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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 19 ( 2017-10-12), p. 11929-11941
    Abstract: Abstract. Large and effective reductions in emissions of long-lived ozone-depleting substance (ODS) are being achieved through the Montreal Protocol, the effectiveness of which can be seen in the declining atmospheric abundances of many ODSs. An important remaining uncertainty concerns the role of very short-lived substances (VSLSs) which, owing to their relatively short atmospheric lifetimes (less than 6 months), are not regulated under the Montreal Protocol. Recent studies have found an unexplained increase in the global tropospheric abundance of one VSLS, dichloromethane (CH2Cl2), which has increased by around 60 % over the past decade. Here we report dramatic enhancements of several chlorine-containing VSLSs (Cl-VSLSs), including CH2Cl2 and CH2ClCH2Cl (1,2-dichloroethane), observed in surface and upper-tropospheric air in East and South East Asia. Surface observations were, on occasion, an order of magnitude higher than previously reported in the marine boundary layer, whilst upper-tropospheric data were up to 3 times higher than expected. In addition, we provide further evidence of an atmospheric transport mechanism whereby substantial amounts of industrial pollution from East Asia, including these chlorinated VSLSs, can rapidly, and regularly, be transported to tropical regions of the western Pacific and subsequently uplifted to the tropical upper troposphere. This latter region is a major provider of air entering the stratosphere, and so this mechanism, in conjunction with increasing emissions of Cl-VSLSs from East Asia, could potentially slow the expected recovery of stratospheric ozone.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 2
    Online Resource
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    Copernicus GmbH ; 2021
    In:  Atmospheric Chemistry and Physics Vol. 21, No. 6 ( 2021-03-23), p. 4487-4502
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 6 ( 2021-03-23), p. 4487-4502
    Abstract: Abstract. Climate is critically affected by aerosols, which alter cloud lifecycles and precipitation distribution through radiative and microphysical effects. In this study, aerosol and cloud property datasets from MODIS (Moderate Resolution Imaging Spectroradiometer), onboard the Aqua satellite, and surface observations, including aerosol concentrations, raindrop size distribution, and meteorological parameters, were used to statistically quantify the effects of aerosols on low-level warm-cloud microphysics and drizzle over northern Taiwan during multiple fall seasons (from 15 October to 30 November of 2005–2017). Our results indicated that northwestern Taiwan, which has several densely populated cities, is dominated by low-level clouds (e.g., warm, thin, and broken clouds) during the fall season. The observed effects of aerosols on warm clouds indicated aerosol indirect effects (i.e., increased aerosol loading caused a decrease in cloud effective radius (CER)), an increase in cloud optical thickness, an increase in cloud fraction, and a decrease in cloud-top temperature under a fixed cloud water path. Quantitatively, aerosol–cloud interactions (ACI=-∂ln⁡CER∂ln⁡α|CWP, changes in CER relative to changes in aerosol amounts) were 0.07 for our research domain and varied between 0.09 and 0.06 in the surrounding remote (i.e., ocean) and polluted (i.e., land) areas, respectively, indicating aerosol indirect effects were stronger in the remote area. From the raindrop size distribution analysis, high aerosol loading resulted in a decreased frequency of drizzle events, redistribution of cloud water to more numerous and smaller droplets, and reduced collision–coalescence rates. However, during light rain (≤1 mm h−1), high aerosol concentrations drove raindrops towards smaller droplet sizes and increased the appearance of drizzle drops. This study used long-term surface and satellite data to determine aerosol variations in northern Taiwan, effects on clouds and precipitation, and observational strategies for future research on aerosol–cloud–precipitation interactions.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 14 ( 2020-07-27), p. 8867-8908
    Abstract: Abstract. In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2009–2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 4
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 8 ( 2020-08-17), p. 4353-4392
    Abstract: Abstract. Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2505596-3
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  • 5
    In: Biogeosciences, Copernicus GmbH, Vol. 13, No. 6 ( 2016-03-23), p. 1787-1800
