ALBERT

Description: An intensive aerosol characterization experiment was performed at the Taipei Aerosol and Radiation Observatory (TARO, 25.02° N, 121.53° E) in the urban area of Taipei, Taiwan, during July 2012. Number concentration and size distribution of aerosol particles were measured continuously, which were accompanied by concurrent measurements of mass concentration of submicron particles, PM1 (d ≤ 1 μm), and photolysis rate of ozone, J(O1D). The averaged number concentrations of total (Ntotal), accumulation mode (Nacu), Aitken mode (NAitken), and nucleation mode (Nnuc) particles were 13.9 × 103 cm−3, 1.2 × 103 cm−3, 6.1 × 103 cm−3, and 6.6 × 103 cm−3, respectively. Accordingly, the ultrafine particles (UFPs, d ≤ 100 nm) accounted for 91% of the total number concentration of particles measured in this study (10 ≤ d ≤ 429 nm), indicating the importance of UFPs to the air quality and radiation budget in Taipei and its surrounding areas. An averaged Nnuc / NOx ratio of 192.4 cm−3 ppbv−1 was derived from nighttime measurements, which was suggested to be the characteristic of vehicle emissions that contributed to the "urban background" of nucleation mode particles throughout a day. On the contrary, it was found that the number concentration of nucleation mode particles was independent of NOx and could be elevated up to 10 times of the "urban background" levels during daytime, suggesting a substantial amount of nucleation mode particles produced from photochemical processes. Averages (± 1σ) of the diameter growth rate (GR) and formation rate of nucleation mode particles, J10, were 11.9 ± 10.6 nm h−1 and 6.9 ± 3.0 cm−3 s−1, respectively. Consistency in the time series of the nucleation mode particle concentration and the proxy of H2SO4 production, UVB · SO2/CS, for new particle formation (NPF) events suggested that photooxidation of SO2 was likely one of the major mechanisms for the formation of new particles in our study area. Moreover, it was revealed that the particle growth rate correlated exponentially with the photolysis of ozone, implying that the condensable vapors were produced mostly from photooxidation reactions. In addition, this study also revealed that Nnuc exhibited a quadratic relationship with J10. The quadratic relationship was inferred as a result of aerosol dynamics and featured NPF processes in urban areas.

Description: To investigate the physico-chemical properties of aerosols in Taiwan, an observation network was initiated in 2003. In this work, the measurements of the mass concentration and carbonaceous composition of PM10 and PM2.5 are presented. Analysis on the data collected in the first 5-years, from 2003 to 2007, showed that there was a very strong contrast in the aerosol concentration and composition between the rural and the urban/suburban stations. The five-year means of EC at the respective stations ranged from 0.9±0.04 to 4.2±0.1 μgC m−3. In rural areas, EC accounted for 2–3% of PM10 and 3–5% of PM2.5 mass loadings, comparing to 4–6% of PM10 and 4–8% of PM2.5 in the urban areas. It was found that the spatial distribution of EC was consistent with CO and NOx across the network stations, suggesting that the levels of EC over Taiwan were dominated by local sources. The measured OC was split into POC and SOC counterparts following the EC tracer method. Five-year means of POC ranged from 1.8±0.1 to 9.7±0.2 μgC m−3 among the stations. It was estimated that the POM contributed 5–17% of PM10 and 7–18% of PM2.5 in Taiwan. On the other hand, the five-year means of SOC ranged from 1.5±0.1 to 3.8±.3 μgC m−3. The mass fractions of SOM were estimated to be 9–19% in PM10 and 14–22% in PM2.5. The results showed that the SOC did not exhibit significant urban-rural contrast as did the POC and EC. A significant cross-station correlation between SOC and total oxidant was observed, which means the spatial distribution of SOC in Taiwan was dominated by the oxidant mixing ratio. Besides, correlation was also found between SOC and particulate nitrate, implying that the precursors of SOA were mainly from local anthropogenic sources. In addition to the spatial distribution, the carbonaceous aerosols also exhibited distinct seasonality. In northern Taiwan, the concentrations of all the three carbonaceous components (EC, POC, and SOC) reached their respective minima in the fall season. POC and EC increased drastically in winter and peaked in spring, whereas the SOC was characterized by a bimodal pattern with the maximal concentration in winter and a second mode in summertime. In southern Taiwan, minimal levels of POC and EC occurred consistently in summer and the maxima were observed in winter, whereas the SOC peaked in summer and declined in wintertime. The discrepancies in the seasonality of carbonaceous aerosols between northern and southern Taiwan were most likely caused by the seasonal meteorological settings that dominated the dispersion of air pollutants. Moreover, it was inferred that the Asian pollution outbreaks could have shifted the seasonal maxima of air pollutants from winter to spring in the northern Taiwan, and that the increases in biogenic SOA precursors and the enhancement in SOA yield were responsible for the elevated SOC concentrations in summer.

