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Sample records for carbonaceous aerosol components

  1. CARES: Carbonaceous Aerosol and Radiative Effects Study Science Plan

    SciTech Connect

    Zaveri, RA; Shaw, WJ; Cziczo, DJ

    2010-05-27

    Carbonaceous aerosol components, which include black carbon (BC), urban primary organic aerosols (POA), biomass burning aerosols, and secondary organic aerosols (SOA) from both urban and biogenic precursors, have been previously shown to play a major role in the direct and indirect radiative forcing of climate. The primary objective of the CARES 2010 intensive field study is to investigate the evolution of carbonaceous aerosols of different types and their effects on optical and cloud formation properties.

  2. Inorganic markers, carbonaceous components and stable carbon isotope from biomass burning aerosols in northeast China

    NASA Astrophysics Data System (ADS)

    Cao, F.; Zhang, Y.; Kawamura, K.

    2015-12-01

    To better characterize the sources of fine particulate matter (i.e. PM2.5) in Sanjiang Plain, Northeast China, aerosol chemical composition such total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied as well as stable carbon isotopic composition (δ13C) of TC. Intensively open biomass burning episodes were identified from late September to early October by satellite fire and aerosol optical depth maps. During the biomass burning episodes, concentrations of PM2.5, OC, EC, and WSOC increased by a factor of 4-12 compared to non-biomass-burning periods. Non-sea-salt potassium is strongly correlated with PM2.5, OC, EC and WSOC, suggesting an important contribution of biomass burning emission. The enrichment in both the non-sea-salt potassium and chlorine is significantly larger than other inorganic species, indicating that biomass burning aerosols in Sanjiang Plain is mostly fresh and less aged. In addition, WSOC to OC ratio is relatively lower compared to that reported in biomass burning aerosols in tropical regions, supporting that biomass burning aerosols in Sanjiang Plain is mostly primary and secondary organic aerosols is not significant. A lower average δ13C value (-26.2‰) is found for the biomass-burning aerosols, suggesting a dominant contribution from combustion of C3 plants in the studied region.

  3. Physical and Chemical Characterization of Carbonaceous Aerosols in Korea

    NASA Astrophysics Data System (ADS)

    Choung, S.; Jin, J. S.; Hwang, G. S.; Jang, K. S.; Han, W. S.; OH, J.; Kwon, Y.

    2014-12-01

    Atmospheric aerosols have been recently paid attention more in environmental research due to their negative effects on air quality, public health, and climate change. The aerosols contain approximately >20-50% carbonaceous components such as organic carbon (OC) and black carbon (BC) (or elemental carbon [EC]) derived from organic compounds, biomass burning, and incomplete combustion of fossil fuels. The physical, chemical, and biological properties of atmospheric aerosols are strongly dependent on the carbonaceous components. In particular, the BC could significantly affect the regional air quality in the northeastern Asia, because China is one of the foremost BC emission country in the world. Previous studies have mainly focused on the quantification and source identification for carbonaceous aerosols. However, understanding of physical and chemical properties for the carbonaceous aerosols related to environmental contamination and toxicity was still incomplete due to analytical difficulties. This study is addressed to evaluate the contribution of carbonaceous aerosols to air pollution through the surface, mass spectroscopic, and electron microscopic analyses, and determination of chemical composition and structure using the air particulate matter (PM2.5 and >PM2.5) samples.

  4. Seasonality of Forcing by Carbonaceous Aerosols

    NASA Astrophysics Data System (ADS)

    Habib, G.; Bond, T.; Rasch, P. J.; Coleman, D.

    2006-12-01

    Aerosols can influence the energy balance of Earth-Atmosphere system with profound effect on regional climate. Atmospheric processes, such as convection, scavenging, wet and dry deposition, govern the lifetime and location of aerosol; emissions affect its quantity and location. Both affect climate forcing. Here we investigate the effect of seasonality in emissions and atmospheric processes on radiative forcing by carbonaceous aerosols, focusing on aerosol from fossil fuel and biofuel. Because aerosol lifetime is seasonal, ignoring the seasonality of sources such as residential biofuel may introduce a bias in aerosol burden and therefore in predicted climate forcing. We present a global emission inventory of carbonaceous aerosols with seasonality, and simulate atmospheric concentrations using the Community Atmosphere Model (CAM). We discuss where and when the seasonality of emissions and atmospheric processes has strong effects on atmospheric burden, lifetime, climate forcing and aerosol optical depth (AOD). Previous work has shown that aerosol forcing is higher in summer than in winter, and has identified the importance of aerosol above cloud in determining black carbon forcing. We show that predicted cloud height is a very important factor in determining normalized radiative forcing (forcing per mass), especially in summer. This can affect the average summer radiative forcing by nearly 50%. Removal by cloud droplets is the dominant atmospheric cleansing mechanism for carbonaceous aerosols. We demonstrate the modeled seasonality of removal processes and compare the importance of scavenging by warm and cold clouds. Both types of clouds contribute significantly to aerosol removal. We estimate uncertainty in direct radiative forcing due to scavenging by tagging the aerosol which has experienced cloud interactions. Finally, seasonal variations offer an opportunity to assess modeled processes when a single process dominates variability. We identify regions where aerosol

  5. Climate impacts of carbonaceous and other non-sulfate aerosols: A proposed study

    SciTech Connect

    Andreae, M.O.; Crutzen, P.J.; Cofer, W.R. III; Hollande, J.M.

    1995-06-01

    In addition to sulfate aerosols, carbonaceous and other non-sulfate aerosols are potentially significant contributors to global climate change. We present evidence that strongly suggests that current assessments of the effects of aerosols on climate may be inadequate because major aerosol components, especially carbonaceous aerosols, are not included in these assessments. Although data on the properties and distributions of anthropogenic carbonaceous aerosols are insufficient to allow quantification of their climate impacts, the existing information suggests that climate forcing by this aerosol component may be significant and comparable to that by sulfate aerosols. We propose that a research program be undertaken to support a quantitative assessment of the role in climate forcing of non-sulfate, particularly carbonaceous, aerosols.

  6. Hydrocarbon components in carbonaceous meteorites

    NASA Astrophysics Data System (ADS)

    Kissin, Y. V.

    2003-05-01

    Currently, the presence of free n-alkanes and isoprenoid alkanes in carbonaceous meteorites is usually explained either by microbial contamination during the period between the meteorite fall and collection or by contamination from the environment of analytical laboratories and museums. The goal of this research was to repeat analysis of hydrocarbon components in meteorites and to investigate possible meteorite contamination routes discussed in the literature. Experimental analysis of free organic constituents in five carbonaceous meteorites by infrared spectroscopy (IR) and gas chromatographic (GC) methods confirmed the presence of extractable aliphatic components, n-alkanes in the C 15H 32-C 27H 56 range and isoprenoid alkanes (phytane, pristane, and norpristane), in some of these meteorites. The contents of these compounds vary depending on the source. Insoluble organic components of two meteorites (meteorite kerogens) were isolated, and their composition was analyzed by IR and cracking/GC methods. Comparison with the data on several terrestrial contamination sources proposed in the literature shows that the presence of free saturated hydrocarbons in meteorites and the composition of the meteorite kerogen could not be explained either by microbial contamination or by contamination from the laboratory environment. The types of the hydrocarbons in meteorites resemble those typical of ancient terrestrial deposits of organic-rich sediments, except for the absence of lighter hydrocarbons, which apparently slowly evaporated in space, and multi-ring naphthenic compounds of the biologic origin, steranes, terpanes, etc. The prevailing current explanation for the presence of free linear saturated hydrocarbons in carbonaceous meteorites, apart from contamination, is the abiotic route from hydrogen and carbon monoxide. However, the data on the structure of meteorite kerogens require a search for different routes that initially produce complex polymeric structures containing

  7. Carbonaceous aerosols influencing atmospheric radiation: Black and organic carbon

    SciTech Connect

    Penner, J.E.

    1994-09-01

    Carbonaceous particles in the atmosphere may both scatter and absorb solar radiation. The fraction associated with the absorbing component is generally referred to as black carbon (BC) and is mainly produced from incomplete combustion processes. The fraction associated with condensed organic compounds is generally referred to as organic carbon (OC) or organic matter and is mainly scattering. Absorption of solar radiation by carbonaceous aerosols may heat the atmosphere, thereby altering the vertical temperature profile, while scattering of solar radiation may lead to a net cooling of the atmosphere/ocean system. Carbonaceous aerosols may also enhance the concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the fine particle (D < 2.5 {mu}m) source rates of both OC and BC. The source rates for anthropogenic organic aerosols may be as large as the source rates for anthropogenic sulfate aerosols, suggesting a similar magnitude of direct forcing of climate. The role of BC in decreasing the amount of reflected solar radiation by OC and sulfates is discussed. The total estimated forcing depends on the source estimates for organic and black carbon aerosols which are highly uncertain. The role of organic aerosols acting as cloud condensation nuclei (CCN) is also described.

  8. Characterization of carbonaceous aerosols in urban air

    NASA Astrophysics Data System (ADS)

    Husain, Liaquat; Dutkiewicz, Vincent A.; Khan, A. J.; Ghauri, Badar M.

    Concentrations of black carbon, [BC], were determined with an Aethalometer every 5 min at Lahore, a city of about 10 million in Pakistan, from 22 November 2005 to 31 January 2006. [BC] were very high, ranging from about 5 to 110μgm-3, with a mean of 21.7μgm-3. A distinct diurnal variation was observed: concentrations were lowest from about 10 a.m. to 4 p.m. local time (LT), and highest around 5-9 p.m. No clear relationship was observed between surface wind directions and [BC], although some of the highest concentrations were observed when the airflow was from southwest to northwest. The daily variations in concentrations were strongly affected by the diurnal variations in the mixing height; BC concentrations were low during the day when the mixing heights were high, ˜1000m, and very high at night when the mixing heights were low <250m. Periods of light to dense fog occurred from 22 December through 4 January. [BC] were generally lower than average when fog occurred during the night and early morning, but they were not necessarily lower during daytime fogs. We also collected aerosols on quartz filters every 3, 6, or 12 h and determined the concentrations of elemental, [EC], and organic carbon, [OC], using the thermal-optical method. The [BC] were highly correlated with EC (r2=0.71), but on average 25% higher than [EC]. The [EC] and [OC] concentrations were moderately correlated (r2=0.65). The [OC]/[EC] ratios varied from 2.8 to 12, with a mean of 5.6. Although a large component of the carbonaceous aerosols in Lahore originated from fossil fuel combustion, a significant fraction was derived from biomass burning.

  9. Global cloud condensation nuclei influenced by carbonaceous combustion aerosol

    NASA Astrophysics Data System (ADS)

    Spracklen, D. V.; Carslaw, K. S.; Pöschl, U.; Rap, A.; Forster, P. M.

    2011-09-01

    Black carbon in carbonaceous combustion aerosol warms the climate by absorbing solar radiation, meaning reductions in black carbon emissions are often perceived as an attractive global warming mitigation option. However, carbonaceous combustion aerosol can also act as cloud condensation nuclei (CCN) so they also cool the climate by increasing cloud albedo. The net radiative effect of carbonaceous combustion aerosol is uncertain because their contribution to CCN has not been evaluated on the global scale. By combining extensive observations of CCN concentrations with the GLOMAP global aerosol model, we find that the model is biased low (normalised mean bias = -77 %) unless carbonaceous combustion aerosol act as CCN. We show that carbonaceous combustion aerosol accounts for more than half (52-64 %) of global CCN with the range due to uncertainty in the emitted size distribution of carbonaceous combustion particles. The model predicts that wildfire and pollution (fossil fuel and biofuel) carbonaceous combustion aerosol causes a global mean cloud albedo aerosol indirect effect of -0.34 W m-2, with stronger cooling if we assume smaller particle emission size. We calculate that carbonaceous combustion aerosol from pollution sources cause a global mean aerosol indirect effect of -0.23 W m-2. The small size of carbonaceous combustion particles from fossil fuel sources means that whilst pollution sources account for only one-third of the emitted mass they cause two-thirds of the cloud albedo aerosol indirect effect that is due to carbonaceous combustion aerosol. This cooling effect must be accounted for, along with other cloud effects not studied here, to ensure that black carbon emissions controls that reduce the high number concentrations of fossil fuel particles have the desired net effect on climate.

  10. Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

    SciTech Connect

    Mazurek, M.A. ); Cofer, W.R. III; Levine, J.S. . Langley Research Center)

    1990-10-01

    The identity and ambient mass concentrations of radiatively important carbonaceous aerosols were measured for a boreal forest prescribed burn conducted in northern Ontario, CAN in August 1989. Nonsize-segregated airborne particles were collected for smoldering-fire and full-fire conditions using a helicopter sampling platform. Total carbon (TC), organic carbon (OC) and elemental carbon (EC) were measured. Smoke plume mass concentrations of the OC and EC particles were greatest for full-fire conditions and had ranges of 1.560 to 2.160 mg/m{sup {minus}1} (OC) and 0.120 to 0.160 mg/m{sup {minus}3} (EC) with OC:EC ratios of 10 to 18, respectively. Smoldering fire conditions showed smoke plume OC and EC levels of 0.570--1.030 mg/m{sup {minus}3} (OC) and 0.006--0.050 mg/m{sup {minus}3} (EC) and much higher ratios of OC:EC (21 to 95). These aerosol data indicate the formation of EC particles is greatest during full-fire combustion of boreal forest material relative to smoldering combustion. However, EC particles comprise a minor fraction of the particulate carbon smoke aerosols for both full-fire and smoldering conditions; the major component of carbonaceous smoke aerosols emitted during the prescribed burn is OC. Overall, the OC and EC in-plume smoke aerosol data show nonuniform production of these particles during various stages of the prescribed burn, and major differences in the type of carbonaceous aerosol that is generated (OC versus EC).

  11. Carbonaceous aerosols of aviation and shipping emissions

    NASA Astrophysics Data System (ADS)

    Popovicheva, O. B.; Kireeva, E. D.; Timofeev, M. A.; Shonija, N. K.; Mogil'Nikov, V. P.

    2010-06-01

    This is a study of the physical and chemical properties of carbonaceous aerosols emitted by transport systems (namely, by aircraft gas turbine engines and large ship diesel engines) into the atmosphere. A comparative analysis of the morphology, size, elemental composition, and surface chemistry between aviation and diesel soot particles reveals the general and characteristic features of emissions from each source. The high pollution rate of diesel soot particles, considerable fraction of metal admixtures, and availability of char particles characterize the specific features of the formation of particles of this type. The main characteristics characterizing the interaction between aviation and shipping emission aerosols in the moist atmosphere (the composition of organic and water-soluble fractions at the surface) have been obtained. Due to high hygroscopicity, the microparticles can generate cloud condensation nuclei and initiate contrails and additional tropospheric cloudiness.

  12. Global cloud condensation nuclei influenced by carbonaceous combustion aerosol

    NASA Astrophysics Data System (ADS)

    Spracklen, D. V.; Carslaw, K. S.; Pöschl, U.; Rap, A.; Forster, P. M.

    2011-03-01

    Black carbon in carbonaceous combustion aerosol warms the climate by absorbing solar radiation, meaning reductions in black carbon emissions are often perceived as an attractive global warming mitigation option. However, carbonaceous combustion aerosol can also act as cloud condensation nuclei (particles upon which cloud drops form) so they also cool the climate by increasing cloud albedo. The net radiative effect of carbonaceous combustion aerosol is uncertain because their contribution to cloud drops has not been evaluated on the global scale. By combining extensive observations of cloud condensation nuclei concentrations and a global aerosol model, we show that carbonaceous combustion aerosol accounts for more than half of global cloud condensation nuclei. The evaluated model predicts that wildfire and pollution (fossil fuel and biofuel) carbonaceous combustion aerosol causes a global mean aerosol indirect effect of -0.34 W m-2 due to changes in cloud albedo, with pollution sources alone causing a global mean aerosol indirect effect of -0.23 W m-2. The small size of carbonaceous combustion particles from pollution sources means that whilst they account for only one-third of the emitted mass from these sources they cause two-thirds of the cloud albedo indirect effect that is due to carbonaceous combustion aerosol. This cooling effect must be accounted for to ensure that black carbon emissions controls that reduce the high number concentrations of small pollution particles have the desired net effect on climate.

  13. Carbonaceous aerosols from different tropical biomass burning sources

    NASA Astrophysics Data System (ADS)

    Cachier, Hélène; Brémond, Marie-Pierre; Buat-Ménard, Patrick

    1989-08-01

    FOLLOWING a repetitive pattern, biomass burning affects the intertropical belt on a continental scale during the dry season1. The importance of these anthropogenic activities with regard to carbonaceous-component emissions into the global atmosphere is now well recognized2-4. It has been suggested that large injections of black carbon aerosols from the Tropics are of potential importance for the radiative and chemical balance of the troposphere5-10. Studies on carbonaceous aerosols have indicated that, on an annual basis, the intensity of the emissions from tropical biomass burning could compare with that of emissions from fossil-fuel burning in industrial countries7,8. Also, results from combustion chamber experiments have determined the important range of the emission factor for both the organic and the black carbon components of the aerosol1-16. Following on from our earlier studies on total atmospheric particulate carbon (Ct) and isotopic composition (δ13C) (ref. 2), we now present new data on the black carbon content (Cb) of atmospheric particles sampled during the biomass-burning season in the wooden savannah of the Ivory Coast. The Cb/Ct ratio is generally lower than expected and highly variable. This variability indicates that there are drastic changes in source apportionment, which from our isotope studies may be ascribed to the variety of vegetation fuel and also to the mode of combustion. Therefore the Cb/Ct ratio can potentially discriminate biomass-burning emissions from different tropical ecosystems.

  14. A one-year record of carbonaceous components and major ions in aerosols from an urban kerbside location in Oporto, Portugal.

    PubMed

    Custódio, Danilo; Cerqueira, Mário; Alves, Célia; Nunes, Teresa; Pio, Casimiro; Esteves, Valdemar; Frosini, Daniele; Lucarelli, Franco; Querol, Xavier

    2016-08-15

    PM2.5 aerosol samples were collected from January 2013 to January 2014 on the kerbside of a major arterial route in the city of Oporto, Portugal, and later analyzed for carbonaceous fractions and water soluble ions. The average concentrations of organic carbon (OC), elemental carbon (EC) and water soluble organic carbon (WSOC) in the aerosol were 6.2μg/m(3), 5.0μg/m(3) and 3.8μg/m(3), respectively, and fit within the range of values that have been observed close to major roads in Europe, Asia and North America. On average, carbonaceous matter accounted for 56% of the gravimetrically measured PM2.5 mass. The three carbon fractions exhibited a similar seasonal variation, with high concentrations in late autumn and in winter, and low concentrations in spring. SO4(2-) was the dominant water soluble ion, followed by NO3(-), NH4(+), Cl(-), Na(+), K(+), oxalate, Ca(2+), Mg(2+), formate, methanesulfonate and acetate. Some of these ions exhibited a clear seasonal trend during the study period. The average OC/EC ratio for the entire set of samples was 1.28±0.61, which was consistent with a significant influence of vehicle exhaust emissions on aerosol composition. On the other hand, the average WSOC/OC ratio was 0.67±0.23, reflecting the influence of other emitting sources. WSOC was highly correlated with nssK(+), a tracer of biomass combustion, and was not correlated with nssSO4(2-), a species associated with secondary processes, suggesting that the main source of WSOC was biomass burning. Most of the SO4(2-) was anthropogenic in origin and was closely associated with NH4(+), pointing to the formation of secondary aerosols. Na(+), Cl(-) and methanesulfonate were clearly associated with marine sources while NO3(-) was related with combustion of both fossil and non-fossil fuels. Mixed sources explained the occurrence of the other water soluble ions. PMID:27110993

  15. Impact of aging mechanism on model simulated carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Huang, Y.; Wu, S.; Dubey, M. K.; French, N. H. F.

    2013-07-01

    Carbonaceous aerosols including organic carbon and black carbon have significant implications for both climate and air quality. In the current global climate or chemical transport models, a fixed hydrophobic-to-hydrophilic conversion lifetime for carbonaceous aerosol (τ) is generally assumed, which is usually around one day. We have implemented a new detailed aging scheme for carbonaceous aerosols in a chemical transport model (GEOS-Chem) to account for both the chemical oxidation and the physical condensation-coagulation effects, where τ is affected by local atmospheric environment including atmospheric concentrations of water vapor, ozone, hydroxyl radical and sulfuric acid. The updated τ exhibits large spatial and temporal variations with the global average (up to 11 km altitude) calculated to be 2.6 days. The chemical aging effects are found to be strongest over the tropical regions driven by the low ozone concentrations and high humidity there. The τ resulted from chemical aging generally decreases with altitude due to increases in ozone concentration and decreases in humidity. The condensation-coagulation effects are found to be most important for the high-latitude areas, in particular the polar regions, where the τ values are calculated to be up to 15 days. When both the chemical aging and condensation-coagulation effects are considered, the total atmospheric burdens and global average lifetimes of BC, black carbon, (OC, organic carbon) are calculated to increase by 9% (3%) compared to the control simulation, with considerable enhancements of BC and OC concentrations in the Southern Hemisphere. Model evaluations against data from multiple datasets show that the updated aging scheme improves model simulations of carbonaceous aerosols for some regions, especially for the remote areas in the Northern Hemisphere. The improvement helps explain the persistent low model bias for carbonaceous aerosols in the Northern Hemisphere reported in literature. Further

  16. The contribution of carbonaceous aerosols to climate change

    SciTech Connect

    Penner, J.E. |; Chuang, C.C.; Liousse, C.

    1996-04-01

    Contribution of aerosols to climate change results from two effects: clear-sky and cloudy-sky forcing. The clear-sky climate forcing by carbonaceous aerosols from biomass burning and fossil fuel burning depends on the relative contribution of scattering and absorption by the aerosols which in turn depends on the fraction of aerosol mass associated with black carbon and its size distribution. This paper reviews estimates for the emission of carbonaceous aerosols, placing these estimates in the context of estimates for the emissions of anthropogenic and natural sulfate aerosols and natural sources of organic particulate matter. The cloudy-sky forcing from carbonaceous aerosols is difficult to estimate because, among other factors, it depends on the amount of absorption by the aerosols in the cloud. It is also highly sensitive to the assumed pre-existing, natural aerosol abundance. An upper limit for this cloudy-sky forcing is -4.4 W/m{sup 2}, but may range as low as -2.4 W/m{sup 2}, depending on background aerosol concentrations. These estimates do not yet account for absorption of radiation by black carbon associated with cloud or the presence of pre-existing dust particles.

  17. Carbonaceous aerosols at a high altitude location in central Himalayas

    NASA Astrophysics Data System (ADS)

    Cong, Z.; Kang, S.; Cao, J.

    2011-12-01

    Atmospheric aerosols receive increasing attention due to their role in many atmospheric processes. Especially, the carbonaceous aerosols may result in global climate change through scattering/absorbing the solar radiation. In the Himalayan region, the carbonaceous aerosols at high elevations may act as the major reason causing the melting of snow packs and glaciers, posing negative effects on water resources of millions of people. Nevertheless, large uncertainties still exist to evaluate the impact of aerosols in this area, primarily due to the scarcity of adequate information on the aerosol properties. In the study, total suspended particle samples were collected weekly from Aug. 2009 to Jul. 2010 at the north slope of Mt. Qomolangma (Mt. Everest), the summit of the world. Organic carbon (OC) and elemental carbon (EC) were analyzed using the thermal/optical reflectance (TOR) method. EC varied from below detection to 1.12 μg m-3 with the average of 0.26 μg m-3, while OC ranged from 0.23 μg m-3 to 7.22 μg m-3 with the average of 1.58 μg m-3. The OC and EC concentrations at Mt. Qomolangma are generally comparable to other remote sites like McMurdo in Antarctica, representing a regional background. Finally the source region and the warming effect of the carbonaceous aerosols are discussed.

  18. Impact of aging mechanism on model simulated carbonaceous aerosols

    PubMed Central

    Huang, Y.; Wu, S.; Dubey, M.K.; French, N. H. F.

    2013-01-01

    Carbonaceous aerosols including organic carbon and black carbon have significant implications for both climate and air quality. In the current global climate or chemical transport models, a fixed hydrophobic-to-hydrophilic conversion lifetime for carbonaceous aerosol (τ) is generally assumed, which is usually around one day. We have implemented a new detailed aging scheme for carbonaceous aerosols in a chemical transport model (GEOS-Chem) to account for both the chemical oxidation and the physical condensation-coagulation effects, where τ is affected by local atmospheric environment including atmospheric concentrations of water vapor, ozone, hydroxyl radical and sulfuric acid. The updated τ exhibits large spatial and temporal variations with the global average (up to 11 km altitude) calculated to be 2.6 days. The chemical aging effects are found to be strongest over the tropical regions driven by the low ozone concentrations and high humidity there. The τ resulted from chemical aging generally decreases with altitude due to increases in ozone concentration and decreases in humidity. The condensation-coagulation effects are found to be most important for the high-latitude areas, in particular the polar regions, where the τ values are calculated to be up to 15 days. When both the chemical aging and condensation-coagulation effects are considered, the total atmospheric burdens and global average lifetimes of BC, black carbon, (OC, organic carbon) are calculated to increase by 9% (3%) compared to the control simulation, with considerable enhancements of BC and OC concentrations in the Southern Hemisphere. Model evaluations against data from multiple datasets show that the updated aging scheme improves model simulations of carbonaceous aerosols for some regions, especially for the remote areas in the Northern Hemisphere. The improvement helps explain the persistent low model bias for carbonaceous aerosols in the Northern Hemisphere reported in literature. Further

  19. Carbonaceous aerosols in an urban tunnel

    NASA Astrophysics Data System (ADS)

    Ancelet, Travis; Davy, Perry K.; Trompetter, William J.; Markwitz, Andreas; Weatherburn, David C.

    2011-08-01

    Particulate matter in the Mount Victoria Tunnel, an urban road tunnel 623 m in length with an average traffic volume of 2070-2300 vehicles per hour located in Wellington, New Zealand, was studied to gain an understanding of carbonaceous species emitted from motor vehicles. The average PM 2.5 concentration during peak hours in the tunnel was found to be 67.6 ± 19.4 μg m -3. Analysis of carbonaceous species present (OC, EC, TC) was performed by both the NIOSH and IMPROVE thermal/optical protocols and carbonaceous species were found to make up 63-73% of the total PM in the tunnel. Comparison of TC concentrations obtained from each protocol revealed that no significant difference was present between the two protocols. Black carbon (BC), also used as a measure of EC, was determined using light reflection and BC values did not differ significantly from EC concentrations determined using the NIOSH and IMPROVE protocols. TC was also determined using EA/IRMS and it was found that TC concentrations from EA/IRMS directly correlated with TC results obtained using the NIOSH protocol. Stable isotope analysis of the PM 2.5 yielded δ 13C values from -24.7 to -28.3‰, typical of motor vehicles. Analysis of particle-phase PAHs by thermal desorption GC/MS revealed an average total PAH concentration of 70.0 ± 4.1 ng m -3 and PAHs were found to contribute 0.10% of total PM 2.5 in the tunnel. PAH emissions in the tunnel were found to be enriched in low molecular weight PAHs, indicative of emissions from diesel-fueled vehicles. Analysis of individual particle composition and morphology revealed that most particles were carbonaceous species that formed large, amorphous agglomerates made up of smaller spherules.

  20. Observationally constrained estimates of carbonaceous aerosol radiative forcing.

    PubMed

    Chung, Chul E; Ramanathan, V; Decremer, Damien

    2012-07-17

    Carbonaceous aerosols (CA) emitted by fossil and biomass fuels consist of black carbon (BC), a strong absorber of solar radiation, and organic matter (OM). OM scatters as well as absorbs solar radiation. The absorbing component of OM, which is ignored in most climate models, is referred to as brown carbon (BrC). Model estimates of the global CA radiative forcing range from 0 to 0.7 Wm(-2), to be compared with the Intergovernmental Panel on Climate Change's estimate for the pre-Industrial to the present net radiative forcing of about 1.6 Wm(-2). This study provides a model-independent, observationally based estimate of the CA direct radiative forcing. Ground-based aerosol network data is integrated with field data and satellite-based aerosol observations to provide a decadal (2001 through 2009) global view of the CA optical properties and direct radiative forcing. The estimated global CA direct radiative effect is about 0.75 Wm(-2) (0.5 to 1.0). This study identifies the global importance of BrC, which is shown to contribute about 20% to 550-nm CA solar absorption globally. Because of the inclusion of BrC, the net effect of OM is close to zero and the CA forcing is nearly equal to that of BC. The CA direct radiative forcing is estimated to be about 0.65 (0.5 to about 0.8) Wm(-2), thus comparable to or exceeding that by methane. Caused in part by BrC absorption, CAs have a net warming effect even over open biomass-burning regions in Africa and the Amazon. PMID:22753522

  1. Artifact free denuder method for sampling of carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Mikuška, P.; Vecera, Z.; Broškovicová, A.

    2003-04-01

    Over the past decade, a growing attention has been focused on the carbonaceous aerosols. Although they may account for 30--60% of the total fine aerosol mass, their concentration and formation mechanisms are not well understood, particularly in comparison with major fine particle inorganic species. The deficiency in knowledge of carbonaceous aerosols results from their complexity and because of problems associated with their collection. Conventional sampling techniques of the carbonaceous aerosols, which utilize filters/backup adsorbents suffer from sampling artefacts. Positive artifacts are mainly due to adsorption of gas-phase organic compounds by the filter material or by the already collected particles, whereas negative artifacts arise from the volatilisation of already collected organic compounds from the filter. Furthermore, in the course of the sampling, the composition of the collected organic compounds may be modified by oxidants (O_3, NO_2, PAN, peroxides) that are present in the air passing through the sampler. It is clear that new, artifact free, method for sampling of carbonaceous aerosols is needed. A combination of a diffusion denuder and a filter in series is very promising in this respect. The denuder is expected to collect gaseous oxidants and gas-phase organic compounds from sample air stream prior to collection of aerosol particles on filters, and eliminate thus both positive and negative sampling artifacts for carbonaceous aerosols. This combination is subject of the presentation. Several designs of diffusion denuders (cylindrical, annular, parallel plate, multi-channel) in combination with various types of wall coatings (dry, liquid) were examined. Special attention was given to preservation of the long-term collection efficiency. Different adsorbents (activated charcoal, molecular sieve, porous polymers) and sorbents coated with various chemical reagents (KI, Na_2SO_3, MnO_2, ascorbic acid) or chromatographic stationary phases (silicon oils

  2. Origin of carbonaceous aerosols over the tropical Indian Ocean: Biomass burning or fossil fuels?

    SciTech Connect

    Novakov, T.; Andreae, M.O.; Gabriel, R.; Kirchstetter, T.; Mayol-Bracero, O.L.; Ramanathan, V.

    2000-08-26

    We present an analysis of the carbon, potassium and sulfate content of the extensive aerosol haze layer observed over the tropical Indian Ocean during the Indian Ocean Experiment (INDOEX). The black carbon (BC) content of the haze is as high as 17% of the total fine particle mass (the sum of carbonaceous and soluble ionic aerosol components) which results in significant solar absorption. The ratio of black carbon to organic carbon (OC) (over the Arabian Sea and equatorial Indian Ocean) was a factor of 5 to 10 times larger than expected for biomass burning. This ratio was closer to values measured downwind of industrialized regions in Japan and Western Europe. These results indicate that fossil fuel combustion is the major source of carbonaceous aerosols, including black carbon during the events considered. If the data set analyzed here is representative of the entire INDOEX study then fossil fuel emissions from South Asia must have similarly contributed to aerosols over the whole study region. The INDOEX ratios are substantially different from those reported f or some source regions of South Asia, thus raising the possibility that changes in composition of carbonaceous aerosol may occur during transport.

  3. An Overview of the 2010 Carbonaceous Aerosol and Radiative Effects Study (CARES) Field Campaign

    NASA Astrophysics Data System (ADS)

    Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.

    2010-12-01

    The primary objective of the DOE Carbonaceous Aerosol and Radiative Effects Study (CARES) in June 2010 was to investigate the evolution of carbonaceous aerosols of different types and their optical and hygroscopic properties in central California, with a focus on the Sacramento urban plume. Carbonaceous aerosol components, which include black carbon (BC), urban primary organic aerosols (POA), biomass burning aerosols, and secondary organic aerosols (SOA) from both urban and biogenic precursors, have been shown to play a major role in the direct and indirect radiative forcing of climate. However, significant knowledge gaps and uncertainties still exist in the process-level understanding of: 1) SOA formation, 2) BC mixing state evolution, and 3) the optical and hygroscopic properties of fresh and aged carbonaceous aerosols. The CARES 2010 field study was designed to address several specific science questions under these three topics. During summer the Sacramento-Blodgett Forest corridor effectively serves as a mesoscale daytime flow reactor in which the urban aerosols undergo significant aging as they are transported to the northeast by upslope flow. The CARES campaign observation strategy consisted of the DOE G-1 aircraft sampling upwind, within, and outside of the evolving Sacramento urban plume in the morning and again in the afternoon. The G-1 payload consisted of a suite of instruments to measure trace gases, aerosol size distribution, composition, and optical properties. The NASA B-200 aircraft carrying a High Spectral Resolution Lidar (HSRL) and a Research Scanning Polarimeter (RSP) was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties. The aircraft measurements were complemented by heavily-instrumented ground sites within the Sacramento urban area and at a downwind site in Cool, California, to characterize the diurnal evolution of meteorological variables, trace gases, aerosol precursors, aerosol

  4. Natural Radionuclides and Isotopic Signatures for Determining Carbonaceous Aerosol Sources, Aerosol Lifetimes, and Washout Processes

    SciTech Connect

    Gaffney, Jeffrey

    2012-12-12

    This is the final technical report. The project description is as follows: to determine the role of aerosol radiative forcing on climate, the processes that control their atmospheric concentrations must be understood, and aerosol sources need to be determined for mitigation. Measurements of naturally occurring radionuclides and stable isotopic signatures allow the sources, removal and transport processes, as well as atmospheric lifetimes of fine carbonaceous aerosols, to be evaluated.

  5. Characteristics and sources of carbonaceous aerosols from Shanghai, China

    NASA Astrophysics Data System (ADS)

    Cao, J.-J.; Zhu, C.-S.; Tie, X.-X.; Geng, F.-H.; Xu, H.-M.; Ho, S. S. H.; Wang, G.-H.; Han, Y.-M.; Ho, K.-F.

    2012-07-01

    An intensive investigation of carbonaceous PM2.5 and TSP from Pudong (China) was conducted as part of the MIRAGE-Shanghai Experiment in 2009. Data for organic and elemental carbon (OC and EC), organic species, including C17 to C40 n-alkanes and 17 polycyclic aromatic hydrocarbons (PAHs), and stable C isotopes OC (δ13COC) and EC (δ13CEC) were used to evaluate the aerosols' temporal variations and identify presumptive sources. High OC/EC ratios indicated a large fraction of secondary organic aerosol (SOA); high char/soot ratios indicated stronger contributions to EC from motor vehicles and coal combustion than biomass burning. Diagnostic ratios of PAHs indicated that much of the SOA was produced via coal combustion. Isotope abundances (δ13COC = -24.5 ± 0.8‰ and δ13CEC = -25.1 ± 0.6‰) indicated that fossil fuels were the most important source for carbonaceous PM2.5, with lesser impacts from biomass burning and natural sources. An EC tracer system and isotope mass balance calculations showed that the relative contributions to total carbon from coal combustion, motor vehicle exhaust, and SOA were 41%, 21%, and 31%: other primary sources such as marine, soil and biogenic emissions contributed 7%. Combined analyses of OC and EC, n-alkanes and PAHs, and stable carbon isotopes provide a new way to apportion the sources of carbonaceous particles.

  6. Encapsulation effects on carbonaceous aerosol light absorption

    SciTech Connect

    Sedlacek, A.J.; Onasch, T.; Davidovits, P.; Cross, E.; Mazzoleni, C.

    2010-03-15

    The contribution of aerosol absorption on direct radiative forcing is still an active area of research, in part, because aerosol extinction is dominated by light scattering and, in part, because the primary absorbing aerosol of interest, soot, exhibits complex aging behavior that alters its optical properties. The consequences of this can be evidenced by the work of Ramanathan and Carmichael (2008) who suggest that incorporating the atmospheric heating due to brown clouds (plumes containing soot byproducts from automobiles, biomass burning, wood-burning kitchen stoves, and coal-fired power plants) will increase black carbon (BC) radiative forcing from the Intergovernmental Panel on Climate Change best estimate of 0.34 Wm-2 (±0.25 Wm-2) (IPCC 2007) to 0.9 Wm-2. This noteworthy degree of uncertainty is due largely to the interdependence of BC optical properties on particle mixing state and aggregate morphology, each of which changes as the particle ages in the atmosphere and becomes encapsulated within a coating of inorganic and/or organic substances. In July 2008, a laboratory-based measurement campaign, led by Boston College and Aerodyne, was initiated to begin addressing this interdependence. To achieve insights into the interdependence of BC optical properties on particle mixing state and aggregate morphology, measurements of both the optical and physical properties of flame-generated soot under nascent, coated, and denuded conditions were conducted. This poster presents data on black carbon (BC) light absorption measured by Photothermal Interferometry (Sedlacek and Lee 2007). In addition to examining nascent BC—to provide a baseline measurement—encapsulation with varying thicknesses of either dioctyl sebacate (DOS) or sulfuric acid was conducted to glean insights into the interplay between particle mixing state and optical properties. Additionally, some experiments were carried out where BC was coated and then denuded. In the case of DOS-coated soot, a

  7. Carbonaceous Components in the Comet Halley Dust

    NASA Technical Reports Server (NTRS)

    Fomenkova, M. N.; Chang, S.; Mukhin, L. M.

    1994-01-01

    Cometary grains containing large amounts of carbon and/or organic matter (CHON) were discovered by in situ measurements of comet Halley dust composition during VEGA and GIOTTO flyby missions. In this paper, we report the classification of these cometary, grains by means of cluster analysis, discuss the resulting compositional groups, and compare them with substances observed or hypothesized in meteorites, interplanetary dust particles, and the interstellar medium. Grains dominated by carbon and/or organic matter (CHON grains) represent approx. 22% of the total population of measured cometary dust particles. They, usually contain a minor abundance of rock-forming elements as well. Grains having organic material are relatively more abundant in the vicinity of the nucleus than in the outer regions of the coma, which suggests decomposition of the organics in the coma environment. The majority of comet Halley organic particles are multicomponent mixtures of carbon phases and organic compounds. Possibly, the cometary CHON grains may be related to kerogen material of an interstellar origin in carbonaceous meteorites. Pure carbon grains, hydrocarbons and polymers of cyanopolyynes, and multi-carbon monoxides are present in cometary dust as compositionally simple and distinctive components among a variety of others. There is no clear evidence of significant presence of pure formaldehyde or HCN polymers in Halley dust particles. The diversity of types of cometary organic compounds is consistent with the inter-stellar dust model of comets and probably reflects differences in composition of precursor dust. Preservation of this heterogeneity among submicron particles suggest the gentle formation of cometary, nucleus by aggregation of interstellar dust in the protosolar nebula without complete mixing or chemical homogenization at the submicron level.

  8. Diurnal variations of carbonaceous components, major ions, and stable carbon and nitrogen isotope ratios in suburban aerosols from northern vicinity of Beijing

    NASA Astrophysics Data System (ADS)

    He, Nannan; Kawamura, Kimitaka; Kanaya, Yugo; Wang, Zifa

    2015-12-01

    We report diurnal variations of organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and major ions as well as stable carbon and nitrogen isotope ratios (δ13C and δ15N) in ambient aerosols at a suburban site (Mangshan), 40 km north of Beijing, China. We found that aerosol chemical compositions were largely controlled by the air mass transport from Beijing in daytime with southerly winds and by relatively fresh air mass in nighttime from the northern forest areas with northerly winds. Higher concentrations of aerosol mass and total carbon were obtained in daytime. Further, higher OC/EC ratios were recorded in daytime (4.0 ± 1.7) than nighttime (3.2 ± 0.7), suggesting that OC is formed by photochemical oxidation of gaseous precursors in daytime. Contributions of WSOC to OC were slightly higher in daytime (38%) than nighttime (34%), possibly due to secondary formation of WSOC in daytime. We also found higher concentrations of Ca2+ in daytime, which was originated from the construction dust in Beijing area and transported to the sampling site. δ13C ranged from -25.3 to -21.2‰ (ave. -23.5 ± 0.9‰) in daytime and -29.0 to -21.4‰ (-24.0 ± 1.5‰) in nighttime, suggesting that Mangshan aerosols were more influenced by fossil fuel combustion products in daytime and by terrestrial C3 plants in nighttime. This study suggests that daytime air mass delivery from megacity Beijing largely influence the air quality at the receptor site in the north together with photochemical processing of organic aerosols during the atmospheric transport, whereas the Mangshan site is covered with relatively clean air masses at night.

  9. Diurnal variations of carbonaceous components, major ions, and stable carbon and nitrogen isotope ratios in suburban aerosols from northern vicinity of Beijing

    NASA Astrophysics Data System (ADS)

    He, Nannan; Kawamura, Kimitaka; Kanaya, Yugo; Wang, Zifa

    2015-12-01

    We report diurnal variations of organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and major ions as well as stable carbon and nitrogen isotope ratios (δ13C and δ15N) in ambient aerosols at a suburban site (Mangshan), 40 km north of Beijing, China. We found that aerosol chemical compositions were largely controlled by the air mass transport from Beijing in daytime with southerly winds and by relatively fresh air mass in nighttime from the northern forest areas with northerly winds. Higher concentrations of aerosol mass and total carbon were obtained in daytime. Further, higher OC/EC ratios were recorded in daytime (4.0 ± 1.7) than nighttime (3.2 ± 0.7), suggesting that OC is formed by photochemical oxidation of gaseous precursors in daytime. Contributions of WSOC to OC were slightly higher in daytime (38%) than nighttime (34%), possibly due to secondary formation of WSOC in daytime. We also found higher concentrations of Ca2+ in daytime, which was originated from the construction dust in Beijing area and transported to the sampling site. δ13C ranged from -25.3 to -21.2‰ (ave. -23.5 ± 0.9‰) in daytime and -29.0 to -21.4‰ (-24.0 ± 1.5‰) in nighttime, suggesting that Mangshan aerosols were more influenced by fossil fuel combustion products in daytime and by terrestrial C3 plants in nighttime. This study suggests that daytime air mass delivery from megacity Beijing largely influence the air quality at the receptor site in the north together with photochemical processing of organic aerosols during the atmospheric transport, whereas the Mangshan site is covered with relatively clean air masses at night.

  10. CARES: Carbonaceous Aerosol and Radiative Effects Study Operations Plan

    SciTech Connect

    Zaveri, RA; Shaw, WJ; Cziczo, DJ

    2010-07-12

    The CARES field campaign is motivated by the scientific issues described in the CARES Science Plan. The primary objectives of this field campaign are to investigate the evolution and aging of carbonaceous aerosols and their climate-affecting properties in the urban plume of Sacramento, California, a mid-size, mid-latitude city that is located upwind of a biogenic volatile organic compound (VOC) emission region. Our basic observational strategy is to make comprehensive gas, aerosol, and meteorological measurements upwind, within, and downwind of the urban area with the DOE G-1 aircraft and at strategically located ground sites so as to study the evolution of urban aerosols as they age and mix with biogenic SOA precursors. The NASA B-200 aircraft, equipped with the High Spectral Resolution Lidar (HSRL), digital camera, and the Research Scanning Polarimeter (RSP), will be flown in coordination with the G-1 to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties, and to provide the vertical context for the G-1 and ground in situ measurements.

