as expressed in relative standard deviation (RSD; N=30) and the detection limits were in the range of pptv for the target halocarbons. A field test by continuous analyzing ambient air with hourly resolution was performed to show the stability of the method as suggested by the homogeneity of certain halocarbons, while also reflecting concentration variation for others when emissions did arise.

This study presents a novel application based on the Deans-switch cutting technique to characterize the thermal-desorption (TD) properties for gas chromatographic (GC) analysis of ambient volatile organic compounds (VOCs). Flash-heating of the sorbent bed at high temperatures to desorb trapped VOCs to GC may easily produce severe asymmetric or tailing GC peaks affecting resolution and sensitivity if care is not taken to optimize the TD conditions. The TD peak without GC separation was first examined for the quality of the TD peak by analyzing a standard gas mixture from C2 to C12 at ppb level. The Deans switch was later applied in two different stages. First, it was used to cut the trailing tail of the TD peak, which, although significantly improved the GC peak symmetry, led to more loss of the higher boiling compounds than the low boiling ones, thus suggesting compound discrimination. Subsequently, the Deans switch was used to dissect the TD peak into six 30 s slices in series, and an uneven distribution in composition between the slices were found. A progressive decrease in low boiling compounds and increase in higher boiling ones across the slices indicated severe inhomogeneity in the TD profile. This finding provided a clear evidence to answer the discrimination problem found with the tail cutting approach to improve peak symmetry. Through the use of the innovated slicing method based on the Deans-switch cutting technique, optimization of TD injection for highly resolved, symmetric and non-discriminated GC peaks can now be more quantitatively assessed and guided.

Continuous measurements of tropospheric ozone were conducted at the Lulin Atmospheric Background Station (LABS) at an altitude of 2862 m from April 2006 to the end of 2009. Distinct seasonal variations in the ozone concentration were observed at the LABS, with a springtime maximum and a summertime minimum. Based on a backward trajectory analysis, CO data, and ozonesondes, the springtime maximum was most likely caused by the long-range transport of air masses from Southeast Asia, where biomass burning was intense in spring. In contrast, a greater Pacific influence contributed to the summertime minimum. In addition to seasonal variations, a distinct diurnal pattern was also observed at the LABS, with a daytime minimum and a nighttime maximum. The daytime ozone minimum was presumably caused by sinks of dry deposition and NO titration during the up-slope transport of surface air. The higher nighttime values, however, could be the result of air subsidence at night bringing ozone aloft to the LABS. After filtering out the daytime data to remove possible local surface contributions, the average background ozone value for the period of 2006–2009 was approximately 36.6 ppb, increased from 32.3 ppb prior to data filtering, without any changes in the seasonal pattern. By applying HYSPLIT4 model analysis, the origins of the air masses contributing to the background ozone observed at the LABS were investigated.

An automated gas chromatographic system aimed at performing unattended measurements of ambient volatile organic compounds was configured and tested. By exploiting various off-the-shelf components, the thermal desorption unit was easily assembled and can be connected with any existing commercial gas chromatograph in the laboratory to minimize cost. The performance of the complete thermal desorption gas chromatographic system was assessed by analyzing a standard mixture containing 56 target nonmethane hydrocarbons from C2 -C12 at sub-ppb levels. Particular attention was given to the enrichment efficiency of the C2 compounds, such as ethane (b.p. = -88.6°C) and ethylene (b.p. = -104.2°C), due to their extremely high volatilities. Quality assurance was performed in terms of the linearity, precision and limits of detection of the target compounds. To further validate the system, field measurements of target compounds in ambient air were compared with those of a commercial total hydrocarbon analyzer and a carbon monoxide analyzer. Highly coherent results from the three instruments were observed during a two-month period of synchronized measurements. Moreover, the phenomenon of opposite diurnal variations between the biogenic isoprene and anthropogenic species was exploited to help support the field applicability of the thermal desorption gas chromatographic method.

