Lulin Atmospheric Background Station Research Articles

Identification of organic constituents on atmospheric particulate matter in the East Asian background air of free troposphere by GC×GC-TOFMS

The presence of organic compounds on the particulate matter (PM) or aerosols can arise from the condensation of gaseous organic compounds on the existing aerosols, or from organic precursors to form secondary organic aerosols (SOA) through photochemistry. The objective of this study is to characterize organic constituents on aerosols relevant to their emission sources and the key compounds revealing the evolution of aerosols with the use of a novel analytical technique. A time-of-flight mass spectrometry (TOFMS) coupled with comprehensive two-dimensional gas chromatography (GC×GC) was developed using a flow type of modulator instead of a thermal type as a prelude to field applications without the need for cryogen. The methodology of GC×GC-TOFMS is discussed in this study in detail.Since the coarse PM (PM10-2.5) may exhibit with a relatively high OC content compared to PM2.5, the GC×GC results have been obtained by analyzing PM10 samples collected in parallel with OC/EC analysis of PM2.5 samples at the Lulin Atmospheric Background Station (LABS, 23.47°N, 120.87°E, 2862 m ASL) as the high-mountain background site in East Asia. We found that the organic analytes were in a majority in the range of 12–30 carbon numbers falling in the category of semi-volatile organic compounds (SVOCs) with 43 compounds of alcohol, aldehyde, ketone, and ester varieties if excluding alkanes. Intriguingly, trace amounts of plasticizers and phosphorus flame retardants such as phthalates (PAEs) and triphenyl phosphate (TPP) were also found, likely originating from regions involved in open burning of household solid waste in Southeast Asia or e-waste recycling in southern China and along the long-range transport route. Compounds such as these are unique to the specific sources, demonstrating the wide spread of these hazardous compounds in the environment.

Transport pathways of carbon monoxide from Indonesian fire pollution to a subtropical high-altitude mountain site in the western North Pacific

Abstract. 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.

Insights into aerosol chemical composition and optical properties at Lulin Atmospheric Background Station (2862 m asl) during two contrasting seasons

Continental outflows from peninsular Southeast Asia and East Asia dominate the widespread dispersal of air pollutants over subtropical western North Pacific during spring and autumn, respectively. This study analyses the chemical composition and optical properties of PM10 aerosols during autumn and spring at a representative high-altitude site, viz., Lulin Atmospheric Background Station (23.47°N, 120.87°E; 2862 m a.s.l.), Taiwan. PM10 mass was reconstructed and the contributions of major chemical components were also delineated. Aerosol scattering (σsp) and absorption (σap) coefficients were regressed on mass densities of major chemical components by assuming external mixing between them, and the site-specific mass scattering efficiency (MSE) and mass absorption efficiency (MAE) of individual components for dry conditions were determined. NH4NO3 exhibited the highest MSE among all components during both seasons (8.40 and 12.58 m2 g−1 at 550 nm in autumn and spring, respectively). (NH4)2SO4 and organic matter (OM) accounted for the highest σsp during autumn (51%) and spring (50%), respectively. Mean MAE (mean contribution to σap) of elemental carbon (EC) at 550 nm was 2.51 m2 g−1 (36%) and 7.30 m2 g−1 (61%) in autumn and spring, respectively. Likewise, the mean MAE (mean contribution to σap) of organic carbon (OC) at 550 nm was 0.84 m2 g−1 (64%) and 0.83 m2 g−1 (39%) in autumn and spring, respectively. However, a classification matrix, based on scattering Ångström exponent, absorption Ångström exponent, and single scattering albedo (ω), demonstrated that the composite absorbing aerosols were EC-dominated (with weak absorption; ω = 0.91–0.95) in autumn and a combination of EC-dominated and EC/OC mixture (with moderate absorption; ω = 0.85–0.92) in spring. This study demonstrates a strong link between chemical composition and optical properties of aerosol and provides essential information for model simulations to assess the imbalance in regional radiation budget with better accuracy over the western North Pacific.