  11. Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem. Revision

    SciTech Connect

    Mazurek, M.A.; Cofer, W.R. III; Levine, J.S.

    1990-10-01

    The identity and ambient mass concentrations of radiatively important carbonaceous aerosols were measured for a boreal forest prescribed burn conducted in northern Ontario, CAN in August 1989. Nonsize-segregated airborne particles were collected for smoldering-fire and full-fire conditions using a helicopter sampling platform. Total carbon (TC), organic carbon (OC) and elemental carbon (EC) were measured. Smoke plume mass concentrations of the OC and EC particles were greatest for full-fire conditions and had ranges of 1.560 to 2.160 mg/m{sup {minus}1} (OC) and 0.120 to 0.160 mg/m{sup {minus}3} (EC) with OC:EC ratios of 10 to 18, respectively. Smoldering fire conditions showed smoke plume OC and EC levels of 0.570--1.030 mg/m{sup {minus}3} (OC) and 0.006--0.050 mg/m{sup {minus}3} (EC) and much higher ratios of OC:EC (21 to 95). These aerosol data indicate the formation of EC particles is greatest during full-fire combustion of boreal forest material relative to smoldering combustion. However, EC particles comprise a minor fraction of the particulate carbon smoke aerosols for both full-fire and smoldering conditions; the major component of carbonaceous smoke aerosols emitted during the prescribed burn is OC. Overall, the OC and EC in-plume smoke aerosol data show nonuniform production of these particles during various stages of the prescribed burn, and major differences in the type of carbonaceous aerosol that is generated (OC versus EC).

  12. Carbonaceous Aerosols and Radiative Effects Study (CARES), g1-aircraft, sedlacek sp2

    DOE Data Explorer

    Sedlacek, Art

    2011-08-30

    The primary objective of the Carbonaceous Aerosol and Radiative Effects Study (CARES) in 2010 was to investigate the evolution of carbonaceous aerosols of different types and their optical and hygroscopic properties in central California, with a focus on the Sacramento urban plume.

  13. Characteristics and sources of carbonaceous aerosols from Shanghai, China

    NASA Astrophysics Data System (ADS)

    Cao, J.-J.; Zhu, C.-S.; Tie, X.-X.; Geng, F.-H.; Xu, H.-M.; Ho, S. S. H.; Wang, G.-H.; Han, Y.-M.; Ho, K.-F.

    2013-01-01

    An intensive investigation of carbonaceous PM2.5 and TSP (total suspended particles) from Pudong (China) was conducted as part of the MIRAGE-Shanghai (Megacities Impact on Regional and Global Environment) experiment in 2009. Data for organic and elemental carbon (OC and EC), organic species, including C17 to C40 n-alkanes and 17 polycyclic aromatic hydrocarbons (PAHs), and stable carbon isotopes OC (δ13COC) and EC (δ13CEC) were used to evaluate the aerosols' temporal variations and identify presumptive sources. High OC/EC ratios indicated a large fraction of secondary organic aerosol (SOA); high char/soot ratios indicated stronger contributions to EC from motor vehicles and coal combustion than biomass burning. Diagnostic ratios of PAHs indicated that much of the SOA was produced via coal combustion. Isotope abundances (δ13COC = -24.5 ± 0.8‰ and δ13CEC = -25.1 ± 0.6‰) indicated that fossil fuels were the most important source for carbonaceous PM2.5 (particulate matter less than 2.5 micrometers in diameter), with lesser impacts from biomass burning and natural sources. An EC tracer system and isotope mass balance calculations showed that the relative contributions to total carbon from coal combustion, motor vehicle exhaust, and SOA were 41%, 21%, and 31%; other primary sources such as marine, soil and biogenic emissions contributed 7%. Combined analyses of OC and EC, n-alkanes and PAHs, and stable carbon isotopes provide a new way to apportion the sources of carbonaceous particles.

  14. Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

    SciTech Connect

    Davidovits, Paul

    2015-10-20

    Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a

  15. Observation of carbonaceous aerosols during 2006-2009 in Nyainqêntanglha Mountains and the implications for glaciers.

    PubMed

    Zhao, Shuyu; Ming, Jing; Sun, Junying; Xiao, Cunde

    2013-08-01

    Atmospheric carbonaceous aerosols were sampled discontinuously from July 2006 to December 2009 at Nam Co Comprehensive Observation and Research Station (NCOS) in the central Tibetan Plateau (TP). The mean daily concentration of carbonaceous aerosols increased from 268 to 330 ng m(-3), and pollution episodes could significantly increase the mean level of carbonaceous aerosols in the total mass concentration. Organic carbon was the main component of carbonaceous aerosols at NCOS, and black carbon (BC) accounted for 5.8 %. Seven-day air masses backward trajectories calculated by the Hybrid Single-Particle Lagrangian Integrated Trajectory model and the aerosol optical depth distribution in the TP and South Asia both suggested that atmospheric pollutants emitted from Northern India and South Asia could penetrate into central TP by southwest winds. Due to the seasonal variations of emission sources and regional atmospheric conditions, calculated BC deposition flux in the nonmonsoon season was higher than that in the monsoon season. Increased BC concentration in snowpack in winter from 2007 to 2009 indicated that the atmospheric environment in central TP became more polluted and the influences from human activities have strengthened. Pollution episodes could significantly increase BC concentrations in the snowpack on a seasonal scale, which would furthermore affect the surface albedo. PMID:23479337

  16. Source apportionment of carbonaceous aerosols over South and East Asia using dual carbon isotopes

    NASA Astrophysics Data System (ADS)

    Gustafsson, O.; Kirillova, E. N.; Andersson, A.-; Kruså, M.; Sheesley, R. J.; Tiwari, S.-; Lee, M.; Chen, B.; Du, K.

    2012-12-01

    Emissions of black carbon (BC) and other components of carbonaceous aerosols affect both climate and health in South and East Asia, yet substantial uncertainties exist regarding their sources. The relative contribution to atmospheric BC from fossil fuel versus biomass combustion is important to constrain both to direct mitigation and as their different properties make their effects on climate forcing and respiratory health different. This study approached the sourcing challenge by applying microscale radiocarbon measurements to aerosol particles collected in both source regions and at regional receptor observatories of both S Asia (New Delhi and the Maldives Climate Observatory) and of E Asia (Beijing, Shanghai, South China Coastal Observatory and the Korea Climate Observatory - Gosan, KCO-G, Jeju Island). The radiocarbon approach is ideally suited to this task as fossil sources are void of 14C whereas biomass combustion products hold a contemporary 14C signal. For S Asia, the 14C-based observations suggest that biomass combustion contributes half to two-thirds of the BC loading. In contrast, for E Asia, fossil fuel combustion account for four-fifths of the BC emitted from China. This source-diagnostic radiocarbon signal in the ambient aerosol over East Asia establishes a much larger role for fossil fuel combustion than suggested by all fifteen BC emission inventory models. There are also poor constraints on the sources of water-soluble organic carbon (WSOC), a large hydrophilic component of carbonaceous aerosols that enhances the propensity of aerosols to form clouds. In a 15-mo continuous campaign in S Asia, radiocarbon-based source apportionment of WSOC shows the dominance of biogenic/biomass combustion sources but also a substantial anthropogenic fossil-fuel contribution (about 20%). WSOC in E Asia reaching KCO-G were 50% from fossil sources. Aerosols reaching the Maldives after long-range over-ocean transport were enriched by 3-4‰ in δ13C-WSOC. This is

  17. Constraining Carbonaceous Aerosol Climate Forcing by Bridging Laboratory, Field and Modeling Studies

    NASA Astrophysics Data System (ADS)

    Dubey, M. K.; Aiken, A. C.; Liu, S.; Saleh, R.; Cappa, C. D.; Williams, L. R.; Donahue, N. M.; Gorkowski, K.; Ng, N. L.; Mazzoleni, C.; China, S.; Sharma, N.; Yokelson, R. J.; Allan, J. D.; Liu, D.

    2014-12-01

    Biomass and fossil fuel combustion emits black (BC) and brown carbon (BrC) aerosols that absorb sunlight to warm climate and organic carbon (OC) aerosols that scatter sunlight to cool climate. The net forcing depends strongly on the composition, mixing state and transformations of these carbonaceous aerosols. Complexities from large variability of fuel types, combustion conditions and aging processes have confounded their treatment in models. We analyse recent laboratory and field measurements to uncover fundamental mechanism that control the chemical, optical and microphysical properties of carbonaceous aerosols that are elaborated below: Wavelength dependence of absorption and the single scattering albedo (ω) of fresh biomass burning aerosols produced from many fuels during FLAME-4 was analysed to determine the factors that control the variability in ω. Results show that ω varies strongly with fire-integrated modified combustion efficiency (MCEFI)—higher MCEFI results in lower ω values and greater spectral dependence of ω (Liu et al GRL 2014). A parameterization of ω as a function of MCEFI for fresh BB aerosols is derived from the laboratory data and is evaluated by field data, including BBOP. Our laboratory studies also demonstrate that BrC production correlates with BC indicating that that they are produced by a common mechanism that is driven by MCEFI (Saleh et al NGeo 2014). We show that BrC absorption is concentrated in the extremely low volatility component that favours long-range transport. We observe substantial absorption enhancement for internally mixed BC from diesel and wood combustion near London during ClearFlo. While the absorption enhancement is due to BC particles coated by co-emitted OC in urban regions, it increases with photochemical age in rural areas and is simulated by core-shell models. We measure BrC absorption that is concentrated in the extremely low volatility components and attribute it to wood burning. Our results support

  18. Carbonaceous aerosol particles from common vegetation in the Grand Canyon

    SciTech Connect

    Hallock, K.A.; Mazurek, M.A. ); Cass, G.R. . Dept. of Environmental Engineering Science)

    1992-05-01

    The problem of visibility reduction in the Grand Canyon due to fine organic aerosol particles in the atmosphere has become an area of increased environmental concern. Aerosol particles can be derived from many emission sources. In this report, we focus on identifying organic aerosols derived from common vegetation in the Grand Canyon. These aerosols are expected to be significant contributors to the total atmospheric organic aerosol content. Aerosol samples from living vegetation were collected by resuspension of surface wax and resin components liberated from the leaves of vegetation common to areas of the Grand Canyon. The samples were analyzed using high-resolution gas chromatography/mass spectrometry (GC/MS). Probable identification of compounds was made by comparison of sample spectra with National Institute of Standards and Technology (NIST) mass spectral references and positive identification of compounds was made when possible by comparison with authentic standards as well as NIST references. Using these references, we have been able to positively identify the presence of n-alkane and n-alkanoic acid homolog series in the surface waxes of the vegetation sampled. Several monoterpenes, sesquiterpenes, and diterpenes were identified also as possible biogenic aerosols which may contribute to the total organic aerosol abundance leading to visibility reduction in the Grand Canyon.

  19. A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects

    NASA Technical Reports Server (NTRS)

    Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

    2010-01-01

    Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

  20. Impact of carbonaceous aerosol emissions on regional climate change

    NASA Astrophysics Data System (ADS)

    Roeckner, E.; Stier, P.; Feichter, J.; Kloster, S.; Esch, M.; Fischer-Bruns, I.

    2006-11-01

    The past and future evolution of atmospheric composition and climate has been simulated with a version of the Max Planck Institute Earth System Model (MPI-ESM). The system consists of the atmosphere, including a detailed representation of tropospheric aerosols, the land surface, and the ocean, including a model of the marine biogeochemistry which interacts with the atmosphere via the dust and sulfur cycles. In addition to the prescribed concentrations of carbon dioxide, ozone and other greenhouse gases, the model is driven by natural forcings (solar irradiance and volcanic aerosol), and by emissions of mineral dust, sea salt, sulfur, black carbon (BC) and particulate organic matter (POM). Transient climate simulations were performed for the twentieth century and extended into the twenty-first century, according to SRES scenario A1B, with two different assumptions on future emissions of carbonaceous aerosols (BC, POM). In the first experiment, BC and POM emissions decrease over Europe and China but increase at lower latitudes (central and South America, Africa, Middle East, India, Southeast Asia). In the second experiment, the BC and POM emissions are frozen at their levels of year 2000. According to these experiments the impact of projected changes in carbonaceaous aerosols on the global mean temperature is negligible, but significant changes are found at low latitudes. This includes a cooling of the surface, enhanced precipitation and runoff, and a wetter surface. These regional changes in surface climate are caused primarily by the atmospheric absorption of sunlight by increasing BC levels and, subsequently, by thermally driven circulations which favour the transport of moisture from the adjacent oceans. The vertical redistribution of solar energy is particularly large during the dry season in central Africa when the anomalous atmospheric heating of up to 60 W m-2 and a corresponding decrease in surface solar radiation leads to a marked surface cooling, reduced

  1. Carbonaceous aerosol and its characteristics observed in Tokyo and south Kanto region

    NASA Astrophysics Data System (ADS)

    Minoura, Hiroaki; Morikawa, Tazuko; Mizohata, Akira; Sakamoto, Kazuhiko

    2012-12-01

    Due to enforcing vehicle emission reduction requirements in Japan, particulate matter (PM) concentration, especially elemental carbon (EC) concentration in roadside atmosphere, obviously decreased in the last decade. In spite of the previous vehicle emission reduction, EC concentration was not shown a clear decrease, recently. To achieve the PM2.5 environmental standard, measurements based on emission source contribution are desirable. However, source apportionment of carbonaceous aerosol was ambiguous because chemical components are complicated, and the components change through photochemical reaction. The goal of this study is to determine source apportionment for carbonaceous aerosols. Examination of PM2.5 was performed in south Kanto including Tokyo in the summer of 2008 and the winter of 2009. Emissions from the industrial area around Tokyo Bay and the agricultural northern area showed transportation and accumulation due to the seasonal prevailing wind. The emissions formed a geographical distribution due to photochemical reactions. The characteristics of carbonaceous aerosol were obtained using carbon profile analysis and carbon isotope analysis, including the source information such as fossil fuel emission origin, vegetation origin, and combustion product, photochemical reaction product, etc. Soot-EC was found as a substance with fossil fuel origin which did not contain biomass combustion matter, and since it is stable, there was no observed difference by site and a uniform concentration was observed in winter. It became apparent from the carbon isotope analysis using 14C that the carbon from the biomass origin involved 29% in total carbon in the summer, and 48% in winter even at Kudan of central Tokyo.

  2. Carbonaceous aerosols in megacity Xi'an, China: Implications of thermal/optical protocols comparison

    NASA Astrophysics Data System (ADS)

    Han, Y. M.; Chen, L.-W. A.; Huang, R.-J.; Chow, J. C.; Watson, J. G.; Ni, H. Y.; Liu, S. X.; Fung, K. K.; Shen, Z. X.; Wei, C.; Wang, Q. Y.; Tian, J.; Zhao, Z. Z.; Prévôt, André S. H.; Cao, J. J.

    2016-05-01

    Carbonaceous aerosol is an important component that influences the environment, climate, and human health. Organic and elemental carbon (OC and EC) are the two main constituents of carbonaceous aerosols that have opposite, i.e., cooling versus warming, effects on the Earth's radiation balance. Knowledge on the variability of OC/EC splits measured by different thermal/optical protocols is useful for understanding the uncertainty in the climate models. This study shows good correlations within OC or EC (r2 > 0.83, P < 0.001) across the IMPROVE, IMPROVE_A, and EUSAAR_2 protocols for both ambient aerosol samples and biomass burning samples. However, EC concentrations differ by more than two folds, and OC/EC ratios differ up to a factor of 2.7. The discrepancies were attributed to the selection between the reflectance and transmittance corrections and the different peak inert-atmosphere temperature. The IMPROVE and IMPROVE_A protocols also quantified different char and soot concentrations, two subtypes of EC with distinct chemical and optical properties. Char, but not soot, was found to correlate with the humic-like substances (HULIS) content in the samples, suggesting that both char and HULIS originate mainly from biomass burning. A one-year (2012-2013) ambient aerosol monitoring in Xi'an, China, shows that OC, EC, and char displayed winter highs and summer lows, while soot had no seasonal trend. The char/soot ratios showed a "single peak" in winter, while OC/EC ratios exhibited "dual peak" feature due to the influence of secondary organic aerosol formation. In addition to commonly measured OC and EC, we recommend both char and soot from a common reference method to be considered in the chemical transport and climate models.

  3. Carbonaceous aerosols in megacity Xi'an, China: Implications of thermal/optical protocols comparison

    NASA Astrophysics Data System (ADS)

    Han, Y. M.; Chen, L.-W. A.; Huang, R.-J.; Chow, J. C.; Watson, J. G.; Ni, H. Y.; Liu, S. X.; Fung, K. K.; Shen, Z. X.; Wei, C.; Wang, Q. Y.; Tian, J.; Zhao, Z. Z.; Prévôt, André S. H.; Cao, J. J.

    2016-05-01

    Carbonaceous aerosol is an important component that influences the environment, climate, and human health. Organic and elemental carbon (OC and EC) are the two main constituents of carbonaceous aerosols that have opposite, i.e., cooling versus warming, effects on the Earth's radiation balance. Knowledge on the variability of OC/EC splits measured by different thermal/optical protocols is useful for understanding the uncertainty in the climate models. This study shows good correlations within OC or EC (r2 > 0.83, P < 0.001) across the IMPROVE, IMPROVE_A, and EUSAAR_2 protocols for both ambient aerosol samples and biomass burning samples. However, EC concentrations differ by more than two folds, and OC/EC ratios differ up to a factor of 2.7. The discrepancies were attributed to the selection between the reflectance and transmittance corrections and the different peak inert-atmosphere temperature. The IMPROVE and IMPROVE_A protocols also quantified different char and soot concentrations, two subtypes of EC with distinct chemical and optical properties. Char, but not soot, was found to correlate with the humic-like substances (HULIS) content in the samples, suggesting that both char and HULIS originate mainly from biomass burning. A one-year (2012-2013) ambient aerosol monitoring in Xi'an, China, shows that OC, EC, and char displayed winter highs and summer lows, while soot had no seasonal trend. The char/soot ratios showed a "single peak" in winter, while OC/EC ratios exhibited "dual peak" feature due to the influence of secondary organic aerosol formation. In addition to commonly measured OC and EC, we recommend both char and soot from a common reference method to be considered in the chemical transport and climate models.

  4. Carbonaceous aerosol tracers in ice-cores record multi-decadal climate oscillations

    PubMed Central

    Seki, Osamu; Kawamura, Kimitaka; Bendle, James A. P.; Izawa, Yusuke; Suzuki, Ikuko; Shiraiwa, Takayuki; Fujii, Yoshiyuki

    2015-01-01

    Carbonaceous aerosols influence the climate via direct and indirect effects on radiative balance. However, the factors controlling the emissions, transport and role of carbonaceous aerosols in the climate system are highly uncertain. Here we investigate organic tracers in ice cores from Greenland and Kamchatka and find that, throughout the period covered by the records (1550 to 2000 CE), the concentrations and composition of biomass burning-, soil bacterial- and plant wax- tracers correspond to Arctic and regional temperatures as well as the warm season Arctic Oscillation (AO) over multi-decadal time-scales. Specifically, order of magnitude decreases (increases) in abundances of ice-core organic tracers, likely representing significant decreases (increases) in the atmospheric loading of carbonaceous aerosols, occur during colder (warmer) phases in the high latitudinal Northern Hemisphere. This raises questions about causality and possible carbonaceous aerosol feedback mechanisms. Our work opens new avenues for ice core research. Translating concentrations of organic tracers (μg/kg-ice or TOC) from ice-cores, into estimates of the atmospheric loading of carbonaceous aerosols (μg/m3) combined with new model constraints on the strength and sign of climate forcing by carbonaceous aerosols should be a priority for future research. PMID:26411576

  5. Spatial and seasonal variability of carbonaceous aerosol across Italy

    NASA Astrophysics Data System (ADS)

    Sandrini, Silvia; Fuzzi, Sandro; Piazzalunga, Andrea; Prati, Paolo; Bonasoni, Paolo; Cavalli, Fabrizia; Bove, Maria Chiara; Calvello, Mariarosaria; Cappelletti, David; Colombi, Cristina; Contini, Daniele; de Gennaro, Gianluigi; Di Gilio, Alessia; Fermo, Paola; Ferrero, Luca; Gianelle, Vorne; Giugliano, Michele; Ielpo, Pierina; Lonati, Giovanni; Marinoni, Angela; Massabò, Dario; Molteni, Ugo; Moroni, Beatrice; Pavese, Giulia; Perrino, Cinzia; Perrone, Maria Grazia; Perrone, Maria Rita; Putaud, Jean-Philippe; Sargolini, Tiziana; Vecchi, Roberta; Gilardoni, Stefania

    2014-12-01

    This paper analyses elemental (EC), organic (OC) and total carbon (TC) concentration in PM2.5 and PM10 samples collected over the last few years within several national and European projects at 37 remote, rural, urban, and traffic sites across the Italian peninsula. The purpose of the study is to obtain a picture of the spatial and seasonal variability of these aerosol species in Italy, and an insight into sources, processes and effects of meteorological conditions. OC and EC showed winter maxima and summer minima at urban and rural locations and an opposite behaviour at remote high altitude sites, where they increase during the warm period due to the rising of the Planetary Boundary Layer (PBL). The seasonal averages of OC are higher during winter compared to summer at the rural sites in the Po Valley (from 1.4 to 3.5 times), opposite to what usually occurs at rural locations, where OC increases during the warm period. This denotes the marked influence of urban areas on the surrounding rural environment in this densely populated region. The different types of sites exhibit marked differences in the average concentrations of carbonaceous aerosol and OC/EC ratio. This ratio is less sensitive to atmospheric processing than OC and EC concentrations, and hence more representative of different source types. Remote locations are characterised by the lowest levels of OC and especially EC, with OC/EC ratios ranging from 13 to 20, while the maximum OC and EC concentrations are observed at road-traffic influenced urban sites, where the OC/EC ratio ranges between 1 and 3. The highest urban impacts of OC and EC relative to remote and rural background sites occur in the Po Valley, especially in the city of Milan, which has the highest concentrations of PM and TC and low values of the OC/EC ratio.

  6. Estimating the Radiative Forcing of Carbonaceous Aerosols over California based on Satellite and Ground Observations

    SciTech Connect

    Xu, Yangyang; Bahadur, R.; Zhao, Chun; Leung, Lai-Yung R.

    2013-10-04

    Carbonaceous aerosols have the potential to impact climate both through directly absorbing incoming solar radiation, and by indirectly affecting the cloud layer. To quantify this impact recent modeling studies have made great efforts to simulate both the spatial and temporal distribution of carbonaceous aerosols and their associated radiative forcing. This study makes the first observationally constrained assessment of the direct radiative forcing of carbonaceous aerosols at a regional scale over California. By exploiting multiple observations (including ground sites and satellites), we constructed the distribution of aerosol optical depths and aerosol absorption optical depths over California for a ten-year period (2000-2010). The total solar absorption was then partitioned into contributions from elemental carbon (EC), organic carbon (OC) and dust aerosols using a newly developed scheme. Aerosol absorption optical depth due to carbonaceous aerosols (EC and OC) at 440 nm is 50%-200% larger than natural dust, with EC contributing the bulk (70%-90%). Observationally constrained EC absorption agrees reasonably well with estimates from regional transport models, but the model underestimates the OC AAOD by at least 50%. We estimate that the TOA warming from carbonaceous aerosols is 0.7 W/m2 and the TOA forcing due to OC is close to zero. The atmospheric heating of carbonaceous aerosols is 2.2-2.9 W/m2, of which EC contributed about 80-90%. The atmospheric heating due to OC is estimated to be 0.1 to 0.4 W/m2, larger than model simulations. The surface brightening due to EC reduction over the last two decades is estimated to be 1.5-3.5 W/m2.

  7. [Study on pollution characteristics of carbonaceous aerosols in Xi'an City during the spring festival].

    PubMed

    Zhou, Bian-Hong; Zhang, Cheng-Zhong; Wang, Ge-Hui

    2013-02-01

    The samples of PM2.5 with 8 times periods were collected using Automated Cartridge Collection Unit (ACCU) of Rupprecht& Patashnick (R&P)Corporation, and monitored by R&P1400a instrument of TEOM series online during 2011 Spring Festival in Xi'an city. The organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and water-insoluble organic carbon (WIOC) contents of 3 h integrated PM2.5 were analyzed to evaluate the influence of firework display on the carbonaceous components in urban air. The mass concentration of PM2.5 was found increased significantly from 00:00 A. M. to 02:59 A. M. at the Chinese Lunar New Year's Eve than the non-firework periods, reaching 1514.8 microg.m-3 at 01:00 A. M. The mass concentrations of OC, EC, WSOC, and WIOC during the same time period were 123.3 microg.m-3, 18.6 microg.m-3, 66.7 microg.m-3, and 56.6 microg.m-3, about 1.7, 1.2, 1.4, and 2.2 times higher than the average in normal days, respectively. Correlation analysis among WSOC, OC, and EC contents in PM25 showed that firework emission was an obvious source of carbonaceous aerosol in the Spring Festival vacation. However, it only contributes to 9. 4% for aerosol in fireworks emission. PMID:23668108

  8. Climate implications of carbonaceous aerosols: An aerosol microphysical study using the GISS/MATRIX climate model

    SciTech Connect

    Bauer, Susanne E.; Menon, Surabi; Koch, Dorothy; Bond, Tami; Tsigaridis, Kostas

    2010-04-09

    Recently, attention has been drawn towards black carbon aerosols as a likely short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and its climate interactions. Black carbon is directly released as particle into the atmosphere, but then interacts with other gases and particles through condensation and coagulation processes leading to further aerosol growth, aging and internal mixing. A detailed aerosol microphysical scheme, MATRIX, embedded within the global GISS modelE includes the above processes that determine the lifecycle and climate impact of aerosols. This study presents a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing change is -0.56 W/m{sup 2} between 1750 and 2000. However, the direct and indirect aerosol effects are very sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing change can vary between -0.32 to -0.75 W/m{sup 2} depending on these carbonaceous particle properties. Assuming that sulfates, nitrates and secondary organics form a coating shell around a black carbon core, rather than forming a uniformly mixed particles, changes the overall net radiative forcing from a negative to a positive number. Black carbon mitigation scenarios showed generally a benefit when mainly black carbon sources such as diesel emissions are reduced, reducing organic and black carbon sources such as bio-fuels, does not lead to reduced warming.

  9. Volcanic influence on background sulfurous and carbonaceous aerosol in the Lowermost Stratosphere

    NASA Astrophysics Data System (ADS)

    Friberg, J.; Martinsson, B. G.; Andersson, S. M.; Brenninkmeijer, C. A. M.; Hermann, M.; van Velthoven, P. F. J.; Zahn, A.

    2012-04-01

    Previous measurements in the upper troposphere (UT) and the lowermost stratosphere (LS) have indicated the presence of a carbonaceous component in the aerosol (Murphy et al.,1998; Nguyen et al., 2008; Martinsson et al., 2009). Here the occurrence of carbonaceous and sulfurous particles around the tropopause is investigated. The data were taken from the CARIBIC (Civil Aircraft for Regular Investigation of the atmosphere Based on an Instrument Container) platform, where instruments onboard a Lufthansa passenger aircraft on inter-continental flights are used for examination of the atmospheric composition in the UT/LS at 8-12 km altitude (Brenninkmeijer et al., 2007). CARIBIC undertakes aerosol sampling for chemical characterization, as well as measurements of particle number concentrations and mixing ratios of a large number of trace gases including O3, CO, NO/NOy, Hg, water (gaseous and condensed), greenhouse gases and halogenated hydrocarbons. The CARIBIC dataset also contains data on meteorological conditions. 500 aerosol samples were collected during 150 flights with a sampling time of 100 minutes by an impaction technique (Nguyen et al., 2006). Specimen are then analyzed by quantitative multi-elemental analysis by PIXE (Particle-Induced X-ray Emission) and PESA (Particle Elastic Scattering Analysis) to obtain elemental concentrations for sulfur, iron, titanium, potassium, hydrogen, carbon, nitrogen and oxygen among others (Nguyen and Martinsson, 2007). The present study is based on samples collected in the LS from May 2005- August 2008. Concentrations of particulate carbon and sulfur in the LS is shown to follow seasonal cycles, correlated with ozone concentrations, with increasing concentrations from the tropopause through the LS. This indicates downward transport from the so-called stratospheric over-world (SOV) as an important source for these species. Sulfuric acid particles are formed in the stratosphere from carbonyl sulfide (OCS) via photochemical

  10. Characteristics of atmospheric depositions of ionic and carbonaceous components at remote sites in Japan

    NASA Astrophysics Data System (ADS)

    Sato, K.; Inomata, Y.; Kajino, M.; Tang, N.; Hayakawa, K.; Hakamata, M.; Morisaki, H.

    2015-12-01

    Atmospheric deposition process is important to evaluate lifetimes and budget of atmospheric components. Deposition amounts of sulfur and nitrogen compounds have been evaluated not only in East Asian region but also worldwide. On the other hand, atmospheric deposition of carbonaceous components including organic carbon (OC), elementary carbon (EC) and Polycyclic Aromatic Hydrocarbons (PAHs) were monitored only at a few sites in Europe, North America and Africa, which will obscure removal process and atmospheric concentration distribution of those components. In this study, ionic and carbonaceous components in precipitation and aerosol are monitored at remote sites in Japan, and the characteristics of atmospheric deposition amounts were evaluated.Field observations have been implemented at the Noto station since November 2013 and the Sado station since May 2011. Wet deposition samples were collected by rain samplers, and dry deposition samples were collected by high volume or low volume aerosol samplers. Concentrations of Cl-, NO3-, SO42-, NH4+, Na+, K+, Mg2+, Ca2+ were measured by ion chromatography, EC and OC by the IMPROVE protocol, and PAHs by HPLC with a fluorescence detector. Wet deposition amounts were calculated as the products of aqueous concentration and precipitation amounts, and dry deposition amounts were as the products of aerosol concentrations and deposition velocity estimated by the Inferential Method.Total (wet and dry) annual deposition amounts of carbonaceous components of NO3-, SO42-, EC, water insoluble OC, Fluoranthene at Noto (Nov. 2013 to Oct. 2014) were 4353.81 mg/m2, 7020.50 mg/m2, 149.84 mg/m2, 1191.09 mg/m2, 28.6 μg/m2, respectively. These amounts are comparable total annual deposition amounts of OC and EC at Sado (May 2011 to Feb. 2012), which were 166.04 mg/m2 and 834.0 mg/m2. Higher deposition amounts of ionic and carbonaceous components were observed, which would be attributable to long range transportation of the East Asian

  11. Inorganic Components of Atmospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Wexler, Anthony Stein

    The inorganic components comprise 15% to 50% of the mass of atmospheric aerosols. For about the past 10 years the mass of these components was predicted assuming thermodynamic equilibrium between the volatile aerosol -phase inorganic species NH_4NO _3 and NH_4Cl and their gas-phase counterparts NH_3, HNO_3, and HCl. In this thesis I examine this assumption and prove that (1) the time scales for equilibration between the gas and aerosol phases are often too long for equilibrium to hold, and (2) even when equilibrium holds, transport considerations often govern the size distribution of these aerosol components. Water can comprise a significant portion of atmospheric aerosols under conditions of high relative humidity, whereas under conditions of sufficiently low relative humidity atmospheric aerosols tend to be dry. The deliquescence point is the relative humidity where the aerosol goes from a solid dry phase to an aqueous or mixed solid-aqueous phase. In this thesis I derive the temperature dependence of the deliquescence point and prove that in multicomponent solutions the deliquescence point is lower than for corresponding single component solutions. These theories of the transport, thermodynamic, and deliquescent properties of atmospheric aerosols are integrated into an aerosol inorganics model, AIM. The predictions of AIM compare well to fundamental thermodynamic measurements. Comparison of the prediction of AIM to those of other aerosol equilibrium models shows substantial disagreement in the predicted water content at lower relative humidities. The disagreement is due the improved treatment in AIM of the deliquescence properties of multicomponent solutions. In the summer and fall of 1987 the California Air Resources Board conducted the Southern California Air Quality Study, SCAQS, during which atmospheric aerosols were measured in Los Angeles. The size and composition of the aerosol and the concentrations of their gas phase counterparts were measured. When the

  12. Spectro-Microscopic Measurements of Carbonaceous Aerosol Aging in Central California

    SciTech Connect

    Moffet, Ryan C.; Rodel, Tobias; Kelly, Stephen T.; Yu, Xiao-Ying; Carroll, Gregory; Fast, Jerome D.; Zaveri, Rahul A.; Laskin, Alexander; Gilles, Mary K.

    2013-10-29

    Carbonaceous aerosols are responsible for large uncertainties in climate models, degraded visibility, and adverse health effects. The Carbonaceous Aerosols and Radiative Effects Study (CARES) was designed to study carbonaceous aerosols in the natural environment of Central Valley, California, and learn more about their atmospheric formation and aging. This paper presents results from spectro-microscopic measurements of carbonaceous particles collected during CARES at the time of pollution accumulation event (June 27-29, 2010), when in situ measurements indicated an increase in the organic carbon content of aerosols as the Sacramento urban plume aged. Computer controlled scanning electron microscopy coupled with an energy dispersive X-ray detector (CCSEM/EDX) and scanning transmission X-ray microscopy coupled with near edge X-ray absorption spectroscopy (STXM/NEXAFS) were used to probe the chemical composition and morphology of individual particles. It was found that the mass of organic carbon on individual particles increased through condensation of secondary organic aerosol. STXM/NEXAFS indicated that the number fraction of homogenous organic particles lacking inorganic inclusions (greater than ~50 nm diameter) increased with plume age as did the organic mass per particle. Comparison of the CARES spectro-microscopic data set with a similar dataset obtained in Mexico City during the MILAGRO campaign showed that individual particles in Mexico City contained twice as much carbon as those sampled during CARES. The number fraction of soot particles at the Mexico City urban site (30%) was larger than at the CARES urban site (10%) and the most aged samples from CARES contained less carbon-carbon double bonds. Differences between carbonaceous particles in Mexico City and California result from different sources, photochemical conditions, gas phase reactants, and secondary organic aerosol precursors. The detailed results provided by these spectro-microscopic measurements

  13. Significant influence of fungi on coarse carbonaceous and potassium aerosols in a tropical rainforest

    NASA Astrophysics Data System (ADS)

    Zhang, Zhisheng; Engling, Guenter; Zhang, Leiming; Kawamura, Kimitaka; Yang, Yihong; Tao, Jun; Zhang, Renjian; Chan, Chuen-yu; Li, Yide

    2015-03-01

    Fungal spores are ubiquitous in the Earth’s atmosphere, especially in the environment of tropical rainforests with intense biological activities. To assess the impact of fungi on chemical components of atmospheric aerosols at a Chinese tropical rainforest site, size-segregated fungal spore tracers (i.e. arabitol and mannitol) were measured along with major aerosol components, including carbonaceous species and water-soluble inorganic ions. The fungal spore tracers were found to be predominately associated with coarse particles, in which organic carbon (OC) and potassium (K+) were also present at significant levels. Enhanced amounts of fungal spore tracers were closely linked to rainfall events. Moreover, fungal spore tracers exhibited positive correlations with relative humidity and negative correlations with wind speed, temperature or radiation. The relationships between fungal spore tracers and meteorological factors are consistent with the emission features of actively discharged fungal spores, which are generally associated with sugar alcohols and by-products such as the inorganic ion K+. The excellent correlations between fungal spore tracers and OC or K+ in the coarse particles further suggested their common emission sources. Absolute principal factor analysis further identified fungi as the largest contributor to coarse OC and K+ (both at ∼66%) in this rainforest.

  14. Atmospheric carbonaceous aerosols from Indo-Gangetic Plain and Central Himalaya: impact of anthropogenic sources.

    PubMed

    Ram, Kirpa; Sarin, M M

    2015-01-15

    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 SO4(2-), 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. PMID:25199599

  15. Carbonaceous Aerosols Emitted from Light-Duty Vehicles Operating on Gasoline and Ethanol Fuel Blends

    EPA Science Inventory

    This study examines the chemical properties of carbonaceous aerosols emitted from three light-duty gasoline vehicles (LDVs) operating on gasoline (e0) and ethanol-gasoline fuel blends (e10 and e85). Vehicle road load simulations were performed on a chassis dynamometer using the t...

  16. SOURCE APPORTIONMENT OF PRIMARY AND SECONDARY CARBONACEOUS AEROSOL IN THE UNITED STATES USING MODELS AND MEASUREMENTS

    EPA Science Inventory

    In this presentation, three diagnostic evaluation methods of model performance for carbonaceous aerosol are reviewed. The EC-tracer method is used to distinguish primary and secondary carbon, radiocarbon data are used to distinguish fossil-fuel and contemporary carbon, and organ...

  17. Sources of excess urban carbonaceous aerosol in the Pearl River delta region, China

    EPA Science Inventory

    Carbonaceous aerosol is one of the important constituents of fine particulate matter (PM2.5) in Southern China, including the Pearl River Delta (PRD) region and Hong Kong (HK). During the study period (October and December of 2002, and March and June of 2003), the monthly average...

  18. Seasonal variation of urban carbonaceous aerosols in a typical city Nanjing in Yangtze River Delta, China

    NASA Astrophysics Data System (ADS)

    Li, Bing; Zhang, Jie; Zhao, Yu; Yuan, Siyu; Zhao, Qiuyue; Shen, Guofeng; Wu, Haisuo

    2015-04-01

    The Yangtze River Delta (YRD) is one of the regions with the most dynamic economy and severe atmospheric pollution in China. In order to characterize the particle features, especially the carbonaceous component in the YRD, particulate matter smaller than 2.5 μm (PM2.5) and 10 μm (PM10) samples in each season were collected in urban Nanjing, a typical city that locates in the west part of the YRD. The organic carbon (OC) and elemental carbon (EC) was differentiated using the thermal optical reflectance method. The average concentrations of PM2.5, OC and EC during the study periods were observed to be 117.6, 13.8, and 5.3 μg/m3 respectively, with all the highest levels in winter. The mass fraction of the Total carbonaceous aerosol (TCA) in PM2.5 was estimated at 23% on average, lower than those reported for other cities in the YRD. The OC and EC correlated well in all the seasons, especially in spring and winter, implying that OC and EC were attributed to common emission sources. Good correlation was observed between OC and estimated K+ from biomass burning in the harvest season in autumn and summer, indicating biomass burning a significant source of carbonaceous aerosols. This could also be confirmed by the lower fraction of OC3 + OC4 in OC during autumn and summer. The secondary organic carbon (SOC) estimated by EC-tracer method was the highest in winter (7.3 μg/m3) followed by autumn (6.7 μg/m3), summer (3.7 μg/m3) and spring (2.0 μg/m3). However, the SOC/OC in winter was not as high as that in summer and autumn, implying the high concentration of OC in winter was probably due to the stable weather but not mainly caused by SOC formation. The high SOC/OC ratio in summer was attributed to stronger oxidation, which could be suggested by higher sulfur oxidation ratio (SOR).

  19. Carbonaceous Aerosols in Fine Particulate Matter of Santiago Metropolitan Area, Chile

    PubMed Central

    Toro Araya, Richard; Flocchini, Robert; Morales Segura, Rául G. E.; Leiva Guzmán, Manuel A.

    2014-01-01

    Measurements of carbonaceous aerosols in South American cities are limited, and most existing data are of short term and limited to only a few locations. For 6 years (2002–2007), concentrations of fine particulate matter and organic and elemental carbon were measured continuously in the capital of Chile. The contribution of carbonaceous aerosols to the primary and secondary fractions was estimated at three different sampling sites and in the warm and cool seasons. The results demonstrate that there are significant differences in the levels in both the cold (March to August) and warm (September to February) seasons at all sites studied. The percent contribution of total carbonaceous aerosol fine particulate matter was greater in the cool season (53 ± 41%) than in the warm season (44 ± 18%). On average, the secondary organic carbon in the city corresponded to 29% of the total organic carbon. In cold periods, this proportion may reach an average of 38%. A comparison of the results with the air quality standards for fine particulate matter indicates that the total carbonaceous fraction alone exceeds the World Health Organization standard (10 µg/m3) and the United States Environmental Protection Agency standard (15 µg/m3) for fine particulate matter. PMID:24587753

  20. Primary carbonaceous aerosols and climate modeling: Classifications, global emission inventories, and observations

    NASA Astrophysics Data System (ADS)

    Sun, H.; Bond, T.

    2004-12-01

    Carbonaceous aerosols, including black carbon (BC) and organic carbon (OC), make up a large fraction of the atmospheric aerosols and affect the radiative balance of the earth either by directly scattering and absorbing solar radiation or through indirect influence on cloud optical properties and cloud lifetimes. The major sources of BC and OC emissions are from combustion processes, mainly.fossil-fuel burning, biofuels burning, and open biomass burning. OC is nearly always emitted with BC. Because different combustion practices contribute to the emission of BC and OC to the atmosphere, the magnitude and characteristics of carbonaceous aerosols vary between regions. Since OC mainly scatters light and BC absorbs it, it is possible that OC can oppose the warming effect of BC, so that the net climatic effect of carbonaceous aerosols is not known. There is presently disagreement on whether carbonaceous aerosols produce a net warming or cooling effect on climate. Some differences in model prediction may result from model differences, such as dynamics and treatment of cloud feedbacks. However, large differences also result from initial assumptions about the properties of BC and OC: optical properties, size distribution, and interaction with water. Although there are hundreds of different organic species in atmospheric aerosols, with widely varying properties, global climate models to date have treated organics as one ¡°compound.¡± In addition, emissions of OC are often derived by multiplying BC emissions by a constant factor, so that the balance between these different compounds is assumed. Addressing these critical model assumptions is a necessary step toward estimating the net climatic impact of carbonaceous aerosols, and different human activities. We aim to contribute to this effort by tabulating important climate-relevant properties of both emissions and ambient measurements. Since one single organic ¡°compound¡± is not sufficient to represent all the

  1. Carbonaceous aerosols observed at Ieodo Ocean Research Station and implication for the role of secondary aerosols in fog formation

    NASA Astrophysics Data System (ADS)

    Han, J.; Shin, B.; Hwang, G.; Kim, J.; Lee, M.; Shim, J.

    2014-12-01

    Carbonaceous components and soluble ions of PM2.5 were measured at Ieodo Ocean Research Station (IORS) from December 2004 to June 2008. IORS is a 40-m research tower and located in the East China Sea (32.07°N, 125.10°E). As IORS is distanced equally from South Korea, China, and Japan, it is an ideal place to monitor Asian outflows with the least influence of local emissions. The mean concentration of PM2.5 mass was 21.8 ± 14.9 μg/m3 with the maximum of 35.3 μg/m3 (March) and the minimum of 11.2 μg/m3 (September). The monthly variation of PM2.5 mass was similar to that of O3 due to meteorological conditions, which determines the degree of influence from nearby lands. Chinese outflows were mostly responsible for the enhancement of mass and major constituents of PM2.5 such as sulfate, OC, and EC. Their concentrations were the lowest in summer when aged marine air masses were dominant. It is noteworthy that sulfate was also enhanced when air mass passed through Japan, even though its concentration was not as high as that of Chinese outflows. In June, OC concentration was distinctively high with high OC/EC ratio of ~9.5. At IORS, June is characterized by the most frequent occurrence of fog and the lowest visibility with the highest relative humidity. In China, the clearing fire of agricultural residues is the major source of fine aerosols in June, leading to severe haze (e.g., Cheng et al., 2014). In addition, the aerosol optical depth was also observed to be the maximum over northeast Asia in June (Kim et al., 2007). Consequently, our results suggest that organic aerosol played a critical role in fog formation in the study region. References Cheng, Z., et al. (2014) Impact of biomass burning on haze pollution in the Yangtze River delta, China: a case study in summer 2011, Atmos. Chem. Phys., 14, 4573-4585, doi:10.5194/acp-14-4573-2014. Kim, S.-W., et al. (2007) Seasonal and monthly variations of columnar aerosol optical properties over east Asia determined from

  2. Carbonaceous aerosol characteristics over Delhi in Northern India: Seasonal variability and possible sources

    NASA Astrophysics Data System (ADS)

    Srivastava, Atul Kumar; Bisht, Ds; Tiwari, S.

