Long-range Transport Of Aerosols Research Articles

Does the Asian summer monsoon play a role in the stratospheric aerosol budget of the Arctic?

Abstract. The Asian summer monsoon has a strong convectional component with which aerosols are able to be lifted up into the lower stratosphere. Due to usually long lifetimes and long-range transport aerosols remain there much longer than in the troposphere and are also able to be advected around the globe. Our aim of this study is a synergy between simulations by Chemical Lagrangian Model of the Stratosphere (CLaMS) and KARL (Koldewey Aerosol Raman Lidar) at AWIPEV, Ny-Ålesund in the Arctic, by comparing CLaMS results with exemplary days of lidar measurements as well as analyzing the stratospheric aerosol background. We use global three-dimensional Lagrangian transport simulations including surface origin tracers as well as back trajectories to identify source regions of the aerosol particles measured over Ny-Ålesund. We analyzed lidar data for the year 2021 and found the stratosphere generally clear, without obvious aerosol layers from volcanic eruptions or biomass burnings. Still an obvious annual cycle of the backscatter coefficient with higher values in late summer to autumn and lower values in late winter has been found. Results from CLaMS model simulations indicate that from late summer to early autumn filaments with high fractions of air which originate in South Asia – one of the most polluted regions in the world – reach the Arctic at altitudes between 360 and 380 K potential temperature. We found a coinciding measurement between the overpass of such a filament and lidar observations, and we estimated that backscatter and depolarization increased by roughly 15 % during this event compared to the background aerosol concentration. Hence we demonstrate that the Asian summer monsoon is a weak but measurable source for Arctic stratospheric aerosol in late summer to early autumn.

Aerosols in the central Arctic cryosphere: satellite and model integrated insights during Arctic spring and summer

Abstract. The central Arctic cryosphere is influenced by the Arctic amplification (AA) and is warming faster than the lower latitudes. AA affects the formation, loss, and transport of aerosols. Efforts to assess the underlying processes determining aerosol variability are currently limited due to the lack of ground-based and space-borne aerosol observations with high spatial coverage in this region. This study addresses the observational gap by making use of total aerosol optical depth (AOD) datasets retrieved by the AEROSNOW algorithm over the vast cryospheric region of the central Arctic during Arctic spring and summer. GEOS-Chem (GC) simulations combined with AEROSNOW-retrieved data are used to investigate the processes controlling aerosol loading and distribution at different temporal and spatial scales. For the first time, an integrated study of AOD over the Arctic cryosphere during sunlight conditions was possible with the AEROSNOW retrieval and GC simulations. The results show that the spatial patterns observed by AEROSNOW differ from those simulated by GC. During spring, which is characterized by long-range transport of anthropogenic aerosols in the Arctic, GC underestimates the AOD in the vicinity of Alaska in comparison with AEROSNOW retrieval. At the same time, it overestimates the AOD along the Bering Strait, northern Europe, and the Siberian central Arctic sea-ice regions, with differences of −12.3 % and 21.7 %, respectively. By contrast, GC consistently underestimates AOD compared with AEROSNOW in summer, when transport from lower latitudes is insignificant and local natural processes are the dominant source of aerosol, especially north of 70° N. This underestimation is particularly pronounced over the central Arctic sea-ice region, where it is −10.6 %. Conversely, GC tends to overestimate AOD along the Siberian and Greenland marginal sea-ice zones by 19.5 % but underestimates AOD along the Canadian Archipelago by −9.3 %. The differences in summer AOD between AEROSNOW data products and GC-simulated AOD highlight the need to integrate improved knowledge of the summer aerosol process into existing models in order to constrain its effects on cloud condensation nuclei, on ice nucleating particles, and on the radiation budget over the central Arctic sea ice during the developing AA period.

