Atmospheric Carbonaceous Aerosols Research Articles

Mass and Light Absorption Properties of Atmospheric Carbonaceous Aerosols over the Outflow Regions of Indo-Gangetic Plain

The uncertainty associated with carbonaceous aerosols in climate models becomes an obstacle to evaluating their harmful environmental effects. Brown Carbon (BrC) has recently become an eye-catching carbonaceous aerosol in ambient air because of its strong light absorption properties. The optical properties of soluble BrC are well studied in South Asia, one of the largest emitters. However, the absorption property of strong light-absorbing insoluble BrC is highly uncertain because of their complex mixing. Besides, the simultaneous apportionment of light-absorbing carbonaceous aerosol constituents as a function of wavelengths is seldom explored. The present study aims to study mass as well as apportionment of absorption properties of Black Carbon (BC) and different BrC chromophores using a multi-wavelength thermal-optical carbon analyzer over the least explored Eastern part of India to fill the knowledge gap. The output suggested that the primary emission sources dominate the carbonaceous aerosol mass; thus, the primary emission reductions will be helpful in improving the local air quality. The BrC is the dominant light-absorbing carbonaceous aerosol in the ultraviolet wavelengths. Besides, significant light absorption by BrC chromophores in near-infrared wavelengths (up to ∼50% of total aerosol absorption) suggested the absorption by BrC in longer wavelengths cannot be neglected. The insoluble fraction of BrC (Tar-BrC), which has a property identical to BC, contributes significantly to light absorption and is more than 50% of total absorption by aerosols in shorter ≤635 nm wavelengths. The present study also revealed that the contribution of Tar-BrC is more pronounced in the Indo-Gangetic Plain (IGP) outflow region than in the IGP emission source regions.

Emission Factors of Carbonaceous Aerosol and Stable Carbon Isotope for In-use Vehicles

Vehicle exhaust is an important anthropogenic source of atmospheric carbonaceous aerosols; of which, the emission factors and stable carbon isotope composition are important basic data. In-use motor vehicles of different types were selected to conduct dynamometer tests using different test cycles and under cold/hot start conditions. The exhaust of each test stage was collected to analyze the carbonaceous components and stable carbon isotopes and to discuss the influencing factors. The total carbon emission factors follow the order:heavy-duty diesel vehicles>light-duty diesel vehicles>light-duty gasoline vehicles. Although the emission factors of light-duty natural gas vehicles were very low at the low- and medium-speed stages, they were similar to those of heavy-duty diesel vehicles at the high-speed stage. The emission factors of cold start were higher than those of hot start, and the emission factors of the NEDC test cycle were lower than those of WLTC (which should be related to the driving speed). The emission factors of organic carbon (OC) of gasoline and natural gas vehicles were much higher than those of elemental carbon (EC) in every test stage. The emission factors of OC and EC of diesel vehicles were similar. The OC/EC of all types of vehicles increased with the increase in driving speed. Stable carbon isotopes in EC were higher than those in OC. The stable carbon isotope in different vehicles follow the order:light-duty gasoline vehicles<light-duty natural gas vehicles<light-duty diesel vehicles<heavy-duty diesel vehicles. The results revealed that the source signatures of stable carbon isotope in vehicles used in current source apportionment could not well represent gasoline vehicles and natural gas vehicles. In future emission control and source apportionment, attention should be paid to the changes in emission factors and isotope signatures caused by the use of natural gas and the aging of motor vehicles.

Molecular Composition of Beijing PM2.5 Brown Carbon Revealed by an Untargeted Approach Based on Gas Chromatography and Time-of-Flight Mass Spectrometry.

The knowledge of the chemical composition of brown carbon (BrC) is limited to the categories of components or parts of specific organic components. In this paper, the light-absorbing properties and molecular compositions of lipid-soluble organic components in fine particulate matter of Beijing from 2016 to 2018, characterized by an ultraviolet-visible spectrometer and gas chromatography coupled with time-of-flight mass spectrometry, respectively, were combined to untargetedly screen the key BrC molecules by a partial least squares regression model for the first time. A total of 421 molecules were obtained, where 61 molecules were identified qualitatively and 22 molecules quantitatively. To the best of our knowledge, 11 molecules were newly identified BrC species. These qualitative molecules included polycyclic aromatic hydrocarbons with higher ambient concentrations and mass absorbing efficiencies (MAEs), as well as oxygen- and nitrogen-containing aromatic components with relatively lower concentrations and MAEs. The absorption contribution at 365 nm of quantified BrC species to lipid-soluble BrC during heating seasons was 39.1 ± 17.0%, which was about 5 times as high as previous studies. These results help establish a complete BrC molecular database and provide data support for better evaluating the climate effect of atmospheric carbonaceous aerosols and formulating air pollution control strategies.

