Organic Carbon Aerosols Research Articles

Long-range transport of air pollutants increases the concentration of hazardous components of PM2.5 in northern South America

Abstract. Long-range transport (LRT) of air pollutants from a range of sources can substantially enhance background pollution levels, especially in urbanized regions, which can exacerbate high-pollution episodes. In the Aburrá Valley (AV), Colombia, and other cities in northern South America, biomass burning (BB), dust, and volcanic degassing have been identified as sources of long-range aerosol transport. However, the impact of these sources on air quality and the characterization of these sources have yet to be thoroughly studied. This work investigates the influence of these sources on the chemical composition of PM2.5 during annual and intra-annual high-load aerosol events in the AV. We identified, tracked, and meteorologically characterized LRT events and evaluated their influence on PM2.5 concentration and chemical composition. We found that the LRT of aerosols from BB, dust, and volcanic degassing influenced approximately 13 %, 8 %, and 13 % of days in the year, respectively. We applied the positive-matrix-factorization (PMF) statistical model to quantify PM2.5 concentrations and chemical compositions for the different LRT event types (e.g., BB). For BB events, we identified large contributions from organic carbon (OC1 and OC2), F−, and secondary aerosol tracers (SO42- and NO3-). For dust LRT events, crustal mineral components, along with Ti and Ca, were the primary contributors to aerosol composition, while SO42-, Na, Al, and Ca were the primary contributors during volcanic events. The concentrations of some ions and toxic heavy metals (Cr, Mn, Cd, and Ni) were also elevated during BB and volcanic-degassing events. BB contributed the most to PM2.5 levels during the LRT events (∼11 µg m−3), while contributions from aerosols arising from dust and volcanic events were also substantial (<7 µg m−3). Our study identifies the Orinoco and the Middle Magdalena Valley as sizable sources of BB aerosols and Nevado del Ruiz as a source of volcanic aerosols. Additionally, we found that African dust reached the Andean region via the Caribbean route. As a result, we identify the need for future chemical-transport modeling studies in the region and new support strategies to manage internal and external pollution sources that degrade air quality in the AV and the surrounding region.

Chemical composition, source characteristics, and hygroscopic properties of organic-enriched aerosols in the high Arctic during summer

Arctic regions are extremely sensitive to global warming. Aerosols are one of the most important short-lived climate-forcing agents affecting the Arctic climate. The present study examines the summertime chemical characteristics and potential sources of various organic and inorganic aerosols at a Norwegian Arctic site, Ny-Ålesund (79°N). The results show that organic matter (OM) accounts for 60 % of the total PM10 mass, followed by sulfate (SO42−). Water-soluble organic carbon (WSOC) contributes 62 % of OC. Photochemical processes involving diverse anthropogenic and biogenic precursor compounds are identified as the major sources of WSOC, while water-insoluble organic carbon (WIOC) aerosols are predominantly linked to primary marine emissions. Despite being a remote pristine site, the aerosols show a sign of chemical aging, evidenced by a significant chloride depletion, which was about 82 % on average during the study period. Nitrogen-containing aerosols are likely stemming from migratory seabird colonies and local dust sources around the sampling site. While biogenic, crustal, and sea salt-derived SO42- account for 37%, 8%, and 5% respectively, the remaining 50% is attributed to anthropogenic SO42-. Through chemical tracers, Pearson correlation coefficient matrix, and Hierarchical Cluster Analysis (HCA), the present study identifies soil biota (terrestrial biogenic) and marine emissions, along with their photochemical oxidation processes, as potential sources of Arctic aerosols during summer, while biomass burning and combustion-related sources have a minor contribution. The chemical closure of hygroscopicity highlights that while organics predominantly control aerosol hygroscopicity in the Arctic summer, specific inorganic components like (NH4)2SO4 can significantly increase it on certain days, affecting aerosol-cloud interactions and climate processes over the Arctic during summer. The present study highlights the high abundance of organics and their vital role in the Arctic climate during summer when natural aerosols are conquered.