    Carbonaceous aerosols have been the focus of extensive studies during the last decade due to its significant impacts on human health, visibility and climate change. As per Asian regions are concerned, aerosols in south-Asia are gaining considerable importance because of their potential impacts on regional climate, yet their possible sources are poorly understood. Semi-continuous measurements of organic carbon (OC) and elemental carbon (EC) and continuous measurements of black carbon (BC) aerosols were conducted simultaneously at Delhi during the period from January 2011 to May 2012. Delhi is the capital city of India and one of the densely populated and industrialized urban megacities in Asia, located at the Ganga basin in the northern part of India. Being highly polluted region, mass concentrations of OC, EC and BC over Delhi were found to vary from about 6-92 mug m (-3) (mean: 23±16 mug m (-3) ), 3-38 mug m (-3) (mean: 11±7 mug m (-3) ) and 1-24 mug m (-3) (mean: 7±5 mug m (-3) ), respectively during the entire measurement period, with about two times higher concentration during winter as compared to summer. A significant correlation between OC and EC (R=0.95, n=232) and relatively lower OC/EC ratio (range: 1.0-3.6; mean: 2.2±0.5) suggest fossil fuel emission as a dominant source of carbonaceous aerosols over the station. The average mass concentration of EC was found about 38% higher than BC during the study period, which is interestingly different as reported at other locations over Ganga basin. We also determined the associated optical properties of carbonaceous species (e.g. absorption coefficient and mass absorption efficiency) over the station. Significant loading of carbonaceous species over such regions emphasize an urgent need to focus on air quality management and proper impact assessment on health perspective.

  3. The application of thermal methods for determining chemical composition of carbonaceous aerosols: a review.

    PubMed

    Chow, Judith C; Yu, Jian Zhen; Watson, John G; Ho, Steven Sai Hang; Bohannan, Theresa L; Hays, Michael D; Fung, Kochy K

    2007-09-01

    Thermal methods of various forms have been used to quantify carbonaceous materials. Thermal/optical carbon analysis provides measurements of organic and elemental carbon concentrations as well as fractions evolving at specific temperatures in ambient and source aerosols. Detection of thermally desorbed organic compounds with thermal desorption-gas chromatography/mass spectrometry (TD-GC/MS) identifies and quantifies over 100 individual organic compounds in particulate matter (PM) samples. The resulting mass spectra contain information that is consistent among, but different between, source emissions even in the absence of association with specific organic compounds. TD-GC/MS is a demonstrated alternative to solvent extraction for many organic compounds and can be applied to samples from existing networks. It is amenable to field-deployable instruments capable of measuring organic aerosol composition in near real-time. In this review, thermal stability of organic compounds is related to chemical structures, providing a basis for understanding thermochemical properties of carbonaceous aerosols. Recent advances in thermal methods applied to determine aerosol chemical compositions are summarized and their potential for uncovering aerosol chemistry are evaluated. Current limitations and future research needs of the thermal methods are included. PMID:17849294

  4. Source apportionment of PM2.5 carbonaceous aerosol in Baghdad, Iraq

    NASA Astrophysics Data System (ADS)

    Hamad, Samera Hussein; Schauer, James Jay; Heo, Jongbae; Kadhim, Ahmed K. H.

    2015-04-01

    Baghdad is the second largest city in the Middle East and suffers from severe air quality degradation due to the high levels of the atmospheric particulate matter (PM). Limited information exists regarding the sources of PM in Baghdad, and the lack of information on sources inhibits the development of control strategies to reduce air pollution. To better understand the nature of fine particulate matter (PM2.5) in Baghdad and the Middle East, a one year sampling campaign to collect PM2.5 was conducted from September 2012 through September 2013, missing August 2013 samples due to the security situation. 24-hour integrated samples collected on a 1-in-6 day schedule were analyzed for the major components, and monthly average samples were analyzed by gas chromatography mass spectrometry (GCMS) methods to measure particle-phase organic molecular markers. The results of organic molecular markers were used in a chemical mass balance (CMB) model to quantify the sources of PM2.5 organic carbon (OC) and PM2.5 mass. Primary sources accounted for 44% of the measured PM2.5, and secondary sources were estimated to make up 28% of the measured PM2.5. Picene, a tracer of coal combustion detected in Baghdad where there is no evidence for coal combustion, can be attributed to burning crude oil and other low quality fuels in Baghdad. Source apportionment results showed that the dominant sources of the carbonaceous aerosols in Baghdad are gasoline (37 ± 6%) and diesel engines (17 ± 3%) which can be attributed to the extensive use of gasoline and diesel powered generators in Baghdad. Wood burning and residual oil combustion contributed to 5 ± 0.4 and 1 ± 0.2% respectively of OC. The unresolved sources contributed to 42 ± 19% of the OC which represented the secondary organic aerosol (SOA) and the unidentified sources.

  5. Properties of Carbonaceous Aerosols during CARDEX 2012: an Instrument Intercomparison

    NASA Astrophysics Data System (ADS)

    Beres, N. D.; Praveen, P. S.; Arnold, I. J.; Chakrabarty, R. K.; Arnott, W. P.; Moosmuller, H.; Schauer, J. J.; Gustafsson, O.; Ramanathan, V.

    2012-12-01

    Quantification of black carbon (BC) aerosol in the atmosphere is becoming increasingly important due to its role in radiative forcing. As advances in measurement techniques continue, BC measurements can be performed using a variety of instruments, employing optical, thermal, and photoacoustic methods. However, the relationship between data obtained with these methods is dependent on multiple properties of the ambient air sampled (e.g., aerosol composition, wavelength-dependence of light- and mass-absorbing efficiencies) and on the instruments and their data analysis algorithms (e.g., scattering correction factors for aethalometer data). Previous studies have utilized theoretical corrections to estimate BC concentrations and their corresponding radiative properties, but with limited confidence. In this study, we present comparisons of in-situ and filter-based measurements of aerosol light absorption, black carbon (BC) concentration, elemental carbon (EC), and organic carbon (OC) from the 2012 CARDEX (Clouds, Aerosol, Radiative forcing, and Dynamics EXperiment) campaign based on the island of Hanimaadhoo in the Republic of Maldives. The instruments used for this comparison study include two photoacoustic spectrometers (PAS, λ = 870 and 405 nm), a 7-wavelength aethalometer (λ = 370, 430, 470, 520, 590, 700, and 880 nm), and independent 12- and 24-hour integrated filter samples, analyzed for EC - OC using the NIOSH thermal evolution protocol. During the dry monsoon season (December to April), anthropogenic aerosols from India and Southeast Asia are characteristically transported to the Maldives at surface level. Data shown here were collected between February and April of 2012 at the Maldives Climate Observatory-Hanimaadhoo (MCOH). Using correction factors adopted from Corrigan et al., (2006), we show reasonable agreement between absorption coefficients obtained with the aethalometer and the photoacoustic spectrometer and between BC mass concentrations obtained with

  6. Interpretation of Aerosol Optical and Morphological Properties during the Carbonaceous Aerosols and Radiative Effects Study in Sacramento, June 2010

    NASA Astrophysics Data System (ADS)

    Gorkowski, K.; Mazzoleni, C.; China, S.; Sharma, N.; Flowers, B. A.; Dubey, M. K.; Gyawali, M. S.; Arnott, W. P.; Zaveri, R. A.

    2010-12-01

    The Sacramento Carbonaceous Aerosols and Radiative Effects Study (CARES) utilized two ground sites T0 and T1 along with an aircraft platform to characterize carbonaceous aerosol chemical and physical properties and their evolution. The T0 site was chosen within the Sacramento metropolitan area for measuring primary and secondary aerosols generated in the city. The T1 site was chosen East of Sacramento on the Sierra foothill to study the evolution and processing of the Sacramento aerosol plume and to assess the characteristics of the background air. To reach T1, the Sacramento aerosols traveled often over the Blodgett Forest resulting in significant aging due coagulation, condensation, and photochemical processes. The ground sites were chosen for this unique and reoccurring transport pattern of the aerosols. The campaign took place in June 2010. Six Integrated Photoacoustic/Nephelometer Spectrometers (IPNSs) were installed at the sites to simultaneously record aerosol light scattering and absorption data. The optical properties of the aerosols were measured at 355nm (ultraviolet), 375nm (ultraviolet), 405nm (blue), 532nm (green), and 781nm (red). In conjugation with the IPNSs, aerosol filters for electron microscopy analysis were collected at each site; these were examined using a field emission scanning electron microscope to study the aerosol morphology. The origins of the air masses did vary daily, but a few general trends emerged. The processing of the IPNS data with a wavelet denoising technique greatly enhanced the signal to noise ratio of the measurements enabling a better understanding of the aerosol optical properties for various airmasses with different characteristics. Typically signals at both sites were lower than expected, however the processed signals from T0 clearly showed a daily rise and dilution of the Sacramento plume. Using the processed signals from both sites the transportation of the Sacramento plume was detectable. The IPNS data were

  7. Source apportionment of the summer time carbonaceous aerosol at Nordic rural background sites

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Simpson, D.; Nøjgaard, J. K.; Kristensen, K.; Genberg, J.; Stenström, K.; Swietlicki, E.; Hillamo, R.; Aurela, M.; Bauer, H.; Offenberg, J. H.; Jaoui, M.; Dye, C.; Eckhardt, S.; Burkhart, J. F.; Stohl, A.; Glasius, M.

    2011-06-01

    In the present study, natural and anthropogenic sources of particulate organic carbon (OCp) and elemental carbon (EC) have been quantified based on weekly filter samples of PM10 collected at four Nordic rural background sites (Birkenes (Norway), Hyytiälä (Finland) Vavihill (Sweden), Lille Valby (Denmark)) during late summer (5 August-2 September 2009). Levels of source specific tracers, i.e. cellulose, levoglucosan, mannitol and the 14C/12C ratio of total carbon (TC), have been used as input for source apportionment of the carbonaceous aerosol, whereas Latin Hypercube Sampling (LHS) was used to statistically treat the multitude of possible combinations resulting from this approach. The carbonaceous aerosol (here: TCp; i.e. particulate TC) was totally dominated by natural sources (69-86 %), with biogenic secondary organic aerosol (BSOA) being the single most important source (48-57 %). Interestingly, primary biological aerosol particles (PBAP) were the second most important source (20-32 %). The anthropogenic contribution was mainly attributed to fossil fuel sources (OCff and ECff (10-24 %), whereas no more than 3-7 % was explained by combustion of biomass (OCbb and ECbb in this late summer campaign i.e. emissions from residential wood burning and/or wild/agricultural fires. Fossil fuel sources totally dominated the ambient EC loading, accounting for 4-12 % of TCp, whereas <1.5 % was attributed to combustion of biomass. The carbonaceous aerosol source apportionment showed only minor variation between the four selected sites. However, Hyytiälä and Birkenes showed greater resemblance to each other, as did Lille Valby and Vavihill, the two latter being somewhat more influenced by anthropogenic sources. Ambient levels of organosulphates and nitrooxy-organosulphates in the Nordic rural background environment are reported for the first time in the present study. The most abundant organosulphate compounds were an organosulphate of isoprene and nitrooxy

  8. Carbonaceous aerosol over semi-arid region of western India: Heterogeneity in sources and characteristics

    NASA Astrophysics Data System (ADS)

    Sudheer, A. K.; Aslam, M. Y.; Upadhyay, M.; Rengarajan, R.; Bhushan, R.; Rathore, J. S.; Singh, S. K.; Kumar, S.

    2016-09-01

    Carbonaceous species (elemental carbon (EC), organic carbon (OC), water-soluble organic carbon (WSOC)) and water-soluble inorganic species (Na+, NH4+, K+, Ca2 +, Mg2 +, Cl-, NO3-, SO42 -) in PM10 and PM2.5 from Ahmedabad and Jodhpur (urban and semi-urban locations, respectively) in western India were measured during May-September, 2011. Stable isotope composition of carbonaceous aerosol (δ13C of TC) in PM10 samples was also determined. Average EC concentration in PM10 at Ahmedabad was 1 μg m- 3 (range: 0.34 to 3.4 μg m- 3), almost 80% of which remained in PM2.5. Similarly, 70% of EC in PM10 (average: 0.9 μg m- 3) resided in PM2.5 at Jodhpur. Average OC concentration at Ahmedabad was 6.4 μg m- 3 and ~ 52% of this was found in PM2.5. On the contrary, OC concentration at Jodhpur was 40 μg m- 3, 80% of which was found in coarse particles contributing substantially to aerosol mass. δ13C of TC (average: - 27.5‰, range: - 29.6 to - 25.8‰) along with WSOC/EC ratio shows an increasing trend at Jodhpur suggesting the possibility of aging of aerosol, since aging results in enrichment of heavier isotope. OC and WSOC show significant correlations with K+ and not with EC, indicating biogenic origin of OC. Different size distributions are also exhibited by WSOC at the two stations. On the other hand, δ13C exhibits an inverse trend with sea-salt constituents at Ahmedabad, indicating the influence of air masses transported from the western/south-western region on carbonaceous aerosol. These results suggest that a strong heterogeneity exists in the sources of carbonaceous aerosol over this region and potential sources of non-combustion emissions such as bio-aerosol that need further investigation.

  9. Factors affecting the indoor concentrations of carbonaceous aerosols of outdoor origin

    SciTech Connect

    Lunden, Melissa M.; Kirchstetter, Thomas W.; Thatcher, Tracy L.; Hering, Susanne V.; Brown, Nancy J.

    2007-06-25

    A field study was conducted in an unoccupied single story residence in Clovis, California to provide data to address issues important to assess the indoor exposure to particles of outdoor origin. Measurements of black and organic carbonaceous aerosols were performed using a variety of methods, resulting in both near real-time measurements as well as integrated filter based measurements. Comparisons of the different measurement methods show that it is crucial to account for gas phase adsorption artifacts when measuring organic carbon (OC). Measured concentrations affected by the emissions of organic compounds sorbed to indoor surfaces imply a higher degree of infiltration of outdoor organic carbon aerosols into the indoor environment for our unoccupied house. Analysis of the indoor and outdoor data for black carbon (BC) aerosols show that, on average, the indoor concentration of black carbon aerosols behaves in a similar manner to sulfate aerosols. In contrast, organic carbon aerosols are subject to chemical transformations indoors that, for our unoccupied home, resulted in lower indoor OC concentrations than would be expected by physical loss mechanisms alone. These results show that gas to particle partitioning of organic compounds, as well as gas to surface interactions within the residence, are an important process governing the indoor concentration to OC aerosols of outdoor origin.

  10. Carbonaceous aerosol at two rural locations in New York State: Characterization and behavior

    NASA Astrophysics Data System (ADS)

    Sunder Raman, Ramya; Hopke, Philip K.; Holsen, Thomas M.

    2008-06-01

    Fine particle samples were collected to determine the chemical constituents in PM2.5 at two rural background sites (Potsdam and Stockton, N. Y.) in the northeastern United States from November 2002 to August 2005. Samples were collected every third day for 24 h with a speciation network sampler. The measured carbonaceous species included thermal-optical organic carbon (OC), elemental carbon (EC), pyrolytic carbon (OP), black carbon (BC), and water-soluble, short-chain (WSSC) organic acids. Concentration time series, autocorrelations, and seasonal variations of the carbonaceous species were examined. During this multiyear period, the contributions of the total carbon (OC + EC) to the measured fine particle mass were 31.2% and 31.1% at Potsdam and Stockton, respectively. The average sum of the WSSC acids carbon accounted for approximately 2.5% of the organic carbon at Potsdam and 3.0% at Stockton. At Potsdam, the seasonal differences in the autocorrelation function (ACF) and partial autocorrelation function (PACF) values for carbonaceous species suggest that secondary formation may be an important contributor to the observed concentrations of species likely to be secondary in origin, particularly during the photochemically active time of the year (May to October). This study also investigated the relationships between carbonaceous species to better understand the behavior of carbonaceous aerosol and to assess the contribution of secondary organic carbon (SOC) to the total organic carbon mass (the EC tracer method was used to estimate SOC). At Potsdam the average SOC contribution to total OC varied between 66% and 72%, while at Stockton it varied between 58% and 64%.

  11. Aerosol chemical characterization and role of carbonaceous aerosol on radiative effect over Varanasi in central Indo-Gangetic Plain

    NASA Astrophysics Data System (ADS)

    Tiwari, S.; Dumka, U. C.; Kaskaoutis, D. G.; Ram, Kirpa; Panicker, A. S.; Srivastava, M. K.; Tiwari, Shani; Attri, S. D.; Soni, V. K.; Pandey, A. K.

    2016-01-01

    This study investigates the chemical composition of PM10 aerosols at Varanasi, in the central Indo-Gangetic Plain (IGP) during April to July 2011, with emphasis on examining the contribution of elemental carbon (EC) to the estimates of direct aerosol radiative effect (DARE). PM10 samples are analysed for carbonaceous aerosols (Organic Carbon, OC and EC) and water-soluble ionic species (WSIS: Cl-, SO42-, NO3-, PO42- NH4+, Na+, K+, Mg2+ and Ca2+) and several diagnostic ratios (OC/EC, K+/EC, etc) have been also used for studying the aerosol sources at Varanasi. PM10 mass concentration varies between 53 and 310 μg m-3 (mean of 168 ± 73 μg m-3), which is much higher than the National and International air quality standards. The OC mass concentration varies from 6 μg m-3 to 24 μg m-3 (mean of 12 ± 5 μg m-3; 7% of PM10 mass), whereas EC ranges between 1.0 and 14.3 μg m-3 (4.4 ± 3.9 μg m-3; ˜3% of PM10 mass). The relative low OC/EC of 3.9 ± 2.0 and strong correlation (R2 = 0.82) between them suggest the dominance of primary carbonaceous aerosols. The contribution of WSIS to PM10 is found to be ˜12%, out of which ˜57% and 43% are anions and cations, respectively. The composite DARE estimates via SBDART model reveal significant radiative effect and atmospheric heating rates (0.9-2.3 K day-1). Although the EC contributes only ˜3% to the PM10 mass, its contribution to the surface and atmospheric forcing is significantly high (37-63% and 54-77%, respectively), thus playing a major role in climate implications over Varanasi.

  12. Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

    SciTech Connect

    Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.; Schmid, B.; Ferrare, R. A.; Alexander, M. L.; Alexandrov, M.; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Baidar, S.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.; Cahill, J. F.; Cairns, B.; Cappa, C. D.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Erickson, M. H.; Fast, J. D.; Floerchinger, C.; Flowers, B. A.; Fortner, E.; Gaffney, J. S.; Gilles, M. K.; Gorkowski, K.; Gustafson, W. I.; Gyawali, M.; Hair, J.; Hardesty, R. M.; Harworth, J. W.; Herndon, S.; Hiranuma, N.; Hostetler, C.; Hubbe, J. M.; Jayne, J. T.; Jeong, H.; Jobson, B. T.; Kassianov, E. I.; Kleinman, L. I.; Kluzek, C.; Knighton, B.; Kolesar, K. R.; Kuang, C.; Kubátová, A.; Langford, A. O.; Laskin, A.; Laulainen, N.; Marchbanks, R. D.; Mazzoleni, C.; Mei, F.; Moffet, R. C.; Nelson, D.; Obland, M. D.; Oetjen, H.; Onasch, T. B.; Ortega, I.; Ottaviani, M.; Pekour, M.; Prather, K. A.; Radney, J. G.; Rogers, R. R.; Sandberg, S. P.; Sedlacek, A.; Senff, C. J.; Senum, G.; Setyan, A.; Shilling, J. E.; Shrivastava, M.; Song, C.; Springston, S. R.; Subramanian, R.; Suski, K.; Tomlinson, J.; Volkamer, R.; Wallace, H. W.; Wang, J.; Weickmann, A. M.; Worsnop, D. R.; Yu, X. -Y.; Zelenyuk, A.; Zhang, Q.

    2012-01-01

    Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program’s Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites – one within the Sacramento urban area and another about 40 km to the northeast in the foothills area – were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and “aged” urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: a) the scientific background and motivation for the study, b) the operational and logistical information pertinent to the execution of the study, c) an overview of key observations and initial findings from the aircraft and ground-based sampling platforms, and d) a roadmap of

  13. Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

    SciTech Connect

    Zaveri, Rahul A.; Shaw, William J.; Cziczo, D. J.; Schmid, Beat; Ferrare, R.; Alexander, M. L.; Alexandrov, Mikhail; Alvarez, R. J.; Arnott, W. P.; Atkinson, D.; Baidar, Sunil; Banta, Robert M.; Barnard, James C.; Beranek, Josef; Berg, Larry K.; Brechtel, Fred J.; Brewer, W. A.; Cahill, John F.; Cairns, Brian; Cappa, Christopher D.; Chand, Duli; China, Swarup; Comstock, Jennifer M.; Dubey, Manvendra K.; Easter, Richard C.; Erickson, Matthew H.; Fast, Jerome D.; Floerchinger, Cody; Flowers, B. A.; Fortner, Edward; Gaffney, Jeffrey S.; Gilles, Mary K.; Gorkowski, K.; Gustafson, William I.; Gyawali, Madhu S.; Hair, John; Hardesty, Michael; Harworth, J. W.; Herndon, Scott C.; Hiranuma, Naruki; Hostetler, Chris A.; Hubbe, John M.; Jayne, J. T.; Jeong, H.; Jobson, Bertram T.; Kassianov, Evgueni I.; Kleinman, L. I.; Kluzek, Celine D.; Knighton, B.; Kolesar, K. R.; Kuang, Chongai; Kubatova, A.; Langford, A. O.; Laskin, Alexander; Laulainen, Nels S.; Marchbanks, R. D.; Mazzoleni, Claudio; Mei, F.; Moffet, Ryan C.; Nelson, Danny A.; Obland, Michael; Oetjen, Hilke; Onasch, Timothy B.; Ortega, Ivan; Ottaviani, M.; Pekour, Mikhail S.; Prather, Kimberly A.; Radney, J. G.; Rogers, Ray; Sandberg, S. P.; Sedlacek, Art; Senff, Christoph; Senum, Gunar; Setyan, Ari; Shilling, John E.; Shrivastava, ManishKumar B.; Song, Chen; Springston, S. R.; Subramanian, R.; Suski, Kaitlyn; Tomlinson, Jason M.; Volkamer, Rainer M.; Wallace, Hoyt A.; Wang, J.; Weickmann, A. M.; Worsnop, Douglas R.; Yu, Xiao-Ying; Zelenyuk, Alla; Zhang, Qi

    2012-08-22

    Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and 'aged' urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: a) the scientific background and motivation for the study, b) the operational and logistical information pertinent to the execution of the study, c) an overview of key observations and initial results from the aircraft and ground-based sampling platforms, and d) a roadmap of planned data

  14. Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

    NASA Technical Reports Server (NTRS)

    Zaveri, R. A.; Shaw, W. J.; Cahill, J. F.; Cairns, Brian; Cappa, C. D.; Ottaviani, Matteo; Cziczo, D. J.; Ferrare, Richard A.; Alexander, M. L.; Alexandrov, Mikhail Dmitrievic; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Schmid, B.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Erickson, M. H.; Fast, J. D.; Flowers, B. A.; Fortner, E.; Baidar, S.; Hair, J.; Hostetler, C.; Obland, M. D.; Rogers, R. R.; Floerchinger, C.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.

    2012-01-01

    Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climaterelated properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial findings from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data

  15. Global climate impacts of country-level primary carbonaceous aerosol from solid-fuel cookstove emissions

    NASA Astrophysics Data System (ADS)

    Lacey, Forrest; Henze, Daven

    2015-11-01

    Cookstove use is globally one of the largest unregulated anthropogenic sources of primary carbonaceous aerosol. While reducing cookstove emissions through national-scale mitigation efforts has clear benefits for improving indoor and ambient air quality, and significant climate benefits from reduced green-house gas emissions, climate impacts associated with reductions to co-emitted black (BC) and organic carbonaceous aerosol are not well characterized. Here we attribute direct, indirect, semi-direct, and snow/ice albedo radiative forcing (RF) and associated global surface temperature changes to national-scale carbonaceous aerosol cookstove emissions. These results are made possible through the use of adjoint sensitivity modeling to relate direct RF and BC deposition to emissions. Semi- and indirect effects are included via global scaling factors, and bounds on these estimates are drawn from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. Absolute regional temperature potentials are used to estimate global surface temperature changes. Bounds are placed on these estimates, drawing from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. We estimate a range of 0.16 K warming to 0.28 K cooling with a central estimate of 0.06 K cooling from the removal of cookstove aerosol emissions. At the national emissions scale, countries’ impacts on global climate range from net warming (e.g., Mexico and Brazil) to net cooling, although the range of estimated impacts for all countries span zero given uncertainties in RF estimates and fuel characterization. We identify similarities and differences in the sets of countries with the highest emissions and largest cookstove temperature impacts (China, India, Nigeria, Pakistan, Bangladesh and Nepal), those with the largest temperature impact per carbon emitted (Kazakhstan, Estonia, and Mongolia), and those that would provide the

  16. Physiochemical properties of carbonaceous aerosol from agricultural residue burning: Density, volatility, and hygroscopicity

    NASA Astrophysics Data System (ADS)

    Li, Chunlin; Hu, Yunjie; Chen, Jianmin; Ma, Zhen; Ye, Xingnan; Yang, Xin; Wang, Lin; Wang, Xinming; Mellouki, Abdelwahid

    2016-09-01

    Size-resolved effective density, mixing state, and hygroscopicity of smoke particles from five kinds of agricultural residues burning were characterized using an aerosol chamber system, including a volatility/hygroscopic tandem differential mobility analyzer (V/H-TDMA) combined with an aerosol particle mass analyzer (APM). To profile relationship between the thermodynamic properties and chemical compositions, smoke PM1.0 and PM2.5 were also measured for the water soluble inorganics, mineral elements, and carbonaceous materials like organic carbon (OC) and elemental carbon (EC). Smoke particle has a density of 1.1-1.4 g cm-3, and hygroscopicity parameter (κ) derived from hygroscopic growth factor (GF) of the particles ranges from 0.20 to 0.35. Size- and fuel type-dependence of density and κ are obvious. The integrated effective densities (ρ) and hygroscopicity parameters (κ) both scale with alkali species, which could be parameterized as a function of organic and inorganic mass fraction (forg &finorg) in smoke PM1.0 and PM2.5: ρ-1 =finorg · ρinorg-1 +forg · ρorg-1 and κ =finorg ·κinorg +forg ·κorg . The extrapolated values of ρinorg and ρorg are 2.13 and 1.14 g cm-3 in smoke PM1.0, while the characteristic κ values of organic and inorganic components are about 0.087 and 0.734, which are similar to the bulk density and κ calculated from predefined chemical species and also consistent with those values observed in ambient air. Volatility of smoke particle was quantified as volume fraction remaining (VFR) and mass fraction remaining (MFR). The gradient temperature of V-TDMA was set to be consistent with the splitting temperature in the OC-EC measurement (OC1 and OC2 separated at 150 and 250 °C). Combing the thermogram data and chemical composition of smoke PM1.0, the densities of organic matter (OM1 and OM2 correspond to OC1 and OC2) are estimated as 0.61-0.90 and 0.86-1.13 g cm-3, and the ratios of OM1/OC1 and OM2/OC2 are 1.07 and 1.29 on average

  17. Feasibility study for GCOM-C/SGLI: Retrieval algorithms for carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Mukai, Sonoyo; Sano, Itaru; Yasumoto, Masayoshi; Fujito, Toshiyuki; Nakata, Makiko; Kokhanovsky, Alexander

    2016-04-01

    The Japan Aerospace Exploration Agency (JAXA) has been developing the new Earth observing system, GCOM (Global Change Observation Mission) project, which consists of two satellite series of GCOM-W1 and GCOM-C1. The 1st GCOM-C satellite will board the SGLI (second generation global imager) which also includes polarimetric sensor and be planed to launch in early of 2017. The SGLI has multi (19)-channels including near UV channel (380 nm) and two polarization channels at red and near-infrared wavelengths of 670 and 870 nm. EUMETSAT plans to collect polarization measurements with a POLDER follow on 3MI / EPS-SG in 2021. Then the efficient retrieval algorithms for aerosol and/or cloud based on the combination use of radiance and polarization are strongly expected. This work focuses on serious biomass burning episodes in East Asia. It is noted that the near UV measurements are available for detection of the carbonaceous aerosols. The biomass burning aerosols (BBA) generated by forest fire and/or agriculture biomass burning have influenced on the severe air pollutions. It is known that the forest fire increases due to global warming and a climate change, and has influences on them vice versa. It is well known that this negative cycle decreases the quality of global environment and human health. We intend to consider not only retrieval algorithms of remote sensing for severe air pollutions but also detection and/or distinction of aerosols and clouds, because mixture of aerosols and clouds are often occurred in the severe air pollutions. Then precise distinction of aerosols and clouds, namely aerosols in cloudy scenes and/or clouds in heavy aerosol episode, is desired. Aerosol retrieval in the hazy atmosphere has been achieved based on radiation simulation method of successive order of scattering 1,2. In this work, we use both radiance and polarization measurements observed by GLI and POLDER-2 on Japanese ADEOS-2 satellite in 2003 as a simulated data. As a result the

  18. Source apportionment of the summer time carbonaceous aerosol at Nordic rural background sites

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Simpson, D.; Nøjgaard, J. K.; Kristensen, K.; Genberg, J.; Stenström, K.; Swietlicki, E.; Hillamo, R.; Aurela, M.; Bauer, H.; Offenberg, J. H.; Jaoui, M.; Dye, C.; Eckhardt, S.; Burkhart, J. F.; Stohl, A.; Glasius, M.

    2011-12-01

    In the present study, natural and anthropogenic sources of particulate organic carbon (OCp) and elemental carbon (EC) have been quantified based on weekly filter samples of PM10 (particles with aerodynamic diameter <10 μm) collected at four Nordic rural background sites [Birkenes (Norway), Hyytiälä (Finland), Vavihill (Sweden), Lille Valby, (Denmark)] during late summer (5 August-2 September 2009). Levels of source specific tracers, i.e. cellulose, levoglucosan, mannitol and the 14C/12C ratio of total carbon (TC), have been used as input for source apportionment of the carbonaceous aerosol, whereas Latin Hypercube Sampling (LHS) was used to statistically treat the multitude of possible combinations resulting from this approach. The carbonaceous aerosol (here: TCp; i.e. particulate TC) was totally dominated by natural sources (69-86%), with biogenic secondary organic aerosol (BSOA) being the single most important source (48-57%). Interestingly, primary biological aerosol particles (PBAP) were the second most important source (20-32%). The anthropogenic contribution was mainly attributed to fossil fuel sources (OCff and ECff) (10-24%), whereas no more than 3-7% was explained by combustion of biomass (OCbb and ECbb) in this late summer campaign i.e. emissions from residential wood burning and/or wild/agricultural fires. Fossil fuel sources totally dominated the ambient EC loading, which accounted for 4-12% of TCp, whereas <1.5% of EC was attributed to combustion of biomass. The carbonaceous aerosol source apportionment showed only minor variation between the four selected sites. However, Hyytiälä and Birkenes showed greater resemblance to each other, as did Lille Valby and Vavihill, the two latter being somewhat more influenced by anthropogenic sources. Ambient levels of organosulphates and nitrooxy-organosulphates in the Nordic rural background environment are reported for the first time in the present study. The most abundant organosulphate compounds were an

  19. Carbonaceous aerosols and mineral dust in atmospheric outflow from the Indo-Gangetic Plain

    NASA Astrophysics Data System (ADS)

    Sarin, M.; Srinivas, B.; Rengarajan, R.

    2012-12-01

    Atmospheric carbonaceous aerosols and mineral dust over south and south-east Asia has been a subject of major debate over the past two decades because of their potential impact on the regional air quality and climate forcing. A comprehensive study through ground-based measurements and data-base for aerosol chemical composition (involving both organic and inorganic constituents) is, thus, essential to constrain the large uncertainties associated with the climate impact. Our systematic study from a downwind site (Kharagpur: 22.02N, 87.11E) in the Indo-Gangetic Plain (IGP) suggests large temporal variability in the atmospheric mass concentrations of mineral dust, organic and elemental carbon (OC, EC), water-soluble organic carbon (WSOC) and inorganic species (WSIS). This is attributed to seasonally varying anthropogenic emissions, their source strength, boundary layer dynamics, secondary aerosol formation and long-range transport of mineral dust from desert regions. Based on diagnostic ratios [OC/EC ≈ 7.0 ± 2.2, WSOC/OC ≈ 0.6 and K+/EC ≈ 0.48 ± 0.17], we document biomass burning emissions (wood-fuel and post-harvest agricultural-waste burning) as a major source of carbonaceous aerosols. The characteristic ratios: nss-SO42-/EC (3.9 ± 2.1), nss-SO42-/OC (0.61 ± 0.46), high abundance of SO42- (6.9 - 25.3 μg m-3) and SO42-/ΣWSIS = 45 - 77 % in the outflow provide better assessment of aerosol optical properties. The subsequent downwind transport of pollutants from the IGP significantly influences the chemical composition of aerosols over the Bay of Bengal. The dominance of aerosol SO42- in the marine atmospheric boundary layer (MABL) is evident from the wide-spread depletion of chloride with respect to sea-salt composition. The Ca/Al and Fe/Al ratios in the IGP-outflow, used as a proxy for the long-range transport of mineral dust, are consistent with those in the MABL. The mass closure for PM2.5 composition suggests that contribution of mineral dust (20

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

    NASA Astrophysics Data System (ADS)

    Mikhailov, E. F.; Mironova, S. Yu.; Makarova, M. V.; Vlasenko, S. S.; Ryshkevich, T. I.; Panov, A. V.; Andreae, M. O.

    2015-07-01

    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.

  1. Carbonaceous aerosols and pollutants over Delhi urban environment: Temporal evolution, source apportionment and radiative forcing.

    PubMed

    Bisht, D S; Dumka, U C; Kaskaoutis, D G; Pipal, A S; Srivastava, A K; Soni, V K; Attri, S D; Sateesh, M; Tiwari, S

    2015-07-15

    Particulate matter (PM2.5) samples were collected over Delhi, India during January to December 2012 and analysed for carbonaceous aerosols and inorganic ions (SO4(2-) and NO3(-)) in order to examine variations in atmospheric chemistry, combustion sources and influence of long-range transport. The PM2.5 samples are measured (offline) via medium volume air samplers and analysed gravimetrically for carbonaceous (organic carbon, OC; elemental carbon, EC) aerosols and inorganic ions (SO4(2-) and NO3(-)). Furthermore, continuous (online) measurements of PM2.5 (via Beta-attenuation analyser), black carbon (BC) mass concentration (via Magee scientific Aethalometer) and carbon monoxide (via CO-analyser) are carried out. PM2.5 (online) range from 18.2 to 500.6μgm(-3) (annual mean of 124.6±87.9μgm(-3)) exhibiting higher night-time (129.4μgm(-3)) than daytime (103.8μgm(-3)) concentrations. The online concentrations are 38% and 28% lower than the offline during night and day, respectively. In general, larger night-time concentrations are found for the BC, OC, NO3(-)and SO4(2-), which are seasonally dependent with larger differences during late post-monsoon and winter. The high correlation (R(2)=0.74) between OC and EC along with the OC/EC of 7.09 (day time) and 4.55 (night-time), suggest significant influence of biomass-burning emissions (burning of wood and agricultural waste) as well as secondary organic aerosol formation during daytime. Concentrated weighted trajectory (CWT) analysis reveals that the potential sources for the carbonaceous aerosols and pollutants are local emissions within the urban environment and transported smoke from agricultural burning in northwest India during post-monsoon. BC radiative forcing estimates result in very high atmospheric heating rates (~1.8-2.0Kday(-1)) due to agricultural burning effects during the 2012 post-monsoon season. PMID:25864155

  2. Aerosol-Assisted Self-Assembly of Reticulated N-Doped Carbonaceous Submicron Spheres for Effective Removal of Hexavalent Chromium.

    PubMed

    He, Jiawei; Long, Yuan; Wang, Yiyan; Wei, Chaoliang; Zhan, Jingjing

    2016-07-01

    This Research Article described a facile one-step method to prepare reticulated N-doped carbonaceous submicron spheres. Through a simple aerosol-assisted technology, glucosamine sulfate used as a carbon source was aerosolized and carbonized to functionalized carbonaceous submicron spheres. The electrostatic attraction between protonated amino groups and sulfate in the aerosol droplets induced a self-assembly and led to the formation of reticular structure, avoiding the use of templates. Compared to bare carbonaceous materials produced from glucose, reticulated N-doped carbonaceous spheres exhibit higher efficiency in the removal of Cr(VI), where the doping of element nitrogen led to electrostatic attraction between protonated nitrogen and chromium ions, and reticulated structure created relatively higher surface area and pore volume, facilitating materials to contact with Cr(VI) ions. XPS characterization proved these novel N-doped carbonaceous materials could effectively transform Cr(VI) to less toxic Cr(III) because of the surface reducing groups. For the practical application, several factors including the initial pH, materials dosage and recycle numbers on the removal performance were studied. PMID:27299376

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

    NASA Astrophysics Data System (ADS)

    Cui, H.; Mao, P.; Zhao, Y.; Nielsen, C. P.; Zhang, J.

    2015-03-01

    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 76 ± 2, 19 ± 2 and 5 ± 1% of the total emissions of OC, respectively, and 52 ± 3, 32 ± 2 and 16 ± 2% of EC. Updated emission factors based on the most recent local field measurements, particularly for biofuel stoves, lead 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 larger OC/EC and SOC/OC ratios are found in southern cities, due to the joint effects of primary emissions and meteorology. Higher SOC/OC 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

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

    NASA Astrophysics Data System (ADS)

    Cui, H.; Mao, P.; Zhao, Y.; Nielsen, C. P.; Zhang, J.

    2015-08-01

    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

  5. Carbonaceous aerosols on the south edge of the Tibetan Plateau: concentrations, seasonality and sources

    NASA Astrophysics Data System (ADS)

    Cong, Z.; Kang, S.; Kawamura, K.; Liu, B.; Wan, X.; Wang, Z.; Gao, S.; Fu, P.

    2014-10-01

    To quantitatively evaluate the effect of carbonaceous aerosols on the south edge of the Tibetan Plateau, aerosol samples were collected weekly from August 2009 to July 2010 at Mt. Everest (Qomolangma Station for Atmospheric and Environmental Observation and Research, briefly QOMS, 28.36° N, 86.95° E, 4276 m a.s.l.). The samples were analyzed for organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and major ions. The average concentrations of OC, EC and WSOC were 1.43, 0.25 and 0.77 μg m-3, respectively. The concentration levels of OC and EC at QOMS are comparable to those at high elevation sites on the southern slopes of the Himalayas (Langtang and NCO-P), but three to six times lower than those at Manora Peak, India and Godavari, Nepal. Sulfate was the most abundant anion species followed by nitrate, accounting for 25 and 12% of total ionic mass, respectively. Ca2+ was the most abundant cation species (annual average of 0.88 μg m-3). The various aerosol compositions showed distinctive seasonality. The dust loading, represented by Ca2+ concentration, was relatively constant throughout the year. While OC, EC and other ionic species (NH4+, K+, NO3-, and SO42-) exhibited a pronounced peak in the pre-monsoon period and a minimum in the monsoon season. Similar seasonal trends of aerosol composition were also reported previously from the southern slope of the Himalayas, such as Langtang and NCO-P. This phenomenon indicates that both slopes of Himalayas share a common atmospheric environment regime. The strong correlation of OC and EC in QOMS aerosols with K+ and levoglucosan indicates that they were mainly originated from biomass burning. The active fire spots observed by MODIS and their backward trajectories further demonstrate that in pre-monsoon season, agricultural and forest fires in the northern India and Nepal were most likely sources of carbonaceous aerosol at QOMS. In addition to large-scale atmospheric circulation, the unique

  6. Carbonaceous aerosols on the south edge of the Tibetan Plateau: concentrations, seasonality and sources

    NASA Astrophysics Data System (ADS)

    Cong, Z.; Kang, S.; Kawamura, K.; Liu, B.; Wan, X.; Wang, Z.; Gao, S.; Fu, P.

    2015-02-01

    To quantitatively evaluate the effect of carbonaceous aerosols on the south edge of the Tibetan Plateau, aerosol samples were collected weekly from August 2009 to July 2010 at Qomolangma (Mt. Everest) Station for Atmospheric and Environmental Observation and Research (QOMS, 28.36° N, 86.95° E, 4276 m a.s.l.). The average concentrations of organic carbon (OC), elemental carbon (EC) and water-soluble organic carbon were 1.43, 0.25 and 0.77 μg m-3, respectively. The concentration levels of OC and EC at QOMS are comparable to those at high-elevation sites on the southern slopes of the Himalayas (Langtang and Nepal Climate Observatory at Pyramid, or NCO-P), but 3 to 6 times lower than those at Manora Peak, India, and Godavari, Nepal. Sulfate was the most abundant anion species followed by nitrate, accounting for 25 and 12% of total ionic mass, respectively. Ca2+ was the most abundant cation species (annual average of 0.88 μg m-3). The dust loading, represented by Ca2+ concentration, was relatively constant throughout the year. OC, EC and other ionic species (NH4+, K+, NO3- and SO42-) exhibited a pronounced peak in the pre-monsoon period and a minimum in the monsoon season, being similar to the seasonal trends of aerosol composition reported previously from the southern slope of the Himalayas, such as Langtang and NCO-P. The strong correlation of OC and EC in QOMS aerosols with K+ and levoglucosan indicates that they mainly originated from biomass burning. The fire spots observed by MODIS and backward air-mass trajectories further demonstrate that in pre-monsoon season, agricultural and forest fires in northern India and Nepal were most likely sources of carbonaceous aerosol at QOMS. Moreover, the CALIOP observations confirmed that air-pollution plumes crossed the Himalayas during this period. The highly coherent variation of daily aerosol optical depth (500 nm) between QOMS and NCO-P indicates that both slopes of the Himalayas share a common atmospheric environment

  7. Quantifying the sources of atmospheric ice nuclei from carbonaceous combustion aerosol

    NASA Astrophysics Data System (ADS)

    Schill, G. P.; Jathar, S.; Galang, A.; Farmer, D.; Friedman, B.; Levin, E. J.; DeMott, P. J.; Kreidenweis, S. M.