Source apportionment of carbonaceous aerosols in diverse atmospheric environments of China by dual-carbon isotope method

Carbonaceous aerosols are major components in PM2.5 of both polluted and clean atmosphere. Accurate source apportionment of carbonaceous aerosols may support effective PM2.5 control. Dual-carbon isotope method (14C and 13C) was adopted to identify the contribution of three main air pollution sources biogenic and biomass (fbb), liquid fossil (fliq.fossil) and coal (fcoal). The aerosol samples were collected at three types of sites with distinctly different degree of air pollution: urban, rural and regional background. The seasonal variation of source apportionment of the carbonaceous aerosols in urban Beijing was discussed. Modern biogenic and biomass made an absolute dominance of 92.9 ± 0.5% contribution to the carbonaceous aerosols at the background site Mt. Yulong due to long-range transport from Southeast Asia. The three main sources contributed jointly to the atmospheric carbonaceous aerosols at the rural site Wangdu and the urban site Beijing. The biogenic and biomass source was the major contribution in summer (47.0 ± 0.3%) and autumn (49.3 ± 0.3%) of Beijing, while coal source increased from summer (26.8 ± 13.8%) to autumn (34.7 ± 11.5%). Heating significantly increased the coal source to the dominant contribution (47.0 ± 16.9%) in winter of Beijing. Separate day and night time coal contributions were used to evaluate the two origins of coal combustion: industrial use vs. residential use. The results of source apportionment for carbonaceous aerosols provide scientific support for the prevention and control of air pollution.

Postharvest Burning of Crop Residues in Home Stoves in a Rural Site of Daejeon, Korea: Its Impact to Atmospheric Carbonaceous Aerosol

To investigate the impact of burning postharvest crop residues in home stoves, PM2.5 samples (particulate matter with a diameter of &lt;2.5 μm) were collected every 3 h at a rural site in Daejeon, Korea during the postharvest season in 2014. A high concentration of levoglucosan was observed with a peak value of 3.8 µg/m3 during the sampling period. The average mannosan/levoglucosan ratio (0.18) at the rural site during a severe BB episode (levoglucosan &gt; 1 μg/m3) was similar to burnings of pepper stems (0.19) and bean stems (0.18) whereas the average OC/levoglucosan ratio (9.9) was similar to burning of pepper stems (10.0), implying that the severe BB episode was mainly attributed to burning of pepper stems. A very strong correlation was observed between levoglucosan and organic carbon (OC) (R2 = 0.81) during the entire sampling period, suggesting that the emission of organic aerosols at the rural site was strongly associated with the burning of crop residues in home stoves. The average mannosan/levoglucosan ratio (0.17 ± 0.06) in the rural area was similar to that in a nearby urban area in Daejeon (0.16 ± 0.04). It was concluded that crop residue burning in a home stove for space heating is one of the important sources of carbonaceous aerosols not only in a rural area but also in the urban area of Daejeon, Korea during the postharvest season.

Development of a Monitoring System for Semicontinuous Measurements of Stable Carbon Isotope Ratios in Atmospheric Carbonaceous Aerosols: Optimized Methods and Application to Field Measurements.

