Organic Carbon Aerosols Research Articles

Observation of heat wave effects on the urban air quality and PBL in New York City area

Heat waves are of serious health concern in highly populated urban areas due to combined heat stress and poor air quality impacts. In this study, we present an observation-based study of the heat-wave impacts on the planetary-boundary-layer (PBL) and air quality in summer 2017 in New York City (NYC). Synergy of remote sensing, in-situ observations with model forecast is applied to quantify and characterize the diurnal variation of PBL height (PBLH), ozone (O3) and PM2.5 during the heat wave period of June 11–13, 2017. The ground O3 concentration attains a maximum of 110 ppb largely exceeding the U.S. National Ambient Air Quality Standard (NAAQS) while the organic carbon (OC) and sulfate aerosols show a coincident increase. The higher O3 in the downwind suburb than those in the urban area are likely associated with the urban pollution transport and local meteorological condition. We observe a dramatic and consistent PBLH growth from 0.5- to 2.5-km at 11:00–13:00 local time from the turbulence-based and aerosol-based PBLH estimate by co-located ceilometer, wind lidar, and aerosol lidar measurement. Regional and high residual layers of aerosols at night are observed from the NASA space-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and Cloud and Aerosol Transport System (CATS) lidars. Furthermore, we evaluate the NOAA National Air Quality Forecasting Capability (NAQFC) products of PBLH, temperature, O3, PM2.5 and NOx (NO2+NO) with the observations. Under the strong convective PBL condition, all the products above show good agreement between the NAQFC predictions and observations. However, in the early morning and night, the model shows dramatic discrepancies with an underestimate of temperature, PBLH and O3 but an overestimate of PM2.5 and NOx. Such bias may be associated with the improper representations of vertical mixing, complex chemical processes and emissions in the model.

Experimental rainwater divalent mercury speciation and photoreduction rates in the presence of halides and organic carbon

Mercury (Hg) photochemical redox reactions control atmospheric Hg lifetime and therefore play an important role in global Hg cycling. Oxidation of Hg(0) to Hg(II) is currently thought to be a Br-initiated two-stage reaction with end-products HgBr2, HgBrOH, HgBrONO, HgBrOHO. Atmospheric photoreduction of these Hg(II) compounds can take place in both the gas and aqueous phase. Here we present new experimental observations on aqueous Hg(II) photoreduction rates in the presence of dissolved organic carbon and halides and compare the findings to rainfall Hg(II) photoreduction rates. The pseudo first-order, gross photoreduction rate constant, kred, for 0.5 μM Hg(II) in the presence of 0.5 mg/ L of dissolved organic carbon (DOC) is 0.23 h−1, which is similar to the mean kred (0.15 ± 0.01 h−1(σ, n = 3)) in high altitude rainfall and at the lower end of the median kred (0.41 h−1, n = 24) in continental and marine waters. Addition of bromide (Br−) to experimental Hg(II)-DOC solutions progressively inhibits Hg(II) photoreduction to reach 0.001 h−1 at total Br− of 10 mM. Halide substitution experiments give Hg(II)Xn(n-2) photoreduction rate constants of 0.016, 0.004 h−1, and < detection limit for X = Cl−, Br−, and I− respectively and reflect increasing stability of the Hg(II)-halide complex. We calculate equilibrium Hg(II) speciation in urban and high-altitude rainfall using Visual Minteq, which indicates Hg(II)-DOC to be the dominant Hg species. The ensemble of observations suggests that atmospheric gaseous HgBr2, HgCl2, HgBrNO2, HgBrHO2 forms, scavenged by aqueous aerosols and cloud droplets, are converted to Hg(II)-DOC forms in rainfall due to abundant organic carbon in aerosols and cloud water. Eventual photoreduction of Hg(II)-DOC in aqueous aerosols and clouds is, however, too slow to be relevant in global atmospheric Hg cycling.