Measurements of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM), and particulate mercury (PHg) have been conducted at Lulin Atmospheric Background Station (LABS) in Taiwan since April 2006. This was the first long-term free tropospheric atmospheric Hg monitoring program in the downwind region of East Asia, which is a major Hg emission source region. Between April 13, 2006 and December 31, 2007, the mean concentrations of GEM, RGM, and PHg were 1.73 ng m −3 , 12.1 pg m −3 , and 2.3 pg m −3 , respectively. A diurnal pattern was observed for GEM with afternoon peaks and nighttime lows, whereas the diurnal pattern of RGM was opposite to that of GEM. Spikes of RGM were frequently observed between midnight and early morning with concurrent decreases in GEM and relative humidity and increases in O 3 , suggesting the oxidation of GEM and formation of RGM in free troposphere (FT). Upslope movement of boundary layer (BL) air in daytime and subsidence of FT air at night resulted in these diurnal patterns. Considering only the nighttime data, which were more representative of FT air, the composite monthly mean GEM concentrations ranged between 1.06 and 2.06 ng m −3 . Seasonal variation in nighttime GEM was evident, with lower concentrations usually occurring in summer when clean marine air masses prevailed. Between fall and spring, air masses passed the East Asian continent prior to reaching LABS, contributing to the elevated GEM concentrations. Analysis of GEM/CO correlation tends to support the argument. Good GEM/CO correlations were observed in fall, winter, and spring, suggesting influence of anthropogenic emission sources. Our results demonstrate the significance of East Asian Hg emissions, including both anthropogenic and biomass burning emissions, and their long-range transport in the FT. Because of the pronounced seasonal monsoon activity and the seasonal variation in regional wind field, export of the Asian Hg emissions to Taiwan occurs mainly during fall, winter, and spring.

Recent biomass burning in Southeast Asia has raised global concerns over its adverse effects on visibility, human health, and global climate. The concentrations of total suspended particles (TSPs) and other vapor-phase pollutants (CO and ozone) were monitored at Lulin, an atmospheric background station in central Taiwan in 2008. To evaluate the long-range transport of persistent organic pollutants (POPs) during the Southeast Asia biomass burning event, the atmospheric polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) were also measured at Lulin station. The atmospheric PCDD/F and TSP concentrations measured at Lulin station ranged from 0.71-3.41 fg I-TEQ/m(3) and 5.32-55.6 microg/m(3), respectively, during the regular sampling periods. However, significantly higher concentrations of PCDD/Fs, TSPs, CO, and ozone were measured during the spring season. These high concentrations could be the result of long-range transport of the products of Southeast Asia biomass burning. During the Southeast Asia biomass burning event (March 18-24, 2008), an intensive observation program was also carried out at the same station. The results of this observation program indicated that the atmospheric PCDD/F concentration increased dramatically from 2.33 to 390 fg I-TEQ/m(3) (March 19, 2008). The trace gas (CO) of biomass burning also significantly increased to 232 ppb during the same period, while the particle-bound PCDD/Fs in the TSP increased from 28.7 to 109 pg I-TEQ/g-TSP at Lulin station during the burning event. We conclude that there was a significant increase in the PCDD/F concentration in ambient air at a high-altitude background station in central Taiwan during the Southeast Asia biomass burning event.

Continuous monitoring of ambient non-methane hydrocarbons (NMHCs) by automated gas chromatographs equipped with flame ionization detection (termed in-situ GC/FID) with hourly data resolution was instated in ozone non-attainment areas throughout Taiwan. Performance of these on-site in-situ GCs was validated by manual flask sampling, as well as by in-lab gas chromatography/mass spectrometry (GC/MS) analysis. More than 50 VOCs from C 2 to C 11 were analyzed by both methods. Ninety flask samples were collected in series near an in-situ GC monitoring station in order to closely compare with the in-situ measurements. Both time-series and scatter plots from the two methods are displayed and discussed. It was found that over-simplified, un-humidified single-point calibration leading to surface loss was responsible for the bias in the in-situ method, resulting in greater error in accuracy as VOC volatility decreased. Although this over-estimate of the concentrations was found across all target VOCs, both methods were able to consistently capture the variability of ambient VOCs, with R 2 values greater than 0.9 for most of the major VOCs.