Carbon content constitutes a major fraction of atmospheric particulate matter (PM) and directly influences the earth's climate and human health. The stable carbon isotope ratios (δ13C) can be used to track potential sources and atmospheric processes of carbonaceous aerosols. Previously, determination of δ13C was always conducted in offline carbonaceous aerosol samples. The poor time-resolution results cannot provide information regarding the temporal evolution of δ13C at a short-time scale. In this study, we developed a new system for online measurements of δ13C in atmospheric carbonaceous aerosols by combining a semicontinuous organic carbon/elemental carbon (OC/EC) analyzer and online cavity ring-down spectroscopy (CRDS) (OC/EC analyzer-CRDS). To provide better stability in the determination of δ13C, a carrier gas with CO2 (∼200 ppm) in "balance gas" was used, and Keeling analysis was employed to separate the δ13C signal of the sample from background CO2 gas. Our results showed that the accuracy and absolute precision of the δ13C measurements by the OC/EC analyzer-CRDS system were better than 0.1‰ and 0.5‰, respectively, for the samples containing carbon content more than 5 μg. Furthermore, we employed this system to monitor δ13C (δ13C-TC) in particulate total carbon (TC) with a time resolution of 2-4 h over Beijing in late summer and early autumn, 2019. During the sampling period, the TC concentrations varied from 0.1 to 12.0 μg m-3 with a mean value of 6.0 ± 2.4 μg m-3. The δ13C-TC ranged from -28.2 to -24.2‰ (mean value was -25.9 ± 0.9‰) without significant diurnal variations, suggesting similar contributing sources to TC. Comparing the δ13C signatures of different emissions, we found that liquid fuels and primary and secondary C3 plants were likely the dominant sources of particulate TC. Finally, we found that atmospheric heavy precipitation washed out the aged aerosols from the polluted air, resulting in significant depletion (∼2.4‰) of δ13C-TC in the atmosphere. This paper described a novel system for conducting online measurements of δ13C in atmospheric carbonaceous aerosols and provided us information to better understand the temporal evolution of emission sources and atmospheric processes of carbonaceous aerosols.

Near infrared hyperspectral imaging as a tool for quantifying atmospheric carbonaceous aerosol

The quantitative determination of atmospheric organic carbon (OC), elemental carbon (EC) and total carbon (TC) is of utmost relevance due to its influence on global warming, visibility degradation, and human health. Thermal-optical transmission (TOT) is the most common analytical method used to analyze them. Nevertheless, it is destructive, time-consuming, and only a small portion of the sample is analyzed. Here, near infrared spectroscopy coupled with a hyperspectral detector (HSI-NIR), together with multivariate data analysis, comes as a reliable alternative.This work aims at establishing a methodology for the quantitation of the carbonaceous content in atmospheric particulate matter (PM) fusing HSI-NIR and multivariate data analysis, and being validated with TOT analysis. Principal Component Analysis and Multivariate Curve Resolution analysis, used as qualitative tools, confirmed concentration trends in the PM samples, and contributions from the chemical composition of both the filter material and aerosol samples. The Partial Least Squares (PLS) regression models developed were optimized using interval Partial Least Squares (iPLS) selection and showed a high correlation between the HSI-NIR spectra and TOT measurements: R2Cal = 0.99, 0.94 and 0.99 for the OC, EC and TC contents, respectively. Finally, the spatial distribution of the carbonaceous content in the filter samples was assessed using a homogeneity percentage (%H). This showed values higher than 50% for all cases, which indicated that no distributional inhomogeneities were observed in the filters and corroborated the efficient operation of the sampling system. This study demonstrated the feasibility of using HSI-NIR for the quantitative assessment of carbonaceous particulate matter in air pollution monitoring.

An environmental evaluation of carbonaceous aerosols in PM10 at micro- and nano-scale levels reveals the formation of carbon nanodots.

Carbonaceous aerosols play significant roles in air quality and the climate; their oxidation at the nano-scale level may possibly increase the reactivity and toxicity of atmospheric particulates. In the present study, a laboratory experiment on the atmospheric carbonaceous aerosol was done by using H2O2 as an oxidizing agent. An extensive study made with advanced analytical tools revealed the formation of photoluminescent carbon nanoparticles (carbon nanodots) in the carbonaceous aerosol. The carbon nanoparticles are mostly at the sp2 hybridization state and contain various surface functional groups such as carboxyl and carbonyl groups. The properties of these carbon nanoparticles resemble the engineered carbon nanoparticles such as carbon dots (CDs). The carbon nanoparticles, mainly less than 10nm, are composed of carbon nanocrystals containing a few other elements such as Ca and Fe. Fluorescence spectroscopy revealed the characteristic excitation-dependent emission spectra of blue fluorescent carbon nanoparticles. The results indicate the presence of characteristic carbon nanoparticles in the carbonaceous aerosol in PM10, opening a new road for predicting environmental processes occurring in the atmospheric environment.