    2015-12-01

    Ice nucleation on particles is a fundamental atmospheric process, which governs precipitation, cloud lifetimes, and climate. Despite being a basic atmospheric process, our current understanding of ice nucleation in the atmosphere is low. One reason for this low understanding is that ice nuclei concentrations are low (only ~1 in 105 particles in the free troposphere nucleate ice), making it challenging to identify both the composition and sources of ambient ice nuclei. Carbonaceous combustion aerosol produced from biomass and fossil fuel combustion are one potential source of these ice nuclei, as they contribute to over one-third of all aerosol in the North American free troposphere. Unfortunately, previous results from field measurements in-cloud, aircraft measurements, and laboratory studies are in conflict, with estimates of the impact of combustion aerosol ranging from no effect to rivaling the well-known atmospheric ice nuclei mineral dust. It is, however, becoming clear that aerosols from combustion processes are more complex than model particles, and their ice activity depends greatly on both fuel type and combustion conditions. Given these dependencies, we propose that sampling from real-world biomass burning and fossil fuel sources would provide the most useful new information on the contribution of carbonaceous combustion aerosols to atmospheric ice nuclei particles. To determine the specific contribution of refractory black carbon (rBC) to ice nuclei concentrations, we have coupled the Single Particle Soot Photometer (SP2) to the Colorado State University Continuous Flow Diffusion Chamber (CFDC). The SP2 utilizes laser-induced incandescence to quantify rBC mass on a particle-by-particle basis; in doing so, it also selectively destroys rBC particles by heating them to their vaporization temperature. Thus, the SP2 can be used as a selective pre-filter for rBC into the CFDC. In this work, we will present recent results looking at contribution of diesel

  8. Modal characteristics of carbonaceous aerosol size distribution in an urban atmosphere of South China

    NASA Astrophysics Data System (ADS)

    Lan, Zi-Juan; Chen, Dong-Lei; Li, Xiang; Huang, Xiao-Feng; He, Ling-Yan; Deng, Yan-Ge; Feng, Ning; Hu, Min

    2011-04-01

    Size distributions can provide important information about aerosol sources, formation, and growth mechanisms. However, compared to size distributions of inorganic aerosols, size distributions of carbonaceous aerosols have been much less studied and reported in the literature. In this paper, we systematically measured size distributions of elemental carbon (EC), organic carbon (OC), oxalate, polycyclic aromatic hydrocarbons (PAHs), as well as major inorganic ions in urban aerosols in Shenzhen, China. Totally 24 sets of samples were collected using a ten-stage micro orifice uniform deposit impactor (MOUDI) during October 2009 to February 2010. Three lognormal modes contained in the size distributions of species were resolved based on positive matrix factorization (PMF) analysis of the measured dataset, corresponding to the condensation (peak = 0.34 μm), droplet (peak = 0.84 μm), and coarse (peak = 5.4 μm) modes, respectively. The mean concentrations of EC in the condensation, droplet, and coarse modes were 2.20, 1.18, and 0.64 μg m -3, respectively, and the modal characteristics of EC indicate that fresher local combustion emissions contributed mostly to aerosol EC in the urban atmosphere of Shenzhen. The mean concentrations of OC in the condensation, droplet, and coarse modes were 2.29, 3.34, and 3.51 μg m -3, respectively, and the modal characteristics of OC indicate that its sources were more primary in the condensation mode while more secondary in the droplet mode. The modal characteristics of aerosol oxalate and PAHs suggest that they were predominantly from in-cloud secondary formation and local emissions, respectively.

  9. Combined measurements of organic aerosol isotopic and chemical composition to investigate day-night differences in carbonaceous aerosol

    NASA Astrophysics Data System (ADS)

    Dusek, Ulrike; Holzinger, Rupert; Meijer, Harro A. J.; Röckmann, Thomas

    2014-05-01

    PM2.5 filter samples have been collected during the Pegasos (Mai, 2012) and Actris (June/July 2012) campaigns at the CESAR site near Cabauw, the Netherlands. This site lies in a rural location surrounded by major urban centers and highways and is a good location for measuring the regional aerosol contamination in the Netherlands. High volume filter samples were taken over several days, but the aerosol was collected on separate filters during day and night time periods. We analyzed these filters for carbon isotopes (14C and 13C) and detailed chemical composition of the organic fraction, which can be a powerful tool, for investigating sources and processing of the organic aerosol. Measurement of the radioactive carbon isotope 14C in aerosols can provide a direct estimate of the contribution of fossil fuel sources to aerosol carbon. The stable carbon isotopes 12C and 13C can be used to get information about sources and processing of organic aerosol. We use a method to measure d13C values of OC desorbed from the filter samples in He at different temperature steps. The chemical composition of the organic fraction at the same temperature steps can be determined using a Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS). The PTR-MS method is applied to the filter samples as well to aerosol collected in situ by a impaction using a Collection-Thermal-Desorption Cell. First results show that the mass concentration of the carbonaceous aerosol is higher during night time than during day time, dominated by a strong increase of biogenic organic aerosol. This is at least partially caused by a shallow night time boundary layer combined with decreased traffic sources and increased condensation of semi-volatile biogenic gases during night-time. Evidence for the role of semi-volatile compounds in enhancing organic carbon (OC) night time concentrations comes from several observations: (1) semi-volatile OC with desorption temperatures lower than 250 °C increases

  10. Morphological characterization of carbonaceous aggregates in soot and free fall aerosol samples

    NASA Astrophysics Data System (ADS)

    Sachdeva, Kamna; Attri, Arun K.

    The morphological characteristics of BC aggregates present in the soot and carbonaceous aerosol (CA) samples were investigated. The process of soot formation under laboratory conditions took into account the commonly used practice of burning fuel in the households in India. The fractal morphology was determined by using box counting algorithm and maximum projected area of the aggregates by using their digital electron microscopic images. Former provided the estimates of perimeter fractal dimension (PD f) of each aggregate, and later estimated the average density fractal dimension (DD f) of aggregate groups. Numbers of particles constituting the aggregates, using projected area approach, were significantly higher than the estimates based on pixel counting. The measured average diameter of the primary particles in aggregates, ranged between 24 and 57 nm. The fractal dimensions, PD f, for the laboratory-generated soot aggregates varied from 1.36 to 1.88. The PD f for aggregates derived from diesel-vehicles and biomass burning showed significant variation: biomass, 1.27; diesel vehicle, 1.82 and 1.7. The size and the dimensions estimated for the free fall CA samples showed large deviation. The ratio L/ Rg (length/radius of gyration) for soot aggregates (gasoline, kerosene, diesel, mustard oil and hexane) ranged from 3.5 to 4.8. Surface morphology of these aggregates, using scanning electron microscope (SEM), showed the presence of spherical "charred cenosphere" like particles in gasoline and free fall aerosol aggregates. FTIR investigations revealed the presence of a large number of organic groups (OC) associated with carbonaceous aggregates present in soot and free fall aerosol samples.

  11. Measurements of non-volatile aerosols with a VTDMA and their correlations with carbonaceous aerosols in Guangzhou, China

    NASA Astrophysics Data System (ADS)

    Cheung, Heidi H. Y.; Tan, Haobo; Xu, Hanbing; Li, Fei; Wu, Cheng; Yu, Jian Z.; Chan, Chak K.

    2016-07-01

    Simultaneous measurements of aerosol volatility and carbonaceous matters were conducted at a suburban site in Guangzhou, China, in February and March 2014 using a volatility tandem differential mobility analyzer (VTDMA) and an organic carbon/elemental carbon (OC / EC) analyzer. Low volatility (LV) particles, with a volatility shrink factor (VSF) at 300 °C exceeding 0.9, contributed 5 % of number concentrations of the 40 nm particles and 11-15 % of the 80-300 nm particles. They were composed of non-volatile material externally mixed with volatile material, and therefore did not evaporate significantly at 300 °C. Non-volatile material mixed internally with the volatile material was referred to as medium volatility (MV, 0.4 < VSF < 0.9) and high volatility (HV, VSF < 0.4) particles. The MV and HV particles contributed 57-71 % of number concentration for the particles between 40 and 300 nm in size. The average EC and OC concentrations measured by the OC / EC analyzer were 3.4 ± 3.0 and 9.0 ± 6.0 µg m-3, respectively. Non-volatile OC evaporating at 475 °C or above, together with EC, contributed 67 % of the total carbon mass. In spite of the daily maximum and minimum, the diurnal variations in the volume fractions of the volatile material, HV, MV and LV residuals were less than 15 % for the 80-300 nm particles. Back trajectory analysis also suggests that over 90 % of the air masses influencing the sampling site were well aged as they were transported at low altitudes (below 1500 m) for over 40 h before arrival. Further comparison with the diurnal variations in the mass fractions of EC and the non-volatile OC in PM2.5 suggests that the non-volatile residuals may be related to both EC and non-volatile OC in the afternoon, during which the concentration of aged organics increased. A closure analysis of the total mass of LV and MV residuals and the mass of EC or the sum of EC and non-volatile OC was conducted. It suggests that non-volatile OC, in addition to EC, was

  12. CHEMICAL ANALYSIS METHODS FOR ATMOSPHERIC AEROSOL COMPONENTS

    EPA Science Inventory

    This chapter surveys the analytical techniques used to determine the concentrations of aerosol mass and its chemical components. The techniques surveyed include mass, major ions (sulfate, nitrate, ammonium), organic carbon, elemental carbon, and trace elements. As reported in...

  13. Evolution of wavelength-dependent mass absorption cross sections of carbonaceous aerosols during the 2010 DOE CARES campaign

    NASA Astrophysics Data System (ADS)

    Flowers, B. A.; Dubey, M. K.; Subramanian, R.; Sedlacek, A. J.; Kelley, P.; Luke, W. T.; Jobson, B. T.; Zaveri, R. A.

    2011-12-01

    Predictions of aerosol radiative forcing require process level optical property models that are built on precise and accurate field observations. Evolution of aerosol optical properties for urban influenced carbonaceous aerosol undergoing transport and mixing with rural air masses was a focal point of the DOE Carbonaceous Aerosol and Radiative Effects (CARES) campaign near Sacramento, CA in summer 2010. Urban aerosol was transported from Sacramento, CA (T0) to the foothills of the Sierra Nevada Mountains to a rural site located near Cool, CA (T1). Aerosol absorption and scattering coefficients were measured at the T0 and T1 sites using integrated photoacoustic acoustic/nephelometer instruments (PASS-3 and PASS-UV) at 781, 532, 405, and 375 nm. Single particle soot photometry (SP2) instrumentation was used to monitor black carbon (BC) mass at both sites. Combining data from these sensors allows estimate of the wavelength-dependent mass absorption coefficient (MAC(λ)) and partitioning of MAC(λ) into contributions from the BC core and from enhancements from coating of BC cores. MAC(λ) measured in this way is free of artifacts associated with filter-based aerosol absorption measurements and takes advantage of the single particle sensitivity of the SP2 instrument, allowing observation of MAC(λ) on 10 minute and faster time scales. Coating was observed to enhance MAC(λ) by 20 - 30 % and different wavelength dependence for MAC(λ) was observed for urban and biomass burning aerosol. Further, T0 - T1 evolution of MAC(λ) was correlated with separately measured NO/NOy ratios and CO/CO2 ratios to understand the effects of aging & transport on MAC(λ) and the implications of aerosol processing that links air quality to radiative forcing on a regional scale. Aircraft observations made from the Gulfstream-1 during CARES are also analyzed to enhance process level understanding of the optical properties of fresh and aged carbonaceous aerosol in the urban-rural interface.

  14. Characteristics of fine particle carbonaceous aerosol at two remote sites in Central Asia

    NASA Astrophysics Data System (ADS)

    Miller-Schulze, Justin P.; Shafer, Martin M.; Schauer, James J.; Solomon, Paul A.; Lantz, Jeffrey; Artamonova, Maria; Chen, Boris; Imashev, Sanjar; Sverdlik, Leonid; Carmichael, Greg R.; Deminter, Jeff T.

    2011-12-01

    Central Asia is a relatively understudied region of the world in terms of characterizing ambient particulate matter (PM) and quantifying source impacts of PM at receptor locations, although it is speculated to have an important role as a source region for long-range transport of PM to Eastern Asia, the Pacific Ocean, and the Western United States. PM is of significant interest not only because of its adverse effect on public health but also due to its more recently realized role in climate change. To investigate the sources and characteristics of PM in the region, a series of PM 2.5 and PM 10 samples were collected on an every-other-day basis at two sites (termed "Bishkek" and "Teploklyuchenka") in the Central Asian nation of the Kyrgyz Republic (also known as Kyrgyzstan) for a full year from July 2008 to July 2009. These samples were analyzed using standard methods for mass, organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), water-insoluble organic carbon by difference (OC minus WSOC) and a variety of molecular marker chemical species to be used in a chemical mass balance (CMB) model to apportion the sources of OC. These analyses indicate that approximately 19 ± 6.4% of the PM 2.5 mass at both sites throughout the year consists of OC. The carbonaceous component of PM 2.5 is dominated by OC, with OC/Total Carbon (TC) ratios being around 0.8 in the winter to almost 0.95 in the summer months. The CMB analysis indicated that mobile sources, i.e., gasoline and diesel engine exhaust, biomass combustion, and biogenic secondary organic aerosol (SOA) formation from isoprene and α-pinene precursors in the summer months were the dominant sources of OC. A strong positive correlation was observed between non-biomass burning WSOC and the un-apportioned OC from the CMB analysis, indicating that some of this un-apportioned OC is WSOC and likely the result of SOA-forming atmospheric processes that were not estimated by the CMB analysis performed. In

  15. The distribution of PM10 and PM2.5 carbonaceous aerosol in Baotou, China

    NASA Astrophysics Data System (ADS)

    Zhou, Haijun; He, Jiang; Zhao, Boyi; Zhang, Lijun; Fan, Qingyun; Lü, Changwei; Dudagula; Liu, Tao; Yuan, Yinghui

    2016-09-01

    Particulate matter (PM), including PM10 and PM2.5, is one of the major impacts on air quality, visibility, climate change, earth radiation balance, and public health. Organic carbon (OC) and elemental carbon (EC) are the major components of PM. 804 samples (PM10 and PM2.5) were simultaneously collected from six urban sites covering 3 districts in Baotou, in January, April, September, and November 2014. As to a long-term study on the effects of carbonaceous aerosol, data were collected annually at Environmental Protection Agency of Baotou (EPB). The concentrations of PM10 and PM2.5, the spatial distribution and content of OC and EC, the relationship between OC and EC, and the formation of secondary organic carbon (SOC) have been investigated. The findings indicated that the concentrations of these particle matter are higher than that in US or European standards. The average concentrations of OC in PM10 and PM2.5 follow the order: January > November > April > September; and for EC in PM10 and PM2.5 follow the order: January > November > September > April. Affected by metrological factors, it was indicated that high wind speed and low relative humidity were beneficial for removal of OC and EC in January and November. Pearson correlations and cluster analysis on OC and EC concentrations in PM10 and PM2.5 with gaseous pollutants (SO2, NO2, and CO) suggested that OC shared the same emission sources with SO2 and CO from combustion, while EC's sources mainly came from vehicles exhaust and combustion which contributed to NO2 as well. The OC concentration is mainly primary in warm months, while it appears secondary in cold months in Baotou. There is a common characteristic among the cities with higher SOC in winter, wherever the coal combustion can lead to the severe pollution. This work is important for the construction of the database of OC and EC concentrations in PM10 and PM2.5 at spatial and time intervals, and it can provide scientific suggestion for similar PM

  16. Sources of excess urban carbonaceous aerosol in the Pearl River Delta Region, China

    NASA Astrophysics Data System (ADS)

    Zheng, Mei; Wang, Fu; Hagler, G. S. W.; Hou, Ximei; Bergin, Michael; Cheng, Yuan; Salmon, L. G.; Schauer, James J.; Louie, Peter K. K.; Zeng, Limin; Zhang, Yuanhang

    2011-02-01

    Carbonaceous aerosol is one of the important constituents of fine particulate matter (PM 2.5) in southern China, including the Pearl River Delta (PRD) region and Hong Kong (HK). During the study period (October and December of 2002, and March and June of 2003), the monthly average organic carbon (OC) ranged from 3.52 to 7.87 μg m -3 in Hong Kong and 4.14-20.19 μg m -3 in the PRD from simultaneous measurements at three sites in HK and four sites in the PRD. Compared to the PRD, the spatial distribution of carbonaceous aerosol in Hong Kong was relatively homogeneous. Sources contributing to excess OC in the PRD were examined, which is the difference between OC concentrations measured at the PRD sites to the average level in Hong Kong. Eight primary sources contributing to excess OC were identified with chemical mass balance modeling in a combination with molecular markers analyzed by gas chromatography/mass spectrometry. Excess OC at Guangzhou, the capital city of Guangdong province, was consistently high, ranging from 9.77 to 13.6 μg m -3. Four primary sources including gasoline engine exhaust, diesel engine exhaust, biomass burning, and coal combustion accounted for more than 50% of excess OC in the PRD, especially in December (up to 76%). Mobile source emissions alone can contribute about 30% of excess OC. The unexplained or other excess OC was the highest at the rural site, but in general less than 20% at other sites. The coal combustion source contribution was unique in that it exhibited relatively homogeneous spatial distribution, indicating it was still an important source of carbonaceous aerosol in the PRD (17% of excess OC) during the study period. This analysis revealed that primary emissions are important sources of excess OC in the PRD and there is a need to reduce the emissions of mobile sources, biomass burning, and coal combustion in order to improve air quality in southern China.

  17. Determination of primary and secondary sources of organic acids and carbonaceous aerosols using stable carbon isotopes

    NASA Astrophysics Data System (ADS)

    Fisseha, Rebeka; Saurer, Matthias; Jäggi, Maya; Siegwolf, Rolf T. W.; Dommen, Josef; Szidat, Sönke; Samburova, Vera; Baltensperger, Urs

    Stable carbon isotope ratio ( δ13C) data can provide important information regarding the sources and the processing of atmospheric organic carbon species. Formic, acetic and oxalic acid were collected from Zurich city in August-September 2002 and March 2003 in the gas and aerosol phase, and the corresponding δ13C analysis was performed using a wet oxidation method followed by isotope ratio mass spectrometry. In August, the δ13C values of gas phase formic acid showed a significant correlation with ozone (coefficient of determination ( r2) = 0.63) due to the kinetic isotope effect (KIE). This indicates the presence of secondary sources (i.e. production of organic acids in the atmosphere) in addition to direct emission. In March, both gaseous formic and acetic acid exhibited similar δ13C values and did not show any correlation with ozone, indicating a predominantly primary origin. Even though oxalic acid is mainly produced by secondary processes, the δ13C value of particulate oxalic acid was not depleted and did not show any correlation with ozone, which may be due to the enrichment of 13C during the gas - aerosol partitioning. The concentrations and δ13C values of the different aerosol fractions (water soluble organic carbon, water insoluble organic carbon, carbonate and black carbon) collected during the same period were also determined. Water soluble organic carbon (WSOC) contributed about 60% to the total carbon and was enriched in 13C compared to other fractions indicating a possible effect of gas - aerosol partitioning on δ13C of carbonaceous aerosols. The carbonate fraction in general was very low (3% of the total carbon).

  18. The mixing state of carbonaceous aerosol particles in northern and southern California measured during CARES and CalNex 2010

    SciTech Connect

    Cahill, John F.; Suski, Kaitlyn; Seinfeld, John H.; Zaveri, Rahul A.; Prather, Kimberly A.

    2012-11-21

    Carbonaceous aerosols impact climate directly by scattering and absorbing radiation, and hence play a major, although highly uncertain, role in global radiative forcing. Commonly, ambient carbonaceous aerosols are internally mixed with secondary species such as nitrate, sulfate, and ammonium, which influence their climate impacts through optical properties, hygroscopicity, and atmospheric lifetime. Aircraft-aerosol time-of-flight mass spectrometry (A-ATOFMS), which measures single-particle mixing state, was used to determine the fraction of organic and soot aerosols that were internally mixed and the variability of their mixing state in California during the Carbonaceous Aerosol and Radiative Effects Study (CARES) and the Research at the Nexus of Air Quality and Climate Change (CalNex) field campaigns in the late spring and early summer of 2010. Nearly 88% of all A-ATOFMS measured particles (100-1000 nm in diameter) were internally mixed with secondary species, with 96% and 75% of particles internally mixed with nitrate and/or sulfate in southern and northern California, respectively. Even though atmospheric particle composition in both regions was primarily influenced by urban sources, the mixing state was found to vary greatly, with nitrate and soot being the dominant species in southern California, and sulfate and organic carbon in northern California. Furthermore, mixing state varied temporally in northern California, with soot becoming the prevalent particle type towards the end of the study as regional pollution levels increased. The results from these studies demonstrate that the majority of ambient carbonaceous particles are internally mixed and are heavily influenced by secondary species that are most predominant in each region. Based on these findings, considerations of regionally dominant sources and secondary species, as well as temporal variations of aerosol physical and optical properties, will be required to obtain more accurate predictions of the

  19. Composition of carbonaceous smoke particles from prescribed burning of a Canadian boreal forest: 1. Organic aerosol characterization by gas chromatography

    SciTech Connect

    Mazurek, M.A.; Laterza, C.; Newman, L.; Daum, P.; Cofer, W.R. III; Levine, J.S.; Winstead, E.L.

    1995-06-01

    In this study we examine the molecular organic constituents (C8 to C40 lipid compounds) collected as smoke particles from a Canadian boreal forest prescribed burn. Of special interest are (1) the molecular identity of polar organic aerosols, and (2) the amount of polar organic matter relative to the total mass of aerosol particulate carbon. Organic extracts of smoke aerosol particles show complex distributions of the lipid compounds when analyzed by capillary gas chromatography/mass spectrometry. The molecular constituents present as smoke aerosol are grouped into non-polar (hydrocarbons) and polar {minus}2 oxygen atoms) subtractions. The dominant chemical species found in the boreal forest smoke aerosol are unaltered resin compounds (C20 terpenes) which are abundant in unburned conifer wood, plus thermally altered wood lignins and other polar aromatic hydrocarbons. Our results show that smoke aerosols contain molecular tracers which are related to the biofuel consumed. These smoke tracers can be related structurally back to the consumed softwood and hardwood vegetation. In addition, combustion of boreal forest materials produces smoke aerosol particles that are both oxygen-rich and chemically complex, yielding a carbonaceous aerosol matrix that is enriched in polar substances. As a consequence, emissions of carbonaceous smoke particles from large-scale combustion of boreal forest land may have a disproportionate effect on regional atmospheric chemistry and on cloud microphysical processes.

  20. Elucidating carbonaceous aerosol sources by the stable carbon δ13CTC ratio in size-segregated particles

    NASA Astrophysics Data System (ADS)

    Masalaite, A.; Remeikis, V.; Garbaras, A.; Dudoitis, V.; Ulevicius, V.; Ceburnis, D.

    2015-05-01

    Carbonaceous aerosol sources were investigated by measuring the stable carbon isotope ratio (δ13CTC) in size-segregated aerosol particles. The samples were collected with a micro-orifice uniform deposit impactor (MOUDI) in 11 size intervals ranging from 0.056 μm to 18 μm. The aerosol particle size distribution obtained from combined measurements with a scanning mobility particle sizer (SMPS; TSI 3936) and an aerosol particle sizer (APS; TSI 3321) is presented for comparison with MOUDI data. The analysis of δ13CTC values revealed that the total carbonaceous matter in size-segregated aerosol particles significantly varied from - 23.4 ± 0.1‰ in a coarse mode to - 30.1 ± 0.5‰ in a fine mode. A wide range of the δ13CTC values of size-segregated aerosol particles suggested various sources of aerosol particles contributing to carbonaceous particulate matter. Therefore, the source mixing equation was applied to verify the idea of mixing of two sources: continental non-fossil and fossil fuel combustion. The obtained δ13CTC value of aerosol particles originating from fossil fuel combustion was - 28.0 to - 28.1‰, while the non-fossil source δ13CTC value was in the range of - 25.0 to - 25.5‰. The two source mixing model applied to the size-segregated samples revealed that the fossil fuel combustion source contributed from 100% to 60% to the carbonaceous particulate matter in the fine mode range (Dp < 1 μm). Meanwhile, the second source, continental non-fossil, was the main contributor in the coarse fraction (Dp > 2 μm). The particle range from 0.5 to 2.0 μm was identified as a transition region where two sources almost equally contributed to carbonaceous particulate matter. The proposed mixing model offers an alternative method for determining major carbonaceous matter sources where radiocarbon analysis may lack the sensitivity (as in size-segregated samples).

  1. Derivation of optical properties of carbonaceous aerosols by monochromated electron energy-loss spectroscopy.

    PubMed

    Zhu, Jiangtao; Crozier, Peter A; Ercius, Peter; Anderson, James R

    2014-06-01

    Monochromated electron energy-loss spectroscopy (EELS) is employed to determine the optical properties of carbonaceous aerosols from the infrared to the ultraviolet region of the spectrum. It is essential to determine their optical properties to understand their accurate contribution to radiative forcing for climate change. The influence of surface and interface plasmon effects on the accuracy of dielectric data determined from EELS is discussed. Our measurements show that the standard thin film formulation of Kramers-Kronig analysis can be employed to make accurate determination of the dielectric function for carbonaceous particles down to about 40 nm in size. The complex refractive indices of graphitic and amorphous carbon spherules found in the atmosphere were determined over the wavelength range 200-1,200 nm. The graphitic carbon was strongly absorbing black carbon, whereas the amorphous carbon shows a more weakly absorbing brown carbon profile. The EELS approach provides an important tool for exploring the variation in optical properties of atmospheric carbon. PMID:24735494

  2. Isotope source apportionment of carbonaceous aerosol as a function of particle size and thermal refractiveness

    NASA Astrophysics Data System (ADS)

    Masalaite, Agne; Holzinger, Rupert; Remeikis, Vidmantas; Röckmann, Thomas; Dusek, Ulrike

    2016-04-01

    The stable carbon isotopes can be used to get information about sources and processing of carbonaceous aerosol. We will present results from source apportionment of carbonaceous aerosol as a function of particle size thermal refractiveness. Separate source apportionment for particles smaller than 200 nm and for different carbon volatility classes are rarely reported and give new insights into aerosol sources in the urban environment. Stable carbon isotope ratios were measured for the organic carbon (OC) fraction and total carbon (TC) of MOUDI impactor samples that were collected on a coastal site (Lithuania) during the winter 2012 and in the city of Vilnius (Lithuania) during the winter of 2009. The 11 impactor stages spanned a size range from 0.056 to 18 μm, but only the 6 stages in the submicron range were analysed. The δ13C values of bulk total carbon (δ13CTC) were determined with an elemental analyser (Flash EA 1112) coupled with an isotope ratio mass spectrometer (Thermo Finnigan Delta Plus Advantage) (EA - IRMS). Meanwhile δ13COC was measured using thermal-desorption isotope ratio mass spectrometry (IRMS) system. This allows a rough separation of the more volatile OC fraction (desorbed in the oven of IRMS up to 250 0C) from the more refractory fraction (desorbed up to 400 0C). In this study we investigated the composition of organic aerosol desorbed from filter samples at different temperatures using the thermal-desorption proton-transfer-reaction mass spectrometry (TD-PTR-MS) technique. During winter-time in Lithuania we expect photochemistry and biogenic emissions to be of minor importance. The main sources of aerosol carbon should be fossil fuel and biomass combustion. In both sites, the coastal and the urban site, δ13C measurements give a clear indication that the source contributions differ for small and large particles. Small particles < 200 nm are depleted in 13C with respect to larger particles by 1 - 2 ‰Ṫhis shows that OC in small particle

  3. Assessment of the Aerosol Optics Component of the Coupled WRF-CMAQ Model usingCARES Field Campaign data and a Single Column Model

    EPA Science Inventory

    The Carbonaceous Aerosols and Radiative Effects Study (CARES), a field campaign held in central California in June 2010, provides a unique opportunity to assess the aerosol optics modeling component of the two-way coupled Weather Research and Forecasting (WRF) – Community Multisc...

  4. Radiative Effects of Carbonaceous and Inorganic Aerosols over California during CalNex and CARES: Observations versus Model Predictions

    NASA Astrophysics Data System (ADS)

    Vinoj, V.; Fast, J. D.; Liu, Y.

    2012-12-01

    Aerosols have been identified to be a major contributor to the uncertainty in understanding the present climate. Most of this uncertainty arises due to the lack of knowledge of their micro-physical and chemical properties as well as how to adequately represent their spatial and temporal distributions. Increased process level understanding can be achieved through carefully designed field campaigns and experiments. These measurements can be used to elucidate the aerosol properties, mixing, transport and transformation within the atmosphere and also to validate and improve models that include meteorology-aerosol-chemistry interactions. In the present study, the WRF-Chem model is used to simulate the evolution of carbonaceous and inorganic aerosols and their impact on radiation during May and June of 2010 over California when two field campaigns took place: the California Nexus Experiment (CalNex) and Carbonaceous Aerosol and Radiative Effects Study (CARES). We merged CalNex and CARES data along with data from operational networks such as, California Air Resources Board (CARB's) air quality monitoring network, the Interagency Monitoring of Protected Visual Environments (IMPROVE) network, the AErosol RObotic NETwork (AERONET), and satellites into a common dataset for the Aerosol Modeling Test bed. The resulting combined dataset is used to rigorously evaluate the model simulation of aerosol mass, size distribution, composition, and optical properties needed to understand uncertainties that could affect regional variations in aerosol radiative forcing. The model reproduced many of the diurnal, multi-day, and spatial variations of aerosols as seen in the measurements. However, regionally the performance varied with reasonably good agreement with observations around Los Angeles and Sacramento and poor agreement with observations in the vicinity of Bakersfield (although predictions aloft were much better). Some aerosol species (sulfate and nitrate) were better represented

  5. Long-term Observations of Carbonaceous Aerosols (including C isotope) at Alert: Inferring Emission Sources of Black Carbon Transported to the Arctic

    NASA Astrophysics Data System (ADS)

    Huang, Lin; Sharma, Sangeeta; Zhang, Wendy; Brook, Jeff; Leaitch, Richard; He, Kebin; Duan, Fengkui; Yang, Fumo

    2015-04-01

    Black carbon is a major component of carbonaceous aerosols and formed by incomplete combustion of fossil fuels and biomass burning (including biofuels and open fires). It plays unique roles in Earth's climate system through both direct and indirect effects. Identifying and attributing its emission sources, tracking source changes with time and relating them to radiative forcing are important for understanding the impacts of BC on climate at the global and regional levels, as well as necessary for the strategies targeted to reduce BC emission. However, there are many challenges and uncertainties regarding those aspects, particularly for BC aerosols transported to the Arctic region. To address the concerns of BC in the Arctic, carbonaceous aerosol observations, including elemental carbon (EC) content as BC mass, C isotopes as a source tracer, and light absorption coefficient as BC's optical property, have been conducted at Alert, a WMO GAW station (82° 27'N, 62° 31'W) since the early 2000s. In this presentation, nearly a decade of measurements will be presented, with a focus on the isotope results in EC (corresponding data from Beijing will also be shown for the purpose of comparison). Seasonal and inter-annual variations in δ13C (EC) have been characterized, inferring emission sources and suggesting source changes over last 5-6 years. Based on the C isotope results, the possible emission sources of BC contributed to the Arctic will be also discussed.

  6. Urban impacts on regional carbonaceous aerosols: case study in central Texas.

    PubMed

    Barrett, Tate E; Sheesley, Rebecca J

    2014-08-01

    Rural and background sites provide valuable information on the concentration and optical properties of organic, elemental, and water-soluble organic carbon (OC, EC, and WSOC), which are relevant for understanding the climate forcing potential of regional atmospheric aerosols. To quantify climate- and air quality-relevant characteristics of carbonaceous aerosol in the central United States, a regional background site in central Texas was chosen for long-term measurement. Back trajectory (BT) analysis, ambient OC, EC, and WSOC concentrations and absorption parameters are reported for the first 15 months of a long-term campaign (May 2011-August 2012). BT analysis indicates consistent north-south airflow connecting central Texas to the Central Plains. Central Texas aerosols exhibited seasonal trends with increased fine particulate matter (< 2.5 microm aerodynamic diameter, PM2.5) and OC during the summer (PM2.5 = 10.9 microg m(-3) and OC = 3.0 microg m(-3)) and elevated EC during the winter (0.22 microg m(-3)). When compared to measurements in Dallas and Houston, TX, central Texas OC appears to have mixed urban and rural sources. However central Texas EC appears to be dominated by transport of urban emissions. WSOC averaged 63% of the annual OC, with little seasonal variability in this ratio. To monitor brown carbon (BrC), absorption was measured for the aqueous WSOC extracts. Light absorption coefficients for EC and BrC were highest during summer (EC MAC = 11 m2 g(-1) and BRC MAE365 = 0.15 m2 g(-1)). Results from optical analysis indicate that regional aerosol absorption is mostly due to EC with summertime peaks in BrC attenuation. This study represents the first reported values of WSOC absorption, MAE365, for the central United States. Implications: Background concentration and absorption measurements are essential in determining regional potential radiative forcing due to atmospheric aerosols. Back trajectory, chemical, and optical analysis of PM2.5 was used to

  7. Composition and sources of carbonaceous aerosols at three contrasting sites in Hong Kong

    NASA Astrophysics Data System (ADS)

    Zheng, Mei; Hagler, Gayle S. W.; Ke, Lin; Bergin, Michael H.; Wang, Fu; Louie, Peter K. K.; Salmon, Lynn; Sin, Della W. M.; Yu, Jian Zhen; Schauer, James J.

    2006-10-01

    A significant fraction of the fine particulate matter in Hong Kong is made up of organic carbon. In order to quantitatively assess the contributions of various sources to carbonaceous aerosol in Hong Kong, a chemical mass balance (CMB) receptor model in combination with organic tracers was employed. Organic tracers including n-alkanes, polycyclic aromatic hydrocarbons (PAHs), steranes, hopanes, resin acids, cholesterol, levoglucosan, and picene in PM2.5 collected from three air monitoring sites located at roadside, urban, and rural areas in Hong Kong are quantified using gas chromatography-mass spectrometry (GC/MS) in the present study. Analyses of some overlapping species from two separate laboratories will be compared for the first time. Spatial and seasonal source contributions to organic carbon (OC) in PM2.5 from up to nine air pollution sources are assessed, including diesel engine exhaust, gasoline engine exhaust, meat cooking, cigarette smoke, biomass burning, road dust, vegetative detritus, coal combustion, and natural gas combustion. Diesel engine exhaust dominated fine organic carbon in Hong Kong (57 ± 13% at urban sites and 25 ± 2% at the rural site). Other sources that play an important role are meat cooking and biomass burning, which can account for as much as 14% of fine organic carbon. The primary sources identified by this technique explained 49%, 79%, and 94% of the measured fine organic carbon mass concentration at the rural, the urban, and the roadside sites, respectively. The unexplained fine OC is likely due to secondary organic aerosol formation.

  8. A general circulation model study of the global carbonaceous aerosol distribution

    NASA Astrophysics Data System (ADS)

    Cooke, W. F.; Ramaswamy, V.; Kasibhatla, P.

    2002-08-01

    Atmospheric distributions of carbonaceous aerosols are simulated using the Geophysical Fluid Dynamics Laboratory SKYHI general circulation model (GCM) (latitude-longitude resolution of ~3° × 3.6°). A number of systematic analyses are conducted to investigate the seasonal and interannual variability of the concentrations at specific locations and to investigate the sensitivity of the distributions to various physical parameters. Comparisons are made with several observational data sets. At four specific sites (Mace Head, Mauna Loa, Sable Island, and Bondville) the monthly mean measurements of surface concentrations of black carbon made over several years reveal that the model simulation registers successes as well as failures. Comparisons are also made with averages of measurements made over varying time periods, segregated by geography and rural/remote locations. Generally, the mean measured remote surface concentrations exceed those simulated. Notwithstanding the large variability in measurements and model simulations, the simulations of both black and organic carbon tend to be within about a factor of 2 at a majority of the sites. There are major challenges in conducting comparisons with measurements due to inadequate sampling at some sites, the generally short length of the observational record, and different methods used for estimating the black and organic carbon amounts. The interannual variability in the model and in the few such measurements available points to the need for doing multiyear modeling and to the necessity of comparing with long-term measurements. There are very few altitude profile measurements; notwithstanding the large uncertainties, the present comparisons suggest an overestimation by the model in the free troposphere. The global column burdens of black and organic carbon in the present standard model integration are lower than in previous studies and thus could be regarded as approximately bracketing a lower end of the simulated

  9. Source apportionment of carbonaceous aerosol in Sao Paulo using 13C and 14C measurements

    NASA Astrophysics Data System (ADS)

    Oyama, Beatriz; Andrade, Maria de Fatima; Holzinger, Rupert; Röckmann, Thomas; Meijer, Harro A. J.; Dusek, Ulrike

    2016-04-01

    The Metropolitan Area of Sao Paulo is affected by high aerosol concentrations, which contain a large fraction of organic material. Up to date, not much is known about the composition and origin of the organic aerosol in this city. We present the first source apportionment of the carbonaceous aerosol fraction in Sao Paulo, using stable (13C) and radioactive carbon isotopes (14C). 14C provides a clear-cut distinction between fossil sources, which contain no 14C, and contemporary sources such as biofuels, biomass burning, or biogenic sources, which contain a typical contemporary 14C/12C ratio. 13C can be used to distinguish C3 plants, such as maize and sugarcane, from C4 plants. This can help to identify a possible impact of sugarcane field burning in the rural areas of Sao Paulo State on the aerosol carbon in the city. In the first part of the study, we compare two tunnel studies: Tunnel 1 is frequented only by light duty vehicles, which run mainly on mixtures of gasoline with ethanol (gasohol, 25% ethanol and 85% gasoline) or hydrated ethanol (5% water and 95% ethanol). Tunnel 2 contains a significant fraction of heavy-duty diesel vehicles, and therefore the fraction of biofuels in the average fleet is lower. Comparison of 14C in organic and elemental carbon (OC and EC) shows that in both tunnels there is no significant contribution of biofuels to EC. Combusting ethanol-gasoline fuels in a vehicle engine does apparently not result in significant EC formation from ethanol. Biofuels contribute around 45% to OC in Tunnel 1 an only 20% in Tunnel 2, reflecting a strong impact of diesel vehicles in Tunnel 2. In the second part of the study we conduct a source apportionment of ambient aerosol carbon collected in a field study during winter (July-August) 2012. Ambient EC has two main sources, vehicular emissions and biomass burning. We estimate a contribution of vehicular sources to EC of roughly 90% during weekdays and 80% during weekends, using the 14C values measured in

  10. Observationally-constrained carbonaceous aerosol source estimates for the Pearl River Delta area of China

    NASA Astrophysics Data System (ADS)

    Li, N.; Fu, T.-M.; Cao, J. J.; Zheng, J. Y.; He, Q. Y.; Long, X.; Zhao, Z. Z.; Cao, N. Y.; Fu, J. S.; Lam, Y. F.

    2015-11-01

    We simulated elemental carbon (EC) and organic carbon (OC) aerosols over the Pearl River Delta (PRD) area of China and compared the results to seasonal surface measurements, with the aim of quantifying carbonaceous aerosol sources from a "top-down" perspective. Our regional model was driven by current-best estimates of PRD EC (39.5 Gg C yr-1) and OC (32.8 Gg C yr-1) emissions and included updated secondary organic aerosol formation pathways. The simulated annual mean EC and OC concentrations were 4.0 and 7.7 μg C m-3, respectively, lower than the observed annual mean EC and OC concentrations (4.5 and 13.1 μg C m-3, respectively). We used multiple regression to match the simulated EC against seasonal mean observations. The resulting top-down estimate for EC emission in the PRD area was 52.9 ± 8.0 Gg C yr-1. We estimated the OC emission in the PRD area to be 60.2 ± 10.3 Gg C yr-1, based on the top-down EC emission estimate and the primary OC / EC ratios derived from bottom-up statistics. Using these top-down emission estimates, the simulated average annual mean EC and OC concentrations were improved to 4.4 and 9.5 μg C m-3, respectively, closer to the observations. Secondary sources accounted for 42 % of annual mean surface OC in our top-down simulations, with biogenic VOCs being the most important precursors.

  11. Characteristics of carbonaceous aerosol in the region of Beijing, Tianjin, and Hebei, China

    NASA Astrophysics Data System (ADS)

    Zhao, Pusheng; Dong, Fan; Yang, Yadong; He, Di; Zhao, Xiujuan; Zhang, Wenzong; Yao, Qing; Liu, Huaiyu

    2013-06-01

    More than 400 PM2.5 samples were collected at four urban sites in Beijing (BJ), Tianjin (TJ), Shijiazhuang (SJZ), and Chengde (CD), and also one site in Shangdianzi (SDZ), which was used as a regional background station, over four seasons from 2009 to 2010. The organic carbon (OC) and elemental carbon (EC) in each sample were analyzed. The average annual concentrations were 71.8-191.2 μg m-3 for PM2.5, 10.8-26.4 μg m-3 for OC, and 3.9-9.7 μg m-3 for EC at the five sites. OC and EC concentrations were lower in the spring and summer and much higher in the autumn and winter, mainly due to aerosol emissions from additional fuel combustion for heating. OC/EC ratios were lowest in the summer and highest in the winter at SDZ, BJ, TJ, and SJZ. These seasonal trends indicate that the characteristics of carbonaceous aerosol pollution were spatially similar and season-dependent in the plain area of Beijing, Tianjin, and Hebei (BTH). An EC tracer method was used to calculate the concentrations for secondary organic carbon (SOC); SOC concentrations were also higher in the autumn and winter and lowest during the summer at all five sites. A stable atmosphere and low temperatures, which were more frequent during the winter and autumn, facilitated the accumulation of air pollutants and accelerated the condensation or adsorption of volatile organic compounds in the BTH area. Over the past ten years (1999-2009), Beijing had observed a decrease in the EC concentrations during every season and a remarkable reduction in aerosol emissions from coal combustion for heating.

  12. Carbonaceous PM(2.5) and secondary organic aerosol across the Veneto region (NE Italy).

    PubMed

    Khan, Md Badiuzzaman; Masiol, Mauro; Formenton, Gianni; Di Gilio, Alessia; de Gennaro, Gianluigi; Agostinelli, Claudio; Pavoni, Bruno

    2016-01-15

    Organic and elemental carbon (OC-EC) were measured in 360 PM2.5 samples collected from April 2012 to February 2013 at six provinces in the Veneto region, to determine the factors affecting the carbonaceous aerosol variations. The 60 daily samples have been collected simultaneously in all sites during 10 consecutive days for 6 months (April, June, August, October, December and February). OC ranged from 0.98 to 22.34 μg/m(3), while the mean value was 5.5 μg/m(3), contributing 79% of total carbon. EC concentrations fluctuated from 0.19 to 11.90 μg/m(3) with an annual mean value of 1.31 μg/m(3) (19% of the total carbon). The monthly OC concentration gradually increased from April to December. The EC did not vary in accordance with OC. However the highest values for both parameters were recorded in the cold period. The mean OC/EC ratio is 4.54, which is higher than the values observed in most of the other European cities. The secondary organic carbon (SOC) contributed for 69% of the total OC and this was confirmed by both the approaches OC/EC minimum ratio and regression. The results show that OC, EC and SOC exhibited higher concentration during winter months in all measurement sites, suggesting that the stable atmosphere and lower mixing play important role for the accumulation of air pollutant and hasten the condensation or adsorption of volatile organic compounds over the Veneto region. Significant meteorological factors controlling OC and EC were investigated by fitting linear models and using a robust procedure based on weighted likelihood, suggesting that low wind speed and temperature favour accumulation of emissions from local sources. Conditional probability function and conditional bivariate probability function plots indicate that both biomass burning and vehicular traffic are probably the main local sources for carbonaceous particulate matter emissions in two selected cities. PMID:26519578

  13. Transport and Mixing Patterns over Central California during the Carbonaceous Aerosol and Radiative Effects Study (CARES)

    SciTech Connect

    Fast, Jerome D.; Gustafson, William I.; Berg, Larry K.; Shaw, William J.; Pekour, Mikhail S.; Shrivastava, ManishKumar B.; Barnard, James C.; Ferrare, R.; Hostetler, Chris A.; Hair, John; Erickson, Matthew H.; Jobson, Tom; Flowers, Bradley; Dubey, Manvendra K.; Springston, Stephen R.; Pirce, Bradley R.; Dolislager, Leon; Pederson, J. R.; Zaveri, Rahul A.