    Abstract: Abstract. Increases in nitrogen (N) availability and mobility resulting from anthropogenic activities have substantially altered the N cycle, both locally and globally. Taiwan characterized by the subtropical montane landscape with abundant rainfall, downwind of the most rapidly industrializing eastern coast of China, can be a demonstration site for extremely high N input and riverine DIN (dissolved inorganic N) export. We used 49 watersheds with similar climatic and landscape settings but classified into low, moderate, and highly disturbed categories based on population density to illustrate their differences in nitrogen inputs (through atmospheric N deposition, synthetic fertilizers, and human emission) and DIN export ratios. Our results showed that the island-wide average riverine DIN export is ∼ 3800 kg N km−2 yr−1, approximately 18 times the global average. The average riverine DIN export ratios are 0.30–0.51, which are much higher than the averages of 0.20–0.25 of large rivers around the world, indicating excessive N input relative to ecosystem demand or retention capacity. The low disturbed watersheds have a high N retention capacity and DIN export ratios of 0.06–0.18 in spite of the high N input (∼ 4900 kg N km−2 yr−1). The high retention capacity is likely due to effective uptake by secondary forests in the watersheds. The moderately disturbed watersheds show a linear increase in DIN export with increases in total N inputs and mean DIN export ratios of 0.20 to 0.31. The main difference in land use between low and moderately disturbed watersheds is the greater proportion of agricultural land cover in the moderately disturbed watersheds. Thus, their greater DIN export could be attributed to N fertilizers used in the agricultural lands. The greater export ratios also imply that agricultural lands have a lower proportional N retention capacity and that reforestation could be an effective land management practice to reduce riverine DIN export. The export ratios of the highly disturbed watersheds are very high, 0.42–0.53, suggesting that much of the N input is transported downstream directly, and urges the need to increase the proportion of households connected to a sewage system and improve the effectiveness of wastewater treatment systems. The increases in the riverine DIN export ratio along the gradient of human disturbance also suggest a gradient in N saturation in subtropical Taiwan. Our results help to improve our understanding of factors controlling riverine DIN export and provide empirical evidence that calls for sound N emission/pollution control measures.
    Type of Medium: Online Resource
    ISSN: 1726-4189
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2158181-2
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  • 6
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 22 ( 2021-11-25), p. 17185-17223
    Abstract: Abstract. Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50 % and 60 % were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (∼ 102 cm−3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day–night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (∼ 103–104 cm−3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (∼ 102–103 cm−3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either 〉50 nm or 〉100 nm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on the order of ∼ 10 to 1000 cm−3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol–cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 7
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 16 ( 2021-08-20), p. 12521-12541
    Abstract: Abstract. Plumes from the boreal spring biomass burning (BB) in northern peninsular Southeast Asia (nPSEA) are lifted into the subtropical jet stream and transported and deposited across nPSEA, South China, Taiwan and even the western North Pacific Ocean. This paper as part of the Seven SouthEast Asian Studies (7-SEAS) project effort attempts to improve the chemical weather prediction capability of the Weather Research and Forecasting coupled with the Community Multiscale for Air Quality (WRF–CMAQ) model over a vast region, from the mountainous near-source burning sites at nPSEA to its downwind region. Several sensitivity analyses of plume rise are compared in the paper, and it is discovered that the initial vertical allocation profile of BB plumes and the plume rise module (PLMRIM) are the main reasons causing the inaccuracies of the WRF–CMAQ simulations. The smoldering emission from the Western Regional Air Partnership (WRAP) empirical algorithm included has improved the accuracies of PM10, O3 and CO at the source. The best performance at the downwind sites is achieved with the inline PLMRIM, which accounts for the atmospheric stratification at the mountainous source region with the FINN burning emission dataset. Such a setup greatly improves not only the BB aerosol concentration prediction over near-source and receptor ground-based measurement sites but also the aerosol vertical distribution and column aerosol optical depth of the BB aerosol along the transport route. The BB aerosols from nPSEA are carried by the subtropical westerlies in the free troposphere to the western North Pacific, while BB aerosol has been found to interact with the local pollutants in the Taiwan region through three conditions: (a) overpassing western Taiwan and entering the central mountain area, (b) mixing down to western Taiwan, (c) transport of local pollutants upwards and mixing with a BB plume on higher ground. The second condition, which involves the prevailing high-pressure system from Asian cold surge, is able to impact most of the population in Taiwan.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 16 ( 2018-08-24), p. 12289-12313