Applications of High-Resolution Mass Spectrometry in Studies of Brown Carbon

Abstract Brown carbon is a hotspot in the field of atmospheric carbonaceous aerosol research. It has significant influence on regional radiative forcing and exerts climatic effects due to its apparent absorbance in the near ultraviolet-visible region. Brown carbon is mainly derived from incomplete combustion of biomass or coal, as well as secondary sources, such as a series of atmospheric photochemical reactions from volatile organic compounds. Although the composition of brown carbon is complex, high-resolution mass spectrometry, with its ultra-high mass resolution and precision, enables elucidation of the characteristics of the organic components of brown carbon at the molecular level. Here, high-resolution mass spectrometry combined with traditional analytical methods was used for the study of brown carbon. The development of high-resolution mass spectrometry for brown carbon separation is reviewed, as well as compositional analysis, source apportionment, and formation mechanism of brown carbon based on high-resolution data. In addition, the issues and prospects for the application of high-resolution mass spectrometry to evaluate brown carbon are discussed.

Characteristics of carbonaceous aerosols analyzed using a multiwavelength thermal/optical carbon analyzer: A case study in Lanzhou City

Characteristics of atmospheric carbonaceous aerosols in Lanzhou City from December 2014 to November 2015 are analyzed using a multiwavelength thermal/optical carbon analyzer. Results reveal that average concentrations of black carbon (BC) and organic carbon in atmospheric aerosols at Lanzhou are 6.7 and 25.4 µg m–3, respectively, showing obvious seasonality (higher in winter and lower in summer). This is consistent with findings in cities of northern China. Primary organic aerosols and secondary organic aerosols respectively account for approximately 60% and 17% of carbonaceous aerosols. No significant seasonality is found for secondary organic carbon, indicating that its potential sources do not vary significantly throughout the study period. The mass absorption cross-section (MAC632 nm) of BC is 7.1 m2 g−1, slightly higher than that of immediately emitted BC. MAC values of BC at different wavelengths vary drastically; they are higher for ultraviolet and visible light (8.5–10.2 m2 g–1) than for near-infrared light (4.9–5.7 m2 g–1). The aerosol absorption optical depth generally declines from the near-infrared to the near-ultraviolet region. The values are higher in winter than in summer, thus showing there are different contributions of BC deposition in different seasons. Brown carbon (BrC) has an Angstrom absorption exponent (AAE) value of approximately 2.75, which is similar to the AAE value of BrC generated by diesel combustion (2.3). The contribution of BrC to light absorption is as much as 34% at a wavelength of 635 nm. This study demonstrates that the multiwavelength thermal/optical carbon analyzer can quantify absorption properties of BrC in atmospheric aerosols. This can enhance understanding of carbonaceous aerosols and provide key parameters for simulations of climate models.

Characteristics and Source Analysis of Atmospheric Carbonaceous Aerosols in the Cities of Hangzhou and Ningbo

To investigate the seasonal variations and sources of carbonaceous aerosols in the cities of Hangzhou and Ningbo, field PM2.5 sampling was conducted at four representative sites (two urban, one suburban, and one rural) in this region from December 2014 to November 2015. A thermal/optical carbon analyzer was employed to analyze both organic carbon (OC) and elemental carbon (EC) contents in PM2.5 by identifying eight different carbon fractions, including OC1, OC2, OC3, OC4+OPC, EC1-OPC, EC2, and EC3. Based on these fractions, OC and EC were defined as OC1+OC2+OC3+OC4+OPC and EC1+EC2+EC3-OPC, respectively; total carbon (TC) was calculated as the sum of OC and EC; and total carbonaceous aerosols (TCAs) were quantified via the sum of organic aerosols (OAs; converted from OC) and EC. The results showed the following. ①The annual average level of TC in this region was (14.3±4.1) μg·m-3, accounting for (26.2±6.5)% of the annual average PM2.5 concentration. The annual average OC and EC concentrations were (11.3±3.4) μg·m-3 and (3.0±0.9) μg·m-3, respectively. The highest TC level was observed in winter among the four seasons. ②The annual average TCA concentration in this region was (25.6±7.5) μg·m-3, contributing (42.2±10.0)% of PM2.5. In addition, secondary organic carbon (SOC) was also estimated by the commonly applied EC method. It was found that SOC contributed (41.1±5.5)% to OC on an annual average basis. ③The sources of carbonaceous aerosols were determined using the correlation between OC and EC, OC/EC mass ratio, and different carbon fraction characteristics. The annual average OC/EC ratio in this region was 4.7±1.7, which falls in the diagnostic ratio range for vehicular emissions, coal combustion, and biomass burning, indicating these sources are probably the major contributors of the regional carbonaceous aerosols. Moreover, a higher char-EC/soot-EC ratio was observed during winter and autumn at all sites, possibly implying the enhanced biomass burning activities during these two seasons.