    2012-02-17

    We describe the synoptic and regional-scale meteorological conditions that affected the transport and mixing of trace gases and aerosols in the vicinity of Sacramento, California during June 2010 when the Carbonaceous Aerosol and Radiative Effects Study (CARES) was conducted. The meteorological measurements collected by various instruments deployed during the campaign and the performance of the chemistry version of the Weather Research and Forecasting model (WRF-Chem) are both discussed. WRF-Chem was run daily during the campaign to forecast the spatial and temporal variation of carbon monoxide emitted from 20 anthropogenic source regions in California to guide aircraft sampling. The model is shown to reproduce the overall circulations and boundary-layer characteristics in the region, although errors in the upslope wind speed and boundary-layer depth contribute to differences in the observed and simulated carbon monoxide. Thermally-driven upslope flows that transported pollutants from Sacramento over the foothills of the Sierra Nevada occurred every afternoon, except during three periods when the passage of mid-tropospheric troughs disrupted the regional-scales flow patterns. The meteorological conditions after the passage of the third trough were the most favorable for photochemistry and likely formation of secondary organic aerosols. Meteorological measurements and model forecasts indicate that the Sacramento pollutant plume was likely transported over a downwind site that collected trace gas and aerosol measurements during 23 periods; however, direct transport occurred during only eight of these periods. The model also showed that emissions from the San Francisco Bay area transported by intrusions of marine air contributed a large fraction of the carbon monoxide in the vicinity of Sacramento, suggesting that this source likely affects local chemistry. Contributions from other sources of pollutants, such as those in the Sacramento Valley and San Joaquin Valley

  14. Transport and mixing patterns over Central California during the carbonaceous aerosol and radiative effects study (CARES)

    SciTech Connect

    Fast J. D.; Springston S.; Gustafson Jr., W. I.; Berg, L. K.; Shaw, W. J.; Pekour, M.; Shrivastava, M.; Barnard, J. C.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. A.; Erickson, M.; Jobson, B. T.; Flowers, B.; Dubey, M. K.; Pierce, R. B.; Dolislager, L.; Pederson, J.; Zaveri, R. A.

    2012-02-17

    We describe the synoptic and regional-scale meteorological conditions that affected the transport and mixing of trace gases and aerosols in the vicinity of Sacramento, California during June 2010 when the Carbonaceous Aerosol and Radiative Effects Study (CARES) was conducted. The meteorological measurements collected by various instruments deployed during the campaign and the performance of the chemistry version of the Weather Research and Forecasting model (WRF-Chem) are both discussed. WRF-Chem was run daily during the campaign to forecast the spatial and temporal variation of carbon monoxide emitted from 20 anthropogenic source regions in California to guide aircraft sampling. The model is shown to reproduce the overall circulations and boundary-layer characteristics in the region, although errors in the upslope wind speed and boundary-layer depth contribute to differences in the observed and simulated carbon monoxide. Thermally-driven upslope flows that transported pollutants from Sacramento over the foothills of the Sierra Nevada occurred every afternoon, except during three periods when the passage of mid-tropospheric troughs disrupted the regional-scale flow patterns. The meteorological conditions after the passage of the third trough were the most favorable for photochemistry and likely formation of secondary organic aerosols. Meteorological measurements and model forecasts indicate that the Sacramento pollutant plume was likely transported over a downwind site that collected trace gas and aerosol measurements during 23 time periods; however, direct transport occurred during only eight of these periods. The model also showed that emissions from the San Francisco Bay area transported by intrusions of marine air contributed a large fraction of the carbon monoxide in the vicinity of Sacramento, suggesting that this source likely affects local chemistry. Contributions from other sources of pollutants, such as those in the Sacramento Valley and San Joaquin

  15. Characteristics of carbonaceous aerosols at a pair of suburban and downtown sites in Nanjing, China

    NASA Astrophysics Data System (ADS)

    Cui, H.; Zhang, J.; Zhao, Y.

    2014-12-01

    Carbonaceous species in PM2.5 were measured in three seasons (except winter) in downtown and around a year in suburban in Nanjing. In particular, the OC and EC concentrations were continuously measured with 1-h interval at both sites. The mean concentrations of PM2.5, OC, EC were 85.9 μg/m3, 10.4 μg/m3, 4.2 μg/m3 and 63.4 μg/m3, 8.1 μg/m3, 5.3μg/m3 for downtown and suburban respectively. At the suburban site, compared to the lowest average concentration in spring, the relatively higher concentration of carbonaceous aerosol in summer was caused by biomass-burning activities. Significant increasing peaks of OC (up to 122.9 ug/m3) and EC (up to 35.8 ug/m3) in suburban were recorded in the June 10th night, and it is indicated using back trajectory that the air mass came through nearby agriculture areas. On the other hand, the OC and EC concentrations during the 2nd AYG (Asian Youth Games, Aug 16th - 24th in 2013) compared to that in rest days in August reduced by 21% and 10%, respectively, attributing to the effective control measures on reduction of industrial point sources, temporary control of motor vehicle and fugitive dusts. Rations of OC/EC in suburban were much lower than that in downtown. This might be due to the fact that the sampling point in suburban is quite close (in 400 meters) to a main highway. Both OC and EC concentrations in suburban were higher in nighttime than daytime, except OC in summer, indicating the existence of strong SOC and supported by high OC/EC and O3 at noon. The annual average SOC estimated by EC-tracer methods occupied 34.5% and 36.7% of the total OC for the downtown and suburban areas, respectively. OC/EC correlations in suburban were much weaker than those from downtown areas, which shows suburban areas is much more affected by long-range transport of pollution and/or complex sources including domestic coal combustion, biomass burning, industrial and transportation, especially in three other seasons except winter, which is

  16. Characteristics and sources of PM2.5-bound carbonaceous aerosols in the Yangtze River Delta, China

    NASA Astrophysics Data System (ADS)

    Hong, Youwei; Hong, Zhenyu; Chen, Jinsheng

    2016-04-01

    An investigation of atmospheric fine particle (PM2.5) from Shanghai, Nanjing and Ningbo in the Yangtze River Delta was conducted during Nov 2014 and Aug 2015. Organic species, including 16 polycyclic aromatic hydrocarbons (PAHs), 10 nitro-PAHs and C8 to C40 n-alkanes, and stable carbon isotopes OC (δ13COC) and EC (δ13CEC) were used to evaluate carbonaceous aerosols' spatiotemporal variations and identify their potential sources. The averaged concentrations of total PAHs and n-alkanes in Shanghai, Nanjing and Ningbo were 16.5 and 101.1 ng m-3, 21.1 and 128.2 ng m-3, 33.0 and 241.1 ng m-3, respectively, while the mean concentrations of 10 nitro-PAHs was 2.02, 2.37 and 2.70 ng m-3. Seasonal variations of organic compounds were listed in the following order: winter > autumn > spring > summer. N-alkanes detected in PM2.5 were characterized by odd carbon number preference, with a unimodal peak shape. The maximum carbon number (Cmax) was C29, followed by C27 and C31. According to diagnostic ratios and principle components analysis (PCA) methods, vehicle emissions and coal burning were the dominant sources of PAHs. The ratios of 2-nitrofluoranthene to 1-nitropyrene were larger than 5, indicating that atmospheric transformation from PAHs was a major source of nitro-PAHs. Meanwhile, primary emissions tracers i.e., 1-nitropyrene (the mean concentration of 0.024 ng m-3 in all cities) was observed, suggesting primary contribution of motor vehicle exhaust to the fine particulate organic aerosols. In addition, isotope abundances (δ13COC=‑24.6±0.8‰ and δ13CEC = ‑23.9±1.4‰) and EC/TC ratio (0.2 < EC/TC < 0.5) in Shanghai demonstrated that fossil fuels (e.g. motor vehicles) were the most important source for carbonaceous PM2.5. We further focus on radiocarbon (14C) analysis and gas/particle partitioning of organic tracers on different size particles. Keywords: organic tracers; stable carbon isotopes; spatiotemporal variations; sources apportionment; Yangtze River Delta

  17. Spatial variability of carbonaceous aerosols and associated source tracers in two cites in the Midwestern United States

    NASA Astrophysics Data System (ADS)

    Snyder, David C.; Rutter, Andrew P.; Worley, Chris; Olson, Mike; Plourde, Anthony; Bader, Rebecca C.; Dallmann, Timothy; Schauer, James J.

    2010-05-01

    Semi-continuous and 24-h averaged measurements of fine carbonaceous aerosols were made concurrently at three sites within each of two U.S. Midwestern Cities; Detroit, Michigan and Cleveland, Ohio; during two, one-month intensive campaigns conducted in July of 2007 and January & February of 2008. A comparison of 24-h measurements revealed substantial intra-urban variability in carbonaceous aerosols consistent with the influence of local sources, and excesses in both PM 2.5 organic carbon (OC) and elemental carbon (EC) were identified at individual sites within each city. High time-resolved black carbon (BC) measurements indicated that elemental carbon concentrations were higher at sites adjacent to freeways and busy surface streets, and temporal patterns suggested that excess EC at sites adjacent to freeways was dominated by mobile source emissions while excesses in EC away from traffic corridors was dominated by point/area source emissions. The site-to-site variability in OC concentrations was approximately 7% within the neighborhood scale (0.5-4 km) and between 4 and 27% at the urban scale (4-100 km). In contrast, measurements of organic source tracers, in conjunction with a Chemical Mass Balance (CMB) source-apportionment model, indicated that the spatial variation in the contribution of both mobile and stationary sources to PM 2.5 OC often exceeded the variation in OC mass concentration by a factor of 3 or more. Markers for mobile sources, biomass smoke, natural gas, and coal combustion differed by as much as 60% within the neighborhood scale and by greater than 200% within the urban scale. The observations made during this study suggest that the urban excess of carbonaceous aerosols is much more complex than has been previously reported and that a more rigorous, source-oriented approach should be taken in order to assess the risk associated with exposure to carbonaceous aerosols within the industrialized environments of the Midwestern United States.

  18. Formation of secondary organic carbon and cloud impact on carbonaceous aerosols at Mount Tai, North China

    NASA Astrophysics Data System (ADS)

    Wang, Zhe; Wang, Tao; Guo, Jia; Gao, Rui; Xue, Likun; Zhang, Jiamin; Zhou, Yang; Zhou, Xuehua; Zhang, Qingzhu; Wang, Wenxing

    2012-01-01

    Carbonaceous aerosols measured at Mount Tai in north China in 2007 were further examined to study the formation of secondary organic carbon (SOC) and the impact of clouds on carbonaceous species. A constrained EC-tracer method and a multiple regression model showed excellent agreement in estimating SOC concentration. The average concentrations of non-volatile and semi-volatile SOC (SOC NV and SOC SV) were 2.61, 5.58 μg m -3 in spring and 2.81, 10.44 μg m -3 in summer. The total SOC accounted for 57.3% and 71.2% of total organic carbon in spring and summer, respectively, indicating the presence of high loading of secondary organic aerosol (SOA) in the North China Plain. The fraction of SOC NV increased with photochemical age (as indicated by NO x/NO y ratios) of air mass, whereas SOC SV was also influenced by the dynamic equilibrium between formation and sink. Significant scavenging by clouds of non-volatile organic carbon (OC NV) and elemental carbon (EC) was observed, whereas semi-volatile organic carbon (OC SV) concentrations increased during clouds, suggesting substantial SOA formation through aqueous-phase reactions in clouds. A mass balance model was proposed to quantify the scavenging coefficients for OC NV, EC and formation rates of OC SV in clouds. The scavenging coefficient constant of EC ( KEC) varied from 0.11 to 0.90 h -1, and was higher than that of OC NV ( KNV-OC: 0.07-0.55 h -1), implying internal mixing of EC with more hygroscopic species. The formation rate constant ( JSV-OC) and sink constant ( SSV-OC) of OC SV ranged from 0.09 to 1.39 h -1 and 0.001 to 1.07 h -1, respectively. These field derived parameters could be incorporated into atmospheric models to help close the gap between predicted and observed SOA loadings in the atmosphere.

  19. Carbonaceous aerosols recorded in a Southeastern Tibetan glacier: variations, sources and radiative forcing

    NASA Astrophysics Data System (ADS)

    Wang, M.; Xu, B.; Cao, J.; Tie, X.; Wang, H.; Zhang, R.; Qian, Y.; Rasch, P. J.; Zhao, S.; Wu, G.; Zhao, H.; Joswiak, D. R.; Li, J.; Xie, Y.

    2014-07-01

    High temporal resolution measurements of black carbon (BC) and organic carbon (OC) covering the time period of 1956-2006 in an ice core over the southeastern Tibetan Plateau show a distinct seasonal dependence of OC / BC ratio with higher values in the non-monsoon season than during the summer monsoon. We use a global aerosol-climate model, in which BC emitted from different source regions can be explicitly tracked, to quantify BC source-receptor relationships between four Asian source regions and the southeastern Tibetan Plateau as a receptor. The model results show that South Asia is a primary contributor during the non-monsoon season (October to May) (81%) and on an annual basis (74%), followed by East Asia (14% and 21%, respectively). The ice-core record also indicates stable and relatively low BC and OC deposition fluxes from late 1950s to 1980, followed by an overall increase to recent years. This trend is consistent with the BC and OC emission inventories and the fuel consumption of South Asia as the primary contributor. Moreover, the increasing trend of OC / BC ratio since the early 1990s indicates a growing contribution of coal combustion and biomass burning to the emissions. The estimated radiative forcing induced by BC and OC impurities in snow has increased since 1980, suggesting an increasing influence of carbonaceous aerosols on the Tibetan glacier melting and the availability of water resources in the surrounding regions. Our study indicates that more attention to OC is merited because of its non-negligible light absorption and the recent rapid increases evident in the ice core record.

  20. Dual carbon isotope characterization of total organic carbon in wintertime carbonaceous aerosols from northern India

    NASA Astrophysics Data System (ADS)

    Bikkina, Srinivas; Andersson, August; Sarin, M. M.; Sheesley, R. J.; Kirillova, E.; Rengarajan, R.; Sudheer, A. K.; Ram, K.; Gustafsson, Örjan

    2016-05-01

    Large-scale emissions of carbonaceous aerosols (CA) from South Asia impact both regional climate and air quality, yet their sources are not well constrained. Here we use source-diagnostic stable and radiocarbon isotopes (δ13C and Δ14C) to characterize CA sources at a semiurban site (Hisar: 29.2°N, 75.2°E) in the NW Indo-Gangetic Plain (IGP) and a remote high-altitude location in the Himalayan foothills (Manora Peak: 29.4°N, 79.5°E, 1950 m above sea level) in northern India during winter. The Δ14C of total aerosol organic carbon (TOC) varied from -178‰ to -63‰ at Hisar and from -198‰ to -1‰ at Manora Peak. The absence of significant differences in the 14C-based fraction biomass of TOC between Hisar (0.81 ± 0.03) and Manora Peak (0.82 ± 0.07) reveals that biomass burning/biogenic emissions (BBEs) are the dominant sources of CA at both sites. Combining this information with δ13C, other chemical tracers (K+/OC and SO42-/EC) and air mass back trajectory analyses indicate similar source regions in the IGP (e.g., Punjab and Haryana). These results highlight that CA from BBEs in the IGP are not only confined to the atmospheric boundary layer but also extend to higher elevations of the troposphere, where the synoptic-scale circulations could substantially influence their abundances both to the Himalayas and over the downwind oceanic regions such as the Indian Ocean. Given the vast emissions of CA from postharvest crop residue combustion practices in the IGP during early Northeast Monsoon, this information is important for both improved process and model understanding of climate and health effects, as well as in guiding policy decision aiming at reducing emissions.

  1. Organic composition of carbonaceous aerosols in an aged prescribed fire plume

    NASA Astrophysics Data System (ADS)

    Yan, B.; Zheng, M.; Hu, Y. T.; Lee, S.; Kim, H. K.; Russell, A. G.

    2007-12-01

    Aged smoke from a prescribed fire (dominated by conifers) impacted Atlanta, GA on 28 February 2007 and dramatically increased hourly ambient concentrations of PM2.5 and organic carbon (OC) up to 140 and 72 μg m-3, respectively. It was estimated that over 1 million residents were exposed to the smoky air lasting from the late afternoon to midnight. To better understand the processes impacting the aging of fire plumes, a detailed chemical speciation of carbonaceous aerosols was conducted by gas chromatography/mass spectrometry (GC/MS) analysis. Ambient concentrations of many organic species (levoglucosan, resin acids, retene, n-alkanes, n-alkanoic acids) associated with wood burning emission were significantly elevated on the event day. Levoglucosan increased by a factor of 10, while hopanes, steranes, cholesterol and major polycyclic aromatic hydrocarbons (PAHs) did not show obvious increases. Strong odd over even carbon number predominance was found for n-alkanes versus even over odd predominance for n-alkanoic acids. Alteration of resin acids during transport from burning sites to monitors is suggested by the observations. Our study also suggests that large quantities of biogenic volatile organic compounds (VOCs) and semivolatile organic compounds (SVOCs) were released both as products of combustion and unburned vegetation heated by the fire. Higher leaf temperature can stimulate biogenic VOC and SVOC emissions, which enhanced formation of secondary organic aerosols (SOA) in the atmosphere. This is supported by elevated ambient concentrations of secondary organic tracers (dicarboxylic acids, 2-methyltetrols, pinonic acid and pinic acid). An approximate source profile was built for the aged fire plume to help better understand evolution of wood smoke emission and can be used for source apportionment.

  2. Organic composition of carbonaceous aerosols in an aged prescribed fire plume

    NASA Astrophysics Data System (ADS)

    Yan, B.; Zheng, M.; Hu, Y. T.; Lee, S.; Kim, H. K.; Russell, A. G.

    2008-11-01

    Aged smoke from a prescribed fire (dominated by conifers) impacted Atlanta, GA on 28 February 2007 and dramatically increased hourly ambient concentrations of PM2.5 and organic carbon (OC) up to 140 and 72 μg m-3, respectively. It was estimated that over 1 million residents were exposed to the smoky air lasting from the late afternoon to midnight. To better understand the processes impacting the aging of fire plumes, a detailed chemical speciation of carbonaceous aerosols was conducted by gas chromatography/mass spectrometry (GC/MS) analysis. Ambient concentrations of many organic species (levoglucosan, resin acids, retene, n-alkanes and n-alkanoic acids) associated with wood burning emission were significantly elevated on the event day. Levoglucosan increased by a factor of 10, while hopanes, steranes, cholesterol and major polycyclic aromatic hydrocarbons (PAHs) did not show obvious increases. Strong odd over even carbon number predominance was found for n-alkanes versus even over odd predominance for n-alkanoic acids. Alteration of resin acids during transport from burning sites to monitors is suggested by the observations. Our study also suggests that large quantities of biogenic volatile organic compounds (VOCs) and semivolatile organic compounds (SVOCs) were released both as products of combustion and unburned vegetation heated by the fire. Higher leaf temperature can stimulate biogenic VOC and SVOC emissions, which enhanced formation of secondary organic aerosols (SOA) in the atmosphere. This is supported by elevated ambient concentrations of secondary organic tracers (dicarboxylic acids, 2-methyltetrols, pinonic acid and pinic acid). An approximate source profile was built for the aged fire plume to help better understand evolution of wood smoke emission and for use in source impact assessment.

  3. Comparison of PM2.5 carbonaceous aerosols in the northeast Asian regions

    NASA Astrophysics Data System (ADS)

    Chang, M.; Lee, M.; Lim, S.; Kim, J.

    2009-12-01

    Aerosols are composed of various chemical species such as ions, organic carbon (OC) and elemental carbon (EC). Among these, organic carbon and elemental carbon were analyzed as 8 fractions (OC1,OC2,OC3,OC4,EC1,EC2,EC3) by TOT/TOR (Thermal Optical transmission/Reflectance method),using IMPROVED protocol method. This study had been performed at Seoul metropolis, Gosan supersite in Jeju and Ieodo in the East China Sea from August 2007 to June 2008. Mean concentrations of OC and EC in PM2.5 are 9.757μg/m3, 4.648μg/m3 (Seoul), 3.95μg/m3, 1.69μg/m3 (Jeju) and 2.43μg/m3, 1.01μg/m3 (Ieodo). OC to EC ratios were 2.39, 2.63 and 2.82 at Seoul, Jeju and Ieodo in respectively. Organic matter and elemental carbon are composed 47% and 16% (Seoul), 23.3% and 10.0% (Jeju) and 26% and 5% (Ieodo). Three stations showed different behaviors of OC and EC. Detailed results for Characteristics of carbonaceous compositions will be discussed in the meeting.

  4. Characteristics and origins of carbonaceous aerosol in the Sichuan Basin, China

    NASA Astrophysics Data System (ADS)

    Chen, Yuan; Xie, Shaodong; Luo, Bin; Zhai, Chongzhi

    2014-09-01

    The Sichuan Basin is a low visibility area in southwest China, where the hilly and basin topography, plus humid and stagnant weather, lead to unique pollution patterns. To identify the characteristics and sources of carbonaceous aerosols, one-year record of 24-h PM2.5 samples were analyzed for organic carbon (OC) and elemental carbon (EC) content following the thermal/optical transmission protocol at three cities (Chengdu (CD), Neijiang (NJ), and Chongqing (CQ)) in the region during May 2012 to April 2013. The annual average concentrations were 19.0 ± 13.3 μg OC m-3 and 4.6 ± 2.6 μg EC m-3 in CD, 18.3 ± 8.4 μg OC m-3 and 4.1 ± 1.8 μg EC m-3 in NJ, and 15.2 ± 8.4 μg OC m-3 and 4.0 ± 1.6 μg EC m-3 in CQ, respectively. Organic matter (1.6OC) plus EC contributed about 40% of PM2.5 mass and displayed weak regional uniformity. Relatively high ratios of OC to EC were observed in the region with 4.3 for CD, 4.6 for NJ, and 3.8 for CQ, respectively. OC and EC pollution in the region exhibited interesting season-dependent characteristics with the lowest concentrations and OC/EC ratios in summer, but higher levels in other seasons. Higher OC/EC ratios in spring and autumn resulted from biomass burning, and in winter were from the enhanced secondary organic aerosol formation under favorable conditions. The exceptionally high OC and EC levels in May and October, mostly notable in CD, resulted from the burning of agricultural residues during harvest period. The high K+ concentrations and the high Kexcess/EC ratios implied the persistent influence of biomass burning throughout the year. Using a novel technique combing the EC tracer method and potassium mass balance in the aerosols, a K/EC ratio of 1.22 was used to retrieve the OC from biomass burning and the estimated contributions were 30.8%, 28.3%, and 21.9% in CD, NJ, and CQ, respectively, while secondary OC contributions to OC were 26.7%, 24.6%, and 25.7% in CD, NJ, and CQ, respectively.

  5. Characteristics of PM2.5 Carbonaceous Aerosol in Urban New York State

    NASA Astrophysics Data System (ADS)

    Khwaja, H. A.; Dutkiewicz, V.; Briggs, R.; Siddique, A.; Regan, J.

    2008-12-01

    In order to investigate the characteristics of carbonaceous fine aerosols, PM2.5 and size-segregated particulate samples (< 2.5 um, 2.5 - 4.2 um, 4.2 - 10 um, and 10 um) were collected during the summer in two urban sites of New York State viz., Botanical Garden (BTG), New York City and Empire State Plaza (ESP), Albany. Gas phase organic compounds were sampled with polyurethane foam (PUF) plugs. Particulate samples were acquired on quartz fiber filters using a high-volume air sampler (Hi-Vol) attached with a slotted impactor. Filters were sonicated in dichloromethane:methanol (9:1); extracts concentrated. A suite of more than 200 individual organic compounds was identified in the PM2.5 samples. Molecular markers, homologous compound series, and non-polar and polar organic compounds were detected at ng/m3 ambient concentrations using gas chromatography/mass spectrometry (GC/MS). Measurements of the organic carbon (OC) and elemental carbon (EC) were also made. Organic compounds detected in the size-segregated samples were grouped into different classes including phthalates and adipates, n-alkanes, alkanoic acids, cyclic siloxanes, waxes, benzoates, polyethylene glycols, squalene, and 4-nitro-butylated phenol. Results indicated that these organic species were predominantly associated in the fine particle mode (< 2.5 um). Gaseous organic compounds trapped in the PUF appeared rich in phenol, 4-nitro-2,6-ditertbutylphenol, pentachlorophenol, benzoic acid, alkanoic acids (C6 - C16 ), PAHs (naphthalene to pyrene), and phthalates. The major part of the extractable and elutable organic carbon was found to correspond to a complex mixture of phthalates and adipates, benzoate esters, n-alkanes, methyl silicates, phosphate esters, aldehydes and ketones, alcohols, alkyl amines, nitrosamines, formamides, amides, morpholines, carboxylic acids, methyl and isopropyl esters, dicarboxylic acids, waxes, lactones, hopanes, ionol 2, and PAHs. The most abundant classes of compounds are

  6. Powder X-Ray Diffraction of the Grain Components of Carbonaceous Chondrite Meteorites.

    NASA Astrophysics Data System (ADS)

    Furton, D. G.; Hurt, Kendra; Bos, Abram

    Carbonaceous chondrite meteorites are thought to bring to Earth samples of primordial interstellar material. Detailed chemical analysis of meteorites representative of this class (i.e., Allende, Murchison, and Orgueil) establish the primordial character of the material they include and, among other things, reveal that nanometer-sized diamond grains are present in the carbonaceous component of these meteorites at about the 1,000 ppm level (Lewis et al. 1987, Nature, 326, 160). The high abundance of nanodiamonds in these meteoritic samples contributes to the hypothesis that nanodiamonds are present in the interstellar medium at relatively high abundance, but direct observational support of this hypothesis is not so conclusive. (It may also be, according to Dai et al. (2002, Nature, 418, 157), that the nanodiamond grains were formed in situ). On the other hand, there is a growing body of observational evidence that indicates nanometer-sized silicon grains are present in the interstellar medium at relatively high abundance (e.g., Smith & Witt 2001, ApJ, 565, 304). But, silicon nanoparticles have yet to be discovered in a sample of carbonaceous chondrite meteorite. It is relevant in this context that the chemical process that has been used to extract nanodiamond grains from meteoritic samples involves dissolving in strong acid the silicate component of the meteorite. The process is ultimately destructive to any silicon grains that may be present and possibly even alters the nanodiamonds it is used to extract (Mutschke et al. 1995, ApJL, 454, L160). There does not appear to be a similar chemical process that could be used to extract silicon nanoparticles from meteoritic samples. We are in the process of establishing to what extent powder X-ray diffraction can be use as a non-destructive analytical tool to examine nanometer-sized grain components of carbonaceous chondrite meteorites. We present powder X-ray diffraction patterns obtained from samples of the Murchison and

  7. Carbonaceous aerosol characteristics over a Pinus taeda plantation: Results from the CELTIC experiment

    NASA Astrophysics Data System (ADS)

    Geron, Chris

    2011-01-01

    Carbonaceous particles smaller than 2.5 μm aerodynamic diameter (PM 2.5) were collected in July, 2003 over a Loblolly Pine plantation at Duke Forest, NC during the Chemical Emission, Loss, Transformation and Interactions within Canopies (CELTIC) field study. Organic (OC) and elemental (EC) carbon in PM 2.5 ranged from 1.4-6.3 and 0.08-0.41 μg C m -3, respectively, and concentrations measured above and below the pine canopy were in good agreement. Ambient OC was lower (<3 μg C m -3) during cooler periods (daytime maximum temperatures < 28 °C) and for periods following precipitation events, and was higher (>3 μg C m -3) during warm humid periods. Radiocarbon analysis indicates that on average 83% (range 78-91%) of the PM 2.5 carbon was derived from contemporary (biogenic VOC and biomass burning) sources. This is higher than previous estimates from urban and suburban sites, and in good agreement with recently published data from other rural sites throughout the U.S. The estimates of contemporary PM 2.5 carbon may represent a lower limit for this site since the sampler was located above the center of a 30 meter diameter plot fumigated with 200 ppm CO 2 derived from fossil carbon sources. However, this effect is likely to be negligible. The regression relationship between OC/EC ratios and percent biogenic carbon in aerosol is very similar to those observed in recent summertime data from Tennessee and Florida. However, our values for both OC/EC and percent biogenic carbon are higher than those observed in the latter studies, likely due to the more rural character of the site. Simple box model estimates indicate that biogenic VOC (BVOC) emissions measured at the site provide sufficient reactive carbon sources to account for the observed levels of aerosol biogenic carbon. The magnitude and temporal pattern in the box model secondary organic aerosol estimates correlate well with the ambient aerosol carbon measurements. The model estimates of the relative contribution

  8. Enhanced UV Absorption in Carbonaceous Aerosols during MILAGRO and Identification of Potential Organic Contributors.

    NASA Astrophysics Data System (ADS)

    Mangu, A.; Kelley, K. L.; Marchany-Rivera, A.; Kilaparty, S.; Gunawan, G.; Gaffney, J. S.; Marley, N. A.

    2007-12-01

    Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) during the month of March, 2006 by using a 7- channel aethalometer (Thermo-Anderson). These measurements, obtained at 370, 470, 520, 590, 660, 880, and 950 nm at a 5 minute time resolution, showed an enhanced absorption in the UV over that expected from carbon soot alone. Samples of fine atmospheric aerosols (less than 0.1micron) were also collected at site T0 and T1 (Universidad Technologica de Tecamac, State of Mexico) from 5 am to 5 pm (day) and from 5 pm to 5 am (night) during the month of March 2006. The samples were collected on quartz fiber filters with high volume impactor samplers. The samples have been characterized for total carbon content (stable isotope ratio mass spectroscopy) and natural radionuclide tracers (210Pb, 210Po, 210Bi, 7Be, 13C, 14C, 40K, 15N). Continuous absorption spectra of these aerosol samples have been obtained in the laboratory from 280 to 900nm with the use of an integrating sphere coupled to a UV-visible spectrometer (Beckman DU with a Labsphere accessory). The integrating sphere allows the detector to collect and spatially integrate the total radiant flux reflected from the sample and therefore allows for the measurement of absorption on highly reflective or diffusely scattering samples (1). The continuous spectra also show an enhanced UV absorption over that expected from carbon soot and the general profiles are quite similar to those observed for humic and fulvic acids found as colloidal materials in surface and groundwaters (2), indicating the presence of humic-like substances (HULIS) in the fine aerosols. The spectra also show evidence of narrow band absorbers below 400 nm typical of polycyclic aromatics (PAH) and nitrated aromatic compounds. Spectra were also obtained on NIST standard diesel soot (SRM 2975), NIST standard air particulate matter (SRM 8785

  9. Variability of carbonaceous aerosols in remote, rural, urban and industrial environments in Spain: implications for air quality policy

    NASA Astrophysics Data System (ADS)

    Querol, X.; Alastuey, A.; Viana, M.; Moreno, T.; Reche, C.; Minguillón, M. C.; Ripoll, A.; Pandolfi, M.; Amato, F.; Karanasiou, A.; Pérez, N.; Pey, J.; Cusack, M.; Vázquez, R.; Plana, F.; Dall'Osto, M.; de la Rosa, J.; de la Campa Sánchez, A.; Fernández-Camacho, R.; Rodríguez, S.; Pío, C.; Alados-Arboledas, L.; Titos, G.; Artíñano, B.; Salvador, P.; Dos Santos García, S.; Patier Fernández, R.

    2013-03-01

    We interpret here the variability of levels of carbonaceous aerosols based on a 12-yr database from 78 monitoring stations across Spain especially compiled for this article. Data did not evidence any spatial trends of carbonaceous aerosols across the country. Conversely, results show marked differences in average concentrations from the cleanest, most remote sites (around 1 μg m-3 of non-mineral carbon (nmC), mostly made of organic carbon (OC), with very little elemental carbon (EC) 0.1 μg m-3; OC/EC = 12-15), to the highly polluted major cities (8-10 μg m-3 of nmC; 3-4 μg m-3 of EC; 4-5 μg m-3 of OC; OC/EC = 1-2). Thus, urban (and very specific industrial) pollution was found to markedly increase levels of carbonaceous aerosols in Spain, with much lower impact of biomass burning. Correlations between yearly averaged OC/EC and EC concentrations adjust very well to a potential equation (OC/EC = 3.37 EC-0.67 R2 = 0.94). A similar equation is obtained when including average concentrations obtained at other European sites (y = 3.61x-0.5, R2 = 0.78). A clear seasonal variability in OC and EC concentrations was detected. Both OC and EC concentrations were higher during winter at the traffic and urban sites, but OC increased during the warmer months at the rural sites. Hourly equivalent black carbon (EBC) concentrations at urban sites accurately depict road traffic contributions, varying with distance to road, traffic volume and density, mixing layer height and wind speed. Weekday urban rush-hour EBC peaks are mimicked by concentrations of primary gaseous emissions from road traffic, whereas a single midday peak is characteristic of remote and rural sites. Decreasing annual trends for carbonaceous aerosols were observed between 1999 and 2011 at a large number of stations, probably reflecting the impact of the EURO4 and EURO5 standards in reducing the diesel PM emissions. This has resulted in some cases in an increasing trend of NO2/OC+EC ratios, because these

  10. Variability of carbonaceous aerosols in remote, rural, urban and industrial environments in Spain: implications for air quality policy

    NASA Astrophysics Data System (ADS)

    Querol, X.; Alastuey, A.; Viana, M.; Moreno, T.; Reche, C.; Minguillón, M. C.; Ripoll, A.; Pandolfi, M.; Amato, F.; Karanasiou, A.; Pérez, N.; Pey, J.; Cusack, M.; Vázquez, R.; Plana, F.; Dall'Osto, M.; de la Rosa, J.; Sánchez de la Campa, A.; Fernández-Camacho, R.; Rodríguez, S.; Pio, C.; Alados-Arboledas, L.; Titos, G.; Artíñano, B.; Salvador, P.; García Dos Santos, S.; Fernández Patier, R.

    2013-07-01

    We interpret here the variability of levels of carbonaceous aerosols based on a 12 yr database from 78 monitoring stations across Spain specially compiled for this article. Data did not evidence any spatial trends of carbonaceous aerosols across the country. Conversely, results show marked differences in average concentrations from the cleanest, most remote sites (around 1 μg m-3 of non-mineral carbon (nmC), mostly made of organic carbon (OC) with very little elemental carbon (EC), around 0.1 μg m-3; OC / EC = 12-15), to the highly polluted major cities (8-10 μg m-3 of nmC; 3-4 μg m-3 of EC; 4-5 μg m-3 of OC; OC / EC = 1-2). Thus, urban (and very specific industrial) pollution was found to markedly increase levels of carbonaceous aerosols in Spain, with much lower impact of biomass burning and of biogenic emissions. Correlations between yearly averaged OC / EC and EC concentrations adjust very well to a potential equation (OC = 3.37 EC0.326, R2 = 0.8). A similar equation is obtained when including average concentrations obtained at other European sites (OC = 3.60EC0.491, R2 = 0.7). A clear seasonal variability in OC and EC concentrations was detected. Both OC and EC concentrations were higher during winter at the traffic and urban sites, but OC increased during the warmer months at the rural sites. Hourly equivalent black carbon (EBC) concentrations at urban sites accurately depict road traffic contributions, varying with distance from road, traffic volume and density, mixing-layer height and wind speed. Weekday urban rush-hour EBC peaks are mimicked by concentrations of primary gaseous emissions from road traffic, whereas a single midday peak is characteristic of remote and rural sites. Decreasing annual trends for carbonaceous aerosols were observed between 1999 and 2011 at a large number of stations, probably reflecting the impact of the EURO4 and EURO5 standards in reducing the diesel PM emissions. This has resulted in some cases in an increasing trend for

  11. Origins and composition of fine atmospheric carbonaceous aerosol in the Sierra Nevada Mountains, California

    NASA Astrophysics Data System (ADS)

    Worton, D. R.; Goldstein, A. H.; Farmer, D. K.; Docherty, K. S.; Jimenez, J. L.; Gilman, J. B.; Kuster, W. C.; de Gouw, J.; Williams, B. J.; Kreisberg, N. M.; Hering, S. V.; Bench, G.; McKay, M.; Kristensen, K.; Glasius, M.; Surratt, J. D.; Seinfeld, J. H.

    2011-10-01

    In this paper we report chemically resolved measurements of organic aerosol (OA) and related tracers during the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX) at the Blodgett Forest Research Station, California from 15 August-10 October 2007. OA contributed the majority of the mass to the fine atmospheric particles and was predominately oxygenated (OOA). The highest concentrations of OA were during sporadic wildfire influence when aged plumes were impacting the site. In situ measurements of particle phase molecular markers were dominated by secondary compounds and along with gas phase compounds could be categorized into six factors or sources: (1) aged biomass burning emissions and oxidized urban emissions, (2) oxidized urban emissions (3) oxidation products of monoterpene emissions, (4) monoterpene emissions, (5) anthropogenic emissions and (6) local methyl chavicol emissions and oxidation products. There were multiple biogenic components that contributed to OA at this site whose contributions varied diurnally, seasonally and in response to changing meteorological conditions, e.g. temperature and precipitation events. Concentrations of isoprene oxidation products were larger when temperatures were higher during the first half of the campaign (15 August-12 September) due to more substantial emissions of isoprene and enhanced photochemistry. The oxidation of methyl chavicol, an oxygenated terpene emitted by ponderosa pine trees, contributed similarly to OA throughout the campaign. In contrast, the abundances of monoterpene oxidation products in the particle phase were greater during the cooler conditions in the latter half of the campaign (13 September-10 October), even though emissions of the precursors were lower, although the mechanism is not known. OA was correlated with the anthropogenic tracers 2-propyl nitrate and carbon monoxide (CO), consistent with previous observations, while being comprised of mostly non-fossil carbon (>75%). The

  12. Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996-2010

    NASA Astrophysics Data System (ADS)

    Lu, Z.; Streets, D. G.

    2011-07-01

    China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2) and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC) emissions from these two countries for the period 1996-2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly fractions for major sectors and gridded emissions at a resolution of 0.1° × 0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %-17 %) due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD) equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs) of SO2, BC, and OC emissions are estimated to be -16 %-17 %, -43 %-93 %, and -43 %-80 % for China, and -15 %-16 %, -41 %-87 %, and -44 %-92 % for India, respectively. Sulfur content, fuel use, and sulfur retention of hard coal and the actual

  13. Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996-2010

    NASA Astrophysics Data System (ADS)

    Lu, Z.; Zhang, Q.; Streets, D. G.

    2011-09-01

    China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2) and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC) emissions from these two countries for the period 1996-2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly temporal distributions for major sectors and gridded emissions at a resolution of 0.1°×0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %-17 %) due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD) equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs) of SO2, BC, and OC emissions are estimated to be -16 %-17 %, -43 %-93 %, and -43 %-80 % for China, and -15 %-16 %, -41 %-87 %, and -44 %-92 % for India, respectively. Sulfur content, fuel use, and sulfur retention of hard coal and

  14. Sources and characteristics of carbonaceous aerosols at Agra "World heritage site" and Delhi "capital city of India".

    PubMed

    Pipal, A S; Tiwari, S; Satsangi, P G; Taneja, Ajay; Bisht, D S; Srivastava, A K; Srivastava, M K

    2014-01-01

    Agra, one of the oldest cities "World Heritage site", and Delhi, the capital city of India are both located in the border of Indo-Gangetic Plains (IGP) and heavily loaded with atmospheric aerosols due to tourist place, anthropogenic activities, and its topography, respectively. Therefore, there is need for monitoring of atmospheric aerosols to perceive the scenario and effects of particles over northern part of India. The present study was carried out at Agra (AGR) as well as Delhi (DEL) during winter period from November 2011 to February 2012 of fine particulate (PM₂.₅: d < 2.5 μm) as well as associated carbonaceous aerosols. PM₂.₅ was collected at both places using medium volume air sampler (offline measurement) and analyzed for organic carbon (OC) and elemental carbon (EC). Also, simultaneously, black carbon (BC) was measured (online) at DEL. The average mass concentration of PM₂.₅ was 165.42 ± 119.46 μg m(-3) at AGR while at DEL it was 211.67 ± 41.94 μg m(-3) which is ~27% higher at DEL than AGR whereas the BC mass concentration was 10.60 μg m(-3). The PM₂.₅ was substantially higher than the annual standard stipulated by central pollution control board and United States Environmental Protection Agency standards. The average concentrations of OC and EC were 69.96 ± 34.42 and 9.53 ± 7.27 μm m(-3), respectively. Total carbon (TC) was 79.01 ± 38.98 μg m(-3) at AGR, while it was 50.11 ± 11.93 (OC), 10.67 ± 3.56 μg m(-3) (EC), and 60.78 ± 14.56 μg m(-3) (TC) at DEL. The OC/EC ratio was 13.75 at (AGR) and 5.45 at (DEL). The higher OC/EC ratio at Agra indicates that the formation of secondary organic aerosol which emitted from variable primary sources. Significant correlation between PM₂.₅ and its carbonaceous species were observed indicating similarity in sources at both sites. The average concentrations of secondary organic carbon (SOC) and primary organic carbon (POC) at AGR were 48.16 and 26

  15. Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas

    NASA Astrophysics Data System (ADS)

    Stone, Elizabeth A.; Schauer, James J.; Pradhan, Bidya Banmali; Dangol, Pradeep Man; Habib, Gazala; Venkataraman, Chandra; Ramanathan, V.

    2010-03-01

    This study focuses on improving source apportionment of carbonaceous aerosol in South Asia and consists of three parts: (1) development of novel molecular marker-based profiles for real-world biofuel combustion, (2) application of these profiles to a year-long data set, and (3) evaluation of profiles by an in-depth sensitivity analysis. Emissions profiles for biomass fuels were developed through source testing of a residential stove commonly used in South Asia. Wood fuels were combusted at high and low rates, which corresponded to source profiles high in organic carbon (OC) or high in elemental carbon (EC), respectively. Crop wastes common to the region, including rice straw, mustard stalk, jute stalk, soybean stalk, and animal residue burnings, were also characterized. Biofuel profiles were used in a source apportionment study of OC and EC in Godavari, Nepal. This site is located in the foothills of the Himalayas and was selected for its well-mixed and regionally impacted air masses. At Godavari, daily samples of fine particulate matter (PM2.5) were collected throughout the year of 2006, and the annual trends in particulate mass, OC, and EC followed the occurrence of a regional haze in South Asia. Maximum concentrations occurred during the dry winter season and minimum concentrations occurred during the summer monsoon season. Specific organic compounds unique to aerosol sources, molecular markers, were measured in monthly composite samples. These markers implicated motor vehicles, coal combustion, biomass burning, cow dung burning, vegetative detritus, and secondary organic aerosol as sources of carbonaceous aerosol. A molecular marker-based chemical mass balance (CMB) model provided a quantitative assessment of primary source contributions to carbonaceous aerosol. The new profiles were compared to widely used biomass burning profiles from the literature in a sensitivity analysis. This analysis indicated a high degree of stability in estimates of source

  16. On the variability of Black Smoke and carbonaceous aerosols in the Netherlands

    NASA Astrophysics Data System (ADS)

    Schaap, M.; Denier van der Gon, H. A. C.