Long range transport of South and East Asian anthropogenic aerosols counteracting Arctic warming

The large-scale convection during the Asian summer monsoon plays an important role in the rapid transport of boundary layer aerosols into the Asian summer monsoon anticyclone. Here, using the state-of-the-art ECHAM6–HAMMOZ aerosol-chemistry-climate model, we show that these aerosols are further transported to the Arctic along isentropic surfaces by the Brewer-Dobson-Circulation (BDC) during the monsoon season. Our model simulations show that East and South Asian anthropogenic emissions contribute significantly to the aerosol transported to the Arctic, which causes a higher negative net aerosol radiative forcing at the surface (dimming) of −0.09 ± 0.02 Wm−2 and −0.07 ± 0.02 Wm−2, respectively. Over the Arctic, the East Asian anthropogenic aerosols that include large amounts of sulfate cause a seasonal mean net radiative forcing at the top of the atmosphere (TOA) of −0.003 ± 0.001Wm−2 and a surface cooling of −0.56 K while the black carbon dominated aerosol from South Asia shows a positive TOA forcing of +0.004 ± 0.001Wm−2 with an only minor surface cooling of −0.043 K. Overall, the long-range transport of South Asian aerosols results in a notably warming throughout the atmospheric column but minimal temperature response at the Arctic surface. Conversely, East Asian aerosols cool the troposphere and heat the lower stratosphere in the Arctic. The Asian aerosol thus plays an ambivalent role, with the East Asian sources in particular having the potential to counteract the rapid rise in Arctic temperatures and the associated melting of snow and ice.

Lidar depolarization characterization using a reference system

Abstract. In this study, we present a new approach for the determination of polarization parameters of the Nicosia Cimel CE376 lidar system, using the PollyXT in Limassol as a reference instrument. The method is applied retrospectively to the measurements obtained during the 2021 Cyprus Fall Campaign. Lidar depolarization measurements represent valuable information for aerosol typing and for the quantification of some specific aerosol types such as dust and volcanic ash. An accurate characterization is required for quality measurements and to remove instrumental artifacts. In this article, we use the PollyXT, a widely used depolarization lidar, as our reference to evaluate the CE376 system's gain ratio and channel cross-talk. We use observations of transported dust from desert regions for this approach, with layers in the free troposphere. Above the boundary layer and the highest terrain elevation of the region, we can expect that, for long-range transport of aerosols, local effects should not affect the aerosol mixture enough for us to expect similar depolarization properties at the two stations (separated by ∼ 60 km). Algebraic equations are used to derive polarization parameters from the comparison of the volume depolarization ratio measured by the two systems. The applied methodology offers a promising opportunity to evaluate the polarization parameters of a lidar system, in cases where a priori knowledge of the cross-talk parameters is not available, or to transfer the polarization parameters from one system to the other.

Mass spectrometric analysis of unprecedented high levels of carbonaceous aerosol particles long-range transported from wildfires in the Siberian Arctic

Abstract. Wildfires in Siberia generate large amounts of aerosols, which may be transported over long distances and pose a threat to the sensitive ecosystem of the Arctic. Particulate matter (PM) of aged wildfire plumes originating from Yakutia in August 2021 was collected in Nadym and on Bely Island (both in northwestern Siberia). An advanced analysis of the chemical composition of aerosol particles was conducted through a multi-wavelength thermal–optical carbon analyzer (TOCA) coupled to resonance-enhanced multiphoton ionization time-of-flight mass spectrometry (REMPI-TOFMS) as well as through ultra-high-resolution Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS). In Nadym, concentrations of organic carbon (OC) and elemental carbon (EC) peaked at 100 and 40 µg m−3, respectively, associated with Angström absorption exponents for 405 and 808 nm (AAE405/808) between 1.5 and 3.3. The weekly average on Bely Island peaked at 8.9 µg m−3 of OC and 0.3 µg m−3 of EC and AAE405/808 close to unity. In particular, ambient aerosol in Nadym had a distinct biomass burning profile with pyrolysis products from carbohydrates, such as cellulose and hemicellulose, as well as lignin and resinoic acids. However, temporarily higher concentrations of five- and six-ring polycyclic aromatic hydrocarbons (PAHs), different from the PAH signature of biomass burning, suggest a contribution of regional gas flaring. FT-ICR MS with electrospray ionization (ESI) revealed a complex mixture of highly functionalized compounds, containing up to 20 oxygen atoms, as well as nitrogen- and sulfur-containing moieties. Concentrations of biomass burning markers on Bely Island were substantially lower than in Nadym, flanked by the appearance of unique compounds with higher oxygen content, higher molecular weight, and lower aromaticity. Back-trajectory analysis and satellite-derived aerosol optical depth suggested long-range transport of aerosol from the center of a Yakutian wildfire plume to Nadym and from the plume periphery to Bely Island. Owing to lower aerosol concentrations in the plume periphery than in its center, it is demonstrated how dilution affects the chemical plume composition during atmospheric aging.