20th Century Changes of DOC and Its 14C Signature Archived in Caucasus Ice‐Core: Implications for Past Sources of Organic Carbon Aerosol in South‐Eastern Europe

AbstractTo reconstruct the history of organic carbon (OC) aerosol over south‐eastern Europe, dissolved organic carbon (DOC) and its 14C signature (DO14C) were investigated along an ice core drilled at the Mount Elbrus (ELB) in Caucasus. In summer, compared to pre‐1945 levels, the DOC concentrations increased by 45% after 1960, the mean DO14C depletion in recent ELB ice relative to atmospheric 14CO2 of 32% being attributed to fossil‐fuel sources. DO14C content of ice deposited during the bomb‐peak era (1955–1980) closely followed atmospheric 14CO2 changes caused by atmospheric nuclear tests, suggesting the living biosphere as the main biogenic source of DOC in summer in this region. ELB data contrast with those previously obtained in summer Alpine (western Europe) ice in which a post‐1950 doubling of DOC was observed and attributed to enhanced emissions of organic compounds from vegetation in France. This regional difference is discussed with respect to changes of biogenic organic compound emissions in response to past change of use‐land and global warming. ELB data document, for the first time, changes of DOC and DO14C in winter mountain ice showing an increase by 44% of DOC levels associated with a 14C signature being 47% lower than that of atmospheric 14CO2 in ELB ice deposited after 1960. The 14C winter ELB ice record followed atmospheric 14CO2 changes with a delay of ∼3 years, suggesting that remaining emissions from the living biosphere, together with a small contribution from wood burning, are the main biogenic sources of DOC in winter in this region.

Polar Aerosol Atmospheric Rivers: Detection, Characteristics, and Potential Applications

AbstractAerosols play a key role in polar climate, and are affected by long‐range transport from the mid‐latitudes, both in the Arctic and Antarctic. This work investigates poleward extreme transport events of aerosols, referred to as polar aerosol atmospheric rivers (p‐AAR), leveraging the concept of atmospheric rivers (AR) which signal extreme transport of moisture. Using reanalysis data, we build a detection catalog of p‐AARs for black carbon, dust, sea salt and organic carbon aerosols, for the period 1980–2022. First, we describe the detection algorithm, discuss its sensitivity, and evaluate its validity. Then, we present several extreme transport case studies, in the Arctic and in the Antarctic, illustrating the complementarity between ARs and p‐AARs. Despite similarities in transport pathways during co‐occurring AR/p‐AAR events, vertical profiles differ depending on the species, and large‐scale transport patterns show that moisture and aerosols do not necessarily originate from the same areas. The complementarity between AR and p‐AAR is also evidenced by their long‐term characteristics in terms of spatial distribution, seasonality and trends. p‐AAR detection, as a complement to AR, can have several important applications for better understanding polar climate and its connections to the mid‐latitudes.

Roles of tropical cyclones with varying intensities in the re-distribution of aerosols

The study analyzes three tropical cyclones (TC) with varying intensities, namely BOB02, a deep depression in the Bay of Bengal; Tauktae, an extremely severe cyclone in the Arabian Sea (AS); and Amphan, a supercyclone in the Bay of Bengal, which developed on October 11, 2020, May 13, 2021, and May 16, 2020, respectively. The analysis focuses on studying the re-distribution of the aerosols over the Indian region using these distinct datasets: Modern-Era Retrospective Analysis for Research and Application, version 2 (MERRA2), Integrated Multi-Satellite Retrievals for GPM (IMERG), and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). Throughout the cyclonic period, which includes the period from the inception of the low-pressure area to its dissipation as well as the pre-cyclonic and post-cyclonic periods (one week prior to and after the cyclonic period, respectively), various parameters related to aerosols and background meteorological conditions were collected. The primary parameter of interest was the aerosol optical depth (AOD). The analysis revealed significant variations in meteorological parameters such as wind speed, temperature, relative humidity, and rainfall along the cyclone track during both the cyclonic and post-cyclonic conditions compared to the pre-cyclonic conditions of these TCs. The AOD surrounding the cyclone track decreases during cyclonic and post-cyclonic conditions compared to pre-cyclonic conditions. This is due to the scavenging of both anthropogenic and natural (dust) aerosols. Conversely, AOD increases along the cyclone track, mainly due to an increase in natural (sea salt) aerosols. During pre-cyclonic conditions, both natural (dust) and anthropogenic (black carbon, organic carbon, and sulfate) aerosols contribute significantly to the total AOD, whereas during pre-cyclonic conditions, the main contributors are natural (sea-salt) aerosols. The coarse-mode particles are more dominant during cyclonic and post-cyclonic conditions than pre-cyclonic ones. Furthermore, our observations indicate that the atmospheric boundary layer (ABL) height increases by ∼0.1–0.6 km along the cyclone track during cyclonic conditions compared to pre-cyclonic conditions. While AOD from the free troposphere (FT) contributes more to the total AOD, contributions from ABL increase, while those from the FT decrease during cyclonic and post-cyclonic conditions.