Characterization of carbonaceous aerosols in Asian outflow in the spring of 2015: Importance of non-fossil fuel sources

The sources of elemental (EC) and organic carbon (OC) aerosols in Asian outflow were investigated in the spring of 2015 in terms of radiocarbon (14C) and molecular marker analyses. The contribution of fossil fuel (FF) sources to carbonaceous aerosols (TC) significantly increased in polluted air masses with enhancements in the concentrations of carbon monoxide. For EC, FF sources dominated in the polluted air masses. For OC, the contributions of non-FF sources other than biomass burning (BB) were found to be significant (comparable to or higher than those of FF sources), especially in air masses with higher values of the water-soluble fraction of OC (fWSOC) and 14C concentrations (F14C). Positive correlations between fWSOC and F14C indicate that the origins of TC (mainly OC) have great impacts on the water solubility variability and the subsequent cloud formation processes of OC during transport. We found the importance of natural sources as possible origins of OC in non-polluted (i.e., background) air. This study raises the need to further investigate the source apportionment of OC, especially its natural origins, for more accurately assessing the climatic impacts of EC and OC in East Asia.

Spatial-temporal Distribution of Aerosol Optical Depth and Its Main Influence Types in China During 1990-2017

In order to accurately understand the optical characteristics of aerosols in China, based on Mann-Kendall(MK) and Sen's slope trend analysis methods, the spatiotemporal variations of aerosol optical depth(AOD) derived from MERRA-2 reanalysis datasets were estimated in China for the period of 1990-2017. The results showed that ① for the interannual scale, there was a significant increasing trend in the annual mean AOD in China during 1990-2017. Besides, high aerosol loadings were observed in spring and summer, and the seasonal difference between the eastern and western regions was large. This was mainly due to the topographic and meteorological factors. ② At the spatial scale, the annual mean AOD values increased from the northwest to the southeast, with characteristically high AOD values occurring in Sichuan Pendi and the Tarim and Turpan basins and low values in the Qinghai-Xizang plateau region. Similarly, the AOD MK value and Sen's slope value showed significant decreasing trends from the southeast to the northwest, which was closely related to climate change and the human activity intensity. ③ In regard to black carbon aerosol, dust aerosol, organic carbon aerosol, sea salt aerosol, and SO4 aerosol, dust and SO4 aerosols were affected by the air humidity and human activity intensity, which have obvious regional differences in China.

Carbonaceous Aerosols Generated from Wood Charcoal Production Plants in the South Korea Context

Herein, a case study discussing the effect of carbonaceous aerosol pollution, which is emitted during the charcoal kiln manufacturing processes or carbonization processes, on the atmospheric environment is presented . In South Korea, in situ analysis of different charcoal production plants specialized in the production of charcoal sauna indicate that the emitted organic carbon (OC) and elemental carbon (EC) aerosols are significantly influenced by the nature of the biomass and technological processes, i.e., treatment or emissions abatement systems for the exhaust effluent gases. In detail, total carbon (TC), which is calculated as the sum of OC and EC emission factors, varied widely from a charcoal production site to another ranging from 21.8 to 35.8 gTC/kg-oak, where the mean value for the considered production sites was approximately 28 gTC/kg-oak (N = 7 and sum = 196.4). Results indicate that the emission factors from a modern charcoal production process in South Korea are quantitatively lower in comparison with the traditional kiln. This study aims to propose advanced wood processes for the production of charcoal from the viewpoint of environmental protection policy and green engineering.

Long-term observation of global black carbon, organic carbon and smoke using CALIPSO and MERRA-2 data

ABSTRACTBlack carbon (BC), organic carbon (OC) and smoke are some of the aerosols that are emitted during combustion reactions. These air pollutants impact human health and the environment negatively, hence it is important to study their sources and distributions. This work concentrates on three global regions; central South America (CSA), central Africa (CA) and east Asia (EA). The study reveals that biomass burning is responsible for the major emissions of BC, OC and smoke aerosols in the CSA and CA regions during the JJA and SON seasons. The EA region is dominated by BC and smoke aerosols emanating from industrial activities during all seasons. However, a high OC aerosol optical depth is only observed in the MAM season indicating biomass burning during this period. High altitude smoke aerosols up to 10 km are observed in CSA and CA regions in the DJF season. The CSA and CA regions further shows the highest planetary boundary layer height at 1400 m in the JJA and SON seasons.

Technical Note: An Automated System for Separate Combustion of Elemental and Organic Carbon for 14C Analysis of Carbonaceous Aerosol

We present the design and evaluation of an automated system for the conversion of elemental and organic carbon aerosol to CO2 for subsequent radiocarbon analysis. The system allows heating the sample in pure oxygen or helium at user defined temperature steps, followed by catalytic conversion of incomplete carbonaceous combustion products to CO2. The resulting CO2 is quantified using an NDIR detector and can be separated from other combustion by-products in a reduction oven. The purified CO2 is cryogenically collected in glass ampoules that can be sealed for storage until 14C analysis. We show that (1) the CO2 amount measured by the calibrated NDIR sensor compares well to an independent manometric method, (2) that we successfully remove combustion by-products such as SO2, H2O, and NOx, resulting in pure CO2 samples, and (3) that the system has low contamination and negligible cross contamination making it ideal for the analysis of very small samples in the order of 10–50 µgC.