Impact of 21 June 2020 Annular Solar Eclipse on Meteorological Parameters, O3 and CO at a High Mountain Site in Taiwan

The annular solar eclipse observed on 21 June 2020 over Taiwan provided a rare opportunity to follow the responses of various meteorological parameters and trace gases to the solar eclipse. For the first time, the impact of the solar eclipse on solar radiation, air temperature (T), relative humidity (RH), atmospheric pressure (P), wind speed (WS), and trace gases (ozone and carbon monoxide) is delineated at the Lulin Atmospheric Background Station (LABS; 23.47°N, 120.87°E; 2,862 m MSL) in Taiwan. Over the Taiwan region, the solar eclipse began at 14:49 local time (LT; UTC+8), reached maximum obscuration at 16:13 LT, and finished at 17:24 LT. Compared to the control period (average of 13–20 June 2020), the weather parameters and trace gases show pronounced changes on the day of the eclipse (21 June 2020). A significant decrease in UV-B and solar irradiance at LABS was observed during the peak phase of the solar eclipse due to the occultation of the Sun by the Moon. On the eclipse day, the T decreased significantly (~4°C) after 17 minutes of maximum solar darkening. Due to the cloudiness and low temperatures on the day of the eclipse, 100% RH was apparent during the period of the eclipse at LABS. We also noticed a steady decline in WS just after the onset of the eclipse at LABS. Interestingly, a marked decline in ozone and carbon monoxide was seen during the eclipse day at LABS. Ozone was reduced by about 10 ppb (40%), with a delay of about 2 hours from the peak phase of the eclipse. Overall, our results show the impact of the solar eclipse on high altitude measurements for the first time, and further this work provides a useful new contribution to the literature examining solar eclipse-induced atmospheric changes.

Humic-like substances (HULIS) in springtime aerosols at a high-altitude background station in the western North Pacific: Source attribution, abundance, and light-absorption

Atmospheric humic-like substances (HULIS) are important components of biomass-burning (BB) emissions and highly associated with light-absorbing organic aerosols (often referred to as brown carbon). This study highlights the importance of BB-emitted HULIS aerosols in peninsular Southeast Asian outflow to the subtropical western North Pacific. We determined various key light-absorbing characteristics of HULIS i.e. mass absorption cross-section (MACHULIS), absorbing component of the refractive index (kHULIS), and absorption Ångström exponent (AAEHULIS) based on ground-based aerosol light absorption measurements along with HULIS concentrations in springtime aerosols at Lulin Atmospheric Background Station (LABS; 2862 m above mean sea level), which is a representative high-altitude remote site in the western North Pacific. Daily variations of HULIS (0.58–12.92 μg m−3) at LABS were mostly linked with the influence from incoming air-masses, while correlations with BB tracers and secondary aerosols indicated the attribution of primary and secondary sources. Stronger light absorption capability of HULIS was clearly evident from MACHULIS and kHULIS values at 370 nm, which were about ~1.5 times higher during BB-dominated days (1.16 ± 0.75 m2 g−1 and 0.05 ± 0.03, respectively) than that during non-BB days (0.77 ± 0.89 m2 g−1 and 0.03 ± 0.04, respectively). Estimates from a simple radiative transfer model showed that HULIS absorption can add as much as 15.13 W g−1 to atmospheric warming, and ~46% more during BB-dominated than non-BB period, highlighting that HULIS light absorption may significantly affect the Earth–atmosphere system and tropospheric photochemistry over the western North Pacific.

Long-range transport of La Soufrière volcanic plume to the western North Pacific: Influence on atmospheric mercury and aerosol properties

Volcanic eruptions are important natural sources of gases and aerosols to the environment. However, their impact on the global cycle of trace elements, including mercury (Hg), remains poorly understood. On 9 April 2021, La Soufrière volcano (13.33°N, 61.18°W) erupted in the Caribbean Sea. Ozone Monitoring Instrument (OMI) measurements of sulfur dioxide (SO2) tracked the transport of volcanic SO2 in the troposphere over long distances from the source, including to the western North Pacific ∼10 day after eruption. A spike in gaseous and particle-bound mercury concentrations along with a peak in aerosol back-scattering coefficient at Lulin Atmospheric Background Station (LABS, 23.47°N, 120.87°E; 2862 m AMSL) coincided with the volcanic plume transport on 19 April. The slope of gaseous elemental mercury vs. carbon monoxide concentrations during the event was 0.027, which is distinctly higher than for Southeast Asia biomass burning (slope = 0.005) and East Asia outflow (0.011) pollution sources. Arrival of the plume high above Taiwan was confirmed by significant changes in signature aerosol properties. Thus, with critical observational evidence, our study reported for the first time enhanced mercury levels ∼18000 km downwind from a volcano source, providing an important check on volcanic Hg emission strength.