Spatiotemporal Variations in Summertime Arctic Aerosol Optical Depth Caused by Synoptic‐Scale Atmospheric Circulation in Three Reanalyses

AbstractAtmospheric aerosol affects the radiation budget, cloud cover and properties, and surface albedo of sea ice and snow over the Arctic with obvious climatological significance. However, observations are scarce and have large uncertainties. Aerosol optical depth (AOD) variability in the Arctic and its relationship with atmospheric disturbances on synoptic timescales were investigated on the basis of the JRAero, CAMSRA, and MERRA2 reanalyses. Total AODs of the three reanalyses were spatiotemporally consistent in summer, although contributions of individual aerosol species differed. Summertime AOD variability was strongly correlated with observations in all reanalyses. The predominance of organic carbon aerosol indicates that aerosols are derived mainly from biomass burning over northern Eurasia and northern North America. Differences in composites of atmospheric fields between high‐ and low‐loading days indicate that locations of synoptic disturbances are related to high‐AOD events in the Arctic. Furthermore, empirical orthogonal function analysis indicates that the first‐ and second‐largest AOD variabilities in synoptic timescales occur over northern Eurasia. This AOD variability is related to two different types of Arctic cyclone, the development of which is important in aerosol transport, aging, and deposition in summer.

Metrological traceable calibration of organic carbon and elemental carbon based on laboratory-generated reference materials

Carbonaceous aerosol, including organic carbon (OC) and elemental carbon (EC), has significant influence on human health, air quality and climate change. Accurate measurement of carbonaceous aerosol is essential to reduce the uncertainty of radiative forcing estimation and source apportionment. The accurate separation of OC and EC is controversial due to the charring of OC. Therefore, the development of reference materials (RM) for the validation of OC/EC separation is an important basis for further study. Previous RMs were mainly based on ambient air sampling, which could not provide traceability of OC and EC concentration. To develop traceable RMs with known OC/EC contents, our study applied an improved aerosol generation and mixing technique, providing uniform deposition of particles on quartz filters. To generate OC aerosol with similar pyrolytic property of ambient aerosol, both water soluble organic carbon (WSOC) and water insoluble organic carbon (WIOC) were used, and amorphous carbon was selected for EC surrogate. The RMs were analyzed using different protocols. The homogeneity within the filter was validated, reaching below 2%. The long-term stability of RMs has been validated with RSD ranged from 1.7%–3.2%. Good correlation was observed between nominal concentration of RMs with measured concentration by two protocols, while the difference of EC concentration was within 20%. The results indicated that the newly developed RMs were acceptable for the calibration of OC and EC, which could improve the accuracy of carbonaceous aerosol measurement. Moreover, the laboratory-generated EC-RMs could be suitable for the calibration of equivalent BC concentration by Aethalometers.

Comparison of the Performance of the GRASP and MERRA2 Models in Reproducing Tropospheric Aerosol Layers

Two approaches, based on Generalized Retrieval of Aerosol and Surface Properties (GRASP) and Modern-Era Retrospective Analysis for Research and Applications version 2 (MERRA-2) models, are investigated for reproducing aerosol layers in the troposphere. The GRASP algorithm is supplied with synergistic LIDAR and sunphotometer measurements to obtain aerosol extinction profiles. MERRA-2 is an atmospheric reanalysis coupling model that includes an external mixture of sea salt, dust, organic carbon, black carbon, and sulfate aerosols. A data set from Racibórz observatory, obtained with LIDAR and a sunphotometer in the 2017–2020 period, is analysed with GRASP along with the closest grid point data given by MERRA-2. The models demonstrate satisfactory agreement, yet some discrepancies were observed, indicating the presence of biases. For vertically integrated profiles, the correlation coefficient (R) between aerosol optical thickness was calculated to be 0.84, indicating a strong linear relationship. The Pearson correlation coefficient calculated between profiles for the selected altitude sectors varies between 0.428 and 0.824, indicating moderate to good agreement at all altitudes. GRASP shows denser aerosol layers in the mid-troposphere, while MERRA-2 gives higher aerosol extinctions throughout the high troposphere to low stratosphere region. Moreover, GRASP does not provide vertical variability in the extinction profile near the ground, due to a lack of data in the LIDAR’s incomplete overlap range. Lastly, the aerosol layer identification and type recognition are validated with statistical analysis of air mass backward trajectories with endpoints spatially and temporally collocated with individual identified layers. These reveal potential source regions that are located within areas known to be significant sources for the different identified aerosol types.