Carbonaceous aerosol in ambient air: Parallel measurements between water cyclone and carbon analyzer

A water cyclone, developed to collect and preserve biological aerosols in a small liquid flow, was interfaced with a total organic carbon analyzer to measure the aerosol organic and inorganic carbon fractions. The total carbon was compared against parallel measurements of elemental carbon (EC) and organic carbon (OC) using a Sunset Real Time ECOC Analyzer between 12–29 January 2009. A National Institute for Occupational Safety and Health (NIOSH) like protocol for the measurements included four temperature steps ending at 840°C for OC under a helium atmosphere followed by two temperature steps ramped to 850°C for EC in a helium–oxygen atmosphere. Carbon data comparison between the water cyclone-TOC and the TOC measured by the analyzer indicated good agreement (r2=0.82, linear regression slope=0.98, p<0.001). Analyses of the relationship between total water organic carbon and OC, investigated using data sets from case studies spanning two different events, suggested it was possible to distinguish between the primary and secondary sources.

Retrieval of desert dust and carbonaceous aerosol emissions over Africa from POLDER/PARASOL products generated by the GRASP algorithm

Abstract. Understanding the role atmospheric aerosols play in the Earth–atmosphere system is limited by uncertainties in the knowledge of their distribution, composition and sources. In this paper, we use the GEOS-Chem based inverse modelling framework for retrieving desert dust (DD), black carbon (BC) and organic carbon (OC) aerosol emissions simultaneously. Aerosol optical depth (AOD) and aerosol absorption optical depth (AAOD) retrieved from the multi-angular and polarimetric POLDER/PARASOL measurements generated by the GRASP algorithm (hereafter PARASOL/GRASP) have been assimilated. First, the inversion framework is validated in a series of numerical tests conducted with synthetic PARASOL-like data. These tests show that the framework allows for retrieval of the distribution and strength of aerosol emissions. The uncertainty of retrieved daily emissions in error free conditions is below 25.8 % for DD, 5.9 % for BC and 26.9 % for OC. In addition, the BC emission retrieval is sensitive to BC refractive index, which could produce an additional factor of 1.8 differences for total BC emissions. The approach is then applied to 1 year (December 2007 to November 2008) of data over the African and Arabian Peninsula region using PARASOL/GRASP spectral AOD and AAOD at six wavelengths (443, 490, 565, 670, 865 and 1020 nm). Analysis of the resulting retrieved emissions indicates 1.8 times overestimation of the prior DD online mobilization and entrainment model. For total BC and OC, the retrieved emissions show a significant increase of 209.9 %–271.8 % in comparison to the prior carbonaceous aerosol emissions. The model posterior simulation with retrieved emissions shows good agreement with both the AOD and AAOD PARASOL/GRASP products used in the inversion. The fidelity of the results is evaluated by comparison of posterior simulations with measurements from AERONET that are completely independent measurements and more temporally frequent than PARASOL observations. To further test the robustness of our posterior emissions constrained using PARASOL/GRASP, the posterior emissions are implemented in the GEOS-5/GOCART model and the consistency of simulated AOD and AAOD with other independent measurements (MODIS and OMI) demonstrates promise in applying this database for modelling studies.

The impact of biomass burning on total suspended particulate matter in the southeastern Tibetan Plateau

To investigate the impact of biomass burning (BB) emissions on total suspended particulate (TSP) in the southeastern Tibetan Plateau (TP), BB tracers (including levoglucosan, mannosan, and galactosan) were measured at Lulang (a remote site, ∼3300 m above sea level) during the period 2015–2016. The concentrations of levoglucosan and mannosan showed large variability of more than 8-fold (range: 0.029–0.253 μg m−3) and 6-fold (range: 0.01–0.061 μg m−3), respectively. The highest seasonal average concentrations of levoglucosan (0.131 ± 0.073 μg m−3) and mannosan (0.028 ± 0.019 μg m−3) were observed during the winter season. The BB contributions to the TSP organic carbon (OC) and TSP mass were estimated with positive matrix factorization (PMF) by using BB tracers, inorganic ions, elements, OC, and EC. The BB contributions to the TSP OC and TSP mass were quite substantial in winter with 26% and 14%, respectively. The results evidenced a major contribution of BB to the aerosol OC during winter season. Major potential source distributions of BB were identified, which included the pollution bands along the Indo-Gangetic Plain, the Yarlung Tsangpo River Valley and the interior of the TP. In addition to the long-range transport of BB, the sources of anthropogenic emissions (residential BB for cooking and heating) in the TP may be an important contributor. The results facilitated understanding of the characteristics and effects of BB in the TP.