    The study addresses the characteristics of elemental carbon (EC) and organic carbon (OC) distributions in the Netherlands by using Black Smoke (BS) data in combination with dedicated measurements and modelling. The BS levels indicate a large-scale background concentration over the Netherlands with low spatial variability and a gradient with highest levels (˜9 μg m -3) in the south gradually decreasing to the north-west (˜5.5 μg m -3). The BS concentrations at rural sites in the Netherlands are highly correlated due to common (diffuse) sources and large-scale meteorology. Superimposed on the regional background are the contributions of local/urban sources. Urban and rural BS levels show a distinct variation over the week with minimum levels on Sundays. BS levels do not reflect a real concentration as they are obtained via an optical measurement in combination with an outdated calibration curve to arrive at total suspended particles (TSP). We have found that the relation between BS and EC in the Netherlands is linear and highly correlated but dependent on station type. Application of these relations to the BS time series yields a gradient in the rural background EC concentration from 0.5 μg m -3 in the north to 0.7 μg m -3 in the south of the Netherlands. The relationship between OC and BS appears to be location specific and is determined by the BS-EC relation in combination with a characteristic OC/EC ratio. OC/EC ratios are ˜5 at regional background sites and ˜2 at traffic locations. Minimum OC/EC ratios at the traffic sites reflect the primary OC/EC ratio of traffic. We argue that estimation of secondary organic aerosol by assuming the minimum OC/EC ratio to be a proxy for the primary OC/EC is not allowed since this approach does not account for sources with high OC/EC ratios. Based on European scale modelling and the measured data, we estimate that national sources contribute ˜40-60% to Dutch EC levels. The rather costly and laborious EC measurements

  17. Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns

    NASA Astrophysics Data System (ADS)

    Fountoukis, Christos; Megaritis, Athanasios G.; Skyllakou, Ksakousti; Charalampidis, Panagiotis E.; Denier van der Gon, Hugo A. C.; Crippa, Monica; Prévôt, André S. H.; Fachinger, Friederike; Wiedensohler, Alfred; Pilinis, Christodoulos; Pandis, Spyros N.

    2016-03-01

    We use a three-dimensional regional chemical transport model (PMCAMx) with high grid resolution and high-resolution emissions (4 × 4 km2) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 µg m-3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m-3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d-1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00-14:00 LT) and 20 % during dinner time (20:00-22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias = -2.3 µg m-3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

  18. Radiative Forcing Due to Enhancements in Tropospheric Ozone and Carbonaceous Aerosols Caused by Asian Fires During Spring 2008

    NASA Technical Reports Server (NTRS)

    Natarajan, Murali; Pierce, R. Bradley; Lenzen, Allen J.; Al-Saadi, Jassim A.; Soja, Amber J.; Charlock, Thomas P.; Rose, Fred G.; Winker, David M.; Worden, John R.

    2012-01-01

    Simulations of tropospheric ozone and carbonaceous aerosol distributions, conducted with the Real-time Air Quality Modeling System (RAQMS), are used to study the effects of major outbreaks of fires that occurred in three regions of Asia, namely Thailand, Kazakhstan, and Siberia, during spring 2008. RAQMS is a global scale meteorological and chemical modeling system. Results from these simulations, averaged over April 2008, indicate that tropospheric ozone column increases by more than 10 Dobson units (DU) near the Thailand region, and by lesser amounts in the other regions due to the fires. Widespread increases in the optical depths of organic and black carbon aerosols are also noted. We have used an off-line radiative transfer model to evaluate the direct radiative forcing due to the fire-induced changes in atmospheric composition. For clear sky, the monthly averaged radiative forcing at the top of the atmosphere (TOA) is mostly negative with peak values less than -12 W/sq m occurring near the fire regions. The negative forcing represents the increased outgoing shortwave radiation caused by scattering due to carbonaceous aerosols. At high latitudes, the radiative forcing is positive due to the presence of absorbing aerosols over regions of high surface albedo. Regions of positive forcing at TOA are more pronounced under total sky conditions. The monthly averaged radiative forcing at the surface is mostly negative, and peak values of less than -30 W/sq m occur near the fire regions. Persistently large negative forcing at the surface could alter the surface energy budget and potentially weaken the hydrological cycle.

  19. Radiative forcing due to enhancements in tropospheric ozone and carbonaceous aerosols caused by Asian fires during spring 2008

    NASA Astrophysics Data System (ADS)

    Natarajan, Murali; Pierce, R. Bradley; Schaack, Todd K.; Lenzen, Allen J.; Al-Saadi, Jassim A.; Soja, Amber J.; Charlock, Thomas P.; Rose, Fred G.; Winker, David M.; Worden, John R.

    2012-03-01

    Simulations of tropospheric ozone and carbonaceous aerosol distributions, conducted with the Real-time Air Quality Modeling System (RAQMS), are used to study the effects of major outbreaks of fires that occurred in three regions of Asia, namely Thailand, Kazakhstan, and Siberia, during spring 2008. RAQMS is a global scale meteorological and chemical modeling system. Results from these simulations, averaged over April 2008, indicate that tropospheric ozone column increases by more than 10 Dobson units (DU) near the Thailand region, and by lesser amounts in the other regions due to the fires. Widespread increases in the optical depths of organic and black carbon aerosols are also noted. We have used an off-line radiative transfer model to evaluate the direct radiative forcing due to the fire-induced changes in atmospheric composition. For clear sky, the monthly averaged radiative forcing at the top of the atmosphere (TOA) is mostly negative with peak values less than -12 W/m2 occurring near the fire regions. The negative forcing represents the increased outgoing shortwave radiation caused by scattering due to carbonaceous aerosols. At high latitudes, the radiative forcing is positive due to the presence of absorbing aerosols over regions of high surface albedo. Regions of positive forcing at TOA are more pronounced under total sky conditions. The monthly averaged radiative forcing at the surface is mostly negative, and peak values of less than -30 W/m2 occur near the fire regions. Persistently large negative forcing at the surface could alter the surface energy budget and potentially weaken the hydrological cycle.

  20. Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns

    NASA Astrophysics Data System (ADS)

    Fountoukis, C.; Megaritis, A. G.; Skyllakou, K.; Charalampidis, P. E.; Denier van der Gon, H. A. C.; Crippa, M.; Prévôt, A. S. H.; Freutel, F.; Wiedensohler, A.; Pilinis, C.; Pandis, S. N.

    2015-09-01

    We use a three dimensional regional chemical transport model (PMCAMx) with high grid resolution and high resolution emissions (4 km × 4 km) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (Megacities: Emissions, urban, regional, and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 μg m-3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 μg m-3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d-1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00-14:00 LT) and 20 % during dinner time (20:00-22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias = -2.3 μg m-3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

  1. Emission sources and atmospheric processing of carbonaceous aerosols in India and China: Insights from dual carbon isotope techniques

    NASA Astrophysics Data System (ADS)

    Andersson, A.; Kirillova, E. N.; Bosch, C.; Suresh, T.; Lee, M.; Du, K.; Sheesley, R. J.; Budhavant, K.; Gustafsson, O. M.

    2013-12-01

    The large emissions of carbonaceous aerosols, e.g., black carbon (BC), in India and China have detrimental effects on both human health and the regional climate. However, mitigation efforts as well as accurate modeling of these effects are currently hampered by large uncertainties regarding the contributions from different emission sources, including both primary and secondary processes. Here, we present dual carbon isotope constraints on emissions sources and atmospheric processing from multiple sites capturing the outflow from India and China. Radiocarbon (14C) studies of elemental carbon (EC) - a tracer for BC - show larger relative fossil contributions than expected from bottom-up emission inventories, for both India (49+-5) and China (80 +-6%). Similarly to EC, radiocarbon constraints of water soluble organic carbon (WSOC) shows substantially larger relative fossil contributions in Chinese outflow (30-50%) as compared with India, but also compared to Europe and USA (10-20%). In contrast to the radiocarbon data, stable carbon (d13C) analysis of WSOC shows substantial variability for different sites capturing the Indian outflow. Strong enrichment of heavy isotopes in WSOC is coupled to expected transport time from sources, indicating the influence of photochemical aging during transport. Such trends in the d13C signature are not observed for the EC fraction. Taken together this work show that carbon isotope techniques provide firm constraints on emission sources of different fractions of carbonaceous aerosols, and may also offer insights into atmospheric processing of these constituents during air mass transport.

  2. Development of a preparation system for the radiocarbon analysis of organic carbon in carbonaceous aerosols in China

    NASA Astrophysics Data System (ADS)

    Zhang, Y. L.; Liu, D.; Shen, C. D.; Ding, P.; Zhang, G.

    2010-09-01

    Carbonaceous aerosols comprising a large fraction of elemental carbon (EC) and organic carbon (OC) are considered to affect both global climate and human health. Radiocarbon measurements have been proved to be a useful isotopic tracer for distinguishing contemporary and fossil emissions. An optimized system of a two-step thermal preparation system for radiocarbon ( 14C) measurement of OC/TC is firstly established in China. In this system, OC/TC are converted into carbon dioxide under a pure oxygen flow at 340 °C/650 °C and then reduced to graphite for AMS target using the method of zinc reduction. Afterwards, radiocarbon measurements of the targets performed by the NEC Compact AMS System at the Institute of Heavy Ion Physics, Peking University. The measured results for estimated reference martial including HOx I, HOx II and IAEA-C6 are consistent with internationally accepted values. The radiocarbon-based source appointment of carbonaceous aerosols in China would be much more convenient and faster with the preparation system developed in this work.

  3. Quantitative determination of carbonaceous particle mixing state in Paris using single particle mass spectrometer and aerosol mass spectrometer measurements

    NASA Astrophysics Data System (ADS)

    Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

    2013-04-01

    Single particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been estimated using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulphate and potassium were compared with concurrent measurements from an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal/optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and ten discrete mixing states for carbonaceous particles were identified and quantified. Potassium content was used to identify particles associated with biomass combustion. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorization, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulphate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidized OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the heterogeneity of primary and

  4. Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements

    NASA Astrophysics Data System (ADS)

    Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

    2013-09-01

    Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal-optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA / EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal

  5. A global emission inventory of carbonaceous aerosol from historic records of fossil fuel and biofuel consumption for the period 1860-1997

    NASA Astrophysics Data System (ADS)

    Junker, C.; Liousse, C.

    2008-03-01

    Country by country emission inventories for carbonaceous aerosol for the period 1860 to 1997 have been constructed on the basis of historic fuel production, use and trade data sets published by the United Nation's Statistical Division UNSTAT (1997), Etemad et al. (1991) and Mitchell (1992, 1993, 1995). The inventories use emission factors variable over time, which have been determined according to changes in technological development. The results indicate that the industrialisation period since 1860 was accompanied by a steady increase in black carbon (BC) and primary organic carbon (POC) emissions up to 1910. The calculations show a moderate decrease of carbonaceous aerosol emissions between 1920 and 1930, followed by an increase up to 1990, the year when emissions began to decrease again. Changes in BC and POC emissions prior to the year 1950 are essentially driven by the USA, Germany and the UK. The USSR, China and India become substantial contributors to carbonaceous aerosol emissions after 1950. Emission maps have been generated with a 1°×1° resolution based on the relative population density in each country. They will provide a helpful tool for assessing the effect of carbonaceous aerosol emissions on observed climate changes of the past.

  6. A global emission inventory of carbonaceous aerosol from historic records of fossil fuel and biofuel consumption for the period 1860-1997

    NASA Astrophysics Data System (ADS)

    Junker, C.; Liousse, C.

    2006-06-01

    Country by country emission inventories for carbonaceous aerosol for the period 1860 to 1997 have been constructed on the basis of historic fuel production, use and trade data sets published by the United Nation's Statistical Division UNSTAT (1997), Etemad et al. (1991) and Mitchell (1992, 1993, 1995). The inventories use emission factors variable over time, which have been determined according to changes in technological development. The results indicate that the industrialisation period since 1860 was accompanied by a steady increase in black carbon (BC) and organic carbon (OC) emissions up to 1910. The calculations show a moderate decrease of carbonaceous aerosol emissions between 1920 and 1930, followed by an increase up to 1990, the year when emissions began to decrease again. Changes in BC and OC emissions prior to the year 1950 are essentially driven by the USA, Germany and the UK. The USSR, China and India become substantial contributors to carbonaceous aerosol emissions after 1950. Emission maps have been generated with a 1°×1° resolution based on the relative population density in each country. They will provide a helpful tool for assessing the effect of carbonaceous aerosol emissions on observed climate changes of the past.

  7. ANALYSIS OF CARBONACEOUS AEROSOLS USING THE THERMAL OPTICAL TRANSMITTANCE AND THERMAL OPTICAL REFLECTANCE METHODS

    EPA Science Inventory

    Carbonaceous particulate typically represents a large fraction of PM2.5 (20 - 40%). Two primary techniques presently used for the analysis of particulate carbon are Thermal Optical Transmission (TOT - NIOSH Method 5040) and Thermal Optical Reflectance (TOR). These two methods b...

  8. Carbonaceous Aerosol Characteristics over a Pinus taeda plantation: Results from the CELTIC experiment

    EPA Science Inventory

    Carbonaceous particles smaller than 2.5 um aerodynamic diameter (PM2.5) were collected in July, 2003 over a Loblolly Pine plantation at Duke Forest, NC during the Chemical Emission, Loss, Transformation and Interactions within Canopies (CELTIC) field study. Organic (OC) and eleme...

  9. SOURCE APPORTIONMENT OF PRIMARY CARBONACEOUS AEROSOL USING THE COMMUNITY MULTISCALE AIR QUALITY MODEL

    EPA Science Inventory

    A substantial fraction of fine particulate matter (PM) across the United States is composed of carbon, which may be either emitted in particulate form (i.e., primary) or formed in the atmosphere through gas-to-particle conversion processes (i.e., secondary). Primary carbonaceous...

  10. Characterization of carbonaceous aerosols during the MINOS campaign in Crete, July-August 2001: a multi-analytical approach

    NASA Astrophysics Data System (ADS)

    Sciare, J.; Cachier, H.; Oikonomou, K.; Ausset, P.; Sarda-Estève, R.; Mihalopoulos, N.

    2003-07-01

    During the major part of the Mediterranean Intensive Oxidant Study (MINOS) campaign (summer 2001, Crete Isl.), the Marine Boundary Layer (MBL) air was influenced by long range transport of biomass burning from the northern and western part of the Black Sea. During this campaign, carbonaceous aerosols were collected on quartz filters at a Free Tropospheric (FT) site, and at a MBL site together with size-resolved distribution of aerosols. Three Evolution Gas Analysis (EGA) protocols have been tested in order to better characterize the collected aged biomass burning smoke: A 2-step thermal method (Cachier et al., 1989) and a thermo-optical technique using two different temperature programs. The later temperature programs are those used for IMPROVE (Interagency Monitoring of Protected Visual Environments) and NIOSH 5040 (National Institute of Occupational Safety and Health). Artifacts were observed using the NIOSH temperature program and identified as interactions between carbon and dust deposited on the filter matrix at high temperature (T=550°C) under the pure helium step of the analysis. During the MINOS campaign, Black Carbon (BC) and Organic Carbon (OC) concentrations were on average respectively 1.19±0.56 and 3.62±1.08 μgC/m3 for the IMPROVE temperature program, and 1.09±0.36 and 3.75±1.24 μgC/m3 for the thermal method. Though these values compare well on average and the agreement between the Total Carbon (TC) measurements sample to sample was excellent (slope = 1.00, r2=0.93, n=56), important discrepancies were observed in determining BC concentrations from these two methods (average error of 33±22%). BC from the IMPROVE temperature program compared well with non-sea-salt potassium (nss-K) pointing out an optical sensitivity to biomass burning. On the other hand, BC from the thermal method showed a better agreement with non-sea-salt sulfate (nss-SO4), considered as a tracer for fossil fuel combustion during the MINOS campaign. The coupling between

  11. Characterization of carbonaceous aerosols during the MINOS campaign in Crete, July August 2001: a multi-analytical approach

    NASA Astrophysics Data System (ADS)

    Sciare, J.; Cachier, H.; Oikonomou, K.; Ausset, P.; Sarda-Estève, R.; Mihalopoulos, N.

    2003-10-01

    During the major part of the Mediterranean Intensive Oxidant Study (MINOS) campaign (summer 2001, Crete Isl.), the Marine Boundary Layer (MBL) air was influenced by long range transport of biomass burning from the northern and western part of the Black Sea. During this campaign, carbonaceous aerosols were collected on quartz filters at a Free Tropospheric (FT) site, and at a MBL site together with size-resolved distribution of aerosols. Three Evolution Gas Analysis (EGA) protocols have been tested in order to better characterize the collected aged biomass burning smoke: A 2-step thermal method (Cachier et al., 1989) and a thermo-optical technique using two different temperature programs. The later temperature programs are those used for IMPROVE (Interagency Monitoring of Protected Visual Environments) and NIOSH 5040 (National Institute of Occupational Safety and Health). Artifacts were observed using the NIOSH temperature program and identified as interactions between carbon and dust deposited on the filter matrix at high temperature (T>550ºC) under the pure helium step of the analysis. During the MINOS campaign, Black Carbon (BC) and Organic Carbon (OC) mass concentrations were on average respectively 1.19±0.56 and 3.62±1.08 mgC/m3 for the IMPROVE temperature program, and 1.09±0.36 and 3.75±1.24 mgC/m3 for the thermal method. Though these values compare well on average and the agreement between the Total Carbon (TC) measurements sample to sample was excellent (slope=1.00, r2=0.93, n=56), important discrepancies were observed in determining BC concentrations from these two methods (average error of 33±22%). BC from the IMPROVE temperature program compared well with non-sea-salt potassium (nss-K) pointing out an optical sensitivity to biomass burning. On the other hand, BC from the thermal method showed a better agreement with non-sea-salt sulfate (nss-SO4), considered as a tracer for fossil fuel combustion during the MINOS campaign. The coupling between these

  12. Individual Aerosol Particles from Biomass Burning in Southern Africa. 1; Compositions and Size Distributions of Carbonaceous Particles

    NASA Technical Reports Server (NTRS)

    Posfai, Mihaly; Simonics, Renata; Li, Jia; Hobbs, Peter V.; Buseck, Peter R.

    2003-01-01

    Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy (TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic (K-salt) inclusions, tar ball particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged (1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/sulfate and soot/sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea-salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles.

  13. Synthesizing Scientific Progress: Outcomes from US EPA’s Carbonaceous Aerosols and Source Apportionment STAR Grants

    EPA Science Inventory

    ABSTRACTA number of studies in the past decade have transformed the way we think about atmospheric aerosols. The advances include, but are not limited to, source apportionment of organics using aerosol mass spectrometer data, the volatility basis set approach, quantifying isopre...

  14. Chapter 3: Evaluating the impacts of carbonaceous aerosols on clouds and climate

    SciTech Connect

    Menon, Surabi; Del Genio, Anthony D.

    2007-09-03

    Any attempt to reconcile observed surface temperature changes within the last 150 years to changes simulated by climate models that include various atmospheric forcings is sensitive to the changes attributed to aerosols and aerosol-cloud-climate interactions, which are the main contributors that may well balance the positive forcings associated with greenhouse gases, absorbing aerosols, ozone related changes, etc. These aerosol effects on climate, from various modeling studies discussed in Menon (2004), range from +0.8 to -2.4 W m{sup -2}, with an implied value of -1.0 W m{sup -2} (range from -0.5 to -4.5 W m{sup -2}) for the aerosol indirect effects. Quantifying the contribution of aerosols and aerosol-cloud interactions remain complicated for several reasons some of which are related to aerosol distributions and some to the processes used to represent their effects on clouds. Aerosol effects on low lying marine stratocumulus clouds that cover much of the Earth's surface (about 70%) have been the focus of most of prior aerosol-cloud interaction effect simulations. Since cumulus clouds (shallow and deep convective) are short lived and cover about 15 to 20% of the Earth's surface, they are not usually considered as radiatively important. However, the large amount of latent heat released from convective towers, and corresponding changes in precipitation, especially in biomass regions due to convective heating effects (Graf et al. 2004), suggest that these cloud systems and aerosol effects on them, must be examined more closely. The radiative heating effects for mature deep convective systems can account for 10-30% of maximum latent heating effects and thus cannot be ignored (Jensen and Del Genio 2003). The first study that isolated the sensitivity of cumulus clouds to aerosols was from Nober et al. (2003) who found a reduction in precipitation in biomass burning regions and shifts in circulation patterns. Aerosol effects on convection have been included in other

  15. Characterization of carbonaceous aerosols over the East China Sea: The impact of the East Asian continental outflow

    NASA Astrophysics Data System (ADS)

    Wang, Fengwen; Guo, Zhigang; Lin, Tian; Hu, Limin; Chen, Yingjun; Zhu, Yifang

    2015-06-01

    Seventy-five paired PM2.5 (aerodynamic diameter less than 2.5 μm) and TSP (total suspended particle) samples collected from a pristine island in the East China Sea (ECS) between October 2011 and August 2012 were analyzed for organic carbon (OC), elemental carbon (EC), and n-alkanes. The island lies in the pathway of continental outflow from Mainland China to the northwest Pacific Ocean driven by the East Asian Monsoon. The concentrations of OC, EC (in μg/m3), and n-alkanes (in ng/m3) were highest in winter (means: 4.7, 1.3, 140.1, respectively) and lowest in summer (means: 1.1, 0.3, 17.0, respectively). PM2.5 contained approximately 88% of the OC, 80% of the EC, and 61% of the n-alkanes in TSP. Petroleum residue was the dominant contributor to the n-alkanes. C12-C22n-alkanes with strong even-to-odd predominance observed in winter were attributed to the microbial contribution from sea spray aerosol (SSA) driven by the higher wind speed. There was a higher secondary organic carbon (SOC)/OC ratio in warm seasons (summer and fall) than that in cold seasons (spring and winter). The dominance of primary organic carbon (POC) and EC in cold seasons was possibly mainly due to the influence of the East Asian continental outflow. Three episodes of high concentrations of carbonaceous aerosols were observed, and we focused on the impact of these pollutants from East Asia on the air quality over the ECS. Carbonaceous pollutants were more concentrated in PM2.5 during the fall episode triggered by biomass burning in East China. The winter haze associated with intensive indoor heating in North China brought substantial carbonaceous pollutants, with a minor influence on their size distribution. The dust episode in spring was related to coarse particles (i.e., TSP-PM2.5), yielding a distinctly different size distribution.

  16. Effect of Increasing Temperature on Carbonaceous Aerosol Direct Radiative Effect over Southeastern US

    NASA Astrophysics Data System (ADS)

    Mielonen, Tero; Kokkola, Harri; Hienola, Anca; Kühn, Thomas; Merikanto, Joonas; Korhonen, Hannele; Arola, Antti; Kolmonen, Pekka; Sogacheva, Larisa; de Leeuw, Gerrit

    2016-04-01

    Aerosols are an important regulator of the Earth's climate. They scatter and absorb incoming solar radiation and thus cool the climate by reducing the amount of energy reaching the atmospheric layers and the surface below (direct effect). A certain subset of the particles can also act as initial formation sites for cloud droplets and thereby modify the microphysics, dynamics, radiative properties and lifetime of clouds (indirect effects). The magnitude of aerosol radiative effects remains the single largest uncertainty in current estimates of anthropogenic radiative forcing. One of the key quantities needed for accurate estimates of anthropogenic radiative forcing is an accurate estimate of the radiative effects from natural unperturbed aerosol. The dominant source of natural aerosols over Earth's vast forested regions are biogenic volatile organic compounds (BVOC) which, following oxidation in the atmosphere, can condense onto aerosol particles to form secondary organic aerosol (SOA) and significantly modify the particles' properties. In accordance with the expected positive temperature dependence of BVOC emissions, several previous studies have shown that some aerosol properties, such as mass concentration and ability to act as cloud condensation nuclei (CCN), also correlate positively with temperature at many forested sites. There is conflicting evidence as to whether the aerosol direct effects have a temperature dependence due to increased BVOC emissions. The main objective of this study is to investigate the causes of the observed effect of increasing temperatures on the aerosol direct radiative effect, and to provide a quantitative estimate of this effect and of the resulting negative feedback in a warming climate. More specifically, we will investigate the causes of the positive correlation between aerosol optical depth (AOD) and land surface temperature (LST) over southeastern US where biogenic emissions are a significant source of atmospheric particles. In

  17. Impacts of controlling biomass burning emissions on wintertime carbonaceous aerosol in Europe

    NASA Astrophysics Data System (ADS)

    Fountoukis, C.; Butler, T.; Lawrence, M. G.; Denier van der Gon, H. A. C.; Visschedijk, A. J. H.; Charalampidis, P.; Pilinis, C.; Pandis, S. N.

    2014-04-01

    We use a 3-D regional chemical transport model, with the latest advancements in the organic aerosol (OA) treatment, and an updated emission inventory for wood combustion to study the organic aerosol change in response to the replacement of current residential wood combustion technologies with pellet stoves. Simulations show a large decrease of fine organic aerosol (more than 60%) in urban and suburban areas during winter and decreases of 30-50% in elemental carbon levels in large parts of Europe. There is also a considerable decrease (around 40%) of oxidized OA, mostly in rural and remote regions. Total PM2.5 mass is predicted to decrease by 15-40% on average during the winter in continental Europe. Accurate representation of the intermediate volatility precursors of organic aerosol in the emission inventory is crucial in assessing the efficiency of such abatement strategies.

  18. Highly Siderophile Elements and Osmium Isotope Systematics in Ureilites: Are the Carbonaceous Veins Primary Components?

    NASA Technical Reports Server (NTRS)

    Rankenburg, K.; Brandon, A. D.; Humayun, M.

    2005-01-01

    Ureilites are an enigmatic group of primitive carbon-bearing achondrites of ultramafic composition. The majority of the 143 ureilite meteorites consist primarily of olivine and pyroxene (and occasionally chromite) [1]. They are coarse-grained, slowly cooled, and depleted in incompatible lithophile elements. Minor amounts of dark interstitial material consisting of carbon, metal, sulfides, and fine-grained silicates occur primarily along silicate grain boundaries, but also intrude the silicates along fractures and cleavage planes. Variable degrees of impact shock features have also been imparted on ureilites. The prevailing two origins proposed for these rocks are either as melting residues of carbonaceous chondritic material [2], [3], or alternatively, derivation as mineral cumulates from such melts [4], [5], [6]. It has recently been proposed that ureilites are the residues of a smelting event, i.e. residues of a partial melting event under highly reducing conditions, where a solid Fe-bearing phase reacts with a melt and carbon to form Fe metal and carbon monoxide [7]. Rapid, localized extraction and loss of the basaltic component into space resulting from high eruption velocities could preserve unequilibrated oxygen isotopes and produce the observed olivine-pyroxene residues via 25-30% partial melting of chondritic-like precursor material.

  19. Thermal characteristics and mass absorption efficiency of carbonaceous aerosol measured during a post-harvest burning period

    NASA Astrophysics Data System (ADS)

    Batmunkh, T.; Kim, Y. J.; Cayetano, M. G.; Lee, K.; Kim, K.; Park, K.

    2012-12-01

    In order to better understand the characteristics of carbonaceous aerosol time-resolved OC, EC, and BC were measured by a Sunset OC/EC analyzer and an Aethalometer, respectively, during a post-harvest burning period from November 22 to December 20, 2011 at a sub-urban site in Gwangju, Korea. OC and EC were analyzed by the thermal-optical transmittance (TOT) method with NIOSH temperature protocol. The spectral light absorption coefficient (babs) was determined based on the Aethalometer data. Overall average OC and EC concentrations were found to be 5.0±2.4 ugC/ m3 and 1.5±0.9 ugC/ m3, respectively for the sampling period. On average, babs at seven Aethalometer wavelengths was found to be 38.4±27.8 Mm-1, 24.3±17.8 Mm-1, 20.8±15.4 Mm-1, 17.9±13.3 Mm-1, 14.9±11.1 Mm-1, 9.9±7.4 Mm-1, and 8.8±6.6 Mm-1 at 370 nm, 470 nm, 520 nm, 590 nm, 660 nm, 880 nm, and 950 nm, respectively. Clear diurnal variations with morning (7:00 AM~9:00 AM) and evening (7:00 PM~11:00 PM) peaks were observed for OC, EC, and babs mostly due to local burning activities. Based on the 4-day back-trajectory analyses conducted using the HYSPLIT model. Event cases were classified into four categories, based on the 4-day air mass back trajectories, as Clean(C), Stagnant(ST), Continental(CC), and Local Burning(LB) events. In order to better investigate the characteristics of atmospheric carbonaceous aerosol, thermal evolution patterns of carbonaceous aerosol measured by the Sunset analyzer were characterized as OC1, OC2, and EC, which were detected in temperature steps of 600 C, 840 C in an non-oxidizing atmosphere, and 870 C in an oxidizing atmosphere, respectively. High ratio of OC2/OC1; 1.39~1.41 was observed in the evening 9:00~11:00 PM due to local burning event. Concentration of OC2 was higher up to 1.4 times than that of OC1 for the LB cases, showing that higher molecular weight fraction of organic aerosol was dominant for the time. As expected, higher correlation was found between EC and

  20. Characteristics of carbonaceous aerosols: Impact of biomass burning and secondary formation in summertime in a rural area of the North China Plain.

    PubMed

    Yao, Lan; Yang, Lingxiao; Chen, Jianmin; Wang, Xinfeng; Xue, Likun; Li, Weijun; Sui, Xiao; Wen, Liang; Chi, Jianwei; Zhu, Yanhong; Zhang, Junmei; Xu, Caihong; Zhu, Tong; Wang, Wenxing

    2016-07-01

    To determine the characteristics of carbonaceous aerosols in rural areas of the North China Plain, field measurements were conducted at Yucheng (YC) in the summers of 2013 and 2014. The concentrations of carbonaceous aerosols at YC exhibited clear diurnal variation, with higher concentrations in the early morning and at night and lower concentrations during the afternoon hours. The mass-balance method designed for particulate matter smaller than 2.5μm (PM2.5) was used to calculate the organic matter (OM)/organic carbon (OC) ratio. The value obtained, 2.07±0.05, was suggested as a reference to estimate organics in PM2.5 in rural areas of the North China Plain. Biomass burning was identified to be a significant source of carbonaceous aerosols; approximately half of the samples obtained at YC were affected by biomass burning during summer 2013. Case studies revealed that biomass burning accounted for up to 52.6% of the OC and 51.1% of the elemental carbon in PM2.5 samples. The organic coatings observed on sulphur-rich and potassium-rich particles indicated the formation of secondary organic aerosols (SOA) from the oxidation of precursor volatile organic compounds (VOCs) during the aging of smoke released from biomass burning. Based on the evolution of the VOCs, the contribution of VOCs oxidation to SOA concentration was 3.21 and 1.07μgm(-3)ppm(-1) CO under conditions of low nitrogen oxide (NOx) and high NOx, respectively. Aromatics (e.g. benzene, toluene, xylene and ethylbenzene) made the greatest contribution to SOA concentration (88.4% in low-NOx conditions and 80.6% in high-NOx conditions). The results of the study offer novel insights into the effects of biomass burning on the carbonaceous aerosols and SOA formation in polluted rural areas. PMID:27031303

  1. Intra-urban spatial variability of PM2.5-bound carbonaceous components

    PubMed Central

    Xie, Mingjie; Coons, Teresa L.; Dutton, Steven J.; Milford, Jana B.; Miller, Shelly L.; Peel, Jennifer L.; Vedal, Sverre; Hannigan, Michael P.

    2014-01-01

    The Denver Aerosol Sources and Health (DASH) study was designed to evaluate associations between PM2.5 species and sources and adverse human health effects. The DASH study generated a five-year (2003–2007) time series of daily speciated PM2.5 concentration measurements from a single, special-purpose monitoring site in Denver, CO. To evaluate the ability of this site to adequately represent the short term temporal variability of PM2.5 concentrations in the five county Denver metropolitan area, a one year supplemental set of PM2.5 samples was collected every sixth day at the original DASH monitoring site and concurrently at three additional sites. Two of the four sites, including the original DASH site, were located in residential areas at least 1.9 km from interstate highways. The other two sites were located within 0.3 km of interstate highways. Concentrations of elemental carbon (EC), organic carbon (OC), and 58 organic molecular markers were measured at each site. To assess spatial variability, site pairs were compared using the Pearson correlation coefficient (r) and coefficient of divergence (COD), a statistic that provides information on the degree of uniformity between monitoring sites. Biweekly co-located samples collected from July 2004 to September 2005 were also analyzed and used to estimate the uncertainty associated with sampling and analytical measurement for each species. In general, the two near-highway sites exhibited higher concentrations of EC, OC, polycyclic aromatic hydrocarbons (PAHs), and steranes than did the more residential sites. Lower spatial heterogeneity based on r and COD was inferred for all carbonaceous species after considering their divergence and lack of perfect correlations in co-located samples. Ratio–ratio plots combined with available gasoline- and diesel-powered motor vehicle emissions profiles for the region suggested a greater impact to high molecular weight (HMW) PAHs from diesel-powered vehicles at the near

  2. Intercomparison of methods for the measurement of carbonaceous aerosol species. Final report

    SciTech Connect

    Appel, B.R.; Cheng, W.; Tokiwa, Y.; Salaymeh, F.; Povard, V.

    1987-01-01

    The principal goal of the study, as part of the Carbonaceous Species Methods Comparison Study, was to perform field trials at Citrus College, Glendora, CA, in August 1986 with a sampler intended to minimize positive and negative artifacts for sampling particulate carbon. In addition, organic and elemental carbon in atmospheric and laboratory-generated samples were analyzed to permit intermethod comparisons. The particulate carbon sampler consisted of a cyclone, parallel-plate diffusion denuder packed with coarse, activated alumina, and a quartz-fiber filter followed by a fluidized bed of activated alumina. The sampler failed to perform effectively in atmospheric trials; alumina showed little activity in decreasing the positive error in filter carbon sampling due to sorption of gas-phase carbonaceous material. The measurement of organic (Co) and elemental carbon (Ce) employed an optical absorption technique for Ce and a coulometer for total C (Ct). Organic carbon was then obtained by difference between Ct and Ce. In addition, organic and elemental carbon in atmospheric and laboratory-generated samples were analyzed to permit intermethod comparisons.

  3. Revisiting AVHRR tropospheric aerosol trends using principal component analysis

    NASA Astrophysics Data System (ADS)

    Li, Jing; Carlson, Barbara E.; Lacis, Andrew A.

    2014-03-01

    The advanced very high resolution radiometer (AVHRR) satellite instruments provide a nearly 25 year continuous record of global aerosol properties over the ocean. It offers valuable insights into the long-term change in global aerosol loading. However, the AVHRR data record is heavily influenced by two volcanic eruptions, El Chichon on March 1982 and Mount Pinatubo on June 1991. The gradual decay of volcanic aerosols may last years after the eruption, which potentially masks the estimation of aerosol trends in the lower troposphere, especially those of anthropogenic origin. In this study, we show that a principal component analysis approach effectively captures the bulk of the spatial and temporal variability of volcanic aerosols into a single mode. The spatial pattern and time series of this mode provide a good match to the global distribution and decay of volcanic aerosols. We further reconstruct the data set by removing the volcanic aerosol component and reestimate the global and regional aerosol trends. Globally, the reconstructed data set reveals an increase of aerosol optical depth from 1985 to 1990 and decreasing trend from 1994 to 2006. Regionally, in the 1980s, positive trends are observed over the North Atlantic and North Arabian Sea, while negative tendencies are present off the West African coast and North Pacific. During the 1994 to 2006 period, the Gulf of Mexico, North Atlantic close to Europe, and North Africa exhibit negative trends, while the coastal regions of East and South Asia, the Sahel region, and South America show positive trends.

  4. Revisiting AVHRR Tropospheric Aerosol Trends Using Principal Component Analysis

    NASA Technical Reports Server (NTRS)

    Li, Jing; Carlson, Barbara E.; Lacis, Andrew A.

    2014-01-01

    The advanced very high resolution radiometer (AVHRR) satellite instruments provide a nearly 25 year continuous record of global aerosol properties over the ocean. It offers valuable insights into the long-term change in global aerosol loading. However, the AVHRR data record is heavily influenced by two volcanic eruptions, El Chichon on March 1982 and Mount Pinatubo on June 1991. The gradual decay of volcanic aerosols may last years after the eruption, which potentially masks the estimation of aerosol trends in the lower troposphere, especially those of anthropogenic origin. In this study, we show that a principal component analysis approach effectively captures the bulk of the spatial and temporal variability of volcanic aerosols into a single mode. The spatial pattern and time series of this mode provide a good match to the global distribution and decay of volcanic aerosols. We further reconstruct the data set by removing the volcanic aerosol component and reestimate the global and regional aerosol trends. Globally, the reconstructed data set reveals an increase of aerosol optical depth from 1985 to 1990 and decreasing trend from 1994 to 2006. Regionally, in the 1980s, positive trends are observed over the North Atlantic and North Arabian Sea, while negative tendencies are present off the West African coast and North Pacific. During the 1994 to 2006 period, the Gulf of Mexico, North Atlantic close to Europe, and North Africa exhibit negative trends, while the coastal regions of East and South Asia, the Sahel region, and South America show positive trends.

  5. Spatial distribution of carbonaceous aerosol in the southeastern Baltic Sea region (event of grass fires)

    NASA Astrophysics Data System (ADS)

    Dudoitis, Vadimas; Byčenkienė, Steigvilė; Plauškaitė, Kristina; Bozzetti, Carlo; Fröhlich, Roman; Mordas, Genrik; Ulevičius, Vidmantas

    2016-05-01

    The aerosol chemical composition in air masses affected by large vegetation fires transported from the Kaliningrad region (Russia) and southeast regions (Belarus and Ukraine) during early spring (March 2014) was characterized at the remote background site of Preila, Lithuania. In this study, the chemical composition of the particulate matter was studied by high temporal resolution instruments, including an Aerosol Chemical Speciation Monitor (ACSM) and a seven-wavelength aethalometer. Air masses were transported from twenty to several hundred kilometres, arriving at the measurement station after approximately half a day of transport. The concentration-weighted trajectory analysis suggests that organic aerosol particles are mainly transported over the Baltic Sea and the continent (southeast of Belarus). Results show that a significant fraction of the vegetation burning organic aerosol is transformed into oxidised forms in less than a half-day. Biomass burning aerosol (BBOA) was quantified from the ACSM data using a positive matrix factorization (PMF) analysis, while its spatial distribution was evaluated using air mass clustering approach.

  6. Organic Aerosol Component (OACOMP) Value-Added Product Report

    SciTech Connect

    Fast, J; Zhang, Q; Tilp, A; Shippert, T; Parworth, C; Mei, F

    2013-08-23

    Significantly improved returns in their aerosol chemistry data can be achieved via the development of a value-added product (VAP) of deriving OA components, called Organic Aerosol Components (OACOMP). OACOMP is primarily based on multivariate analysis of the measured organic mass spectral matrix. The key outputs of OACOMP are the concentration time series and the mass spectra of OA factors that are associated with distinct sources, formation and evolution processes, and physicochemical properties.

  7. Contributions of vehicular carbonaceous aerosols to PM2.5 in a roadside environment in Hong Kong

    NASA Astrophysics Data System (ADS)

    Huang, X. H. H.; Bian, Q. J.; Louie, P. K. K.; Yu, J. Z.

    2014-09-01

    Hourly measurements of elemental carbon (EC) and organic carbon (OC) were made at Mong Kok, a roadside air quality monitoring station in Hong Kong, for a year, from May 2011 to April 2012. The monthly average EC concentrations were 3.8-4.9 μg C m-3, accounting for 9.2-17.7% of the PM2.5 mass (21.5-49.7 μg m-3). The EC concentrations showed little seasonal variation and peaked twice daily, coinciding with the traffic rush hours of a day. Strong correlations were found between EC and NOx concentrations, especially during the rush hours in the morning, confirming vehicular emissions as the dominant source of EC at this site. The analysis by means of the minimum OC / EC ratio approach to determine the OC / EC ratio representative of primary vehicular emissions yields a value of 0.5 for (OC / EC)vehicle. By applying the derived (OC / EC)vehicle ratio to the data set, the monthly average vehicle-related OC was estimated to account for 17-64% of the measured OC throughout the year. Vehicle-related OC was also estimated using receptor modeling of a combined data set of hourly NOx, OC, EC and volatile organic compounds characteristic of different types of vehicular emissions. The OCvehicle estimations by the two different approaches were in good agreement. When both EC and vehicle-derived organic matter (OM) (assuming an OM-to-OC ratio of 1.4) are considered, vehicular carbonaceous aerosols contributed ~ 7.3 μg m-3 to PM2.5, accounting for ~ 20% of PM2.5 mass (38.3 μg m-3) during winter, when Hong Kong received significant influence of air pollutants transported from outside, and ~ 30% of PM2.5 mass (28.2 μg m-3) during summertime, when local emission sources were dominant. A reduction of 3.8 μg m-3 in vehicular carbonaceous aerosols was estimated during 07:00-11:00 (i.e., rush hours on weekdays) on Sundays and public holidays. This could mainly be attributed to less on-road public transportation (e.g., diesel-powered buses) in comparison with non-holidays. These

  8. Contributions of vehicular carbonaceous aerosols to PM2.5 in a roadside environment in Hong Kong

    NASA Astrophysics Data System (ADS)

    Huang, X. H. Hilda; Bian, Q. J.; Louie, P. K. K.; Yu, J. Z.

    2014-01-01

    Hourly measurements of elemental carbon (EC) and organic carbon (OC) were made at Mong Kok, a roadside air quality monitoring station in Hong Kong for a year from May 2011 to April 2012. The monthly average EC concentrations were 3.8-4.9 μgC m-3, accounting for 9.2-17.7% of the PM2.5 mass (21.5-49.7 μg m-3). The EC concentrations showed little seasonal variation and peaked twice daily in coincidence with the traffic rush hours of a day. Good correlations were found between EC and NOx concentrations, especially during the rush hours in the morning. In time periods when diesel-powered vehicles dominated the road traffic, the OC / EC ratio was approximately 0.5. The analysis by the minimum OC / EC ratio approach to determine OC / EC ratio representative of primary emissions also yields a value of 0.5, suggesting that it is a reasonable lower limit estimation of (OC / EC)vehicle in representing vehicular emissions. By applying the derived (OC / EC)vehicle ratio to the dataset, the monthly average vehicle-related OC was estimated to account for 16.6-64.0% of the measured OC throughout the year. Vehicle-related OC was also estimated using receptor modeling of a combined dataset of hourly NOx, OC, EC and select volatile organic compounds. The estimations by the two different approaches were in good agreement. When both EC and vehicle-derived organic matter (OM) (assuming an OM-to-OC ratio of 1.4) are considered, vehicular carbonaceous aerosols contributed ~ 7.3 μg m-3 to PM2.5, accounting for ~ 20% of PM2.5 mass (38.3 μg m-3) during winter when Hong Kong was largely influenced by regional transport of air pollutants and ~ 30% of PM2.5 mass (28.2 μg m-3) during summertime when local emission sources were dominant. A reduction of 3.82 μg m-3 in vehicular carbonaceous aerosols was observed during 07:00-11:00 LT (i.e. rush hours on weekdays) on Sundays and public holidays. This could mainly be attributed to less on-road public transportation (e.g. diesel-powered buses

  9. Variations of carbonaceous aerosols from open crop residue burning with transport and its implication to estimate their lifetimes

    NASA Astrophysics Data System (ADS)

    Pan, X. L.; Kanaya, Y.; Wang, Z. F.; Komazaki, Y.; Taketani, F.; Akimoto, H.; Pochanart, P.