Characteristics of Organic Carbon and Elemental Carbon in Atmospheric Aerosols in the Urban Area in Beibei, a Suburb of Chongqing

To investigate the pollutive characteristics of atmospheric carbonaceous aerosols in Beibei District, a suburb of Chongqing Municipal City, graded aerosol samples were continuously collected by cascade impactors over one year, from March 2014 to February 2015. Carbonaceous aerosols, including organic carbon (OC) and elemental carbon (EC), were detected by a DRI 2001A carbon analyzer. The results showed that the average annual concentrations of OC and EC in the PM2.1 were 16.3 ± 7.6 and 1.8 ± 0.7 µg m–3, and in the PM9.0 were 25.0 ± 9.6 and 3.2 ± 1.2 µg m–3, respectively. On the one hand, a more seasonal distribution of OC concentrations appeared in the PM2.1 (winter > spring > summer > autumn) than in the PM9.0 (winter ≈ spring ≈ summer > autumn); furthermore, whereas the OC significantly positively correlated with wind speed for both the PM2.1 (P spring > summer > autumn), and the EC in the PM2.1 significantly negatively correlated with temperature (P < 0.05). Additionally, both the OC and the EC were concentrated mainly in the fine particles (< 2.10 µm), and the size distributions of the OC in all four seasons displayed a bi-modal pattern that peaked in the size ranges of 0.43–0.65 µm (for fine particles) and 4.7–5.8 µm (for coarse particles), whereas the EC displayed a uni-modal pattern that peaked in the size range of 4.7–5.8 µm (for coarse particles). Furthermore, the correlations between the OC and the EC were analyzed, and the SOC (secondary organic carbon) in the PM2.1 was estimated using the primary OC/EC ratio. It was found that the OC highly significantly correlated with the EC (P < 0.01), with the average annual concentration of the SOC being 6.3 ± 5.9 µg m–3, which accounted for 33.5 ± 22.6% of the OC. Analyzing the sources of the pollutive atmospheric aerosol in Beibei further demonstrated that it mainly originated in biomass burning, gasoline-vehicle exhaust, and coal combustion.

Absorbing Refractive Index and Direct Radiative Forcing of Atmospheric Brown Carbon over Gangetic Plain

Atmospheric carbonaceous aerosols consisting of black carbon and organic carbon influence Earth’s radiative balance by interacting with solar radiation. A subset of organic aerosols known as brown carbon is absorbing in nature and poorly characterized in terms of optical properties. Brown carbon can warm the local and regional atmosphere depending upon its absorbing capacity, mixing state, and meteorological conditions. We report a diurnal spectral absorbing refractive index of brown carbon over North India and its influence on regional radiative forcing. Measurements show the presence of highly absorbing brown carbon consisting of soluble and non-soluble fractions having distinct spectral absorption. The brown carbon refractive index at 365 nm shows a 50% reduction during daytime when compared to nighttime as a result of combined effects of reduced primary emissions and photobleaching/volatilization. Brown carbon and the lensing effect as a result of a thin absorbing coating exert a forcing of −0.93 ± 0....

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

Abstract. In early spring the Baltic region is frequently affected by high-pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m−3 and black carbon (BC) up to 17 µg m−3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OCnf) was the dominant fraction of PM1, with the primary (POCnf) and secondary (SOCnf) fractions contributing 26–44 % and 13–23 % to the total carbon (TC), respectively. 5–8 % of the TC had a primary fossil origin (POCf), whereas the contribution of fossil secondary organic carbon (SOCf) was 4–13 %. Non-fossil EC (ECnf) and fossil EC (ECf) ranged from 13–24 and 7–13 %, respectively. Isotope ratios of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

Description and evaluation of a new four-mode version of the Modal Aerosol Module (MAM4) within version 5.3 of the Community Atmosphere Model