Dissimilar effects of two El Niño types on PM2.5 concentrations in East Asia

We investigate the effects of natural variability of meteorological fields on surface PM2.5 concentration changes in East Asia during El Niño periods for the past three decades (1980–2014) through GEOS-Chem 3D global chemical transport model simulations. First, our evaluation of the model with anthropogenic emissions for 2006 and a comparison against observations show that the simulated results accurately reproduced the observed spatial distribution of annual mean aerosol concentrations for 2006–2007 including inorganic (sulfate, ammonium, and nitrate) and carbonaceous (organic and black carbon) aerosols in the surface air. Based on the Oceanic Niño Index, the assimilated meteorological data used in the model simulations indicate that 10 El Niño events occurred for the past three decades (1980–2014). We further classified the 10 El Niño events into 6 central Pacific El Niño (C-type) and 4 eastern Pacific El Niño (E-type) to examine the different roles of two El Niño types in determining seasonal surface PM2.5 concentrations in East Asia. We find opposite impacts on the seasonal surface PM2.5 concentrations depending on two El Niño types, such that the surface PM2.5 concentrations during the E-type period are higher than the climatological mean value, especially in northern East Asia. The peak increase of as much as 20% occurs in winter and is sustained until the following spring. However, the C-type period shows a decrease in seasonal PM2.5 concentrations in northern East Asia compare to the climatological mean, and the peak decrease of as much as 10% occurs in the following spring. The different of two El Niño types also have dissimilar impacts on surface PM2.5 concentrations in southeastern China. Natural variation of aerosol concentrations driven by the different of two El Niño types appears to be significant and would be an important factor in determining the inter-annual variation of aerosol concentrations in East Asia.

The role of Boundary Layer Height (BLH) variations on pollution dispersion over a coastal station in the Southwest Peninsular India

We report the variability of Boundary Layer Height (BLH) and Ventilation Coefficient (VC) over a coastal station in southwest Peninsular India from vertical soundings. Altitude profile of Virtual Potential Temperature (θv) (derived from balloon-borne GPS radiosonde observations) was used to study the seasonal changes of BLH over Thumba (8.5°N, 77°E), a coastal station in southwest Peninsular India. Variability in the BLH is maximum during the pre-monsoon season and minimum during the winter, whereas the VC was found to be highest in the summer and lowest during winter. It is revealing the excellent efficiency in the dispersion of pollutants during the summer monsoon season. Conversely, low VC during winter and post-monsoon seasons showed great potential for pollution at this site. Role of VC on the dispersion of pollution was also examined using surface mass concentration of Black and Organic Carbon (BC and OC), sulphate and columnar Aerosol Optical Depth (AOD). High value of VC lowers the surface mass concentrations of BC, OC and sulphate during winter and maximises during summer monsoon and decreases the pollution potential.

Mixing State of Carbonaceous Aerosols of Primary Emissions from "Improved" African Cookstoves.

Designs of "improved" stoves are introduced recently to benefit the solid fuel consumption of cooking activities in developing countries, but the uncertainties concerning the combustion processes and particulate emissions remain poorly characterized. To help understand this, combustion in three examples of "improved" African cookstoves was investigated in the laboratory. A typical European heating stove was included for comparison purpose. Detailed aerosol emissions were studied in real-time with an Aerosol Mass Spectrometer and Single Particle Soot Photometer, to explore interactions between black carbon (BC) and organic carbon aerosols, which were parametrized according to modified combustion efficiency (MCE), a common metric used within the atmospheric emission community. Greater than 50% of the total organic matter (OM) was found in BC-containing particles when MCE was >0.95 for dry oak and coal fuels, whereas at lower MCE, over 80% of the total OM for most of the fuels existed in particles without detectable BC. When the OM mass fraction of total particulate matter (PM1) > 0.9, the mass ratio of OM to refractory BC in BC-containing particles was about 2-3, but only ∼0.8 when OM mass fraction <0.9. These findings are not currently included in models and such information should be considered in the future emission scenarios.