Ozone deterioration over North China plain caused by light absorption of black carbon and organic carbon

Previous studies have revealed that the light absorption effect of black carbon (BC) aerosol could influence ozone concentrations via absorbing sunlight and modulating photolysis rates, the so-called aerosol-photolysis interaction (API). However, few studies have quantified the API effect of organic carbon (OC) aerosol, which has recently been found to contribute to about 10%–40% of the total light absorption at 300 nm wavelength. This study tried to quantify and compare the OC and BC aerosols' influence on ozone concentrations through a case study over North China Plain (NCP) in Oct. 2018. By modulating OC's absorption index based on field measurements, we quantified the OC and BC API effect on surface ozone by the WRF-Chem model. The API effect and its uncertainties of OC aerosols were evaluated using the high and low absorption values that have been reported in previous studies. Results showed that, in terms of the pollution periods in NCP, removing all the OC aerosol from the atmosphere could increase the daytime maximum daily average 8-h (MDA8) O3. In this episode, the average (extreme) MDA8 O3 increased by 0.7–2.4 ppb (1.1–3.7 ppb), accounting for 1.5%–5.3% (2.4%–8.8%) of ozone concentration, comparable to that by BC of 2.0 ppb (3.3 ppb), accounting for 4.4% (7.8%), which means the OC's API effect was 35%–120% of BC's API effect on surface ozone in this case. The results also indicated a fact that, though OC has a lower light absorption rate than BC, the API efficiency of OC on surface ozone when reducing aerosols could be compensated by a higher portion of OC aerosols and higher light absorption efficiency due to much more OC was distributed on higher altitude (especially 1–3 km) than BC aerosols, which result in larger ozone changes in both the low troposphere and surface.

A comprehensive reappraisal of long-term aerosol characteristics, trends, and variability in Asia

Abstract. Changes in aerosol loadings and properties are important for the understanding of atmospheric environment and climate change. This study investigates the characteristics and long-term trends of aerosols of different sizes and types in Asia from 2000 to 2020 by considering multi-source aerosol data and novel analysis methods and perspectives, all of which provides the groundwork for promoting the acquisition of new discoveries that are different from the past. The geometric mean aggregation method is applied, and serial autocorrelation is considered to avoid the overestimation of trend significance. Among regions in Asia, high values of aerosol optical depth (AOD) are mainly concentrated in East Asia (EA) and South Asia (SA) and are closely related to the population density. The AOD in EA showed the most significant negative trend, with a value of -5.28×10-4 per year, mainly owing to decreases in organic carbon (OC), black carbon (BC), and dust aerosols. It is also worth noting that this observed large-scale decrease in OC and BC is a unique and significant phenomenon to region of EA and mainly around China. In contrast, the aerosol concentrations in SA generally show a positive trend, with an increased value of AOD of 1.25 × 10−3 per year. This increase is mainly due to large emissions of fine-mode aerosols, such as OC and sulfate aerosol. Additionally, the high aerosol loading in northern SA has a lower AOD variability when compared with that of East China Plain, revealing a relatively more persistent air pollution situation. Over the whole region of Asia, the characteristics of the percentage changes in different types of AOD are seen in the increases in BC (6.23 %) and OC (17.09 %) AOD, together with a decrease in dust (−5.51 %), sulfate (−3.07 %), and sea salt (−9.80 %) AOD. Except for anthropogenic emissions, the large increase in the percentage of OC is also due to wildfires found in northern Asia in the summer, whereas the differently sized AOD only shows slight changes in Asia in that small-sized AOD decreases (−3.34 %) and that the total AOD did not show a significant change. This suggests that, from a trend perspective, decreases in aerosol in recent years have mostly been offsetting earlier increases in the anthropogenic emissions over Asia. To summarize, the above findings analyse the comprehensive characteristics of aerosol distributions and reappraise the long-term trends of different aerosol parameters, which will greatly enhance the understanding of regional and global aerosol environment and climatology, in addition to filling the gaps and breaking through the limitations of past knowledge.