Abstract. Atmospheric carbonaceous aerosols play an important role in the climate system by influencing the Earth's radiation budgets and modifying the cloud properties. Despite the importance, their representations in large-scale atmospheric models are still crude, which can influence model simulated burden, lifetime, physical, chemical and optical properties, and the climate forcing of carbonaceous aerosols. In this study, we improve the current three-mode version of the Modal Aerosol Module (MAM3) in the Community Atmosphere Model version 5 (CAM5) by introducing an additional primary carbon mode to explicitly account for the microphysical ageing of primary carbonaceous aerosols in the atmosphere. Compared to MAM3, the four-mode version of MAM (MAM4) significantly increases the column burdens of primary particulate organic matter (POM) and black carbon (BC) by up to 40 % in many remote regions, where in-cloud scavenging plays an important role in determining the aerosol concentrations. Differences in the column burdens for other types of aerosol (e.g., sulfate, secondary organic aerosols, mineral dust, sea salt) are less than 1 %. Evaluating the MAM4 simulation against in situ surface and aircraft observations, we find that MAM4 significantly improves the simulation of seasonal variation of near-surface BC concentrations in the polar regions, by increasing the BC concentrations in all seasons and particularly in cold seasons. However, it exacerbates the overestimation of modeled BC concentrations in the upper troposphere in the Pacific regions. The comparisons suggest that, to address the remaining model POM and BC biases, future improvements are required related to (1) in-cloud scavenging and vertical transport in convective clouds and (2) emissions of anthropogenic and biomass burning aerosols.

Patterns in atmospheric carbonaceous aerosols in China: emission estimates and observed concentrations

Abstract. China is experiencing severe carbonaceous aerosol pollution driven mainly by large emissions resulting from intensive use of solid fuels. To gain a better understanding of the levels and trends of carbonaceous aerosol emissions and the resulting ambient concentrations at the national scale, we update an emission inventory of anthropogenic organic carbon (OC) and elemental carbon (EC) and employ existing observational studies to analyze characteristics of these aerosols including temporal, spatial, and size distributions, and the levels and shares of secondary organic carbon (SOC) in total OC. We further use ground observations to test the levels and inter-annual trends of the calculated national and provincial emissions of carbonaceous aerosols, and propose possible improvements in emission estimation for the future. The national OC emissions are estimated to have increased 29 % from 2000 (2127 Gg) to 2012 (2749 Gg) and EC by 37 % (from 1356 to 1857 Gg). The residential, industrial, and transportation sectors contributed an estimated 74–78, 17–21, and 4–6 % of the total emissions of OC, respectively, and 49–55, 30–34, and 14–18 % of EC. Updated emission factors (EFs) based on the most recent local field measurements, particularly for biofuel stoves, led to considerably lower emissions of OC compared to previous inventories. Compiling observational data across the country, higher concentrations of OC and EC are found in northern and inland cities, while higher OC / EC ratios are found in southern sites, due to the joint effects of primary emissions and meteorology. Higher OC / EC ratios are estimated at rural and remote sites compared to urban ones, attributed to more emissions of OC from biofuel use, more biogenic emissions of volatile organic compound (VOC) precursors to SOC, and/or transport of aged aerosols. For most sites, higher concentrations of OC, EC, and SOC are observed in colder seasons, while SOC / OC is reduced, particularly at rural and remote sites, attributed partly to weaker atmospheric oxidation and SOC formation compared to summer. Enhanced SOC formation from oxidization and anthropogenic activities like biomass combustion is judged to have crucial effects on severe haze events characterized by high particle concentrations. Several observational studies indicate an increasing trend in ambient OC / EC (but not in OC or EC individually) from 2000 to 2010, confirming increased atmospheric oxidation of OC across the country. Combining the results of emission estimation and observations, the improvement over prior emission inventories is indicated by inter-annual comparisons and correlation analysis. It is also indicated, however, that the estimated growth in emissions might be faster than observed growth, and that some sources with high primary OC / EC, such as burning of biomass, are still underestimated. Further studies to determine changing EFs over time in the residential sector and to compare to other measurements, such as satellite observations, are thus suggested to improve understanding of the levels and trends of primary carbonaceous aerosol emissions in China.

Studying seasonal variations in carbonaceous aerosol particles in the atmosphere over central Siberia

The results of 2-year (2010–2012) measurements of the concentrations of organic carbon (OC) and elemental carbon (EC), which were taken at the Zotino Tall Tower Observatory (ZOTTO) Siberian background station (61° N, 89° E), are given. Despite the fact that this station is located far from populated areas and industrial zones, the concentrations of OC and EC in the atmosphere over boreal forests in central Siberia significantly exceed their background values. In winter and fall, high concentrations of atmospheric carbonaceous aerosol particles are caused by the long-range transport (~1000 km) of air masses that accumulate pollutants from large cities located in both southern and southwestern regions of Siberia. In spring and summer, the pollution level is also high due to regional forest fires and agricultural burning in the steppe zone of western Siberia in the Russian–Kazakh border region. Background concentrations of carbonaceous aerosol particles were observed within relatively short time intervals whose total duration was no more than 20% of the entire observation period. In summer, variations in the background concentrations of OC closely correlated with air temperature, which implies that the biogenic sources of organic-particle formation are dominating.