Characteristic and Driving Factors of Aerosol Optical Depth over Mainland China during 1980–2017

Since the reform and opening up of China, the increasing aerosol emissions have posted great challenges to the country’s climate change and human health. The aerosol optical depth (AOD) is one of the main physical indicators quantifying the atmospheric turbidity and air pollution. In this study, 38-years (1980–2017) of spatial and temporal variations of AOD in China were analyzed using AOD records derived from MODIS atmosphere products and the MERRA-2 dataset. The results showed that the annual mean AOD values throughout China have gone through an increasing, but fluctuating, trend, especially in 1982 and in 1992 due to two volcano eruptions; the AOD values experienced a dramatically increasing period during 2000–2007 with the rapid economic development and “population explosions” in China/after 2008, the AOD values gradually decreased from 0.297 (2008) to 0.257 (2017). The AOD values in China were generally higher in spring than that in other seasons. The Sichuan Basin has always been an area with high AOD values owing to the strong human activity and the basin topography (hindering aerosol diffusions in the air). In contrast, the Qinghai Tibet Plateau has always been an area with low AOD values due to low aerosol emissions and clear sky conditions there. The trend analysis of AOD values during 1980–2017 in China indicated that the significant increasing trend was mainly observed in Southeastern China. By contrast, the AOD values in the northernmost of China showed a significant decreasing trend. Then, the contributions (AODP) of the AOD for black carbon aerosol (BCAOD), dust aerosol (DUAOD), organic carbon aerosol (OCAOD), sea salt aerosol (SSAOD), and SO4 aerosol (SO4AOD) to the total AOD values were calculated. The results showed that DUAOD (25.43%) and SO4AOD (49.51%) were found to be the main driving factors for the spatial and temporal variations of AOD values. Finally, the effects of anthropogenic aerosol emissions, socioeconomic factors, and land-use and land coverage changes on AOD were analyzed. The GDP, population density, and passenger traffic volume were found to be the main socioeconomic drivers for AOD distributions. Relatively larger AOD values were mainly found in urban land and land covered by water, while lower AOD values were found in grassland and permanent glacier areas.

The implementation of NEMS GFS Aerosol Component (NGAC) Version 2.0 for global multispecies forecasting at NOAA/NCEP – Part 1: Model descriptions

Abstract. The NEMS GFS Aerosol Component Version 2.0 (NGACv2) for global multispecies aerosol forecast has been developed at the National Centers of Environment Prediction (NCEP) in collaboration with the NESDIS Center for Satellite Applications and Research (STAR), the NASA Goddard Space Flight Center (GSFC), and the University at Albany, State University of New York (SUNYA). This paper describes the continuous development of the NGAC system at NCEP after the initial global dust-only forecast implementation (NGAC version 1.0, NGACv1). With NGACv2, additional sea salt, sulfate, organic carbon, and black carbon aerosol species were included. The smoke emissions are from the NESDIS STAR's Global Biomass Burning Product (GBBEPx), blended from the global biomass burning emission product from a constellation of geostationary satellites (GBBEP-Geo) and GSFC's Quick Fire Emission Data Version 2 from a polar-orbiting sensor (QFED2). This implementation advanced the global aerosol forecast capability and made a step forward toward developing a global aerosol data assimilation system. The aerosol products from this system have been used by many applications such as for regional air quality model lateral boundary conditions, satellite sea surface temperature (SST) physical retrievals, and the global solar insolation estimation. Positive impacts have been seen in these applications.

Characteristics and temporal variations of organic and elemental carbon aerosols in a high–altitude, tropical Latin American megacity