    2013-08-01

    Studying the correlations of carbonaceous aerosols (element carbon, EC, and organic carbon, OC) from open biomass burning helps to reduce uncertainties in emission inventories and provides necessary constraints for model simulations. In the present study, we measured apparent elemental carbon (ECa) and OC concentrations at the summit of Mount Tai (Mt. Tai) during intensive open crop residue burning (OCRB) episodes using a Sunset OCEC analyzer. In the fine particle mode, OC and ECa showed strong correlations (r > 0.9) with carbon monoxide (CO). Footprint analysis using the FLEXPART_WRF model indicated that OCRB in Central East China had a significant influence on ambient carbonaceous aerosol loadings at the summit of Mt. Tai. During campaign, ΔECa/ΔCO ratios of OCRB plumes were found to be 14.3 ± 1.0 ng m-3 ppbv at Mt. Tai. This ratio was twice larger than those for urban pollution in CEC, demonstrating that significant emissions of soot particles emitted from OCRB. ΔOC/ΔCO ratio of OCRB plumes was found to be 41.9 ± 2.6 ng m-3 ppbv averagely. The transport time of smoke particles was estimated using the FLEXPART_WRF tracer model by releasing particles from the ground layer inside geographical regions where large numbers of hotspots were detected by the MODIS sensor. The relationship between transport time and observed ΔECa/ΔCO and ΔOC/ΔCO ratios was fitted by an e-folding exponential function. Results showed that the loss rate of OC (normalized by CO) with transport was much quicker than that of ECa mass, and the corresponding lifetime of OC mass was estimated to be 28.0-44.2 h (1.2-1.8 days), much shorter than that 98.4-136.9 h (4.1-5.7 days) of ECa. Lifetime of ECa estimated for the OCRB events in CEC in the study was comparably lower than the values normally calculated by the transport models. Short lifetime of OC highlighted its vulnerability to cloud scavenging in the presence of water-soluble organic species from biomass combustion.

  10. Estimation of lifetime of carbonaceous aerosol from open crop residue burning during Mount Tai Experiment 2006 (MTX2006)

    NASA Astrophysics Data System (ADS)

    Pan, X. L.; Kanaya, Y.; Wang, Z. F.; Komazaki, Y.; Taketani, F.; Akimoto, H.; Pochanart, P.; Liu, Y.

    2012-06-01

    Studying the emission ratios of carbonaceous aerosols (element carbon, EC, and organic carbon, OC) from open biomass burning helps to reduce uncertainties in emission inventories and provides necessary constraints for model simulations. We measured apparent elemental carbon (ECa) and OC concentrations at the summit of Mount Tai (Mt. Tai) during intensive open crop residue burning (OCRB) episodes using a Sunset OCEC analyzer. Equivalent black carbon (BCe) concentrations were determined using a Multiple Angle Absorption Photometer (MAAP). In the fine particle mode, OC and EC showed strong correlations (r > 0.9) with carbon monoxide (CO). Footprint analysis using the FLEXPART_WRF model indicated that OCRB in central east China (CEC) had a significant influence on ambient carbonaceous aerosol loadings at the summit of Mt. Tai. ΔECa/ΔCO ratios resulting from OCRB plumes were 14.3 ± 1.0 ng m-3 ppbv-1 at Mt. Tai. This ratio was more than three times those resulting from urban pollution in CEC, demonstrating that significant concentrations of soot particles were released from OCRB. ΔOC/ΔCO ratio from fresh OCRB plumes was found to be 41.9 ± 2.6 ng m-3 ppbv-1 in PM1. The transport time of smoke particles was estimated using the FLEXPART_WRF tracer model by releasing inert particles from the ground layer inside geographical regions where large numbers of hotspots were detected by a MODIS satellite sensor. Fitting regressions using the e-folding exponential function indicated that the removal efficiency of OC (normalized to CO) was much larger than that of ECa mass, with mean lifetimes of 27 h (1.1 days) for OC and 105 h (4.3 days) for ECa, respectively. The lifetime of black carbon estimated for the OCRB events in east China was comparably lower than the values normally adopted in the transport models. Short lifetime of organic carbon highlighted the vulnerability of OC to cloud scavenging in the presence of water-soluble organic species from biomass combustion.

  11. The primitive matrix components of the unique carbonaceous chondrite Acfer 094: a TEM study.

    PubMed

    Greshake, A

    1997-01-01

    The mineralogical and chemical characteristics of the fine-grained matrix (< or = 3 micrometers) of the unique primitive carbonaceous chondrite Acfer 094 have been investigated in detail by scanning electron microscopy (SEM) and analytical transmission electron microscopy (ATEM). Generally, the fine-grained matrix represents a highly unequilibrated assemblage of an amorphous material, small forsteritic olivines (200-300 nm), low Ca-pyroxenes (300-400 nm), and Fe,Ni-sulfides (100-300 nm). The matrix is basically unaffected by secondary processes. Only minor amounts of serpentine and ferrihydrite, as products of hydrous alteration, are present. Texturally, the amorphous material acts as a groundmass to olivines, pyroxenes, and sulfides, mostly exhibiting rounded or elongated morphologies. Only very few clastic mineral grains have been found. The texture and chemical composition of the amorphous material are consistent with an origin by disequilibrium condensation in either the cooling solar nebula or a circumstellar environment. As such, the amorphous material may be considered as a possible precursor of matrix materials in other types of chondrites. The non-clastic matrix olivines (Fo98-99) and pyroxenes (En97-100) are suggested to have formed either by condensation in the solar nebula under highly oxidizing conditions or by recrystallization from the amorphous material. The formation of these grains by fragmentation of chondrule components is unlikely due to chemical and microstructural reasons. Rapid cooling caused the observed intergrowths of clino/orthoenstatite in the Mg-rich matrix pyroxenes. Although some similarities exist comparing the fine-grained matrix of Acfer 094 with the matrices of the unequilibrated CO3 chondrite ALHA77307 and the unique type 3 chondrite Kakangari, Acfer 094 remains unique. Since it contains the highest measured concentrations of circumstellar SiC and the second highest of diamond (highest is Orgueil), it seems reasonable to

  12. Comparison of Bulk Carbon Concentrations and Optical Properties of Carbonaceous Aerosols in the North Slope Alaska from Summer 2012 and Summer 2015

    NASA Astrophysics Data System (ADS)

    Sheesley, R. J.; Barrett, T. E.; Moffett, C.; Gunsch, M.; Pratt, K.

    2015-12-01

    With recent drilling permits being issued for exploratory drilling in the Chukchi Sea, there is a need for characterization of carbonaceous aerosols in the Arctic both prior to and during the exploratory drilling phase. A month-long field sampling campaign will be conducted in Barrow, AK, at the confluence of the Chukchi and Beaufort seas, from August to September 2015. Total suspended particulate (TSP) aerosol samples will be collected at the Department of Energy Atmospheric Radiation Measurement (ARM) climate research facility in Barrow, AK, USA. Samples will be analyzed for organic carbon (OC), elemental carbon (EC) on a Sunset carbon analyzer utilizing the NIOSH 5040 method. Samples will also be analyzed for water soluble organic carbon (WSOC) using a water extraction method and subsequent analysis on a Shimadzu Total Carbon Analyzer. Optical properties of the aqueous extracts will also be measured using an Agilent ultraviolet-visible (UV-Vis) spectrometer. OC, EC and WSOC concentrations will then be compared to aerosol samples collected at the same location in summer 2012, prior to the onset of exploratory drilling in the Chukchi Sea. Back trajectory (BT) analysis will be performed for each sampling campaign to help assess the impact of source region on the carbonaceous aerosol budget and to identify any changes in source region between the two campaigns. A comparison of samples from the same location and season both prior to and post drilling will allow for a more accurate characterization and tracking of the potential impacts of new aerosol emission sources in the region.

  13. Observations of Light-Absorbing Carbonaceous Aerosols in East and South Asia

    NASA Astrophysics Data System (ADS)

    Yoon, S.; Kim, S.; Choi, W.

    2013-05-01

    Light-absorbing aerosols, such as black carbon (BC), brown carbon and mineral dust, typically constitute a small fraction of ambient particle mass but can contribute to solar radiative forcing through absorption of solar radiation and heating of the absorbing aerosol layer. Besides the direct radiative effect, the heating can evaporate clouds and change the atmospheric dynamics. In this study, we investigate the optical and radiative properties of light-absorbing aerosols from ground-based and aircraft measurements in East and South Asia within the framework of UNEP Atmospheric Brown Cloud-Asia (ABC-Asia) project and Sustainable Atmosphere for the Kathmandu Valley (SusKat) campaign (December 2012 ~ February 2013). BC mass concentration, aerosol scattering and absorption coefficients measurements and radiative forcing calculations were performed at four sites: Gosan (Korea), Anmyeon (Korea), Hanimaadhoo (Maldives) and Pyramid (Nepal). No significant seasonal variations of aerosol properties, except for summer due to wet scavenging by rainfall, were observed in East Asia, whereas dramatic changes of light-absorbing aerosol properties were observed in South Asia between dry and wet monsoon periods. Although BC mass concentration in East Asia is generally higher than that observed in South Asia, BC mass concentration at Hanimaadhoo during winter dry monsoon is similar to that of East Asia. The observed solar absorption efficiency (absorption coefficient/extinction coefficient) at 550 nm at Gosan and Anmyeon is higher than that in Hanimaadhoo due to large portions of BC emission from fossil fuel combustion. Interestingly, solar absorption efficiency at Pyramid is 0.14, which is two times great than that in Hanimaadhoo and is about 40% higher than that in East Asia, though BC mass concentration at Pyramid is the lowest among four sites. Throughout the unmanned aerial vehicle experiment in Jeju, Korea during August-September 2008, long-range transport of aerosols from

  14. Carbonaceous aerosols recorded in a southeastern Tibetan glacier: analysis of temporal variations and model estimates of sources and radiative forcing

    NASA Astrophysics Data System (ADS)

    Wang, M.; Xu, B.; Cao, J.; Tie, X.; Wang, H.; Zhang, R.; Qian, Y.; Rasch, P. J.; Zhao, S.; Wu, G.; Zhao, H.; Joswiak, D. R.; Li, J.; Xie, Y.

    2015-02-01

    High temporal resolution measurements of black carbon (BC) and organic carbon (OC) covering the time period of 1956-2006 in an ice core over the southeastern Tibetan Plateau show a distinct seasonal dependence of BC and OC with higher respective concentrations but a lower OC / BC ratio in the non-monsoon season than during the summer monsoon. We use a global aerosol-climate model, in which BC emitted from different source regions can be explicitly tracked, to quantify BC source-receptor relationships between four Asian source regions and the southeastern Tibetan Plateau as a receptor. The model results show that South Asia has the largest contribution to the present-day (1996-2005) mean BC deposition at the ice-core drilling site during the non-monsoon season (October to May) (81%) and all year round (74%), followed by East Asia (14% to the non-monsoon mean and 21% to the annual mean). The ice-core record also indicates stable and relatively low BC and OC deposition fluxes from the late 1950s to 1980, followed by an overall increase to recent years. This trend is consistent with the BC and OC emission inventories and the fuel consumption of South Asia (as the primary contributor to annual mean BC deposition). Moreover, the increasing trend of the OC / BC ratio since the early 1990s indicates a growing contribution of coal combustion and/or biomass burning to the emissions. The estimated radiative forcing induced by BC and OC impurities in snow has increased since 1980, suggesting an increasing potential influence of carbonaceous aerosols on the Tibetan glacier melting and the availability of water resources in the surrounding regions. Our study indicates that more attention to OC is merited because of its non-negligible light absorption and the recent rapid increases evident in the ice-core record.

  15. Carbonaceous aerosols recorded in a southeastern Tibetan glacier: analysis of temporal variations and model estimates of sources and radiative forcing

    SciTech Connect

    Wang, Mo; Xu, B.; Cao, J.; Tie, X.; Wang, Hailong; Zhang, Rudong; Qian, Yun; Rasch, Philip J.; Zhao, Shuyu; Wu, Guangjian; Zhao, Huabiao; Joswiak, Daniel R.; Li, Jiule; Xie, Ying

    2015-02-02

    High temporal resolution measurements of black carbon (BC) and organic carbon (OC) covering the time period of 1956–2006 in an ice core over the southeastern Tibetan Plateau show a distinct seasonal dependence of BC and OC with higher respective concentrations but a lower OC / BC ratio in the non-monsoon season than during the summer monsoon. We use a global aerosol-climate model, in which BC emitted from different source regions can be explicitly tracked, to quantify BC source–receptor relationships between four Asian source regions and the southeastern Tibetan Plateau as a receptor. The model results show that South Asia has the largest contribution to the present-day (1996–2005) mean BC deposition at the ice-core drilling site during the non-monsoon season (October to May) (81%) and all year round (74%), followed by East Asia (14% to the non-monsoon mean and 21% to the annual mean). The ice-core record also indicates stable and relatively low BC and OC deposition fluxes from the late 1950s to 1980, followed by an overall increase to recent years. This trend is consistent with the BC and OC emission inventories and the fuel consumption of South Asia (as the primary contributor to annual mean BC deposition). Moreover, the increasing trend of the OC / BC ratio since the early 1990s indicates a growing contribution of coal combustion and/or biomass burning to the emissions. The estimated radiative forcing induced by BC and OC impurities in snow has increased since 1980, suggesting an increasing potential influence of carbonaceous aerosols on the Tibetan glacier melting and the availability of water resources in the surrounding regions. Our study indicates that more attention to OC is merited because of its non-negligible light absorption and the recent rapid increases evident in the ice-core record.

  16. Carbonaceous aerosols recorded in a southeastern Tibetan glacier: analysis of temporal variations and model estimates of sources and radiative forcing

    DOE PAGESBeta

    Wang, Mo; Xu, B.; Cao, J.; Tie, X.; Wang, Hailong; Zhang, Rudong; Qian, Yun; Rasch, Philip J.; Zhao, Shuyu; Wu, Guangjian; et al

    2015-02-02

    High temporal resolution measurements of black carbon (BC) and organic carbon (OC) covering the time period of 1956–2006 in an ice core over the southeastern Tibetan Plateau show a distinct seasonal dependence of BC and OC with higher respective concentrations but a lower OC / BC ratio in the non-monsoon season than during the summer monsoon. We use a global aerosol-climate model, in which BC emitted from different source regions can be explicitly tracked, to quantify BC source–receptor relationships between four Asian source regions and the southeastern Tibetan Plateau as a receptor. The model results show that South Asia hasmore » the largest contribution to the present-day (1996–2005) mean BC deposition at the ice-core drilling site during the non-monsoon season (October to May) (81%) and all year round (74%), followed by East Asia (14% to the non-monsoon mean and 21% to the annual mean). The ice-core record also indicates stable and relatively low BC and OC deposition fluxes from the late 1950s to 1980, followed by an overall increase to recent years. This trend is consistent with the BC and OC emission inventories and the fuel consumption of South Asia (as the primary contributor to annual mean BC deposition). Moreover, the increasing trend of the OC / BC ratio since the early 1990s indicates a growing contribution of coal combustion and/or biomass burning to the emissions. The estimated radiative forcing induced by BC and OC impurities in snow has increased since 1980, suggesting an increasing potential influence of carbonaceous aerosols on the Tibetan glacier melting and the availability of water resources in the surrounding regions. Our study indicates that more attention to OC is merited because of its non-negligible light absorption and the recent rapid increases evident in the ice-core record.« less

  17. Airborne measurements of carbonaceous aerosols in southern Africa during the dry, biomass burning season

    SciTech Connect

    Kirchstetter, Thomas W.; Novakov, T.; Hobbs, Peter V.; Magi, Brian

    2002-06-17

    Particulate matter collected aboard the University of Washington's Convair-580 research aircraft over southern Africa during the dry, biomass burning season was analyzed for total carbon, organic carbon, and black carbon contents using thermal and optical methods. Samples were collected in smoke plumes of burning savanna and in regional haze. A known artifact, produced by the adsorption of organic gases on the quartz filter substrates used to collect the particulate matter samples, comprised a significant portion of the total carbon collected. Consequently, conclusions derived from the data are greatly dependent on whether or not organic carbon concentrations are corrected for this artifact. For example, the estimated aerosol co-albedo (1 - single scattering albedo), which is a measure of aerosol absorption, of the biomass smoke samples is 60 percent larger using corrected organic carbon concentrations. Thus, the corrected data imply that the biomass smoke is 60 percent more absorbing than do the uncorrected data. The black carbon to (corrected) organic carbon mass ratio (BC/OC) of smoke plume samples (0.18/2610.06) is lower than that of samples collected in the regional haze (0.25/2610.08). The difference may be due to mixing of biomass smoke with background air characterized by a higher BC/OC ratio. A simple source apportionment indicates that biomass smoke contributes about three-quarters of the aerosol burden in the regional haze, while other sources (e.g., fossil fuel burning) contribute the remainder.

  18. Airborne Measurements of Carbonaceous Aerosols in Southern Africa during the Dry Biomass Burning Season

    NASA Technical Reports Server (NTRS)

    Kirchstetter, Thomas W.; Novakov, T.; Hobbs, Peter V.; Magi, Brian

    2003-01-01

    Particulate matter collected aboard the University of Washington's (UW) Convair-580 research aircrafi over southem Afiica during the dry biomass burning season was analyzed for total carbon (TC), organic carbon (OC), and black carbon (BC) contents using thermal and optical methods. Samples were collected in smoke plumes of burning savanna and in regional haze. A known artifact, produced by the adsorption of organic gases on the quartz filter substrates used to collect the particulate matter samples, comprised a significant portion of the TC collected. Consequently, conclusions derived from the data are greatly dependent on whether or not OC concentrations are corrected for this artifact. For example, the estimated aerosol coalbedo (1 - single scattering albedo (SSA)), which is a measure of aerosol absorption, of the biomass smoke samples is 60% larger using corrected OC concentrations. Thus, the corrected data imply that the biomass smoke is 60% more absorbing than do the uncorrected data. The BC to (corrected) OC mass ratio (BC/OC) of smoke plume samples (0.18 plus or minus 0.06) is lower than that of samples collected in the regional haze (0.25 plus or minus 0.08). The difference may be due to mixing of biomass smoke with background air characterized by a higher BC/OC ratio. A simple source apportionment indicates that biomass smoke contributes about three quarters of the aerosol burden in the regional haze, while other souxes (e.g., fossil fuel burning) contribute the remainder.

  19. Historical estimation of carbonaceous aerosol emissions from biomass open burning in China for the period 1990-2005.

    PubMed

    Qin, Y; Xie, S D

    2011-12-01

    Multi-year inventories of carbonaceous aerosol emissions from biomass open burning at a high spatial resolution of 0.5° × 0.5° have been constructed in China using GIS methodology for the period 1990-2005. Black carbon (BC) emissions have increased by 383.03% at an annual average rate of 25.54% from 14.05 Gg in 1990 to 67.87 Gg in 2005; while organic carbon (OC) emissions have increased by 365.43% from 57.37 Gg in 1990 to 267.00 Gg in 2005. Through the estimation period, OC/BC ratio for biomass burning was averagely 4.09, suggesting that it was not the preferred control source from a climatic perspective. Spatial distribution of BC and OC emissions were similar, mainly concentrated in three northeastern provinces, central provinces of Shandong, Jiangsu, Anhui and Henan, and southern provinces of Guangxi, Guangdong, Hunan and Sichuan basin, covering 24.89% of China's territory, but were responsible for 63.38% and 67.55% of national BC and OC emissions, respectively. PMID:21911273

  20. Mixing of anthropogenic dust and carbonaceous aerosols in seasonal snow on snow albedo reduction in 2014 China survey

    NASA Astrophysics Data System (ADS)

    Wang, Xin; Huang, Jianping; Pu, Wei

    2016-04-01

    Anthropogenic dusts produced from the affected by human activities derived from the industrial areas and carbonaceous aerosols (black carbon and organic carbon) deposited into snow or ice core via wet and dry deposition play key roles to the regional and global climate. Recently, a China survey was performed to measure the concentrations of insoluble light-absorbing particles (ILAP) in seasonal snow across northern China in January and February of 2014. The results indicate that the higher concentration of NO3- and SO42- and heavy metals of Zn, Pb, Cd, Ni, and Cu are likely to be attributed to enhanced local industrial emissions due to human activities. The emissions from fossil fuel combustion and biomass burning are likely to be important for the chemical elements in the seasonal snow with long-range transport, while medium enrichment factors of Mg, Ca, and Al were predominantly associated with soil dust, which is the most important natural source. There are large ranges of the BC and AD in seasonal snow over northeast China because of the anthropogenic emissions, which are caused by human activities. In addition, although the values of the snow albedo by model simulations are little higher in the visible to near-infrared wavelength than that during the China survey, the surface snow albedo by field campaign measurements have good agreement with the model simulations in the visible wavelength.

  1. Characteristics and major sources of carbonaceous aerosols in PM2.5 from Sanya, China.

    PubMed

    Wang, Jingzhi; Ho, Steven Sai Hang; Cao, Junji; Huang, Rujin; Zhou, Jiamao; Zhao, Youzhi; Xu, Hongmei; Liu, Suixin; Wang, Gehui; Shen, Zhenxing; Han, Yongming

    2015-10-15

    PM2.5 samples were collected in Sanya, China in summer and winter in 2012/2013. Organic carbon (OC), elemental carbon (EC), and non-polar organic compounds including n-alkanes (n-C14-n-C40) and polycyclic aromatic hydrocarbons (PAHs) were quantified. The concentrations of these carbonaceous matters were generally higher in winter than summer. The estimated secondary organic carbon (OCsec) accounted for 38% and 54% of the total organic carbon (TOC) in winter and summer, respectively. The higher value of OCsec in addition to the presences of photochemically-produced PAHs in summer supports that photochemical conversions of organics are much active at the higher air temperatures and with stronger intense solar radiation. Carbon preference index (CPI) and percent contribution of wax n-alkanes suggest that anthropogenic sources were more dominant than derivation from terrestrial plants in Sanya. Diagnostic ratios of atmospheric PAHs further indicate that there was a wide mix of pollution sources in winter while fossil fuel combustion was the most dominant in summer. Positive Matrix Factorization (PMF) analysis with 18 PAHs in the winter samples found that motor vehicle emissions and biomass burning were the two main pollution sources, contributing 37.5% and 24.6% of the total quantified PAHs, respectively. PMID:26026415

  2. Decadal trend of black carbon and refractory carbonaceous aerosol in the western rim of the North Pacific Ocean: atmospheric concentration and the retrieved record of deposition flux

    NASA Astrophysics Data System (ADS)

    Kaneyasu, Naoki; Yamaguchi, Takashi; Noguchi, Izumi; Akiyama, Masayuki; Matsumoto, Kiyoshi

    2013-04-01

    The long-term trend of light absorbing carbonaceous aerosols (or black carbon: BC) or refractory carbonaceous aerosol (or elemental carbon: EC) concentration is reported at European background sites such as Mace Head, and that of aerosol absorption coefficient are monitored in many GAW sites. On the contrary, such long-term data are relatively scarce at around the western part of the North Pacific Ocean. Thus, to understand the long-term variation of in the area, BC in fine aerosol fraction has been measured at Chichi-jima Islands, Japan. Chichi-jima Island is located 1000 km south of the Japanese mainland, and 1800 km west of the coast line of the Asian continent. BC has been measured with an Aethalometer (Magee, AE-16 and AE-30) since December, 1998 with 1 hr time resolution. Mass flowmeter embedded inside the Aethalometer is calibrated with a rotational dry gas-meter once a year. Monthly averaged BC concentration shows an obvious seasonal variation, i.e. high concentration during late autumn-winter-spring period resulting from the transport from East Asia, with maximum daily concentration above 500 ng m-3. In summer, daily concentration was usually less than 20 ng m-3, due to the clean background airmass originating from the North Pacific Anticyclone. Decadal trend of the annual averaged BC concentration showed a increasing trend from 2000 to 2007 and started to decrease after 2008, which roughly coincides with the reported emission trend of SO2 in China (Lu et al., 2010). In addition, total (i.e., wet + dry) deposition record of refractory carbon at two sites in the northern Japan (Rishiri Island: a remote island site, and Sapporo City: an urban site) are retrieved. At these sites, the local government have been measuring the chemical components in precipitation water collected by deposition gauges. In the deposition gauge, a membrane filter made of cellulose-acetate is fixed at the bottom of the funnel to remove water-insoluble particles from the precipitated

  3. Establishing Global Source-Receptor Relationships for Carbonaceous Aerosol to Characterize Sensitivity of its Climate Forcing to Emission Uncertainties

    NASA Astrophysics Data System (ADS)

    Wang, H.; Rasch, P. J.; Easter, R. C.; Singh, B.; Qian, Y.; Ma, P.; Zhang, R.

    2013-12-01

    Carbonaceous aerosol (CA) has been identified as an important but very uncertain forcing agent in the Earth's climate system. It has cascading radiative, microphysical and dynamical effects across the different scales in the atmosphere. Light-absorbing CA (e.g., black carbon (BC) and brown carbon) deposited on snow, sea ice and glaciers can accelerate their melting, which can induce more profound impact through positive feedback mechanisms, having important implications for climate change and fresh water availability at the global and regional scale. Many factors can affect the amount and impacts of CA in a specific region such as the Arctic, among which the global distribution of emissions is of primary importance. There are many uncertainties in global CA emissions, which are changing over time. To better understand the response of climate to these uncertainties and to potential future CA emission changes, it is useful to characterize the global source-receptor relationships and attribute CA loading and radiative forcing to various regional and sectoral CA sources. Observational evidence has clearly demonstrated the occurrence of intercontinental long-range transport of aerosols and to some extent the characteristic transport pathways. However, the observational approach alone cannot provide quantitative information on global source-receptor relationships. We have recently improved the treatment of aerosol transport and wet removal processes in the Community Atmosphere Model version 5 (CAM5) and introduced a brute-force aerosol source tagging technique in which aerosol particles emitted from many independent source regions and sectors are tagged and explicitly tracked. We run the CAM5 model in an 'offline' mode (i.e., driven by reanalysis data) so the transport processes are less likely to be subject to model biases in meteorology and circulation patterns. This modeling tool is used to quantify the characteristics (e.g., burden, surface deposition rate, lifetime

  4. Microscopic Characterization of Carbonaceous Aerosol Particle Aging in the Outflow from Mexico City

    SciTech Connect

    Moffet, R. C.; Henn, T. R.; Tivanski, A. V.; Hopkins, R. J.; Desyaterik, Y.; Kilcoyne, A. L. D.; Tyliszczak, T.; Fast, J.; Barnard, J.; Shutthanandan, V.; Cliff, S.S.; Perry, K. D.; Laskin, A.; Gilles, M. K.

    2009-09-16

    This study was part of the Megacities Initiative: Local and Global Research Observations (MILAGRO) field campaign conducted in Mexico City Metropolitan Area during spring 2006. The physical and chemical transformations of particles aged in the outflow from Mexico City were investigated for the transport event of 22 March 2006. A detailed chemical analysis of individual particles was performed using a combination of complementary microscopy and micro-spectroscopy techniques. The applied techniques included scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure spectroscopy (NEXAFS) and computer controlled scanning electron microscopy with an energy dispersive X-ray analyzer (CCSEM/EDX). As the aerosol plume evolves from the city center, the organic mass per particle increases and the fraction of carbon-carbon double bonds (associated with elemental carbon) decreases. Organic functional groups enhanced with particle age include: carboxylic acids, alkyl groups, and oxygen bonded alkyl groups. At the city center (T0) the most prevalent aerosol type contained inorganic species (composed of sulfur, nitrogen, oxygen, and potassium) coated with organic material. At the T1 and T2 sites, located northeast of T0 (~;;29 km and ~;;65 km, respectively), the fraction of homogenously mixed organic particles increased in both size and number. These observations illustrate the evolution of the physical mixing state and organic bonding in individual particles in a photochemically active environment.

  5. Characteristics of size-segregated carbonaceous aerosols in the Beijing-Tianjin-Hebei region.

    PubMed

    Guo, Yuhong

    2016-07-01

    Mass concentrations of organic carbon (OC) and elemental carbon (EC) in size-resolved aerosols were investigated at four sites (three cities and one country) in the Beijing-Tianjin-Hebei region from September 2009 to August 2011. The size distributions of OC and EC presented large evolutions among rural and urban sites, and among four seasons, with highest peaks of OC and EC in fine mode in urban areas during winter. Geometric mean diameters (GMDs) of OC and EC in fine particles at urban sites during winter were lower than those at rural site mainly due to effects of fine particle coagulation and organic compound repartitioning. Fossil fuel emissions were a dominant source of OC and EC in urban areas, while biomass burning was a major source of OC and EC at rural site. Trajectory clustering and CWT analysis showed that regional transport was an important contributor to OC and EC in Beijing. PMID:27040539

  6. Laboratory Studies of Processing of Carbonaceous Aerosols by Atmospheric Oxidants/Hygroscopicity and CCN Activity of Secondary & Processed Primary Organic Aerosols

    SciTech Connect

    Ziemann, P.J.; Arey, J.; Atkinson, R.; Kreidenweis, S.M.; Petters, M.D.

    2012-06-13

    The atmosphere is composed of a complex mixture of gases and suspended microscopic aerosol particles. The ability of these particles to take up water (hygroscopicity) and to act as nuclei for cloud droplet formation significantly impacts aerosol light scattering and absorption, and cloud formation, thereby influencing air quality, visibility, and climate in important ways. A substantial, yet poorly characterized component of the atmospheric aerosol is organic matter. Its major sources are direct emissions from combustion processes, which are referred to as primary organic aerosol (POA), or in situ processes in which volatile organic compounds (VOCs) are oxidized in the atmosphere to low volatility reaction products that subsequent condense to form particles that are referred to as secondary organic aerosol (SOA). POA and VOCs are emitted to the atmosphere from both anthropogenic and natural (biogenic) sources. The overall goal of this experimental research project was to conduct laboratory studies under simulated atmospheric conditions to investigate the effects of the chemical composition of organic aerosol particles on their hygroscopicity and cloud condensation nucleation (CCN) activity, in order to develop quantitative relationships that could be used to more accurately incorporate aerosol-cloud interactions into regional and global atmospheric models. More specifically, the project aimed to determine the products, mechanisms, and rates of chemical reactions involved in the processing of organic aerosol particles by atmospheric oxidants and to investigate the relationships between the chemical composition of organic particles (as represented by molecule sizes and the specific functional groups that are present) and the hygroscopicity and CCN activity of oxidized POA and SOA formed from the oxidation of the major classes of anthropogenic and biogenic VOCs that are emitted to the atmosphere, as well as model hydrocarbons. The general approach for this project was

  7. Multi-wavelength optical measurement to enhance thermal/optical analysis for carbonaceous aerosol

    NASA Astrophysics Data System (ADS)

    Chen, L.-W. A.; Chow, J. C.; Wang, X. L.; Robles, J. A.; Sumlin, B.; Lowenthal, D. H.; Zimmermann, R.; Watson, J. G.

    2014-09-01

    A thermal/optical carbon analyzer equipped with seven-wavelength light source/detector (405-980 nm) for monitoring spectral reflectance (R) and transmittance (T) of filter samples allows "thermal spectral analysis (TSA)" and wavelength (λ)-dependent organic carbon (OC)-elemental carbon (EC) measurements. Optical sensing is calibrated with transfer standards traceable to absolute R and T measurements and adjusted for loading effects to determine spectral light absorption (as absorption optical depth [τa, λ]) using diesel exhaust samples as a reference. Tests on ambient and source samples show OC and EC concentrations equivalent to those from conventional carbon analysis when based on the same wavelength (~635 nm) for pyrolysis adjustment. TSA provides additional information that evaluates black carbon (BC) and brown carbon (BrC) contributions and their optical properties in the near-IR to the near-UV parts of the solar spectrum. The enhanced carbon analyzer can add value to current aerosol monitoring programs and provide insight into more accurate OC and EC measurements for climate, visibility, or health studies.

  8. Multi-wavelength optical measurement to enhance thermal/optical analysis for carbonaceous aerosol

    NASA Astrophysics Data System (ADS)

    Chen, L.-W. A.; Chow, J. C.; Wang, X. L.; Robles, J. A.; Sumlin, B. J.; Lowenthal, D. H.; Zimmermann, R.; Watson, J. G.

    2015-01-01

    A thermal/optical carbon analyzer equipped with seven-wavelength light source/detector (405-980 nm) for monitoring spectral reflectance (R) and transmittance (T) of filter samples allowed "thermal spectral analysis (TSA)" and wavelength (λ)-dependent organic-carbon (OC)-elemental-carbon (EC) measurements. Optical sensing was calibrated with transfer standards traceable to absolute R and T measurements, adjusted for loading effects to report spectral light absorption (as absorption optical depth (τa, λ)), and verified using diesel exhaust samples. Tests on ambient and source samples show OC and EC concentrations equivalent to those from conventional carbon analysis when based on the same wavelength (~ 635 nm) for pyrolysis adjustment. TSA provides additional information that evaluates black-carbon (BC) and brown-carbon (BrC) contributions and their optical properties in the near infrared to the near ultraviolet parts of the solar spectrum. The enhanced carbon analyzer can add value to current aerosol monitoring programs and provide insight into more accurate OC and EC measurements for climate, visibility, or health studies.

  9. Improved measurement of carbonaceous aerosol in Beijing, China: intercomparison of sampling and thermal-optical analysis methods

    NASA Astrophysics Data System (ADS)

    Cheng, Y.; He, K. B.; Duan, F. K.; Zheng, M.; Ma, Y. L.; Tan, J. H.; Du, Z. Y.

    2010-06-01

    The sampling artifacts (both positive and negative) and the influence of thermal-optical methods (both charring correction method and the peak inert mode temperature) on the split of organic carbon (OC) and elemental carbon (EC) were evaluated in Beijing. The positive sampling artifact constituted 10% and 23% of OC concentration determined by the bare quartz filter during winter and summer, respectively. For summer samples, the adsorbed gaseous organics were found to continuously evolve off the filter during the whole inert mode when analyzed by the IMPROVE-A temperature protocol. This may be due to the oxidation of the adsorbed organics during sampling (reaction artifact) which would increase their thermal stability. The backup quartz approach was evaluated by a denuder-based method for assessing the positive artifact. The quartz-quartz (QBQ) in series method was demonstrated to be reliable, since all of the OC collected by QBQ was from originally gaseous organics. Negative artifact that could be adsorbed by quartz filter was negligible. When the activated carbon impregnated glass fiber (CIG) filter was used as the denuded backup filter, the denuder efficiency for removing gaseous organics that could be adsorbed by the CIG filter was only about 30%. EC values were found to differ by a factor of about two depending on the charring correction method. Influence of the peak inert mode temperature was evaluated based on the summer samples. The EC value was found to continuously decrease with the peak inert mode temperature. Premature evolution of light absorbing carbon began when the peak inert mode temperature was increased from 580 to 650 °C; when further increased to 800 °C, the OC and EC split frequently occurred in the He mode, and the last OC peak was characterized by the overlapping of two separate peaks. The discrepancy between EC values defined by different temperature protocols was larger for Beijing carbonaceous aerosol compared with North America and

  10. Seasonal variations and sources of ambient fossil and biogenic-derived carbonaceous aerosols based on 14C measurements in Lhasa, Tibet

    NASA Astrophysics Data System (ADS)

    Huang, Jie; Kang, Shichang; Shen, Chengde; Cong, Zhiyuan; Liu, Kexin; Wang, Wei; Liu, Lichao

    2010-06-01

    A total of 30 samples of total suspended particles were collected at an urban site in Lhasa, Tibet from August 2006 to July 2007 for investigating carbonaceous aerosol features. The fractions of contemporary carbon ( fc) in total carbon (TC) of ambient aerosols are presented using radiocarbon ( 14C) measurements. The value of fc represents the biogenic contribution to TC, as the biosphere releases organic compounds with the present 14C/ 12C level ( fc = 1), whereas 14C has become extinct in anthropogenic emissions of fossil carbon ( fc = 0). The fc values in Lhasa ranging from 0.357 to 0.702, are higher than Beijing and Tokyo, but clearly lower than the rural region of Launceston, which indicates a major biogenic influence in Lhasa. Seasonal variations of fc values corresponded well with variations of pollutants concentrations (e.g. NO 2). Higher fc values appeared in winter indicating carbonaceous aerosol is more dominated by wood burning and incineration of agricultural wastes within this season. The lower fc values in summer and autumn may be caused by increased diesel and petroleum emissions related to tourism in Lhasa. δ13C values ranged from - 26.40‰ to - 25.10‰, with relative higher values in spring and summer, reflecting the increment of fossil carbon emissions.

  11. Characteristics of carbonaceous aerosol in PM 2.5: Pearl Delta River Region, China

    NASA Astrophysics Data System (ADS)

    Huang, H.; Ho, K. F.; Lee, S. C.; Tsang, P. K.; Ho, Steven Sai Hang; Zou, C. W.; Zou, S. C.; Cao, J. J.; Xu, H. M.

    2012-02-01

    Simultaneous measurements of atmospheric organic carbon (OC), elemental carbon (EC) and water-soluble organic carbon (WSOC) were made at four sampling sites, namely Guangzhou (GZ), Zhaoqing (ZQ), PolyU Campus (PU) and Hok Tsui (HT), in the Pearl River Delta (PRD) region between 14 August 2006 and 28 August 2007. The highest concentrations of total carbon (TC) were found at the medium-scale roadside site (PU) and the lowest were found at the regional-scale site (HT). Among the four sampling sites, the average WSOC at ZQ showed the highest concentrations, while the lowest were seen at HT. OC and EC concentrations revealed spring/summer minima and autumn/winter maxima at all sites except PU, which had a consistently high EC concentration all over the year. The highest WSOC/OC ratio was found at ZQ with an average of 0.41, suggesting that the OC was more oxidized in the atmosphere of the semi-rural site. The lowest WSOC/OC was found at the roadside site of PU. Moreover, the WSOC/OC ratio increased in autumn, when the photochemical reactions are the most active in the PRD region. This can be attributed to aging and atmospheric processing of the organic compounds during their transportation, or to the formation of secondary organic aerosol (SOA). Average annual secondary organic carbon (SOC) concentrations in PM2.5 were estimated to be 2.2 and 3.5 μg m- 3 for GZ and ZQ, comprising 33.5% and 42.8% of the corresponding OC concentrations, respectively. The results indicate that SOC is significant in the PRD region, and its formation mostly occurs within the region.

  12. Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode in 2013

    NASA Astrophysics Data System (ADS)

    Zhang, Y.-L.; Huang, R.-J.; El Haddad, I.; Ho, K.-F.; Cao, J.-J.; Han, Y.; Zotter, P.; Bozzetti, C.; Daellenbach, K. R.; Canonaco, F.; Slowik, J. G.; Salazar, G.; Schwikowski, M.; Schnelle-Kreis, J.; Abbaszade, G.; Zimmermann, R.; Baltensperger, U.; Prévôt, A. S. H.; Szidat, S.

    2014-10-01

    During winter 2013, extremely high concentrations (i.e. 4-20 times higher than the World Health Organization guideline) of PM2.5 (particulate matter with an aerodynamic diameter <2.5 μm) were reported in several large cities in China. In this work, source apportionment of fine carbonaceous aerosols during this haze episode was conducted at four major cities in China including Xian, Beijing, Shanghai and Guangzhou. An effective statistical analysis of a combined dataset from elemental carbon (EC) and organic carbon (OC), radiocarbon (14C) and biomass-burning marker measurements using Latin-hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. We found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% at all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K+). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K+ ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xian (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was rather from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10% and 48 ± 9% of OC and TC, respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8%, 48 ± 18%, 53 ± 4% and 65 ± 26% of non-fossil OC for Xian, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass-burning were mainly attributed to formation of secondary organic carbon

  13. Distribution of the pre-solar component in Allende and other carbonaceous chondrites

    NASA Technical Reports Server (NTRS)

    Clayton, R. N.; Onuma, N.; Grossman, L.; Mayeda, T. K.

    1977-01-01

    Detailed analyses of separated phases of several Allende Ca-Al-rich inclusions are reported which reveal a consistent pattern of large O-16 enrichments in spinel, pyroxene, and sometimes olivine, and small O-16 enrichments in melilite, feldspathoids, and grossular. The heterogeneous distribution of the O-16 excesses, together with their enhancement in minerals believed to be early solar nebular condensates, suggests the existence of pre-solar carriers of the isotopic anomaly, probably grains or molecules with oxygen which was nearly pure O-16. Pre-solar grains of corundum or spinel, and pre-solar molecules of SiO are considered possibilities. Excess O-16, relative to terrestrial abundances, has been found in all samples of C2, C3 (the Allende is this kind), and C4 carbonaceous chondrites which have been analyzed. No direct correlation has yet been observed between the oxygen anomalies and isotope anomalies in neon, magnesium, or xenon.

  14. Optical-chemical-microphysical relationships and closure studies for mixed carbonaceous aerosols observed at Jeju Island; 3-laser photoacoustic spectrometer, particle sizing, and filter analysis

    NASA Astrophysics Data System (ADS)

    Flowers, B. A.; Dubey, M. K.; Mazzoleni, C.; Stone, E. A.; Schauer, J. J.; Kim, S.-W.; Yoon, S. C.

    2010-11-01

    Transport of aerosols in pollution plumes from the mainland Asian continent was observed in situ at Jeju, South Korea during the Cheju Asian Brown Cloud Plume-Asian Monsoon Experiment (CAPMEX) field campaign throughout August and September 2008 using a 3-laser photoacoustic spectrometer (PASS-3), chemical filter analysis, and size distributions. The PASS-3 directly measures the effects of morphology (e.g. coatings) on light absorption that traditional filter-based instruments are unable to address. Transport of mixed sulfate, carbonaceous, and nitrate aerosols from various Asian pollution plumes to Jeju accounted for 74% of the deployment days, showing large variations in their measured chemical and optical properties. Analysis of eight distinct episodes, spanning wide ranges of chemical composition, optical properties, and source regions, reveals that episodes with higher organic carbon (OC)/sulfate (SO42-) and nitrate (NO3-)/SO42- composition ratios exhibit lower single scatter albedo at shorter wavelengths (ω405). We infer complex refractive indices (n-ik) as a function of wavelength for the high, intermediate, and low OC/SO42- pollution episodes by using the observed particle size distributions and the measured optical properties. The smallest mean particle diameter corresponds to the high OC/SO42- aerosol episode. The imaginary part of the refractive index (k) is greater for the high OC/SO42- episode at all wavelengths. A distinct, sharp increase in k at short wavelength implies enhanced light absorption by OC, which accounts for 50% of the light absorption at 405 nm, in the high OC/SO42- episode. Idealized analysis indicates increased absorption at 781 nm by factors greater than 3 relative to denuded black carbon in the laboratory. We hypothesize that coatings of black carbon cores are the mechanism of this enhancement. This implies that climate warming and atmospheric heating rates from black carbon particles can be significantly larger than have been

  15. Impact of transboundary transport of carbonaceous aerosols on the regional air quality in the United States: A case study of the South American wildland fire of May 1998

    NASA Astrophysics Data System (ADS)

    in, Hee-Jin; Byun, Daewon W.; Park, Rokjin J.; Moon, Nan-Kyoung; Kim, Soontae; Zhong, Sharon

    2007-04-01

    The present work is an attempt to improve the performance of a regional air quality model by means of linking it with a global chemistry transport model in order to provide initial and lateral boundary conditions. The current Community Multiscale Air Quality (CMAQ) model uses a set of constant lateral background condition profiles of the pollutant species, without reflecting temporal and spatial variations at the boundaries. A modeling study of a severe biomass burning event during May 1998 in Mexico and Central America, attributable to an ENSO-related drought, is presented. In this study, the GEOS-Chem global model output is incorporated as the CMAQ lateral boundary and initial values through an interpolation reconciling the differences in the vertical and horizontal coordinates and the chemical species representations of the two models. Simulated daily and monthly mean aerosol concentrations were evaluated by comparing these predicted concentrations with observational data from the Interagency Monitoring of Protected Visual Environments (IMPROVE) surface network. CMAQ, using the GEOS-Chem output to provide the lateral boundary conditions, improves model simulation of carbonaceous aerosols, such as the elemental carbons (EC) and organic carbons (OC). The square of correlation coefficients between overall simulated versus observed monthly mean concentration of EC was 0.36 and OC was 0.72, demonstrating successful simulations of transboundary transport of aerosols. Model sensitivity simulations were performed to assess the carbonaceous emissions in the U.S. EPA's National Emissions Inventory for 1999 (NEI99) and to explore long-range transport and local contributions of wild fire emissions as potential sources for correcting the low bias of EC simulations in CMAQ. In the simulation without the boundary influx from wildfire, the analysis shows a general net export of EC and OC from the continental United States of America, while in the simulations with the GEOS

  16. Characteristics of carbonaceous aerosols in Emilia-Romagna (Northern Italy) based on two fall/winter field campaigns

    NASA Astrophysics Data System (ADS)

    Costa, V.; Bacco, D.; Castellazzi, S.; Ricciardelli, I.; Vecchietti, R.; Zigola, C.; Pietrogrande, M. C.