Changing patterns in the highly contributing aerosol types/species across the globe in the past two decades

With the rapidly changing aerosol emissions due to the increase in urbanization, energy consumption, population density, and industrialization in the past two decades across the globe, there is an evolution of different chemical properties of aerosols that are yet not quantified properly. Therefore, a rigorous attempt is made in this study to obtain the long-term changing patterns in the contribution of different aerosol types/species, to the total aerosol loading. This study is carried out only over those regions exhibiting either increasing or decreasing trends in the aerosol optical depth (AOD) parameter on a global scale. Applying the multivariate linear regression trend analysis on Modern-Era Retrospective Analysis for Research and Application version 2 (MERRA-2) aerosol species dataset obtained between 2001 and 2020, we found that despite the overall statistically significant decrease in total columnar AOD trend values over North-Eastern America, and Eastern and Central China regions, an increase in the dust and organic carbon aerosols is observed, respectively. As the uneven vertical distribution of aerosols can alter the direct radiative effects, the extinction profiles of different aerosol types obtained using Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) dataset between 2006 and 2020, are further partitioned, for the first time, based on their presence in different altitudes (i.e., within the atmospheric boundary layer and free-troposphere) as well as measurement timing (i.e., daytime and night-time) regimes. The detailed analysis showed that there exists an overall higher contribution of aerosols persisting in the free troposphere region which in turn can have a long-term effect on climate due to their higher residence time, particularly absorbing aerosols. As the trends are mostly associated with the changes in energy use, regional regulatory policies, and/or changing background meteorology conditions, therefore this study also elaborates on the effectiveness of these factors with the changes obtained in different aerosol species/types over the region.

Evaluation of PM Chemical Composition in Thessaloniki, Greece Based on Air Quality Simulations

The average PM10 daily levels over the urban area of Thessaloniki, Greece, usually exceed the air quality limits and therefore the improved PM chemical composition and air quality modeling results that will facilitate the design of the most appropriate mitigation measures (e.g., limitations in wood combustion for heating purposes) are essential. The air quality modeling system WRF-CAMx was applied over a 2 × 2 km2 horizontal resolution grid covering the greater area of Thessaloniki for the year 2015, when Greece was still confronting the consequences of the financial crisis. The output hourly surface concentrations of twelve PM species at three sites of different environmental type characterization in the city of Thessaloniki were temporally and spatially analyzed. Carbonaceous aerosols (organic and elemental) are the major contributor to total PM10 levels during winter representing a 35–40% share. During summer, mineral aerosols (excluding dust) distribute by up to 48% to total PM10 levels, being the major contributor attributed to road traffic. PM species, during winter, increase in the morning and in the afternoon mainly due to road transport and residential heating, respectively, in addition with the unfavorable meteorological conditions. An underestimation of the primary organic carbon aerosol levels during winter is identified. The application of the modeling system using a different speciation profile for the fine particles emissions from residential heating based on observational data instead of the CAMS emissions profile revealed an improvement in the simulated OC/EC values for which a 50% increase was identified compared to the base run.

Quantitative evaluation for the sources and aging processes of organic aerosols in urban Guangzhou: Insights from a comprehensive method of dual‑carbon isotopes and macro tracers

Organic carbon aerosol (OC) is a pivotal component of PM2.5 in the atmospheric environment, yet its emission sources and atmospheric behaviors remain poorly constrained in many regions. In this study, a comprehensive method based on the combination of dual‑carbon isotopes (13C and 14C) and macro tracers was employed in the PRDAIO campaign performed in the megacity of Guangzhou, China. The 14C analysis showed that 60 ± 9 % of OC during the sampling campaign was associated with non-fossil sources such as biomass burning activities and biogenic emissions. It should be noted that this non-fossil contribution in OC would significantly decrease when the air masses came from the eastern cities. Overall, we found that non-fossil secondary OC (SOCNF) was the largest contributor (39 ± 10 %) to OC, followed by fossil secondary OC (SOCFF: 26 ± 5 %), fossil primary OC (POCFF: 14 ± 6 %), biomass burning OC (OCbb: 13 ± 6 %) and cooking OC (OCck: 8 ± 5 %). Also, we established the dynamic variation of 13C as a function of aged OC and the volatile organic compounds (VOCs) oxidized OC to explore the impact of aging processes on OC. Our pilot results showed that atmospheric aging was highly sensitive to the emission sources of seed OC particles, with a higher aging degree (86 ± 4 %) when more non-fossil OC particles were transferred from the northern PRD.