Seasonal characterization of aerosols over high altitude location of southern India, Ooty, Tamilnadu

Climate change has been worsened by aerosols which got a significant place in the scientific research to understand climate change dynamics. Hence, the optical properties of the aerosols play an important role in the earth’s energy radiation budget. The Aerosol Optical Depth was measured at high altitude region in Ooty from December 2020 to May 2021. The spectral, monthly and diurnal variation of AOD were assessed and showed their seasonal variability. The mean AOD value at 500 nm was higher during the Summer season (0.625±0.323) than in the Winter season (0.213±0.006). The Black Carbon (BC) was measured using an Aethalo meter from December 2020 to September 2021. The average season wise concentrations of BC were 0.680±0.206µg m-3, 1.128±0.393 µg m-3 and 0.189±0.06 µg m-3 for the Winter, Summer and Monsoon seasons, respectively. The sources of BC mass concentration were apportioned based on fossil fuel (BCff) and biomass burning (BCbb). The fossil fuel based contribution was higher than the biomass based contribution to the total BC concentration. The comparative study of BC concentration with the AOD, it was projected that the AOD had increased in line with surging BC concentration up to April, 2021. The ground-based daily AOD measurements were compared with the MODIS retrieved AOD. The MODIS retrieved AOD was positively correlated with the ground measured AOD during the Winter and Summer seasons. The HYSPLIT trajectory presented the pathways of the source from the long range regions. The Winter season trajectory was attributed to the North-easterly and easterly winds and the Summer season was attributed to the North-westerly and westerly winds that exhibited the long-range transport of aerosols from the neighbouring cities. The meteorological parameters significantly affected the loading of aerosols during all the seasons, denoting that they were supposed to the local prevailing meteorological conditions.

Conditionally Background Level of Aerosol Pollution of Near-Surface Air in Moscow and One of Its Suburbs: Seasonal Variations

The data of continuous observations of aerosol composition in the near-surface atmosphere in Moscow (in the city center) and in Moscow region (near Zvenigorod, Moscow region) for three years, from autumn 2019 to the end of 2022, are analyzed. The obtained data were compared with the results of observations on the Moscow network stations “Mosecomonitoring”. The concept of conditionally background aerosol pollution of the atmosphere in Moscow is introduced for those days when the average daily concentration of PM10 is less than the MPC value (60 µg/m3). Previously, the authors found that all episodes of increased aerosol pollution in Moscow with daily average PM10 concentration higher than the MPC value, are associated either with the presence of a close local source in the city itself, or with the long-range transport of fire aerosols and/or dust from other territories to the Moscow region. The average daily PM2.5 concentration in the city and the suburb is lower than the MPC (35 µg/m3) all year round. The days corresponding to the introduced conditional background make up more than 91% over three years in the center of Moscow. Such a conditional background is formed by both natural and anthropogenic sources of aerosols, and not only of local, but also of remote origin. It implicitly takes into account the influence of meteorological conditions on sources and sinks of aerosols, as well as advective air mass transport of aerosol to and from the city. Seasonal variations in mass concentration of PM10, PM2.5 particles and individual chemical elements, as well as in the distribution of chemical elements by the size of aerosol particles in near-surface atmosphere under conditionally background pollution are analyzed. The emphasis is placed on the similarity and difference in the conditionally background near-surface aerosol for the city and the suburb in different seasons.

Assessment of vertical characterization and potential sources of aerosols in different altitude layers: Combined application of MAX-DOAS observation and the 3D-CWT model