    Abstract: Abstract. High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer (ABL) air masses due to convective transport processes. The local and meso-scale topographical features around the station are involved in the convective boundary layer development and in the formation of thermally induced winds leading to ABL air lifting. The station altitude alone is not a sufficient parameter to characterize the ABL influence. In this study, a topography analysis is performed allowing calculation of a newly defined index called ABL-TopoIndex. The ABL-TopoIndex is constructed in order to correlate with the ABL influence at the high altitude stations and long-term aerosol time series are used to assess its validity. Topography data from the global digital elevation model GTopo30 were used to calculate five parameters for 43 high and 3 middle altitude stations situated on five continents. The geometric mean of these five parameters determines a topography based index called ABL-TopoIndex, which can be used to rank the high altitude stations as a function of the ABL influence. To construct the ABL-TopoIndex, we rely on the criteria that the ABL influence will be low if the station is one of the highest points in the mountainous massif, if there is a large altitude difference between the station and the valleys or high plains, if the slopes around the station are steep, and finally if the inverse drainage basin potentially reflecting the source area for thermally lifted pollutants to reach the site is small. All stations on volcanic islands exhibit a low ABL-TopoIndex, whereas stations in the Himalayas and the Tibetan Plateau have high ABL-TopoIndex values. Spearman's rank correlation between aerosol optical properties and number concentration from 28 stations and the ABL-TopoIndex, the altitude and the latitude are used to validate this topographical approach. Statistically significant (SS) correlations are found between the 5th and 50th percentiles of all aerosol parameters and the ABL-TopoIndex, whereas no SS correlation is found with the station altitude. The diurnal cycles of aerosol parameters seem to be best explained by the station latitude although a SS correlation is found between the amplitude of the diurnal cycles of the absorption coefficient and the ABL-TopoIndex.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 9
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 7 ( 2021-04-09), p. 5533-5547
    Abstract: Abstract. A weak El Niño during 2014–2015 boreal winter developed as a strong boreal summer event in 2015 which continued and even enhanced during the following winter. In this work, the detailed changes in the structure, dynamics, and trace gases within the Asian summer monsoon anticyclone (ASMA) during the extreme El Niño of 2015–2016 is delineated by using Aura Microwave Limb Sounder (MLS) measurements, COSMIC radio occultation (RO) temperature, and National Centers for Environmental Prediction (NCEP) reanalysis products. Our analysis concentrates only on the summer months of July and August 2015 when the Niño 3.4 index started to exceed values of 1.5. The results show that the ASMA structure was quite different in summer 2015 as compared to the long-term (2005–2014) mean. In July, the spatial extension of the ASMA is greater than the long-term mean in all the regions except over northeastern Asia, where it exhibits a strong southward shift in its position. The ASMA splits into two, and the western Pacific mode is evident in August. Interestingly, the subtropical westerly jet (STJ) shifted southward from its normal position over northeastern Asia, and as a result midlatitude air moved southward in 2015. Intense Rossby wave breaking events along with STJ are also found in July 2015. Due to these dynamical changes in the ASMA, pronounced changes in the ASMA tracers are noticed in 2015 compared to the long-term mean. A 30 % (20 %) decrease in carbon monoxide (water vapor) at 100 hPa is observed in July over most of the ASMA region, whereas in August the drop is strongly concentrated at the edges of the ASMA. A prominent increase in O3 (〉 40 %) at 100 hPa is clearly evident within the ASMA in July, whereas in August the increase is strongly located (even at 121 hPa) over the western edges of the ASMA. Further, the temperature around the tropopause shows significant positive anomalies (∼ 5 K) within the ASMA in 2015. The present results clearly reveal the El-Niño-induced dynamical changes caused significant changes in the trace gases within the ASMA in summer 2015.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 8 ( 2023-04-20), p. 4727-4740
    Abstract: 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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
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