Detection of stratospheric intrusion events and their role in ozone enhancement at a mountain background site in sub-tropical East Asia

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.

Relationships between atmospheric mercury and optical properties of spring outflow aerosols from Southeast Asia

Southeast Asia is a major biomass burning (BB) source area and BB has been identified as an important source of mercury (Hg) and aerosols to the atmosphere. Previous studies found correlations between atmospheric Hg and Delta-C (BC370–BC880) during the BB episodes in low-elevation BB source areas; however, whether this relationship persists during long-range transport remains unknown. Lulin Atmospheric Background Station (LABS), a high mountain background site in central Taiwan, has monitored the impact of BB long-range transports from Southeast Asia on atmospheric Hg and aerosols in downwind areas since 2006 and 2008, respectively. As such, these data provide an opportunity to investigate the relationship between atmospheric Hg (PBM and GOM) and aerosol optical properties, such as Delta-C and absorption Ångström exponent (AAE370-880). In this study, three long-range transport BB events were observed at LABS in the springtime during 2014–2016. Significant positive correlations with PBM/GOM were observed for Delta-C and (R2 = 0.34–0.51) and AAE370-880 (R2 = 0.41–0.54) during the BB events, while poor correlations were shown under non-BB episodes. Additionally, the positive correlation between PBM and AAE370-880 suggests that the Hg(II) may be preferably absorbed onto organic aerosols or originated from the same emission sources. This study demonstrated that AAE370-880 can be used to identify the source of Hg(II) from BB long-range transport. In addition, our results also indicated the influences of aerosol chemical compositions on the partitioning of Hg(II), which is important to further the understanding of atmospheric Hg cycling.

Effects of temperature and relative humidity on the partitioning of atmospheric oxidized mercury at a high-altitude mountain background site in Taiwan

Gas-particle partitioning of oxidized mercury (Hg) plays an important role in governing the speciation, transport and deposition of atmospheric Hg. Although studies on gas-particle partitioning of oxidized Hg have been conducted at some urban sites, comparable studies at remote mountain sites are still limited. This study analyzes multi-year (2014–2016) data of speciated atmospheric Hg concentrations from Lulin Atmospheric Background Station (LABS, 2862 m above sea level), Taiwan, to explore the factors that influence the gas-particle partitioning of atmospheric oxidized Hg. Mean concentrations (±S.D.) of gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particulate-bound mercury (PBM) were 1.54 ± 0.34 ng m−3, 14.5 ± 26.5 pg m−3, and 5.0 ± 12.0 pg m−3, respectively. In addition, our results indicated that the partitioning of Hg(II) toward particles was favored in the upper free troposphere and/or lower stratosphere. Both temperature (T) and relative humidity (RH) were found to strongly affect the gas-particle partitioning of oxidized Hg. Significant negative correlations between the partitioning coefficient (Kp) and T were obtained for all seasons, but peaked in summer. When RH<30%, Kp decreased with increasing RH. However, Kp and RH were positively correlated when RH>30%. Two empirical Kp-T and Kp-T-RH regression equations: log(1/Kp) = 15.0 – 3887.6(1/T) and log(1/Kp) = 17.92 – 4390.0(1/T) – 0.016RH were developed for free tropospheric air downwind of continental East Asia, which could be implemented in a chemical transport model to improve our understanding of the Hg biogeochemical cycle.