Emission Characteristics of Organic Carbon and Elemental Carbon in PM10 and PM2.5 from Vehicle Exhaust and Civil Combustion Fuels

To study the emission characteristics of carbonaceous aerosol in particulate matter emitted from vehicle exhaust and main civil combustion fuels, organic carbon (OC) and elemental carbon (EC) in PM10 and PM2.5 samples from vehicle sources (gasoline vehicles, light duty diesel vehicles, and heavy duty diesel vehicles), civil coal (chunk coal and briquette coal), and biomass fuels (wheat straw, wood plank, and grape branches) were collected and analyzed by using a multifunctional portable dilution channel sampler and the Model 5L-NDIR OC/EC analyzer. The results showed that there were significant differences in the proportion of carbonaceous aerosols in PM10 and PM2.5from different emission sources. The proportions of total carbon (TC) in PM10 and PM2.5 of different emission sources were 40.8%-68.5% and 30.5%-70.9%, respectively, and the OC/EC were 1.49-31.56 and 1.90-87.57, respectively. The carbon components produced by different emission sources were dominated by OC, and the OC/TC values in PM10 and PM2.5 were 56.3%-97.0% and 65.0%-98.7%, respectively. The proportions of OC in carbonaceous aerosols in PM10and PM2.5 were in the descending order of:briquette coal>chunk coal>gasoline vehicle>wood plank>wheat straw>light duty diesel vehicle>heavy duty diesel vehicle and briquette coal>gasoline car>grape branches>chunk coal>light duty diesel vehicle>heavy duty diesel vehicle, respectively. The main components of carbonaceous aerosols in PM10 and PM2.5 emitted from the various emission sources were different, and source apportionment of carbonaceous aerosols could be accurately distinguished by their ingredient composition profiles.

Atmospheric nanoparticles hygroscopic growth measurement by a combined surface plasmon resonance microscope and hygroscopic tandem differential mobility analyzer

Abstract. The hygroscopic growth of atmospheric aerosols plays an important role in regional radiation, cloud formation, and hence climate. Aerosol hygroscopic growth is often characterized by hygroscopic tandem differential mobility analyzers (HTDMAs), and Xie et al. (2020) recently demonstrated that hygroscopic growth measurements of a single particle are possible using a surface plasmon resonance microscope-azimuthal rotation illumination (SPRM-ARI). The hygroscopic properties of ambient aerosols are not uniform and often exhibit large relative humidity (RH) and size variabilities due to different chemical compositions and mixing states. To better understand the contribution of different aerosol components and establish a link between the apparent hygroscopic properties of single particles and bulk aerosols, we conduct combined hygroscopic growth measurements using a SPRM-ARI and an HTDMA as a case study to prove the concept (experimental information: 100–200 nm, during noontime on 28 September 2021 and 22 March 2022 in Hefei, China). According to the distinct hygroscopic growth behavior from single-particle probing using a SPRM-ARI, the individual particles can be classified into three categories defined as non-hygroscopic (NH), less hygroscopic (LH), and more hygroscopic (MH). The mean growth factor (GF) of the three categories can be utilized to reproduce the GF distribution obtained from the HTDMA measurement. The chemical compositions of individual particles from the three categories are identified to be organic carbon (OC), soot (mainly elemental carbon), fly ash, and secondary aerosols (mainly OC and sulfate), using scanning electron microscopy (SEM) with an energy-dispersive spectrometer (EDS). The coupled SPRM–HTDMA measurement suggests a size-dependent variation of aerosol chemical components, i.e., an increase of OC fraction with increasing particle sizes, which agrees reasonably well with the chemical compositions from collected aerosol samples. This likely links the hygroscopic properties of individual particles to their bulk hygroscopic growth and chemical composition.