Vertical distribution is essential for understanding the regional transport sources of pollutants accumulated at different altitudes. We investigate aerosol extinction coefficient (AEC) profiles based on ground-based multi-Axis differential optical absorption spectroscopy measurements from August 2020 to June 2021 in Ningbo, East China. AEC vertical structures can be classified into three groups: decreasing with height (51.2%), well-mixed (2.4%), and inverse structures (46.4%), which can be explained by long-range transport, the planetary boundary layer heigh, and temperature inversion. Except in the winter, the vertical profile of the AEC typically extends to higher altitudes, which suggests the accumulation, secondary formation, or long-range transport of aerosols at higher altitudes. The three-dimensional concentration weighted trajectory (3D-CWT) model is utilized to elucidate not only altitudinal atmospheric layers in which aerosol transport occurs, but also the potential source areas of aerosols at multiple air mass arrival altitudes. The 3D-CWT model results indicate the long-range transport of aerosols, mainly through backward air mass trajectories within layers 1 (0–500 m) and 2 (500–1000 m). The potential source areas of aerosols at lower altitudes are mainly distributed in the North China Plain. At air mass arrival altitudes exceeding 600 m, the sources likely to affect aerosols in Ningbo are both land-sourced and marine-sourced (including the East China Sea, Yellow Sea, and the marginal sea between Korea and Japan) air flows. At different air mass arrival altitudes, the estimated contributions of long-range transport to aerosols are approximately 6% (200 m), 11% (600 m), and 18% (1000 m). Our findings provide a scientific basis for revealing different aerosol vertical structures and assessing long-range transport contributions in coastal urban areas.

Diurnal source apportionment of organic and inorganic atmospheric particulate matter at a high-altitude mountain site under summer conditions (Sierra Nevada; Spain)

High-altitude mountain areas are sentinel ecosystems for global environmental changes such as anthropogenic pollution. In this study, we report a source apportionment of particulate material with an aerodynamic diameter smaller than 10 μm (PM10) in a high-altitude site in southern Europe (Sierra Nevada Station; SNS (2500 m a.s.l.)) during summer 2021. The emission sources and atmospheric secondary processes that determine the composition of aerosol particles in Sierra Nevada National Park (Spain) are identified from the concentrations of organic carbon (OC), elemental carbon (EC), 12 major inorganic compounds, 18 trace elements and 44 organic molecular tracer compounds in PM10 filter samples collected during day- and nighttime. The multivariate analysis of the joint dataset resolved five main PM10 sources: 1) Saharan dust, 2) advection from the urbanized valley, 3) local combustion, 4) smoke from a fire-event, and 5) aerosol from regional recirculation with high contribution of particles from secondary inorganic and organic aerosol formation processes. PM sources were clearly associated with synoptic meteorological conditions, and day- and nighttime circulation patterns typical of mountainous areas. Although a local pollution source was identified, the contribution of this source to PM10, OC and EC was small. Our results evidence the strong influence of middle- and long-range transport of aerosols, mainly from anthropogenic origin, on the aerosol chemical composition at this remote site.

The Identification and Analysis of Long-Range Aerosol Transport Pathways with Layered Cloud-Aerosol Lidar with Orthogonal Polarization Datasets from 2006 to 2016

In this study, we used Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aerosol products acquired from 2006 to 2016 to identify global long-range aerosol transport pathways, including the trans-Atlantic, the trans-Pacific, and the trans-Arabian Sea pathways. Deep analyses were subsequently conducted focusing on two significant paths within the range of the trans-Pacific transport pathway, from which we generated a three-stage conceptual model mainly identifying aerosols from the Taklimakan Desert and aerosols from the North China Plain. The results show that in the first stage of the model, the dust or polluted-dust aerosols were emitted, raised, and mixed within the planetary boundary layer (PBL), characterized by high percentages (>70%) of aerosols in the PBL (AODPBL), while in the second stage, some aerosols were further raised into the free troposphere where the AODPBL percentages decreased to less than 40%, driven by vertical movements and turbulences; in the last stage, the aerosols gradually settled back to the surface layer due to gravity and wet deposition, inferred by increasing AODPBL percentages. We demonstrated that the proposed model is capable of characterizing different aerosol types and climate conditions on spatiotemporal scales, providing a straightforward and evident approach to exploring long-range aerosol transport pathways.