Real-time measurements of PM2.5 water-soluble inorganic ions at a high-altitude mountain site in the western North Pacific: Impact of upslope wind and long-range transported biomass-burning smoke

Real-time measurement of PM2.5 (particulate matter with aerodynamic diameter ≤ 2.5 μm) water-soluble inorganic ions (WSIIs) was conducted at Lulin Atmospheric Background Station (LABS; 2862 m above mean sea level) in the western North Pacific (WNP) during the autumn 2015 and spring 2016. During autumn, the mountain-valley (M-V) circulation is effective in increasing the mass concentrations of PM2.5, WSIIs, and carbon monoxide (CO) at LABS from 12:00 to 18:00 local time every day. In sharp contrast to autumn, five high aerosol-loading events were recorded during the spring, with each event persisting for a few days. These events were harmonized with the long-range transport of biomass-burning (BB) smoke emissions from northern peninsular Southeast Asia (PSEA), as disclosed from the fire count map and backward trajectories. The plumes appear to mask their characteristic diurnal features driven by the local M-V circulation. During both seasons, the prominent pathway of SO2 to SO42− conversion was aqueous phase oxidation as revealed from the relationship between sulfur oxidation ratio (SOR) and aerosol liquid-water content. Furthermore, NO3− was found to be produced primarily via homogeneous reactions during the spring season. The optical measurements were also made along with the semi-continuous measurements of WSIIs in this study. The magnitude of aerosol scattering and absorption coefficients exhibited high values when LABS was either under the influence of M-V circulation or long-range BB transport, although the latter event was apparently greater. Large surface cooling (up to −30.8 W m−2) and atmospheric warming (up to +21.3 W m−2) at LABS attributed to absorption enhancement by BB-induced aerosols can potentially influence the regional radiation budget.

Isotopic composition of total gaseous mercury at a high-altitude tropical forest site influenced by air masses from the East Asia continent and the Pacific Ocean

Gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), particulate-bound mercury (PBM), and the isotopic composition of total gaseous mercury (TGM = GEM + GOM) were measured at the Lulin Atmospheric Background Station (LABS), a mountain background site downwind of the East Asia continent, from February 2015 to January 2016. Mean (±S.D.) concentrations of GEM, GOM, and PBM were 1.54 ± 0.34 ng m−3, 14.0 ± 27.8 pg m−3, and 2.6 ± 3.7 pg m−3, respectively. Concentration-Weighted Trajectory (CWT) analysis indicated that East and coastal China were the main source regions of elevated GEM observed at LABS. Weekly integrated TGM showed significant variations in δ202HgTGM (−0.42 to 0.41‰) and Δ199HgTGM (−0.31 to −0.13‰). Both δ202HgTGM and Δ199HgTGM showed clear seasonal variations, but the seasonal pattern of δ202HgTGM was different from that of Δ199HgTGM. The lowest mean δ202HgTGM was observed in spring (−0.15‰), while the lowest mean Δ199HgTGM was observed in summer (−0.24‰). A significant positive correlation (R2 = 0.38, p < 0.01) existed between δ202HgTGM and normalized difference vegetation index (NDVI), suggesting vegetation activity was an important factor controlling the seasonal variation of δ202HgTGM. In contrast, air mass transport path, which influences the source region of TGM to LABS, was likely the driver for the seasonal variations of Δ199HgTGM. Furthermore, results from the air mass classification showed distinguishable Δ199HgTGM signature for different air mass source regions, with air masses from South China Sea and western Pacific Ocean being characterized by more negative Δ199HgTGM (−0.25 ± 0.04‰). Results of this research demonstrated a clear difference in isotopic compositions of atmospheric Hg between continental and marine air masses.

Characterizing a landmark biomass-burning event and its implication for aging processes during long-range transport

Abstract 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.