Three CO instruments, i.e., vacuum ultraviolet resonance fluorescence (VUV-RF), gas chromatography/reduction gas detection (GC/RGD), and non-dispersive infrared (NDIR) spectrometry, were inter-compared at a background site, i.e., Lulin Atmospheric Baseline Station (LABS) in central Taiwan. For a period of 18 days of continuous measurements, highly coherent results were observed between the three instruments. Calibration of the GC/RGD and VUV-RF was based on the same batch of CO standards, producing results that agreed within 4%. Nevertheless, NDIR displayed a significant bias with a large offset compared to the other two instruments (about −63.1 ppb), due mainly to its over-simplified calibration procedure. The NDIR bias was then removed by aligning the NDIR data to those of GC/RGD in a process termed “post-run correction”. Through this practice, the NDIR was linked to the same calibration scale as that of GC/RGD. As a result, by simultaneously exploiting both GC/RGD and NDIR to measure background CO, both time-resolution and accuracy can be secured.

This study investigated a gas chromatographic (GC) method to assess the destruction or removal efficiency (DRE) of local scrubbers on five perfluorocompounds (PFCs), i.e., SF 6 , NF 3 , CF 4 , C 2 F 6 , and C 3 F 8 , which are very potent greenhouse gases used in a semiconductor fabrication plant. Air samples taken at inlets and outlets of local scrubbers were analyzed by a self-constructed multi-column GC system equipped with thermal conductivity detection. Three packed columns were integrated into the heart-cut GC system to allow simultaneous analysis of the five target PFCs. The Porapak Q pre-column performs rough separation and cuts eluent groups to two analytical columns for optimal separation. The Molecular Sieve – 5A column separated NF 3 , CF 4 , and C 3 F 8 and the second Porapak Q separated SF 6 and C 2 F 6 . Linearity was greater than 0.995 ( R 2 ) for the five PFCs, and the reproducibility was about 4% (relative standard deviation) for NF 3 , and better than 0.5% for the other four PFCs. DRE for the combustion (CB) and electric–thermal types of local scrubbers was evaluated by taking into account the in-line dilution from air and fuel gases. Both flow and tracer methods were employed to deduce the dilution factors (DFs). For the tracer method, helium was employed as the tracer and injected upstream of the scrubbers and thus mixed with the exhaust gas. With this method, the DFs were determined to be in the range from 4.8 to 5.9 for the CB unit, significantly higher than the value of 3.3 based on the flow method. The DREs for the CB unit for C 3 F 8 were greater than 90% and between 40% and 50% for CF 4 .

Ambient levels and variability of major atmospheric halocarbons, i.e. CFC-12, CFC-11, CFC-113, CCl4, CH3CCl3, C2HCl3, and C2Cl4 in a major metropolis (Taipei, Taiwan) were re-investigated after fourteen years by flask sampling in 2012. Our data indicates that the variability expressed as standard deviations (SD) of CFC-113 and CCl4 remained small (2.0 ppt and 1.9 ppt, respectively) for the 10th–90th percentile range in both sampling periods; whereas the variability of CFC-12, CFC-11, C2HCl3, and C2Cl4 measured in 2012 became noticeably smaller than observed in 1998, suggesting their emissions were reduced over time. By comparing with the background data of a global network (NOAA/ESRL/GMD baseline observatories), the ambient levels and distribution of these major halocarbons in Taipei approximated those at a background site (Mauna Loa) in 2012, suggesting that the fingerprint of the major halocarbons in a used-to-be prominent source area has gradually approached to that of the background atmosphere.