Description: As a part of the CAREBeijing-2008 campaign, observations of O3, oxides of nitrogen (NOx and NOy), CO, and hydrocarbons (NMHCs) were carried out at the air quality observatory of the Peking University in Beijing, China during August 2008, including the period of the 29th Summer Olympic Games. The measurements were compared with those of the CAREBeijing-2006 campaign to evaluate the effectiveness of the air pollution control measures, which were conducted for improving the air quality in Beijing during the Olympics. The results indicate that significant reduction in the emissions of primary air pollutants had been achieved; the monthly averaged mixing ratios of NOx, NOy, CO, and NMHCs decreased by 42.2, 56.5, 27.8, and 49.7 %, respectively. In contrast to the primary pollutants, the averaged mixing ratio of O3 increased by 42.2 %. Nevertheless, it was revealed that the ambient levels of total oxidant (Ox = O3+NO2+1.5 NOz) and NOz were reduced by 21.3 and 77.4 %, respectively. The contradictions between O3 and Ox were further examined in two case studies. Ozone production rates of 30–70 ppbv h−1 and OPEx of ~8 mole mole−1 were observed on a clear-sky day in spite of the reduced levels of precursors. In that case, it was found that the mixing ratio of O3 increased with the increasing NO2/NO ratio, whereas the NOz mixing ratio leveled off when NO2/NO〉8. Consequently, the ratio of O3 to NOz increased to above 10, indicating the shift from VOC-sensitive regime to NOx-sensitive regime. However, in the other case, it was found that the O3 production was inhibited significantly due to substantial reduction in the NMHCs. According to the observations, it was suggested that the O3 and/or Ox production rates in Beijing should have been reduced as a result of the reduction in the emissions of precursors during the Olympic period. However, the nighttime O3 levels increased due to a decline in the NO-O3 titration, and the midday O3 peak levels were elevated because of the shift in the photochemical regime and the inhibition of NOz formation.

Description: To investigate the physico-chemical properties of aerosols in Taiwan, an observation network was initiated in 2003. In this work, the measurements of the mass concentration and carbonaceous composition of PM10 and PM2.5 are presented. Analysis on the data collected in the first 5-years, from 2003 to 2007, showed that there was a very strong contrast in the aerosol field between the rural and the urban/suburban stations. The five-year means of EC at the respective stations ranged from 0.9±0.04 to 4.2±0.1 μgC m−3. In rural areas, EC accounted for 2–3% of PM10 and 3–5% of PM2.5 mass loadings, comparing to 4–6% of PM10 and 4–8% of PM2.5 in the urban areas. It was found that the spatial distribution of EC was consistent with CO and NOx across the network stations, suggesting that the levels of EC over Taiwan were dominated by local sources. The measured OC was split into POC and SOC counterparts following the EC tracer method. Five-year means of POC ranged from 1.8±0.1 to 9.7±0.2 μgC m−3 among the stations. It was estimated that the POM contributed 5–17% of PM10 and 7–18% of PM2.5 in Taiwan. On the other hand, the five-year means of SOC ranged from 1.5±0.1 to 3.8±0.3 μgC m−3. The mass fractions of SOM were estimated to be 9–19% in PM10 and 14–22% in PM2.5. The results showed that the SOC did not exhibit significant urban-rural contrast as did the POC and EC. A significant cross-station correlation between SOC and total oxidant was observed, which means the spatial distribution of SOC in Taiwan was dominated by the oxidant mixing ratio. Besides, correlation was also found between SOC and particulate nitrate, implying that the precursors of SOA were mainly from local anthropogenic sources. In addition to the spatial distribution, the carbonaceous aerosols also exhibited distinct seasonality. In northern Taiwan, the concentrations of all the three carbonaceous components (EC, POC, and SOC) reached their respective minima in the fall season. POC and EC increased drastically in winter and peaked in spring, whereas the SOC was characterized by a bimodal pattern with the maximal concentration in winter and a second mode in summertime. In southern Taiwan, minimal levels of POC and EC occurred consistently in summer and the maxima were observed in winter, whereas the SOC peaked in summer and declined in wintertime. The discrepancies in the seasonality of carbonaceous aerosols between northern and southern Taiwan were most likely caused by the seasonal meteorological settings that dominated the dispersion of air pollutants. Moreover, it was inferred that the Asian pollution outbreaks could have shifted the seasonal maxima of air pollutants from winter to spring in the northern Taiwan, and that the biogenic SOA precursors were responsible to the elevated SOC concentrations in summer.