Long-term (2003–2018) trends in aerosol chemical components at a high-altitude background station in the western North Pacific: Impact of long-range transport from continental Asia

This study examined the long-term trends in chemical components in PM2.5 (particulate matter with aerodynamic diameter ≤2.5 μm) samples collected at Lulin Atmospheric Background Station (LABS) located on the summit of Mt. Lulin (2862 m above mean sea level) in Taiwan in the western North Pacific during 2003–2018. High ambient concentrations of PM2.5 and its chemical components were observed during March and April every year. This enhancement was primarily associated with the long-range transport of biomass burning (BB) smoke emissions from Indochina, as revealed from cluster analysis of backward air mass trajectories. The decreasing trends in ambient concentrations of organic carbon (−0.67% yr−1; p = 0.01), elemental carbon (−0.48% yr−1; p = 0.18), and non–sea-salt (nss) K+ (−0.71% yr−1; p = 0.04) during 2003–2018 indicated a declining effect of transported BB aerosol over the western North Pacific. These findings were supported by the decreasing trend in levoglucosan (−0.26% yr−1; p = 0.20) during the period affected by the long-range transport of BB aerosol. However, NO3− displayed an increasing trend (0.71% yr−1; p = 0.003) with considerable enhancement resulting from the air masses transported from the Asian continent. Given that the decreasing trends were for the majority of the chemical components, the columnar aerosol optical depth (AOD) also demonstrated a decreasing trend (−1.04% yr−1; p = 0.0001) during 2006–2018. Overall decreasing trends in ambient (carbonaceous aerosol and nss-K+) as well as columnar (e.g., AOD) aerosol loadings at the LABS may influence the regional climate, which warrants further investigations. This study provides an improved understanding of the long-term trends in PM2.5 chemical components over the western North Pacific, and the results would be highly useful in model simulations for evaluating the effects of BB transport on an area.

Eight-year dry deposition of atmospheric mercury to a tropical high mountain background site downwind of the East Asian continent

Atmospheric deposition, either dry or wet, has been identified as an important pathway of mercury (Hg) input to terrestrial and aquatic systems. Although East Asia is the major atmospheric Hg emission source region, very few studies have been conducted to quantify atmospheric Hg deposition in its downwind region. In this study, 8-year (2009–2016) atmospheric Hg dry deposition was reported at the Lulin Atmospheric Background Station (LABS), a high mountain forest site in central Taiwan. Dry deposition of speciated Hg was estimated using a bi-directional air-surface flux exchange model for gaseous elemental mercury (GEM) and dry deposition models for gaseous oxidized mercury (GOM) and particulate-bound mercury (PBM), making use of the monitored speciated atmospheric Hg concentrations. Annual total Hg dry deposition ranged from 51.9 to 84.9 μg m−2 yr−1, with a multi-year average of 66.1 μg m−2 yr−1. Among the three forms of atmospheric Hg, GEM was the main contributor to the total dry deposition, contributing about 77.8% to the total, due to the high density of forest canopy as well as the much higher concentration of GEM than GOM and PBM at LABS. Mercury dry deposition is higher in winter and spring than in summer and fall, partly due to the elevated Hg concentrations associated with air masses from East and Southeast Asia where with high atmospheric Hg emissions. The mean annual dry/wet deposition ratio of 2.8 at LABS indicated that Hg deposition to forest landscape was governed by dry rather than wet deposition.

Temporal changes in atmospheric mercury concentrations at a background mountain site downwind of the East Asia continent in 2006–2016

Atmospheric mercury (Hg) has been monitored at the Lulin Atmospheric Background Station (LABS) in Taiwan since April 2006 and is still continuing. Here we reported the trend in gaseous elemental Hg (GEM) concentrations at LABS between April 2006 and December 2016, before the Minamata Convention on Mercury entered into force in 2017. Previous research indicated nighttime (0–8 am) data collected at LABS are better representative of regional influence. Therefore, only nighttime GEM data were used for trend analysis. A significant decreasing trend in GEM at a rate of −1.5% yr−1 (−0.022 ng m−3 yr−1, p < 0.01) was found, comparable to the decreasing trends observed in Europe, North America, South Africa, and over the North Atlantic Ocean. Five major GEM source regions to the LABS were identified, including northern Indochina Peninsula, China, Northeast Asia, the Pacific Ocean, and South China Sea. Significant decreasing trends in GEM were found for air masses coming from northern Indochina Peninsula (−0.042 ng m−3 yr−1, −2.6% yr−1, p < 0.01), China (−0.041 ng m−3 yr−1, −2.4% yr−1, p < 0.01), Northeast Asia (−0.031 ng m−3 yr−1, −2.0% yr−1, p < 0.05), and the Pacific Ocean (−0.022 ng m−3 yr−1, −1.7% yr−1, p < 0.05). Decreasing GEM trend (−0.020 ng m−3 yr−1, −1.5% yr−1), but insignificant (p > 0.05), was also found for air masses coming from South China Sea. The decreasing trends observed with air from the Pacific Ocean and South China Sea indicated declining background GEM concentrations in Northern Hemisphere. Decrease in GEM concentrations at the LABS was in agreement with the reduction in atmospheric Hg export from the East Asia continent caused by changes in Hg emission quantity and speciation, and temporal and spatial distribution in emission sources that have been suggested by recent research. Additionally, changes in the frequency distribution of air mass origins and transport paths may also contribute to the changes in GEM concentrations at LABS.