Characterization of carbonaceous aerosols at Mount Lu in South China: implication for secondary organic carbon formation and long-range transport.

In order to understand the sources and potential formation processes of atmospheric carbonaceous aerosols in South China, fine particle samples were collected at a high-elevation mountain site--Mount Lu (29°35' N, 115°59' E, 1165 m A.S.L.) during August-September, 2011. Eight carbonaceous fractions from particles were resolved following the IMPROVE thermal/optical reflectance protocol. During the observation campaign, the daily concentrations of PM2.5 at Mount Lu ranged from 7.69 to 116.39 μg/m(3), with an average of 58.76 μg/m(3). The observed average organic carbon (OC) and elemental carbon (EC) concentrations in PM2.5 were 3.78 and 1.28 μg/m(3), respectively. Secondary organic carbon (SOC) concentration, estimated by EC-tracer method, was 2.07 μg/m(3) on average, accounting for 45.0% of the total OC. The enhancement of secondary organic aerosol (SOA) formation was observed during cloud/fog processing, and heterogeneous acid-catalyzed reactions may have contributed to SOA formation as well. Back trajectory analysis indicated that air masses were mainly sourced from southern China during observation period, and this air mass source was featured by highest values of OC and effective carbon ratio (ECR). Relation of carbonaceous species and principal component analysis indicated that multiple sources contributed to the carbonaceous aerosols at Mount Lu.

Atmospheric carbonaceous aerosols from Indo-Gangetic Plain and Central Himalaya: Impact of anthropogenic sources

In the present-day scenario of growing anthropogenic activities, carbonaceous aerosols contribute significantly (∼20–70%) to the total atmospheric particulate matter mass and, thus, have immense potential to influence the Earth's radiation budget and climate on a regional to global scale. In addition, formation of secondary organic aerosols is being increasingly recognized as an important process in contributing to the air-pollution and poor visibility over urban regions. It is, thus, essential to study atmospheric concentrations of carbonaceous species (EC, OC and WSOC), their mixing state and absorption properties on a regional scale. This paper presents the comprehensive data on emission sources, chemical characteristics and optical properties of carbonaceous aerosols from selected urban sites in the Indo-Gangetic Plain (IGP) and from a high-altitude location in the central Himalaya. The mass concentrations of OC, EC and WSOC exhibit large spatio-temporal variability in the IGP. This is attributed to seasonally varying emissions from post-harvest agricultural-waste burning, their source strength, boundary layer dynamics and secondary aerosol formation. The high concentrations of OC and SO42−, and their characteristic high mass scattering efficiency, contribute significantly to the aerosol optical depth and scattering coefficient. This has implications to the assessment of single scattering albedo and aerosol radiative forcing on a regional scale.

Quantitative determination of the biomass-burning contribution to atmospheric carbonaceous aerosols in Daejeon, Korea, during the rice-harvest period

To investigate the impact of biomass-burning emissions on atmospheric carbonaceous aerosols, the biomass burning tracers; levoglucosan, mannonsan, galactosan, and K+ were measured at a suburban site in Daejeon, Korea, during the rice-harvest period, during the fall, 2012. The emissions of K+ from biomass burning (K+_BB) were estimated by subtracting sea-salt K+ and soil K+ concentrations from measured K+ concentrations. Regression analysis of levoglucosan and K+_BB reveals that K+_BB alone is not suitable as a biomass-burning tracer in the Daejeon atmosphere, especially when the biomass-burning contribution is low. Levoglucosan to K+_BB ratios during the study period ranged from 0.40 to 1.39, with an average of 0.89 ± 0.30, whereas levoglucosan to mannosan ratios ranged from 4.61 to 15.45, with an average of 6.70 ± 2.69. The ratios of levoglucosan to mannosan, K+, organic carbon (OC), and elemental carbon (EC) show that biomass-burning aerosols in the Daejeon atmosphere during the rice-harvest period are emitted mainly from crop residue, grass, and leaf burnings. The contributions of biomass-burning emissions to OC and EC concentrations were 45% ± 12% and 12% ± 7.3%, respectively, indicating that a large fraction of OC was emitted from biomass burning.