Bogota is a Latin American megacity located at an average altitude of 2600 m in the tropical Andes. It registers frequent episodes of poor air quality due to high PM10 concentrations. The carbonaceous fraction is the main PM10 component (>50%), but there is a lack of specific studies analyzing the characteristics and temporal variability of organic carbon (OC) and elemental carbon (EC) aerosols. In this study, daily samples (24±1h) were collected from June 2015 to May 2016 (a total of 308 samples) at an urban background site during an El Niño year, and the quartz filters were analyzed using a thermal-optical method. Results showed that EC and organic matter accounted for ~60% of the PM10 mass. The OC and EC averages were 8.92 ± 4.52 μg/m3 and 3.25 ± 1.59 μg/m3, respectively. The months with the highest average OC values were January to March, while EC concentrations were relatively constant throughout the year. Regarding daily values, the highest mean concentrations of OC (10.2 ± 5.13 μg/m3) and EC (3.73 ± 1.74 μg/m3) were obtained on Thursdays, and the lowest on Sundays (OC = 6.67 ± 3.04 μg/m3 and EC = 2.46 ± 0.94 μg/m3). The OC/EC ratio ranged from 1.66 (June) to 4.88 (March), with an annual average of 3.16 ± 2.01. The secondary organic carbon (SOC) contributions, measured using the EC-tracer method, accounted for 45% of the total OC. The effective carbon ratio, which indicates an association between carbonaceous particles and climate change, ranged from 0.12 (July) to 0.74 (May). The study of air-mass origins revealed that days with air mass from E + NE registered the highest OC concentrations. This research provides new data on the variability of carbonaceous aerosols over the course of a year. It also highlights forest fires as a significant source of OC and EC, and indicates the high impact of SOC on OC concentration at the sampling site.

Benzo(a)pyrene parallel measurements in PM1 and PM2.5 in the coastal zone of the Gulf of Gdansk (Baltic Sea) in the heating and non-heating seasons

Parallel measurements of PM1 and PM2.5 aerosols were conducted in the urbanized coastal zone of the southern Baltic Sea. The main aim of the research was to assess and determine annual, seasonal (heating and non-heating), and daily concentration variability of benzo(a)pyrene in aerosols, these being the most dangerous constituents to human health. The average annual concentration of benzo(a)pyrene (B(a)P) was equal to 2.6 ng·m−3 in PM1 and 4.6 ng·m−3 in PM2.5, and both values were several times higher than the level of 1 ng·m−3 which was set out in the CAFE Directive. High mean daily concentrations of B(a)P persisted for 50 and 65% of the study period in PM1 and PM2.5, respectively. In order to determine the sources of B(a)P in both aerosol fractions, organic (OC) and elemental (EC) carbon concentrations were examined. The highest concentrations of all carbon species were reported during the heating season under local or regional land advection and at low air temperatures. The origin of pollutants was the same and was primarily related to the combustion of fossil fuels in the communal-utility sector. During the non-heating period, the role of transportation, both land and marine, increased and may have been significant in creating higher concentrations of carbon compounds in PM1 and PM2.5. Regardless of the size of the aerosol fractions, B(a)P loads introduced into the Baltic coastal zone were several times higher during the heating period compared to the non-heating season.Graphical abstractᅟ

Global radiative effects of solid fuel cookstove aerosol emissions

Abstract. We apply the NCAR CAM5-Chem global aerosol-climate model to quantify the net global radiative effects of black and organic carbon aerosols from global and Indian solid fuel cookstove emissions for the year 2010. Our assessment accounts for the direct radiative effects, changes to cloud albedo and lifetime (aerosol indirect effect, AIE), impacts on clouds via the vertical temperature profile (semi-direct effect, SDE) and changes in the surface albedo of snow and ice (surface albedo effect). In addition, we provide the first estimate of household solid fuel black carbon emission effects on ice clouds. Anthropogenic emissions are from the IIASA GAINS ECLIPSE V5a inventory. A global dataset of black carbon (BC) and organic aerosol (OA) measurements from surface sites and aerosol optical depth (AOD) from AERONET is used to evaluate the model skill. Compared with observations, the model successfully reproduces the spatial patterns of atmospheric BC and OA concentrations, and agrees with measurements to within a factor of 2. Globally, the simulated AOD agrees well with observations, with a normalized mean bias close to zero. However, the model tends to underestimate AOD over India and China by ∼ 19 ± 4 % but overestimate it over Africa by ∼ 25 ± 11 % (± represents modeled temporal standard deviations for n = 5 run years). Without BC serving as ice nuclei (IN), global and Indian solid fuel cookstove aerosol emissions have net global cooling radiative effects of −141 ± 4 mW m−2 and −12 ± 4 mW m−2, respectively (± represents modeled temporal standard deviations for n = 5 run years). The net radiative impacts are dominated by the AIE and SDE mechanisms, which originate from enhanced cloud condensation nuclei concentrations for the formation of liquid and mixed-phase clouds, and a suppression of convective transport of water vapor from the lower troposphere to the upper troposphere/lower stratosphere that in turn leads to reduced ice cloud formation. When BC is allowed to behave as a source of IN, the net global radiative impacts of the global and Indian solid fuel cookstove emissions range from −275 to +154 mW m−2 and −33 to +24 mW m−2, with globally averaged values of −59 ± 215 and 0.3 ± 29 mW m−2, respectively. Here, the uncertainty range is based on sensitivity simulations that alter the maximum freezing efficiency of BC across a plausible range: 0.01, 0.05 and 0.1. BC–ice cloud interactions lead to substantial increases in high cloud (&lt; 500 hPa) fractions. Thus, the net sign of the impacts of carbonaceous aerosols from solid fuel cookstoves on global climate (warming or cooling) remains ambiguous until improved constraints on BC interactions with mixed-phase and ice clouds are available.