Relationship between long-range transported atmospheric black carbon and carbon monoxide at a high-altitude background station in East Asia

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.

Four-year Measurements of Wet Mercury Deposition at a Tropical Mountain Site in Central Taiwan

ABSTRACT Rainwater samples were collected between 2010 and 2013 at Lulin Atmospheric Background Station (LABS) to study the distribution and characteristics of wet mercury (Hg) deposition, and possible driving mechanisms. Sample Hg concentrations ranged from 0.8 to 35.1 ng L–1 with an overall volume-weighted mean (VWM) concentration of 9.2 ng L–1. Annual wet Hg deposition fluxes ranged between 24.4 and 48.9 µg m–2 with a mean value of 32.3 µg m–2. This mean annual wet flux was about 1.5–6.0 times the values measured at 15 sites in the U.S. and 4–16 times the values reported from mountain and high-elevation sites in China. Both rainwater Hg concentration and rainfall amount contributed to this geographical difference, but rainfall amount played a more important role. This indicated that tropical mountains in East and Southeast Asia, especially the windward maritime slopes with abundant rainfall, could be hot spots of wet Hg deposition. Wet Hg deposition flux was high in summer because of elevated rainwater Hg concentrations and high rainfall. The seasonal pattern of rainwater Hg concentrations was different from that of the East Asian air pollutant export, indicating other factors, e.g., rainfall type, were also influencing rainwater Hg concentrations. A clear difference in seasonal frequency distribution of rainfall types was observed, with rain events associated with the Pacific high pressure type (PH) occurring more frequently in summer months. PH rainfall type had the highest VWM Hg concentration (13.5 ng L–1), 2.3–6.2 ng L–1 greater than those of the other rainfall types. Because of intense surface heating under summer PH conditions, precipitation systems usually form locally due to strong convection, resulting in afternoon shower. Therefore, the elevated rainwater Hg levels in summer at LABS were likely due to the scavenging of free tropospheric gaseous oxidized Hg (GOM) by deep convection.

Aerosol optical properties at the Lulin Atmospheric Background Station in Taiwan and the influences of long-range transport of air pollutants

The Lulin Atmospheric Background Station (LABS, 23.47°N 120.87°E, 2862 m ASL) in Central Taiwan was constructed in 2006 and is the only high-altitude background station in the western Pacific region for studying the influence of continental outflow. In this study, extensive optical properties of aerosols, including the aerosol light scattering coefficient (σs) and light absorption coefficient (σa), were collected from 2013 to 2014. The intensive optical properties, including mass scattering efficiency (αs), mass absorption efficiency (αa), single scattering albedo (ω), scattering Ångstrӧm exponent (Å), and backscattering fraction (b), were determined and investigated, and the distinct seasonal cycle was observed. The value of αs began to increase in January and reached a maximum in April; the mean in spring was 5.89 m2 g−1 with a standard deviation (SD) of 4.54 m2 g−1 and a 4.48 m2 g−1 interquartile range (IQR: 2.95–7.43 m2 g−1). The trend was similar in αa, with a maximum in March and a monthly mean of 0.84 m2 g−1. The peak values of ω (Mean = 0.92, SD = 0.03, IQR: 0.90–0.93) and Å (Mean = 2.22, SD = 0.61, IQR: 2.12–2.47) occurred in autumn. These annual patterns of optical properties were associated with different long-range transport patterns of air pollutants such as biomass burning (BB) aerosol in spring and potential anthropogenic emissions in autumn. The optical measurements performed at LABS during spring in 2013 were compared with those simultaneously performed at the Doi Ang Kang Meteorology Station, Chiang Mai Province, Thailand (DAK, 19.93°N, 99.05°E, 1536 m a.s.l.), which is located in the Southeast Asia BB source region. Furthermore, the relationships among αs, αa, and b were used to characterize the potential aerosol types transported to LABS during different seasons, and the data were inspected according to the HYSPLIT 5-day backward trajectories, which differentiate between different regions of air mass origin.