Composition and mixing state of individual aerosol particles from northeast Greenland and Svalbard in the Arctic during spring 2018

The Arctic region is warming about four times faster than the rest of the globe, and thus it is important to understand the processes driving climate change in this region. Aerosols are a significant component of the Arctic climate system as they form ice crystals and liquid droplets that control the dynamics of clouds and also directly interact with solar radiation, depending on the compositions and mixing states of individual particles. Here, we report on the characteristics of submicron-sized aerosol particles using transmission electron microscopy obtained at two high Arctic sites, northeast Greenland (Villum Research Station) and Svalbard (Zeppelin Observatory), during spring 2018. The results showed that a dominant compound in the submicron-sized spring aerosols was sulfate, followed by sea salt particles. Both model simulations and observations at the Zeppelin Observatory showed that sea salt particles became more prevalent when low-pressure systems passed by the station. Model simulations indicate that both sampling sites were affected by diffused and diluted long-range transport of anthropogenic aerosols from lower latitudes with negligible influences of biomass burning emissions during the observation period. Overall, the composition of measured aerosol particles from the two Arctic sites was generally similar and showed no apparent variation except for the sea salt fractions. This study shows a general picture of high Arctic aerosol particles influenced by marine sources and diffused long-range transport of anthropogenic sources during the Arctic spring period. These results will contribute to a better knowledge of the aerosol composition and mixing state during the Arctic spring, which helps to understand the contributions of aerosols to the Arctic climate.

Temporal variability, meteorological influences, and long-range transport of atmospheric aerosols over two contrasting environments Agartala and Patiala in India.

The present study focused on the temporal variability, meteorological influences, potential sources, and long-range transport of atmospheric aerosols over two contrasting environments during 2011-2013. We have chosen Agartala (AGR) city in Northeast India as one of our sites representing the rural-continental environment and Patiala (PTA) as an urban site in Northwest India. The seasonal averaged equivalent black carbon (eBC) concentration in AGR ranges from 1.55 to 38.11µg/m3 with an average value of 9.87 ± 8.17µg/m3, whereas, at an urban location, PTA value ranges from 1.30 to 15.57µg/m3 with an average value of 7.83 ± 3.51µg/m3. The annual average eBC concentration over AGR was observed to be ~ 3 times higher than PTA. Two diurnal peaks (morning and evening) in eBC have been observed at both sites but were observed to be more prominent at AGR than at PTA. Spectral aerosol optical depth (AOD) has been observed to be in the range from 0.33 ± 0.09 (post-monsoon) to 0.85 ± 0.22 (winter) at AGR and 0.47 ± 0.04 (pre-monsoon) to 0.74 ± 0.09 (post-monsoon) at PTA. The concentration of eBC and its diurnal and seasonal variation indicates the primary sources of eBC as local sources, synoptic meteorology, planetary boundary layer (PBL) dynamics, and distant transportation of aerosols. The wintertime higher values of eBC at AGR than at PTA are linked with the transportation of eBC from the Indo-Gangetic Plain (IGP). Furthermore, it is evident that eBC aerosols are transported from local and regional sources, which is supported by concentration-weighted trajectory (CWT) analysis results.

Thermal infrared dust optical depth and coarse-mode effective diameter over oceans retrieved from collocated MODIS and CALIOP observations

Abstract. In this study, we developed a novel algorithm based on the collocated Moderate Resolution Imaging Spectroradiometer (MODIS) thermal infrared (TIR) observations and dust vertical profiles from the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) to simultaneously retrieve dust aerosol optical depth at 10 µm (DAOD10 µm) and the coarse-mode dust effective diameter (Deff) over global oceans. The accuracy of the Deff retrieval is assessed by comparing the dust lognormal volume particle size distribution (PSD) corresponding to retrieved Deff with the in situ-measured dust PSDs from the AERosol Properties – Dust (AER-D), Saharan Mineral Dust Experiment (SAMUM-2), and Saharan Aerosol Long-Range Transport and Aerosol–Cloud-Interaction Experiment (SALTRACE) field campaigns through case studies. The new DAOD10 µm retrievals were evaluated first through comparisons with the collocated DAOD10.6 µm retrieved from the combined Imaging Infrared Radiometer (IIR) and CALIOP observations from our previous study (Zheng et al., 2022). The pixel-to-pixel comparison of the two DAOD retrievals indicates a good agreement (R∼0.7) and a significant reduction in (∼50 %) retrieval uncertainties largely thanks to the better constraint on dust size. In a climatological comparison, the seasonal and regional (2∘×5∘) mean DAOD10 µm retrievals based on our combined MODIS and CALIOP method are in good agreement with the two independent Infrared Atmospheric Sounding Interferometer (IASI) products over three dust transport regions (i.e., North Atlantic (NA; R=0.9), Indian Ocean (IO; R=0.8) and North Pacific (NP; R=0.7)). Using the new retrievals from 2013 to 2017, we performed a climatological analysis of coarse-mode dust Deff over global oceans. We found that dust Deff over IO and NP is up to 20 % smaller than that over NA. Over NA in summer, we found a ∼50 % reduction in the number of retrievals with Deff>5 µm from 15 to 35∘ W and a stable trend of Deff average at 4.4 µm from 35∘ W throughout the Caribbean Sea (90∘ W). Over NP in spring, only ∼5 % of retrieved pixels with Deff>5 µm are found from 150 to 180∘ E, while the mean Deff remains stable at 4.0 µm throughout eastern NP. To the best of our knowledge, this study is the first to retrieve both DAOD and coarse-mode dust particle size over global oceans for multiple years. This retrieval dataset provides insightful information for evaluating dust longwave radiative effects and coarse-mode dust particle size in models.