Carbonaceous aerosols remote sensing from geostationary satellite observation, Part I: Algorithm development using critical reflectance

Current aerosol remote sensing without using multi-view satellite sensors still fail to retrieve its components directly, such as black carbon (BC) and organic carbon (OC) simultaneously due to the limitations on available observations. In this study, A new general carbonaceous aerosol retrieval strategy for geostationary single-view satellite observations is implemented based on a method of critical reflectance, to retrieve the parameters of BC and extra OC concentration from measured radiance without prior quantification of Aerosol Optical Thickness (AOT). The method is based on measuring the change in upward reflectance between clear and hazy days over a varying surface reflectance, with the aim of finding a balance between brightening due to scattering and darkening due to absorption. Since aerosols in the proposed algorithm are considered as a mixture of BC, OC and clustered shell aerosols, this balance can be used to retrieve concentration parameters of these components via radiative transfer models. Sensitivity tests indicate that different scenarios of BC and OC volume fractions can introduce certain sensitivity pattern on critical reflectance. The retrieval is achieved by minimizing the differences between measured critical reflectance and a set of look-up tables (LUTs). Random sampling consensus (RANSAC) is also used in the strategy to reduce the influence of clouds and anomalous pixels on the retrievals. Since critical reflectance should be calculated by comparing geometrically consistent clear and hazy images, the algorithm is more suitable for geostationary satellites with constant viewing geometries. An initial validation and application applied to Himawari images over the North China Plain (NCP) shows that the carbonaceous aerosol retrievals are highly consistent with the expectations in terms of spatial and temporal patterns. The retrievals of BC and OC concentration follow the daily fluctuations of the Aethalometers observations and feature small differences in mean values throughout the month. Additionally, the AOTs at 0.55 μm can be also satisfactorily reproduced based on the carbonaceous aerosol retrievals, resulting in a mean absolute error of 0.089 and a correlation coefficient of 0.870. The main errors in the method arise from shell model assumptions, RANSAC fitting bias, inconsistent clear reference AOT in LUT, and geometric inconsistency between the clear reference and hazy images. This work indicates that the BC and OC concentration in high resolution can be acquired through the geostationary single-view remote sensing for the further air quality and climate studies.

Significant overestimation of black carbon concentration caused by high organic carbon in aerosols of the Tibetan Plateau

Black carbon plays an important role in climate change. Whereas, accurate measurement of black carbon (also known as elemental carbon (EC)) is still a challenging issue because portion of the pyrolytic carbon produced from the organic carbon (OC) can cause the overestimation of EC when measured by thermal-optical method. As one of the remote regions in the world, the Tibetan Plateau (TP) is characterized as high OC/EC ratio in its atmosphere. In this study, potential influence of relative high OC concentration to EC were investigated at three remote sites (Yaze, Everest and Nam Co) in the TP. The results showed that carbonaceous aerosols from different sources can affect the fraction of OC extracted by methanol. Concentration of OC extracted by methanol had a significantly positive correlation with the reduction of pyrolytic carbon and EC concentrations, indicating that part of OC extracted by methanol can decrease the production of pyrolytic carbon and then reduce the overestimation of EC. After considering this effect, it is shown in this study that actual EC concentration at Yaze, Everest and Nam Co were overestimated by approximately 40.0 ± 12.6%, 28.8 ± 9.1% and 24.8 ± 4.7%, respectively. Accordingly, combined with the overestimation of EC concentration by carbonates, actual ratios of solar energy absorbed by organic carbon to EC were 1.67, 2.33 and 2.78 times those of original ones at Yaze, Everest and Nam Co, respectively. Therefore, warming effect caused by EC on the TP should be lower than that previously estimated. This phenomenon needs to be considered for both in situ study and model simulation in the future.

Quantitative evaluation of mixed biomass burning and anthropogenic aerosols over the Indochina Peninsula using MERRA-2 reanalysis products validated by sky radiometer and MAX-DOAS observations