Aerosol transport from Chiang Mai, Thailand to Mt. Lulin, Taiwan – Implication of aerosol aging during long-range transport

The transport of biomass burning (BB) aerosol from Indochina may cause a potential effect on climate change in Southeast Asia, East Asia, and the Western Pacific. Up to now, the understanding of BB aerosol composition modification during long-range transport (LRT) is still very limited due to the lack of observational data. In this study, atmospheric aerosols were collected at the Suthep/Doi Ang Khang (DAK) mountain sites in Chiang Mai, Thailand and the Lulin Atmospheric Background Station (Mt. Lulin) in central Taiwan from March to April 2010 and from February to April 2013, respectively. During the study period, an upwind and downwind relationship between the Suthep/DAK and Lulin sites (2400 km apart) was validated by backward trajectories. Comprehensive aerosol properties were resolved for PM2.5 water-soluble inorganic ions, carbonaceous content, water-soluble/insoluble organic carbon (WSOC/WIOC), dicarboxylic acids and their salts (DCAS), and anhydrosugars. A Modification Factor (MF) is proposed by employing non-sea-salt potassium ion (nss-K+) or fractionalized elemental carbon evolved at 580 °C after pyrolized OC correction (EC1-OP) as a BB aerosol tracer to evaluate the mass fraction changes of aerosol components from source to receptor regions during LRT. The MF values of nss-SO42−, NH4+, NO3−, OC1 (fractionalized organic carbon evolved from room temperature to 140 °C), OP (pyrolized OC fraction), DCAS, and WSOC were above unity, which indicated that these aerosol components were enhanced during LRT as compared with those in the near-source region. In contrast, the MF values of anhydrosugars ranged from 0.1 to 0.3, indicating anhydrosugars have degraded during LRT.

Investigation of the CCN Activity, BC and UVBC Mass Concentrations of Biomass Burning Aerosols during the 2013 BASELInE Campaign

Biomass-burning (BB) aerosols, acting as cloud condensation nuclei (CCN), can influence cloud microphysical and radiative properties. In this study, we present CCN measured near the BB source regions over northern Southeast Asia (Doi Ang Khang, Thailand) and at downwind receptor areas (Lulin Atmospheric Background Station, Taiwan), focusing exclusively on 13–20 March 2013 as part of 2013 spring campaign of the Seven SouthEast Asian Studies (7-SEAS) intensive observation. One of the campaign’s objectives is to characterize BB aerosols serving as CCN in SouthEast Asia (SEA). CCN concentrations were measured by a CCN counter at 5 supersaturation (SS) levels: 0.15%, 0.30%, 0.45%, 0.60%, and 0.75%. In addition, PM2.5 and black carbon mass concentrations were analyzed by using a tapered element oscillating microbalance and an aethalometer. It was found the number-size distributions and the characteristics of hygroscopicity (e.g., activation ratio and κ) of BB aerosols in SEA have a strong diurnal pattern, and different behaviors of patterns were characterized under two distinct weather systems. The overall average κ value was low (0.05–0.1) but comparable with previous CCN studies in other BB source regions. Furthermore, a large fraction of UV-absorbing organic material (UVBC) and high Delta-C among BB aerosols were also observed, which suggest the existence of substantial particulate organic matter in fresh BB aerosols. These data provide the most extensive characterization of BB aerosols in SEA until now.