Triggering of an Epidemic Outbreak via Long-Range Atmospheric Transport of Bio-Aerosols—Application to a Hypothetical Case for COVID-19

In the present work, we investigate the possibility that long-range airborne transport of infectious aerosols could initiate an epidemic outbreak at distances downwind beyond one hundred kilometers. For this, we have developed a simple atmospheric transport box model, which, for a hypothetical case of a COVID-19 outbreak, was compared to a more sophisticated three-dimensional transport-dispersion model (HYSPLIT) calculation. Coupled with an extended Wells–Riley description of infection airborne spread, it shows that the very low probability of outdoor transmission can be compensated for by high numbers and densities of infected and susceptible people in the source upwind and in the target downwind, respectively, such as occur in large urban areas. This may result in the creation of a few primary cases. It is worth pointing out that the probability of being infected remains very small at the individual level. Therefore, this process alone, which depends on population sizes, geography, seasonality, and meteorology, can only “trigger” an epidemic, which could then spread via the standard infection routes.

Exploring geometrical stereoscopic aerosol top height retrieval from geostationary satellite imagery in East Asia

Abstract. Despite the importance of aerosol height information for events such as volcanic eruptions and long-range aerosol transport, spatial coverage of its retrieval is often limited because of a lack of appropriate instruments and algorithms. Geostationary satellite observations in particular provide constant monitoring for such events. This study assessed the application of different viewing geometries for a pair of geostationary imagers to retrieve aerosol top height (ATH) information. The stereoscopic algorithm converts a lofted aerosol layer parallax, calculated using image-matching of two visible images, to ATH. The sensitivity study provides a reliable result using a pair of Advanced Himawari Imager (AHI) and Advanced Geostationary Radiation Imager (AGRI) images at 40∘ longitudinal separation. The pair resolved aerosol layers above 1 km altitude over East Asia. In contrast, aerosol layers must be above 3 km for a pair of AHI and Advanced Meteorological Imager (AMI) images at 12.5∘ longitudinal separation to resolve their parallax. Case studies indicate that the stereoscopic ATH retrieval results are consistent with aerosol heights determined using extinction profiles from the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP). Comparisons between the stereoscopic ATH and the CALIOP 90 % extinction height, defined by extinction coefficient at 532 nm data, indicated that 88.9 % of ATH estimates from the AHI and AGRI are within 2 km of CALIOP 90 % extinction heights, with a root-mean-squared difference (RMSD) of 1.66 km. Meanwhile, 24.4 % of ATH information from the AHI and AMI was within 2 km of the CALIOP 90 % extinction height, with an RMSD of 4.98 km. The ability of the stereoscopic algorithm to monitor hourly aerosol height variations is demonstrated by comparison with a Korea Aerosol Lidar Observation Network dataset.