In this study, we conducted the quantitative evaluation of aerosol optical properties in the Indochina Peninsula (ICP), which is significantly affected yearly by both biomass burning (BB) and anthropogenic aerosols, using Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) aerosol products. To perform spatiotemporal analysis with validated aerosol data, the MERRA-2 aerosol optical depth (AOD) and absorption AOD (AAOD) data were evaluated based on sky radiometer observations at the SKYNET Phimai site (15.18° N, 102.56° E). Furthermore, multi-axis differential optical absorption spectroscopy was conducted, providing additional data for the comparison of the aerosol extinction coefficient (AEC) vertical profile data. MERRA-2 AOD, AAOD, and AEC at altitudes below 1 km were underestimated in the dry season, with relative mean biases of 0.84, 0.54, and 0.48, respectively. These underestimations are attributed to insufficient BB emissions of light-absorbing aerosols near the surface. On the basis of these results, we investigated the factors that determined spatiotemporal variations in AOD over ICP from 2009 to 2020. We found that the seasonal variations in AOD were driven mainly by organic carbon (OC) and sulfate aerosols. OC AOD was dominant during the active BB period (from January to March), whereas sulfate AOD was high all year round, accounting for more than 25% of the total AOD. Sulfate AOD in the northeast ICP (NEIC) was approximately 74% of the total AOD in October, indicating the remarkable effect of sulfate aerosol transportation from southern China (SC). In the period of study, AOD decreased in NEIC and south ICP (SIC) by − 4.40% and − 3.00% year−1, respectively, corresponding to the decrease in sulfur dioxide concentrations in SC and NEIC. Thus, OC AOD was dominant during the active BB periods, whereas a significant amount of anthropogenic aerosols from SC contributed to the atmospheric environment over ICP throughout 2009–2020.

Wavelet Analysis of the Interconnection between Atmospheric Aerosol Types and Direct Irradiation over Cameroon

The comparative analysis of the intra- and interannual dynamics between the Direct Normal Irradiation (DNI) under clear sky conditions and five aerosol types (Dust, Sea Salt, Black Carbon, Organic Carbon, and Sulfate) is the purpose of this study. To achieve this aim, we used fifteen-year DNI and aerosols data downloaded at 3-hour time intervals in nine defined zones throughout Cameroon. The wavelet transform is a powerful tool for studying local variability of amplitudes in a temporal dataset and constitutes our principal tool. The results show unequal distribution of aerosol types according to zones, but the Desert Dusts (DU) and Organic Carbon (OM) aerosols have been found as dominant particles in the studied region. The wavelet coherence analysis between DNI and each aerosol type reveals three bands of periodicity: ∼ 4-month band, 8–16-month band, and sometimes after-32-month band, with the most important frequency at 8–16-month band period. However, the intensity of coherence across bands varies with respect to aerosol type as well as each of the nine climate zones. A significant anticorrelation relationship was obtained between DNI and each type of aerosol, emphasizing that the presence of such atmospheric particles could dampen the renewable energy utilized by power systems. Also, the analysis shows that scattering aerosols such as Sulfate and Sea Salt (SU and SS, respectively) lead DNI in phase while absorbing aerosols such as Organic Carbon, Black Carbon, and Dust (OM, BC, and DU, respectively) give phase lag with DNI.

Saccharides in atmospheric PM2.5 in tropical forest region of southwest China: Insights into impacts of biomass burning on organic carbon aerosols

Biomass burning (BB) in South and Southeast Asia has a strong impact on regional air quality, yet its impact on atmospheric PM2.5 of tropical rainforest regions, a background region occupying a large area in South Asia, has rarely been investigated. In this work, we performed one-year PM2.5 sampling during December 2018 to October 2019 at a tropical rainforest site in southwest China. PM2.5 mass concentration, major chemical components, and ten saccharides were determined to study seasonal variations of PM2.5 chemical composition, and further to understand possible impacts of BB to organic carbon (OC) aerosols at this background region. The concentration levels of PM2.5, major PM2.5 components, and total saccharides were significantly higher in dry season than in wet season. Besides, PM2.5, OC, and total saccharides were highly correlated (R2 > 0.64, p < 0.001) during the sampling period, suggesting they might share common sources. Source apportionment of saccharides revealed that BB was the main source in both seasons. Furthermore, the contributions of BB to OC (BB/OC) were estimated using levoglucosan as a molecular tracer while levoglucosan's chemical degradation was considered. It was found that over 80% of LG was degraded in both seasons, suggesting BB sources were largely from the transport of external air mass. The estimated BB/OC were over 50%, indicating BB was an important source of OC and likely of PM2.5 in both seasons. The air-mass backward trajectory analysis and active fire spots data indicate intense BB emission sources were from South and Southeast Asia in dry season and the BB emissions in southern region of China could impact on the studied area in wet season.