Description: As the host of the 2008 Summer Olympic Games, Beijing implemented a series of stringent, short-term air quality control measures to reduce the emissions of anthropogenic air pollutants. Large reductions in the daily average concentrations of primary pollutants, e.g., non-methane hydrocarbons (NMHCs) and nitrogen oxides (NOx) of approximately 50% were observed at the air quality observatory of Peking University. Nevertheless, high levels of ozone were present during the control period. Although anthropogenic precursors were greatly reduced, the meteorological conditions in summer, including high temperature and light flux, are conducive to the production of large amounts of biogenic isoprene, which is extremely reactive. The diurnal pattern of isoprene showed daily maximum mixing ratios of 0.83 ppbv at noon and a minimum at night, reflecting its primarily biogenic properties. Using the ratio of isoprene to vehicle exhaust tracers, approximately 92% of the daytime isoprene was estimated from biogenic sources, and only 8% was attributed to vehicular emissions. In terms of OH reactivity and the ozone formation potential (OFP), biogenic isoprene with its midday surge can contribute approximately 20% of the total OFPs and 40–50% of the total OH reactivities of the 65 measured NMHCs during the midday hours. The discrepancy between decreased precursor levels and the observed high ozone was most likely caused by a combination of many factors. The changes in the partition among the components of oxidation products (O3, NO2 and NOz) and the contribution of air pollutants from regional sources outside Beijing should be two primary reasons. Furthermore, the influences of biogenic isoprene as well as the non-linearity of O3-VOC-NOx chemistry are other major concerns that can reduce the effectiveness of the control measures for decreasing ozone formation. Although anthropogenic precursors were greatly reduced during the Olympic Games, sufficient biogenic isoprene and moderate NOx were still present in the conditions of high radiation flux and temperature during midday and early afternoon, which can still contribute a significant fraction of midday and early afternoon O3.

Description: An intensive aerosol characterization experiment was performed at the Taipei Aerosol and Radiation Observatory (TARO, 25.02° N, 121.53° E) in the urban area of Taipei, Taiwan during July 2012. Number concentration and size distribution of aerosol particles were measured continuously, which were accompanied by concurrent measurements of mass concentration of submicron particles, PM (d ≤ 1 μm), and photolysis rate of ozone, J(O1D). The averaged number concentrations of total (Ntotal), accumulation mode (Nacu), Aitken mode (Ntotal), and nucleation mode (Nnuc) particles were 7.6 × 103 cm−3, 1.2 × 103 cm−3, 4.4 × 103 cm−3, and 1.9 × 103 cm−3, respectively. Accordingly, the ultrafine particles (UFPs, d ≤ 100 nm) accounted for 83% of the total number concentration of particles measured in this study (10 ≤ d ≤ 429 nm), indicating the importance of UFPs to the air quality and radiation budget in Taipei and its surrounding areas. An averaged Nnuc/NOx ratio of ~60 cm−3 ppbv−1 was derived from nighttime measurements, which was suggested to be the characteristic of vehicle emissions that contributed to the "urban background" of nucleation mode particles throughout a day. On the contrary, it was found that the number concentration of nucleation mode particles was independent of NOx and could be elevated up to 10 times the "urban background" levels during daytime, suggesting a substantial amount of nucleation mode particles produced from photochemical processes. Consistency in the time series of the nucleation mode particle concentration and the proxy of H2SO4 production, UVB·SO2, for new particle formation (NPF) events showed that photo-oxidation of SO2 was responsible for the formation of new particles in our study area. Moreover, analysis upon the diameter growth rate, GR, and formation rate of nucleation mode particles, J10−25, found that the values of GR (8.5 ± 6.8 nm h−1) in Taipei were comparable to other urban areas, whereas the values of J10−25 (2.2 ± 1.2 cm−3 s−1) observed in this study were around the low end of the range of new particle formation rate reported by previous investigations. It was revealed that the particle growth rate correlated exponentially with the photolysis of ozone, suggesting the condensable vapors were produced mostly from photo-oxidation reactions. In addition, this study also revealed that both GR and J10−25 exhibited quadratic relationship with the number concentration of particles. The quadratic relationship was inferred as a result of aerosol dynamics and featured NPF process in urban areas.