Organic aerosols in the inland Tibetan Plateau: New insights from molecular tracers

Aerosols affect the radiative forcing of the global climate and cloud properties. Organic aerosols are among the most important, yet least understood, components of the sensitive Tibetan Plateau atmosphere. Here, the concentration of and the seasonal and diurnal variations in biomass burning and biogenic aerosols, and their contribution to organic aerosols in the inland Tibetan Plateau were investigated using molecular tracers. Biomass burning tracers including levoglucosan and its isomers, and aromatic acids showed higher concentrations during winter than in summer. Molecular tracers of primary and secondary biogenic organic aerosols were more abundant during summer than those in winter. Meteorological conditions were the main factors influencing diurnal variations in most organic molecular tracers during both seasons. According to the tracer-based method, we found that biogenic secondary organic aerosols (38.5 %) and fungal spores (14.4 %) were the two dominant contributors to organic aerosols during summer, whereas biomass burning (15.4 %) was an important aerosol source during winter at remote continental background site. Results from the positive matrix factor source apportionment also demonstrate the importance of biomass burning and biogenic aerosols in the inland Tibetan Plateau. During winter, the long-range transport of biomass burning from South Asia contributes to organic aerosols. In contrast, the precursors, biogenic secondary organic aerosols, and fungal spores from local emissions/long-range transport are the major sources of organic aerosols during summer. Further investigation is required to distinguish between local emissions and the long-range transport of organic aerosols. In-depth insights into the organic aerosols in the Tibetan Plateau are expected to reduce the uncertainties when evaluating aerosol effects on the climate system in the Tibetan Plateau.

Contribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: results from a regionally nested global model

Abstract. Global model studies and observations have shown that downward transport of aerosol nucleated in the free troposphere is a major source of cloud condensation nuclei (CCN) to the global boundary layer. In Amazonia, observations show that this downward transport can occur during strong convective activity. However, it is not clear from these studies over what spatial scale this cycle of aerosol formation and downward supply of CCN is occurring. Here, we aim to quantify the extent to which the supply of aerosol to the Amazonian boundary layer is generated from nucleation within a 1000 km regional domain or from aerosol produced further afield and the effectiveness of the transport by deep convection. We run the atmosphere-only configuration of the HadGEM3 climate model incorporating a 440 km × 1080 km regional domain over Amazonia with 4 km resolution. Simulations were performed over several diurnal cycles of convection. Below 2 km altitude in the regional domain, our results show that new particle formation within the regional domain accounts for only between 0.2 % and 3.4 % of all Aitken and accumulation mode aerosol particles, whereas nucleation that occurred outside the domain (in the global model) accounts for between 58 % and 81 %. The remaining aerosol is primary in origin. Above 10 km, the regional-domain nucleation accounts for up to 66 % of Aitken and accumulation mode aerosol, but over several days very few of these particles nucleated above 10 km in the regional domain are transported into the boundary layer within the 1000 km region, and in fact very little air is mixed that far down. Rather, particles transported downwards into the boundary layer originated from outside the regional domain and entered the domain at lower altitudes. Our model results show that CCN entering the Amazonian boundary layer are transported downwards gradually over multiple convective cycles on scales much larger than 1000 km. Therefore, on a 1000 km scale in the model (approximately one-third the size of Amazonia), trace gas emission, new particle formation, transport and CCN production do not form a “closed loop” regulated by the biosphere. Rather, on this scale, long-range transport of aerosol is a much more important factor controlling CCN in the boundary layer.

Aerosol Characterization of Northern China and Yangtze River Delta Based on Multi-Satellite Data: Spatiotemporal Variations and Policy Implications

Horizontal and vertical distributions of aerosol properties in the Taklimakan Desert (TD), North central region of China (NCR),North China Plain(NCP), and Yangtze River Delta (YRD) were investigated by statistical analysis using Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) L3 data from 2007 to 2020, to identify the similarities and differences in atmospheric aerosols in different regions, and evaluate the impact of pollution control policies developed in China in 2013 on aerosol properties in the study area. The aerosol optical depth (AOD) distribution had substantial seasonal and spatial distribution characteristics. AOD had high annual averages in TD (0.38), NCP (0.49), and YRD (0.52). However, these rates showed a decline post-implementation of the long-term pollution control policies; AOD values declined by 5%, 13.8%, 15.5%, and 23.7% in TD, NCR, NCP, and YRD respectively when comparing 2014–2018 to 2007–2013, and by 7.8%, 11.5%, 16%, and 10.4% when comparing 2019–2020 to 2014–2018. The aerosol extinction coefficient showed a clear regional pattern and a tendency to decrease gradually as height increased. Dust and polluted dust were responsible for the changes in AOD and extinction coefficients between TD and NCR and NCP and YRD, respectively. In TD, with change of longitude, dust aerosol first increased and then decreased gradually, peaking in the middle. Similarly in NCP, polluted dust aerosol first increased and then decreased, with a maximum value in the middle. The elevated smoke aerosols of NCP and YRD were significantly higher than those observed in TD and NCR. The high aerosol extinction coefficient values (>0.1 km−1) were mainly distributed below 4 km, and the relatively weak aerosol extinction coefficients (>0.001 km−1) were mainly distributed between 5–8 km, indicating that the high-altitude long-range transport of TD and NCR dust aerosols affects NCP and YRD.