Simulating Aerosol Size Distribution and Mass Concentration with Simultaneous Nucleation, Condensation/Coagulation, and Deposition with the GRAPES–CUACE

A coupled aerosol–cloud model is essential for investigating the formation of haze and fog and the interaction of aerosols with clouds and precipitation. One of the key tasks of such a model is to produce correct mass and number size distributions of aerosols. In this paper, a parameterization scheme for aerosol size distribution in initial emission, which took into account the measured mass and number size distributions of aerosols, was developed in the GRAPES–CUACE [Global/Regional Assimilation and PrEdiction System–China Meteorological Administration (CMA) Unified Atmospheric Chemistry Environment model]—an online chemical weather forecast system that contains microphysical processes and emission, transport, and chemical conversion of sectional multi-component aerosols. In addition, the competitive mechanism between nucleation and condensation for secondary aerosol formation was improved, and the dry deposition was also modified to be in consistent with the real depositing length. Based on the above improvements, the GRAPES–CUACE simulations were verified against observational data during 1–31 January 2013, when a series of heavy regional haze–fog events occurred in eastern China. The results show that the aerosol number size distribution from the improved experiment was much closer to the observation, whereas in the old experiment the number concentration was higher in the nucleation mode and lower in the accumulation mode. Meanwhile, the errors in aerosol number size distribution as diagnosed by its sectional mass size distribution were also reduced. Moreover, simulations of organic carbon, sulfate, and other aerosol components were improved and the overestimation as well as underestimation of PM2.5 concentration in eastern China was significantly reduced, leading to increased correlation coefficient between simulated and observed PM2.5 by more than 70%. In the remote areas where bad simulation results were produced previously, the correlation coefficient grew from 0.35 to 0.61, and the mean mass concentration went up from 43% to 87.5% of the observed value. Thus, the simulation of particulate matters in these areas has been improved considerably.

Impacts of springtime biomass burning in the northern Southeast Asia on marine organic aerosols over the Gulf of Tonkin, China

Fine particles (PM2.5) samples, collected at Weizhou Island over the Gulf of Tonkin on a daytime and nighttime basis in the spring of 2015, were analyzed for primary and secondary organic tracers, together with organic carbon (OC), elemental carbon (EC), and stable carbon isotopic composition (δ13C) of total carbon (TC). Five organic compound classes, including saccharides, lignin/resin products, fatty acids, biogenic SOA tracers and phthalic acids, were quantified by gas chromatography/mass spectrometry (GC/MS). Levoglucosan was the most abundant organic species, indicating that the sampling site was under strong influence of biomass burning. Based on the tracer-based methods, the biomass-burning-derived fraction was estimated to be the dominant contributor to aerosol OC, accounting for 15.7% ± 11.1% and 22.2% ± 17.4% of OC in daytime and nighttime samples, respectively. In two episodes E1 and E2, organic aerosols characterized by elevated concentrations of levoglucosan as well as its isomers, sugar compounds, lignin products, high molecular weight (HMW) fatty acids and β-caryophyllinic acid, were attributed to the influence of intensive biomass burning in the northern Southeast Asia (SEA). However, the discrepancies in the ratios of levoglucosan to mannosan (L/M) and OC (L/OC) as well as the δ13C values suggest the type of biomass burning and the sources of organic aerosols in E1 and E2 were different. Hardwood and/or C4 plants were the major burning materials in E1, while burning of softwood and/or C3 plants played important role in E2. Furthermore, more complex sources and enhanced secondary contribution were found to play a part in organic aerosols in E2. This study highlights the significant influence of springtime biomass burning in the northern SEA to the organic molecular compositions of marine aerosols over the Gulf of Tonkin.