Description: Iron and phosphorous are essential to marine microorganisms in vast regions in oceans worldwide. Atmospheric inputs are important allochthonous sources of Fe and P. The variability in airborne Fe deposition is hypothesized to serve an important function in previous glacial–interglacial cycles, contributing to the variability in atmospheric CO2 and ultimately the climate. Understanding the mechanisms underlying the mobilization of airborne Fe and P from insoluble to soluble forms is critical to evaluate the biogeochemical effects of these elements. In this study, we present a robust power-law correlation between fractional Fe solubility and non-sea-salt-sulfate / Total-Fe (nss-sulfate / FeT) molar ratio independent of distinct sources of airborne Fe of natural and/or anthropogenic origins over the South China Sea. This area receives Asian dust and pollution outflows and Southeast Asian biomass burning. This correlation is also valid for nitrate and total acids, demonstrating the significance of acid processing in enhancing Fe mobilization. Such correlations are also found for P, yet source dependent. These relationships serve as straightforward parameters that can be directly incorporated into available atmosphere–ocean coupling models that facilitate the assessment of Fe and P fertilization effects. Although biomass burning activity may supply Fe to the bioavailable Fe pool, pyrogenic soils are possibly the main contributors, not the burned plants. This finding warrants a multidisciplinary investigation that integrates atmospheric observations with the resulting biogeochemistry in the South China Sea, which is influenced by atmospheric forcings and nutrient dynamics with monsoons.

Description: The aim of this study is to investigate the seasonal variations in the physicochemical properties of atmospheric ultrafine particles (UFPs, d ≤ 100nm) and submicron particles (PM1, d ≤ 1 μm) in an East-Asian urban area, which are hypothesized to be affected by the interchange of summer and winter monsoons. An observation experiment was conducted at the TARO, an urban aerosol station in Taipei, Taiwan, from October 2012 to August 2013. The measurements included the mass concentration and chemical composition of UFPs and PM1, as well as the particle number concentration (PNC) and size distribution (PSD) with size range of 4–736 nm. The results indicate that the mass concentration of PM1 was elevated during cold seasons with peak level of 18.5 μg m-3 in spring, whereas the highest UFPs concentration was measured in summertime with a seasonal mean of 1.62 μg m-3. Moreover, chemical analysis revealed that the UFPs and PM1 were characterized by distinct composition; UFPs were composed mostly of organics, whereas ammonium and sulfate were the major constituents in PM1. The seasonal median of total PNCs ranged from 13.9 × 103 cm-3 in autumn to 19.4 × 103 cm-3 in spring. The PSD information retrieved from the corresponding PNC measurements indicates that the nucleation mode PNC (N4–25) peaked at 11.6 × 103 cm-3 in winter, whereas the Aitken mode (N25–100) and accumulation mode (N100–736) exhibited summer maxima at 6.0 × 103 and 3.1 × 103 cm-3, respectively. The shift in PSD during summertime is attributed to the enhancement in the photochemical production of condensable organic matter that, in turn, contributes to the growth of aerosol particles in the atmosphere. In addition, remarkable photochemical production of particles was observed in spring and summer seasons, which was characterized with averaged particle growth and formation rates of 4.3 ± 0.8 nm h-1 and 1.6 ± 0.8 cm-3 s-1, respectively. The prevalence of new particle formation (NPF) in summer is suggested as a result of seasonally enhanced photochemical oxidation of SO2, which contributes to the production of H2SO4, and low level of PM10 (d ≤ 10 μm) that serves as the condensation sink. Regarding the sources of aerosol particles, correlation analysis upon the PNCs against NOx revealed that the local vehicular exhaust was the dominant contributor of the UFPs throughout a year. On the contrary, the Asian pollution outbreaks can have significant influence in the PNC of accumulation mode particles during the seasons of winter monsoons. The results of this study underline the significance of secondary organic aerosols in the seasonal variations of UFPs and the influences of continental pollution outbreaks in the downwind areas of Asian outflows.