Long-range transport of CO and aerosols from Siberian biomass burning over northern Japan during 18–20 May 2016

High CO concentration and dense aerosol layers at 1–6 km altitude in the free troposphere were observed over Rikubetsu, Japan, in ground-based Fourier transform spectrometer (FTS) and lidar measurements during 18–20 May 2016, days after intense wildfires east of Lake Baikal, Siberia. The column-averaged dry-air mole fraction of CO (XCO) was observed to be ∼150 ppb from 11:15 to 13:50 JST on 19 May, and peak aerosol optical depths (AODs) of 1.41 and 1.28 were observed at 15:40 JST 18 May and 11:20 JST 19 May, respectively. We used the HYSPLIT model to calculate five-day backward trajectories from Rikubetsu on May 18, 2016 at 2, 3 and 5 km altitude. The results show that the air parcels passed over the Siberian wildfires during 16–17 May. It was found that the high CO concentrations originated from forest fires were transported to the upper layers of Hokkaido. This will contribute to the understanding of the regional effects of air pollution in northern Japan due to air masses originating from forest fires. By combining these independent datasets such as AERONET aerosol optical thickness (AOT), MODIS fire data, and Infrared Atmospheric Sounding Interferometer (IASI) total CO columns, we confirmed that the lidar measurements of enhanced aerosol concentrations and FTS measurements of maximum XCO over Rikubetsu resulted from a persistent smoke plume transported from Siberian wildfires. Relatively large-scale forest fires have been frequently occurring in Siberia recently. However, the effects of CO and other gases released from them over northern Japan are not well known. We observed high concentrations of CO over the TCCON station in Rikubetsu, Japan, which we believe to be of forest fire origin. Therefore, we analyzed it as a case study to confirm its origin and impact on the upper atmosphere over northern Japan.

Using cluster algorithms with a machine learning technique and PMF models to quantify local-specific origins of PM2.5 and associated metals in Taiwan

The influence of long-range transport (LRT) of air pollutants on neighboring regions and countries has been documented. The magnitude of LRT aerosols and related constituents can misdirect control strategies for local air quality management. In this study, we aimed to quantify PM2.5 (diameter less than 2.5 μm, PM2.5) and associated metals derived from local sources and LRT in different geographic locations in Taiwan using advanced receptor models. We collected daily PM2.5 samples (n = ∼1000) and analyzed 28 metals every three days from 2016 to 2018 in the northern, central-south, eastern, and southern areas of Taiwan. We first used a machine learning technique with a cluster algorithm coupled with a backward trajectory to classify local, regional, and LRT-related aerosols. We then quantified the source contributions with a positive matrix factorization (PMF) model for Taiwan weighted by region-specific populations. The northern and eastern regions were found to be more vulnerable to LRT-related PM2.5 and metals than the central-south and southern regions in Taiwan. The LRT increased Pb and As concentrations by 90–200% and ∼40% in the northern and central-south regions. Ambient PM2.5-metals mainly originated from local traffic-related emissions in the northern, central-south, and southern regions, whereas oil combustion was the primary source of PM2.5-metals in the eastern region. By subtracting the influence from the LRT, the contributions of domestic emission sources to ambient PM2.5 metals in Taiwan were 35% from traffic-related emission, 17% from non-ferrous metallurgy, 13% from iron ore and steel factories, 12% from coal combustion, 12% from oil combustion, 10% from incinerator emissions, and <1% from cement manufacturing emissions. This study proposed an advanced method for refining local source contributions to ambient PM2.5 metals in Taiwan, which provides useful information on regional control strategies.