    2016-01-01

    The carbonaceous aerosol in Emilia-Romagna region (Northern Italy) was characterized in two fall/winter monitoring campaigns conducted through the years 2011-2012 and 2012-2013. Nearly 650 PM2.5 samples were collected at three monitoring stations describing urban background (main city Bologna, MS, Parma and Rimini) and one rural background site (San Pietro, SP). OC and EC values were measured by the thermal-optical transmittance method (TOT). Low flow-rate sampling strategy (24 m3 air volume per day) was used to reduce loading of light absorbing material on the filter surface in order to ensure the correct OC/EC discrimination. The TC values measured in winter 2011-2012 ranged from 9.8 μgC m- 3 at San Pietro to 12.0 μgC m- 3 at Parma, consisting of OC from 8.6 μgC m- 3 at SP to 9.9 μgC m- 3 at MS and EC from 1.3 μgC m- 3 at SP to 2.5 μgC m- 3 at Rimini. In winter 2012-2013, lower values were in general found with TC values ranging from 7.8 to 9.1 μgC m- 3 consisting of OC from 5.1 to 7.0 μgC m- 3 and EC from 1.5 to 2.2 μgC m- 3. Such differences can be likely explained by higher pollutant emissions related to domestic heating in colder fall/winter 2011/2012 (mean temperature ≈ 2 °C in comparison with ≈ 7 °C in winter 2012/2013). This hypothesis is supported by high levels of levoglucosan, as unambiguous tracer for biomass burning emission, and of polycyclic aromatic hydrocarbons related to combustion (levoglucosan ≃ 1000 ng m- 3 and burning PAHs ≃ 4 ng m- 3 at MS and SP sites).

  17. Ensemble projections of wildfire activity and carbonaceous aerosol concentrations over the western United States in the mid-21st century

    NASA Astrophysics Data System (ADS)

    Yue, X.; Mickley, L. J.; Logan, J. A.

    2010-12-01

    We estimate future wildfire activity over the western United States during the mid-21st century (2046-2065), based on ensemble results from 16 models following the IPCC A1B scenario. Regression models and a parameterization model of area burned (AB) are developed for the projection. The ecoregion-based regression models consider the meteorological impacts from both the current and previous years on the regional AB; the correlation coefficients between the predicted and observed annual AB range from 0.59 to 0.85 during 1981-2000 for six ecoregions. The parameterization model calculates the effects of temperature, precipitation, and relative humidity on daily AB; the predicted monthly total AB over the western US is highly correlated with observations with a normal (logarithmic) correlation coefficient of 0.73 (0.90) for 300 months (1980-2004). The meteorological fields under the A1B scenario from 15 IPCC models and a general circulation model (NASA/GISS GCM 3) are applied to the fire models to estimate AB during 2046-2065. We calculate that the annual AB will increase by 21~124% (regression models) and 40~198% (parameterization) over six ecoregions in the western US at midcentury relative to present day; the length of fire season will extend by 11.1% for the warmer and drier climate. We also examine the impact of the changing climate on the fuel load with a dynamic vegetation model LPJ driven by future meteorology from the GISS GCM 3; it shows that the fuel load over western US experiences small changes because of the short time period from 2000 to 2050. Based on the projected fuel load and the AB calculations, we estimate that the annual total biomass burning over western US will increase by 68% (regression models) or as much as 161% (parameterization). We further investigate the impact of the changing fire emission on the carbonaceous aerosol concentrations over the western United States in the mid-21st century using the chemistry transport model GEOS-Chem driven

  18. Carbonaceous aerosols in the Western Mediterranean during summertime and their contribution to the aerosol optical properties at ground level: First results of the ChArMEx-ADRIMED 2013 intensive campaign in Corsica

    NASA Astrophysics Data System (ADS)

    Sciare, Jean; Dulac, Francois; Feron, Anais; Crenn, Vincent; Sarda Esteve, Roland; Baisnee, Dominique; Bonnaire, Nicolas; Hamonou, Eric; Mallet, Marc; Lambert, Dominique; Nicolas, Jose B.; Bourrianne, Thierry; Petit, Jean-Eudes; Favez, Olivier; Canonaco, Francesco; Prevot, Andre; Mocnik, Grisa; Drinovec, Luka; Marpillat, Alexandre; Serrie, Wilfrid

    2014-05-01

    As part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx, http://charmex.lsce.ipsl.fr/), the CORSiCA (http://www.obs-mip.fr/corsica) and the ANR-ADRIMED programs, a large set of real-time measurements of carbonaceous aerosols was deployed in June 2013 at the Cape Corsica atmospheric supersite (http://gaw.empa.ch/gawsis/reports.asp?StationID=2076203042). Submicron organic aerosols (OA) were monitored every 30 min using an Aerosol Chemical Speciation Monitor (ACSM; Aerodyne Res. Inc. MA, USA); Fine (PM2.5) Organic Carbon (OC) and Elemental Carbon (EC) were measured every 2h using an OCEC Sunset Field Instrument (Sunset Lab, OR, USA) and every 12h using a low-vol (Leckel) filter sampler running at 2.3m3/h. Equivalent Black Carbon (BC) was monitored using two Aethalometers (models AE31 and AE33, Magee Scientific, US & Aerosol d.o.o., Slovenia) and a MAAP instrument (Thermo). Quality control of this large dataset was performed through chemical mass closure studies (using co-located SMPS and TEOM-FDMS) and direct comparisons with other real-time instruments running in parallel (Particle-Into-Liquid-Sampler-Ion-Chromatograph for ions, filter sampling, ...). Source apportionment of OA was then performed using the SourceFinder software (SoFi v4.5, http://www.psi.ch/acsm-stations/me-2) allowing the distinction between hydrogen- and oxygen-like organic aerosols (HOA and OOA, respectively) and highlighting the major contribution of secondary OA in the Western Mediterranean during summer. Using this time-resolved chemical information, reconstruction of the optical aerosol properties were performed and compared with integrating nephelometer (Model 3563, TSI, US) and photoacoustic extinctiometer (PAX, DMT, US) measurements performed in parallel. Results of these different closure studies (chemical/physical/optical) are presented and discussed here in details. They highlight the central role of carbonaceous aerosols on the optical properties of aerosols at ground level

  19. Monitoring of inorganic ions, carbonaceous matter and mass in ambient aerosol particles with online and offline methods

    NASA Astrophysics Data System (ADS)

    Timonen, H.; Aurela, M.; Saarnio, K.; Frey, A.; Saarikoski, S.; Teinilä, K.; Kulmala, M.; Hillamo, R.

    2011-10-01

    Year-long high timeresolution measurements of major chemical components in atmospheric sub-micrometer particles were conducted at an urban background station in Finland 2006-2007. Ions were analyzed using a particle-into-liquid sampler combined with an ion chromatograph (PILS-IC), organic and elemental carbon (OC and EC) by using a semicontinuos OC/EC aerosol carbon analyzer (RT-OCEC), and PM2.5 mass with a tapered element oscillating microbalance (TEOM). Long time series provides information on differences between the used measurement techniques as well as information about the diurnal and seasonal changes. Chemical mass closure was constructed by comparing the identified aerosol mass with the measured PM2.5. The sum of all components measured online (ions, particulate organic matter (POM), EC) represented only 65% of the total PM2.5 mass. The difference can be explained by the difference in cutoff sizes (PM1 for online measurements, PM2.5 for total mass) and by evaporation of the semivolatile/volatile components. In general, some differences in results were observed when the results of the continuous/semicontinuous instruments were compared with those of the conventional filter samplings. For non-volatile compounds, like sulfate and potassium, correlation between the filter samples and the PILS was good but greater differences were observed for the semivolatile compounds like nitrate and ammonium. For OC the results of the RT-OCEC were on average 10% larger than those of the filters. When compared to filter measurements, high resolution measurements provide important data on short pollution plumes as well as on diurnal changes. Clear seasonal and diurnal cycles were observed for nitrate and EC.

  20. Calibration method for a photoacoustic system for real time source apportionment of light absorbing carbonaceous aerosol based on size distribution measurements

    NASA Astrophysics Data System (ADS)

    Utry, Noemi; Ajtai, Tibor; Pinter, Mate; Orvos, Peter I.; Szabo, Gabor; Bozoki, Zoltan

    2016-04-01

    In this study, we introduce a calibration method with which sources of light absorbing carbonaceous particulate matter (LAC) can be apportioned in real time based on multi wavelength optical absorption measurements with a photoacoustic system. The method is primary applicable in wintry urban conditions when LAC is dominated by traffic and biomass burning. The proposed method was successfully tested in a field campaign in the city center of Szeged, Hungary during winter time where the dominance of traffic and wood burning aerosol has been experimentally demonstrated earlier. With the help of the proposed calibration method a relationship between the measured Aerosol Angström Exponent (AAE) and the number size distribution can be deduced. Once the calibration curve is determined, the relative strength of the two pollution sources can be deduced in real time as long as the light absorbing fraction of PM is exclusively related to traffic and wood burning. This assumption is indirectly confirmed in the presented measurement campaign by the fact that the measured size distribution is composed of two unimodal size distributions identified to correspond to traffic and wood burning aerosols. The proposed method offers the possibility of replacing laborious chemical analysis with simple in-situ measurement of aerosol size distribution data.

  1. The Role of Global Emission Inventory of Carbonaceous Emissions

    NASA Astrophysics Data System (ADS)

    Fatima, H.; Sharma, O. P.; Updhyaya, H.

    2010-12-01

    Aerosols - liquid or solid particles suspended in the air - are important constituents of the global atmosphere. They have a direct effect on climate by scattering and/or absorbing solar radiation modifying the radiative balance of the atmosphere and indirect effect by acting as condensation nuclei, their increase in number concentration may give rise to increased number of cloud condensation nuclei, which might increase the droplet concentration with relatively smaller size droplets for fixed liquid water content, making clouds more reflective (Twomey, 1977). Recent measurements show that atmospheric black carbon (BC) and organic carbon (OC) aerosol particles frequently contribute significantly to the total aerosol mass (Novakov et al. 1997). BC is emitted as primary particles from incomplete combustion process, such as fossil fuel and biomass burning, and therefore much atmospheric BC is of anthropogenic origin. OC is emitted as both primary particles and by secondary production from gaseous compounds via condensation or gas phase oxidation of hydrocarbons. Primary organic aerosols come from both anthropogenic sources (fossil fuel and biomass burning) and from natural sources (such as debris, pollen, spores, and algae). Carbonaceous aerosols make up a large but highly variable fraction of the atmospheric aerosol. Black carbon aerosols absorb the solar radiation and induce positive forcing whereas organic matter aerosols reflect solar radiation and produce negative forcing. Various emission inventories have been developed for carbonaceous aerosols. Detailed emission inventories for both BC and OC have been developed (e.g., Penner et al., 1993; Cooke and Wilson, 1996; Liousse et al., 1996; Cooke et al., 1999, Bond et al. 2004) that consider both fossil fuel and biomass components. The inventories of biomass- burning BC and OC particles are more difficult to constrain than fossil fuel emissions, owing to the paucity of data. In the present study we have compared the

  2. Interannual Variability of Carbonaceous Particles from Boreal Wildland Fires and their Contributions to Aerosol Loading and Deposition in the Arctic (Invited)

    NASA Astrophysics Data System (ADS)

    Lavoue, D.; Zhao, T. L.; Gong, S. L.; Huang, P.; Sharma, S.; Stocks, B. J.

    2009-12-01

    We performed two modeling studies to assess over several consecutive years the emissions of carbonaceous particles from boreal wildland fires and to investigate the synoptic transport of boreal smoke to the Arctic. Firstly, a wildfire emission model based on the Canadian Forest Fire Behavior Prediction (FBP) System was applied to forest fires in Canada from 2000 to 2004. Fire datasets, including final sizes and locations, were compiled from records of provincial, territorial, and federal management agencies. Fuel consumption, rate of spread, and injection heights were calculated hourly for individual fires from forest fuel patterns and meteorological conditions obtained with the Canadian weather forecast model GEM. Wildfire emissions were compared to anthropogenic fossil fuel combustion sources at provincial, territorial, and national levels. Moreover, transport pathways of Canadian smoke plumes to the Arctic were investigated using the Lagrangian dispersion model HYSPLIT. Secondly, 10 years of carbonaceous aerosol atmospheric transport were simulated with the Canadian multi-scale air quality modeling system GEM-AQ/EC from 1995 to 2004. The horizontal grid was configured with a global uniform resolution of 1 deg. Monthly emission inventories from boreal wildland fires were built from a combination of fire agencies' reports and satellite products. For Canada, we used the 1995-1999 large fire database (> 200 ha) to complete the previous emission dataset. With respect to Alaska, Russia, and Mongolia, burn scars were used to determine annual areas burned and monthly variability was obtained from MODIS and ATSR fire pixels. GEM-AQ/EC was run with constant anthropogenic emissions representative of the end of the 1990’s. Simulation outputs were compared to satellite observations and ground measurements at four sites (Alert, Barrow, Ny-Alesund, and Summit) across the Arctic. Boreal smoke contributions to aerosol surface concentrations, aerosol optical depths, and

  3. An Unique On-line Method to Infer Black Carbonaceous contributions to Water-Insoluble Aerosol Compositions

    NASA Astrophysics Data System (ADS)

    Asa-Awuku, A. A.; Short, D.

    2013-12-01

    Particle number, size, and composition information is important for constraining aerosol effects on air quality, climate, and health. The composition of particles, especially from vehicular sources, may contain insoluble material that may modify particle nucleating properties. Changes in fuel properties are known to modify criteria pollutants and particulate matter mass, size, and number. In this work we summarize findings as they pertain to the water-soluble and insoluble composition of particles. In field measuremnts and controlled laboratory studies, a water-based condensation particle counter (CPC) and a butanol-based CPC measure particle number concentration. Both instruments were coupled with a Scanning Mobility Particle Sizer (SMPS) and particle number and size data were recorded. Real time particle insoluble mass fractions are estimated with the SMPS data sets; theoretical soluble fractions are calculated from ideal hygroscopicty single parameter values. This is the first time that this experimental method has been employed and used to infer online insoluble fractions. The results show that near-roadway emissions contain water insoluble and black carbon components. We will discuss the contributions of the organic component to the water-insoluble nature. Time permitting, the emissions of different ethanol and butanol gasoline blends are also explored for light-duty vehicles on a light-duty dynaometer chassis. Laboratory results indicate that soluble vehicular components are strongly correlated with vehicle driving conditions.

  4. Effects of particle shape, hematite content and semi-external mixing with carbonaceous components on the optical properties of accumulation mode mineral dust

    NASA Astrophysics Data System (ADS)

    Mishra, S. K.; Tripathi, S. N.; Aggarwal, S. G.; Arola, A.

    2010-12-01

    The radiative forcing estimation of the polluted mineral dust is limited due to lack of morphological analysis, mixing state with the carbonaceous components and the hematite content in the pure dust. The accumulation mode mineral dust has been found to mix with anthropogenically produced black carbon, organic carbon and brown carbon during long range transport. The above features of the polluted dust are not well accounted in the optical models and lead the uncertainty in the numerical estimation of their radiative impact. The Semi-external mixing being a prominent mixing of dust and carbonaceous components has not been studied in details so for compared to core-shell, internal and external mixing studies. In present study, we consider the pure mineral dust composed of non-metallic components (such as Quartz, Feldspar, Mica and Calcite) and metalic component like hematite (Fe2O3). The hematite percentage in the pure mineral dust governs its absorbance. Based on this hematite variation, the hematite fraction in pure mineral dust has been constrained between 0-8%. The morphological and mineralogical characterization of the polluted dust led to consider the three sphere, two sphere and two spheroid model shapes for polluted dust particle system. The pollution gives rise to various light absorbing aerosol components like black carbon, brown carbon and organic carbon (comprising of HUmic-Like Substances, HULIS) in the atmosphere. The entire above discussed model shapes have been considered for the mineral dust getting polluted with (1) organic carbon (especially HULIS component) (2) Brown carbon and (3) black carbon by making a semi-external mixture with pure mineral dust. The optical properties (like Single Scattering Albedo, SSA; Asymmetry parameter, g and Extinction efficiency, Qext) of above model shapes for the polluted dust have been computed using Discrete Dipole Approximation, DDA code. For above model shapes, the SSA was found to vary depending on hematite

  5. Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013

    NASA Astrophysics Data System (ADS)

    Zhang, Y.-L.; Huang, R.-J.; El Haddad, I.; Ho, K.-F.; Cao, J.-J.; Han, Y.; Zotter, P.; Bozzetti, C.; Daellenbach, K. R.; Canonaco, F.; Slowik, J. G.; Salazar, G.; Schwikowski, M.; Schnelle-Kreis, J.; Abbaszade, G.; Zimmermann, R.; Baltensperger, U.; Prévôt, A. S. H.; Szidat, S.

    2015-02-01

    During winter 2013, extremely high concentrations (i.e., 4-20 times higher than the World Health Organization guideline) of PM2.5 (particulate matter with an aerodynamic diameter < 2.5 μm) mass concentrations (24 h samples) were found in four major cities in China including Xi'an, Beijing, Shanghai and Guangzhou. Statistical analysis of a combined data set from elemental carbon (EC), organic carbon (OC), 14C and biomass-burning marker measurements using Latin hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. Based on 14C measurements of EC fractions (six samples each city), we found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% across all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K+). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K+ ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xi'an (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10 and 48 ± 9% of OC and total carbon (TC), respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8, 48 ± 18, 53 ± 4 and 65 ± 26% of non-fossil OC for Xi'an, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass burning were mainly attributed to formation of secondary organic carbon (SOC) from non-fossil precursors such as biomass

  6. A 1 year record of carbonaceous aerosols from an urban site in the Indo-Gangetic Plain: Characterization, sources, and temporal variability

    NASA Astrophysics Data System (ADS)

    Ram, Kirpa; Sarin, M. M.; Tripathi, S. N.

    2010-12-01

    This study presents a comprehensive 1 year (January 2007-March 2008) data set on the chemical composition of ambient aerosols collected from an urban location (Kanpur) in the Indo-Gangetic Plain (IGP) and suggests that the varying strength of the regional emission sources, boundary layer dynamics, and formation of secondary aerosols all contribute significantly to the temporal variability in the mass concentrations of elemental carbon (EC), organic carbon (OC), and water-soluble OC (WSOC). On average, carbonaceous aerosols contribute nearly one third of the PM10 mass during winter, whereas their fractional mass is only ˜10% during summer. A three- to four-fold increase in the OC and K+ concentrations during winter and a significant linear relation between them suggest biomass burning (wood fuel and agricultural waste) emission as a dominant source. The relatively high OC/EC ratio (average: 7.4 ± 3.5 for n = 66) also supports that emissions from biomass burning are overwhelming for the particulate OC in the IGP. The WSOC/OC ratios vary from 0.21 to 0.70 over the annual seasonal cycle with relatively high ratios in the summer, suggesting the significance of secondary organic aerosols. The long-range transport of mineral aerosols from Iran, Afghanistan, and the Thar Desert (western India) is pronounced during summer months. The temporal variability in the concentrations of selected inorganic constituents and neutralization of acidic species (SO42- and NO3-) by NH4+ (dominant during winter) and Ca2+ (in summer) reflect conspicuous changes in the source strength of anthropogenic emissions.

  7. Real-time measurement of aerosol black carbon during the Carbonaceous Species Methods Comparison Study, Citrus College, Glendora, California, August 12-21, 1986: Final report

    SciTech Connect

    Hansen, A.D.A.; Novakov, T.

    1987-11-01

    During the period August 12-21, 1986, the Atmospheric Aerosol Research Group of Lawrence Berkeley Laboratory participated in the Carbonaceous Species Method Comparison Study (CSMCS) conducted at Citrus College, Glendora, California. The equipment that we used was the aethalometer, an instrument developed at LBL that measures the concentration of aerosol black carbon in real time. In this report we present our results from that study in the form of 1-minute, 1-hour, and multi-hour average concentrations. We found concentrations generally ranging from 2 to 5 ..mu..g (BC)m/sup 3/, usually with increases in the morning traffic hours. We also observed short-duration (2-15 min) peaks in the black carbon concentration that could be directly attributed to the activity of vehicles in a delivery area less than 50 m from the study site. We conclude that mobile sources were the major contributor to the short- and medium-term variability of aerosol black carbon measured at this site. 5 refs., 5 figs., 1 tab

  8. [Investigation of Carbonaceous Airborne Particles by Scanning Proton Microprobe].

    PubMed

    Bao, Liang-man; Liu, Jiang-feng; Lei, Qian-tao; Li, Xiao-lin; Zhang, Gui-lin; Li, Yan

    2016-01-15

    Carbonaceous particles are an important component of the atmospheric aerosol particles and important for global climate change, air quality and human health. The PM₁₀ single particles from two environmental monitor locations and seven pollution emission sources were analyzed using scanning proton microprobe (SPM) techniques. The concentration of carbon in individual particles was quantitatively determined by proton non-Rutherford elastic backscattering spectrometry (EBS). The results of this investigation showed that carbonaceous particles were dominant in the pollution sources of coal and oil combustions, diesel busexhaust and automobile exhaust, while inorganic particles were dominant in the sources of steel industry, cement dust and soil dust. Carbonaceous matter was enriched in particles from the city center, while mineral matter was the main component of airborne particles in the industrial area. Elemental mapping of single aerosol particles yielded important information on the chemical reactions of aerosol particles. The micro-PIXE (particle induced X-ray emission) maps of S, Ca and Fe of individual carbonaceous particles showed that sulfuration reaction occurred between SO₂and mineral particles, which increased the sulfur content of particles. PMID:27078933

  9. Investigation of aerosol components influencing atmospheric transfer of UV radiation in Baltic Sea region

    NASA Astrophysics Data System (ADS)

    Reinart, A.; Kikas, Ü.; Tamm, E.

    2006-01-01

    Linking of atmospheric aerosol size distributions and optical properties via predefined aerosol components was investigated. The measured aerosol volume distributions were decomposed to Optical Properties of Aerosols and Clouds (OPAC) components, and aerosol optical properties were calculated for a mixture of those components. The obtained aerosol optical properties were then used for modeling the surface UV irradiances with the libRadtran radiative transfer code. The results were verified with the columnar aerosol characteristics obtained from Aerosol Robotic Network (AERONET) station Tõravere (58.26°N, 26.46°E) and clear-sky surface UV measurements in Pärnu, Estonia (58.38°N, 24.51°E). The best decomposition results were obtained with four OPAC components, when their lookup characteristics varied within ±10%. Variation of aerosol optical properties in 17 days was influenced by the following aerosol components: soot, 1.2 ± 1.4%; insoluble, 23.1 ± 8.3%; water-soluble, 44.0 ± 10.8%; accumulation mode sea salt, 31.6 ± 6.2% of total aerosol volume. The average refractive index (for λ = 440 nm) of the component mixture was of 1.42 - 0.013i. Interpretation of the soot component was disputable, since similarly high soot concentrations corresponded to the secondary particles in polluted atmosphere and the nucleation bursts in clean atmosphere. The sea-salt component showed a correlation with the aerosol residence time over sea. The water-soluble component and the additional "biomass haze" component represented partly the same aerosol volume in the diameter range of 0.18-1.8 μm. The surface UV irradiances modeled with the AERONET data and the fitted aerosol components were highly correlated with each other, but both model results underestimated the UV extinction by aerosol.

  10. Extinction spectra of mineral dust aerosol components in an environmental aerosol chamber: IR resonance studies

    NASA Astrophysics Data System (ADS)

    Mogili, Praveen K.; Yang, K. H.; Young, Mark A.; Kleiber, Paul D.; Grassian, Vicki H.

    Mineral dust aerosol plays an important role in determining the physical and chemical equilibrium of the atmosphere. To better understand the impact that mineral dust aerosol may have on climate forcing and on remote sensing, we have initiated a study of the optical properties of important components of mineral dust aerosol including silicate clays (illite, kaolinite, and montmorillonite), quartz, anhydrite, and calcite. The extinction spectra are measured in an environmental simulation chamber over a broad wavelength range, which includes both the IR (650-5000 cm -1) and UV-vis (12,500-40,000 cm -1) spectral regions. In this paper, we focus on the IR region from 800 to 1500 cm -1, where many of these mineral dust constituents have characteristic vibrational resonance features. Experimental spectra are compared with Mie theory simulations based on published mineral optical constants. We find that Mie theory generally does a poor job in fitting the IR resonance peak positions and band profiles for nonspherical aerosols in the accumulation mode size range ( D˜0.1-2.5 μm). We explore particle shape effects on the IR resonance line profiles by considering analytic models for extinction of particles with characteristic shapes (i.e. disks, needles, and ellipsoids). Interestingly, Mie theory often appears to give more accurate results for the absorption line profiles of larger particles that fall in the coarse mode size range.

  11. Polycyclic Aromatic Aerosol Components: Chemical Analysis and Reactivity

    NASA Astrophysics Data System (ADS)

    Schauer, C.; Niessner, R.; Pöschl, U.

    Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous environmental pollutants in the atmosphere and originate primarily from incomplete combustion of organic matter and fossil fuels. Their main sources are anthropogenic (e.g. vehicle emissions, domes- tic heating or tobacco smoke), and PAHs consisting of more than four fused aromatic rings reside mostly on combustion aerosol particles, where they can react with atmo- spheric trace gases like O3, NOx or OH radicals leading to a wide variety of partially oxidized and nitrated derivatives. Such chemical transformations can strongly affect the activity of the aerosol particles as condensation nuclei, their atmospheric residence times, and consequently their direct and indirect climatic effects. Moreover some poly- cyclic aromatic compounds (PACs = PAHs + derivatives) are known to have a high carcinogenic, mutagenic and allergenic potential, and are thus of major importance in air pollution control. Furthermore PACs can be used as well defined soot model sub- stances, since the basic structure of soot can be regarded as an agglomerate of highly polymerized PAC-layers. For the chemical analysis of polycyclic aromatic aerosol components a new analyti- cal method based on LC-APCI-MS has been developed, and a data base comprising PAHs, Oxy-PAHs and Nitro-PAHs has been established. Together with a GC-HRMS method it will be applied to identify and quantify PAHs and Nitro-PAHs in atmo- spheric aerosol samples, diesel exhaust particle samples and model soot samples from laboratory reaction kinetics and product studies. As reported before, the adsorption and surface reaction rate of ozone on soot and PAH-like particle surfaces is reduced by competitive adsorption of water vapor at low relative humidity (< 25 %). Recent results at higher relative humidities (ca. 50 %), however, indicate re-enhanced gas phase ozone loss, which may be due to absorbtion of ozone into an aqueous surface layer. The interaction of ozone and nitrogen

  12. Aerosol chemical components in Alaska air masses: 1. Aged pollution

    NASA Astrophysics Data System (ADS)

    Shaw, Glenn E.

    1991-12-01

    A 4-year Alaska chemical data set of aerosols or "dust" in the air clearly reveals a mixture of distinct aerosol components with different and interesting chemical composition, one or two being ascribed to pollution imported to Alaska by winds all the way from other continents. Of particular note is a strong chemical contrast between what we imagine to be highly scavenged, orographically lifted, northern Pacific air (Pacific marine air mass) and stagnant Arctic air (polar air mass), the latter containing seasonal average concentrations of between 2-4 times the concentration of the former, at least for pollution markers noncrustal vanadium, noncrustal manganese, arsenic, selenium, bromine, and antimony. The findings concur our old discovery that Arctic air is persistently polluted (Arctic haze), but Pacific air is relatively clean, in spite of the fact that Alaska is downwind of major pollution sources in the Orient. This is remarkable. In this the first of a two-part paper, we concentrate on the pollution component found primarily during incursion of Arctic polar air. Two major occurrences of visual haze with optical depths of approximately 0.2 and elevated aerosol concentration lasting about a month (spring 1985 and 1986) were affiliated with strong incoming transport of polar air, temperatures ranging from 10° to 20°C below normal (polar air) and air trajectory hindcasts leading back to industrial pollution sources in Eurasia. These long-range transport pollution events brought metal-rich aerosol of removal-resistant submicron particles. The size, chemistry, and meteorology all strongly suggest the presence of a well-aged (10-100 day) polluted air mass. An important implication is that in spring a large fraction of the Arctic polar air mass becomes charged with by-products of industrial pollution. In this multiyear chemical data set one finds a notable summer-winter contrast, changing by factors of 2 to 4 for pollution markers As, Se, Sb, and noncrustal

  13. Source apportionment using radiocarbon and organic tracers for PM2.5 carbonaceous aerosols in Guangzhou, South China: contrasting local- and regional-scale haze events.

    PubMed

    Liu, Junwen; Li, Jun; Zhang, Yanlin; Liu, Di; Ding, Ping; Shen, Chengde; Shen, Kaijun; He, Quanfu; Ding, Xiang; Wang, Xinming; Chen, Duohong; Szidat, Sönke; Zhang, Gan

    2014-10-21

    We conducted a source apportionment and investigated the atmospheric behavior of carbonaceous aerosols during hazy and normal days using radiocarbon ((14)C) and biomass burning/secondary organic aerosol (SOA) tracers during winter in Guangzhou, China. Haze episodes were formed either abruptly by local emissions or through the accumulation of particles transported from other areas. The average contributions of fossil carbon to elemental carbon (EC), water-insoluble organic carbon, and water-soluble organic carbon were 71 ± 10%, 40 ± 6% and 33 ± 3%, respectively. High contributions of fossil carbon to EC (80-90%) were observed for haze samples that were substantially impacted by local emissions, as were the highest (lowest) ratios for NO3(-)/SO4(2-) (OC/EC), which indicates that these particles mainly came from local vehicle exhaust. Low contributions of fossil carbon to EC (60-70%) were found for haze particles impacted by regional transport. Secondary organic carbon (SOC) calculated using SOA tracers accounts for only ∼ 20% of the SOC estimated by (14)C, which is probably because some important volatile organic carbons are not taken into account in the SOA tracer calculation method and because of the large discrepancy in ambient conditions between the atmosphere and smog chambers. A total of 33 ± 11% of the SOC was of fossil origin, a portion of which could be influenced by humidity. PMID:25264588

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

    NASA Astrophysics Data System (ADS)

    Jung, Jinsang; Lee, Sangil; Kim, Hyosun; Kim, Doyeon; Lee, Hyoeun; Oh, Sanghyup

    2014-06-01

    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.

  15. Two-component wind fields from single scanning aerosol lidar

    NASA Astrophysics Data System (ADS)

    Mayor, Shane D.; Derian, Pierre; Mauzey, Christopher F.; Hamada, Masaki

    2015-09-01

    An overview of recent research results on the performance of two motion estimation algorithms used to deduce two-component horizontal wind fields from ground-based scanning elastic backscatter lidar is presented. One motion estimation algorithm is a traditional cross-correlation method optimized for atmospheric lidar data. The second algorithm is a recently-developed wavelet-based optical flow. An intercomparison of experimental results with measurements from an independent Doppler lidar over an agricultural area in Chico, California, during daytime convective conditions in 2013-14 are presented. Finally, early results from application of the algorithms to data collected over the ocean from a compact and portable aerosol lidar that was deployed on the northern California coast in March of 2015 are presented.

  16. Size distribution of carbonaceous aerosols at a high-altitude site on the central Tibetan Plateau (Nam Co Station, 4730 m a.s.l.)

    NASA Astrophysics Data System (ADS)

    Wan, Xin; Kang, Shichang; Wang, Yuesi; Xin, Jinyuan; Liu, Bin; Guo, Yuhong; Wen, Tianxue; Zhang, Guoshuai; Cong, Zhiyuan

    2015-02-01

    The chemical composition and size distribution characteristics of atmospheric aerosols have important effects on the environment, human health and climate change. In this paper, we study the size distribution of carbonaceous aerosols at the remote and pristine site, Nam Co Monitoring and Research Station for Multisphere Interactions, in the inland Tibetan Plateau (TP) based on collected size-segregated aerosols during 2012. The samples were quantified using the thermal/optical (TOR) method. The overall average concentrations of OC and EC in TSP, PM9.0, PM2.1, and PM1.0 were 4.61 μg m- 3 and 0.19 μg m- 3, 4.52 μg m- 3 and 0.18 μg m- 3, 2.72 μg m- 3 and 0.11 μg m- 3, and 2.11 μg m- 3 and 0.09 μg m- 3, respectively. Generally, the highest concentration of OC and EC in different aerosol size occurred during winter. The low level of EC indicated that direct anthropogenic disturbances in the interior of the TP still remain insignificant. The size distributions of OC and EC concentrations presented bimodal variations. In winter, pre-monsoon, monsoon, and post-monsoon seasons, the peaks for OC were in droplet mode (0.43-0.65 μm) and coarse mode (4.7-5.8 μm); while in the monsoon period, the coarse mode shifted to a smaller size bin (3.3-4.7 μm). The coarse mode may be due to dust particles while the droplet mode may be due to the growth process of particles. For EC, the peaks variations in coarse mode were as same as OC, while the other peaks were complicated: the peaks during winter, pre-monsoon, and monsoon seasons exhibited in droplet mode (1.1-2.1 μm, 0.65-1.1 μm, and 0.43-0.65 μm, respectively), and in post-monsoon period, the peak located in condensation mode. The highest peak concentrations for OC and EC occurred in winter and the pre-monsoon period, while the lowest peak values in the monsoon and post-monsoon periods, respectively. The size distribution variations may be caused by deposition, gas/particles exchange, hygroscopic growth, external mixing

  17. Radiocarbon-insights into temporal variations in the sources and concentrations of carbonaceous aerosols in the Los Angeles and Salt Lake City Metropolitan Areas

    NASA Astrophysics Data System (ADS)

    Czimczik, Claudia; Mouteva, Gergana; Simon, Fahrni; Guaciara, Santos; James, Randerson

    2014-05-01

    Increased fossil fuel consumption and biomass burning are contributing to significantly larger emissions of black carbon (BC) aerosols to the atmosphere. Together with organic carbon (OC), BC is a major constituent of fine particulate matter in urban air, contributes to haze and has been linked to a broad array of adverse health effects. Black carbon's high light absorption capacity and role in key (in-)direct climate feedbacks also lead to a range of impacts in the Earth system (e.g. warming, accelerated snow melt, changes in cloud formation). Recent work suggests that regulating BC emissions can play an important role in improving regional air quality and reducing future climate warming. However, BC's atmospheric transport pathways, lifetime and magnitudes of emissions by sector and region, particularly emissions from large urban centers, remain poorly constrained by measurements. Contributions of fossil and modern sources to the carbonaceous aerosol pool (corresponding mainly to traffic/industrial and biomass-burning/biogenic sources, respectively) can be quantified unambiguously by measuring the aerosol radiocarbon (14C) content. However, accurate 14C-based source apportionment requires the physical isolation of BC and OC, and minimal sample contamination with extraneous carbon or from OC charring. Compound class-specific 14C analysis of BC remains challenging due to very small sample sizes (5-15 ug C). Therefore, most studies to date have only analyzed the 14C content of the total organic carbonaceous aerosol fraction. Here, we present time-series 14C data of BC and OC from the Los Angeles (LA) metropolitan area in California - one of two megacities in the United States - and from Salt Lake City (SLC), UT. In the LA area, we analyzed 48h-PM10 samples near the LA port throughout 2007 and 2008 (with the exception of summer). We also collected monthly-PM2.5 samples at the University of California - Irvine, with shorter sampling periods during regional wildfire

  18. Monte Carlo simulation of two-component aerosol processes

    NASA Astrophysics Data System (ADS)

    Huertas, Jose Ignacio

    Aerosol processes have been extensively used for production of nanophase materials. However when temperatures and number densities are high, particle agglomeration is a serious drawback for these techniques. This problem can be addressed by encapsulating the particles with a second material before they agglomerate. These particles will agglomerate but the primary particles within them will not. When the encapsulation is later removed, the resulting powder will contain only weakly agglomerated particles. To demonstrate the applicability of the particle encapsulation method for the production of high purity unagglomerated nanosize materials, tungsten (W) and tungsten titanium alloy (W-Ti) particles were synthesized in a sodium/halide flame. The particles were characterized by XRD, SEM, TEM and EDAX. The particles appeared unagglomerated, cubic and hexagonal in shape, and had a size of 30-50 nm. No contamination was detected even after extended exposure to atmospheric conditions. The nanosized W and W-Ti particles were consolidated into pellets of 6 mm diameter and 6-8 mm long. Hardness measurements indicate values 4 times that of conventional tungsten. 100% densification was achieved by hipping the samples. To study the particle encapsulation method, a code to simulate particle formation in two component aerosols was developed. The simulation was carried out using a Monte Carlo technique. This approach allowed for the treatment of both probabilistic and deterministic events. Thus, the coagulation term of the general dynamic equation (GDE) was Monte Carlo simulated, and the condensation term was solved analytically and incorporated into the model. The model includes condensation, coagulation, sources, and sinks for two-component aerosol processes. The Kelvin effect has been included in the model as well. The code is general and does not suffer from problems associated with mass conservation, high rates of condensation and approximations on particle composition. It has

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

    NASA Astrophysics Data System (ADS)

    Ulevicius, Vidmantas; Byčenkienė, Steigvilė; Bozzetti, Carlo; Vlachou, Athanasia; Plauškaitė, Kristina; Mordas, Genrik; Dudoitis, Vadimas; Abbaszade, Gülcin; Remeikis, Vidmantas; Garbaras, Andrius; Masalaite, Agne; Blees, Jan; Fröhlich, Roman; Dällenbach, Kaspar R.; Canonaco, Francesco; Slowik, Jay G.; Dommen, Josef; Zimmermann, Ralf; Schnelle-Kreis, Jürgen; Salazar, Gary A.; Agrios, Konstantinos; Szidat, Sönke; El Haddad, Imad; Prévôt, André S. H.

    2016-05-01

    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.

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

    NASA Astrophysics Data System (ADS)

    Ulevicius, V.; Byčenkienė, S.; Bozzetti, C.; Vlachou, A.; Plauškaitė, K.; Mordas, G.; Dudoitis, V.; Abbaszade, G.; Remeikis, V.; Garbaras, A.; Masalaite, A.; Blees, J.; Fröhlich, R.; Dällenbach, K. R.; Canonaco, F.; Slowik, J. G.; Dommen, J.; Zimmermann, R.; Schnelle-Kreis, J.; Salazar, G. A.; Agrios, K.; Szidat, S.; El Haddad, I.; Prévôt, A. S. H.

    2015-09-01

    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 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 7-12 %, respectively. Isotope ratio of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

  1. Characterization and sources of regional-scale transported carbonaceous and dust aerosols from different pathways in coastal and sandy land areas of China

    NASA Astrophysics Data System (ADS)

    Zhang, X. Y.; Wang, Y. Q.; Wang, D.; Gong, S. L.; Arimoto, R.; Mao, L. J.; Li, J.

    2005-08-01

    Concentrations of 12-hour averaged organic carbon (OC), elemental carbon (EC), and other trace elements were determined from bulk aerosol samples at a coastal city of Lian Yun Gang (LYG) in east China from June to December 2003 and a sandy land site of Tong Liao in northeast China from June to August 2003. Regional transports from four main source areas accounted for ˜35-49% of the Asian dust and 16-18% of the carbonaceous particles for both sites. The regional mean concentrations of various species, especially EC, were comparable to or lower than those in urban areas of inland China, Korea, and Japan but tended to be higher than those in Hong Kong or rural sites in east Asia. At LYG, OC showed a clear seasonal pattern with a peak loading in winter (24 μg m-3) and a low in summer (10 μg m-3). Seasonality of EC was more pronounced than that of OC with a difference of approximately threefold (3.8 to 11 μg m-3). Three types of air masses with high particulate loadings were found to be responsible for the peak EC and low OC/EC ratios in winter. Clean air masses with more than 50% secondary organic carbon contents were largely of marine origins. Elemental concentrations (Ca, Fe, K, Mn, and Ti) were mainly associated with Asian dust aerosols with a certain fraction of K from biomass burning in mainland China characterized with a ratio of 1.3 for OC/K.

  2. Maritime Aerosol Network (MAN) as a Component of AERONET

    NASA Technical Reports Server (NTRS)

    Smirnov, A.; Holben, B. N.; Slutsker, I.; Giles, D. M.; McClain, C. R.; Eck, T. F.; Sakerin, S. M.; Macke, A.; Croot, P.; Zibordi, G.; Quinn, P. K.

    2008-01-01

    The World Ocean produces a large amount of natural aerosols that have all impact on the Earth's albedo and climate. Sea-salt is the major contributor to aerosol optical depth over the oceans. [Mahowald et al. 2006; Chin et al. 2002; Satheesh et al. 1999; Winter and Chylek, 1997] and therefore affects the radiative balance over the ocean through the direct [Haywood et al. 1999] and indirect aerosol effect [O'Dowd et al. 1999]. Aerosols over the oceans (produced marine and advected from land sources) are important for various atmospheric processes [Lewis and Schwartz, 2004] and remote sensing studies [Gordon, 1997].

  3. Source apportionment and dynamic changes of carbonaceous aerosols during the haze bloom-decay process in China based on radiocarbon and organic molecular tracers

    NASA Astrophysics Data System (ADS)

    Liu, Junwen; Li, Jun; Liu, Di; Ding, Ping; Shen, Chengde; Mo, Yangzhi; Wang, Xinming; Luo, Chunling; Cheng, Zhineng; Szidat, Sönke; Zhang, Yanlin; Chen, Yingjun; Zhang, Gan

    2016-03-01

    Fine carbonaceous aerosols (CAs) is the key factor influencing the currently filthy air in megacities in China, yet few studies simultaneously focus on the origins of different CAs species using specific and powerful source tracers. Here, we present a detailed source apportionment for various CAs fractions, including organic carbon (OC), water-soluble OC (WSOC), water-insoluble OC (WIOC), elemental carbon (EC) and secondary OC (SOC) in the largest cities of North (Beijing, BJ) and South China (Guangzhou, GZ), using the measurements of radiocarbon and anhydrosugars. Results show that non-fossil fuel sources such as biomass burning and biogenic emission make a significant contribution to the total CAs in Chinese megacities: 56 ± 4 in BJ and 46 ± 5 % in GZ, respectively. The relative contributions of primary fossil carbon from coal and liquid petroleum combustions, primary non-fossil carbon and secondary organic carbon (SOC) to total carbon are 19, 28 and 54 % in BJ, and 40, 15 and 46 % in GZ, respectively. Non-fossil fuel sources account for 52 in BJ and 71 % in GZ of SOC, respectively. These results suggest that biomass burning has a greater influence on regional particulate air pollution in North China than in South China. We observed an unabridged haze bloom-decay process in South China, which illustrates that both primary and secondary matter from fossil sources played a key role in the blooming phase of the pollution episode, while haze phase is predominantly driven by fossil-derived secondary organic matter and nitrate.

  4. Source apportionment and dynamic changes of carbonaceous aerosols during the haze bloom-decay process in China based on radiocarbon and organic molecular tracers

    NASA Astrophysics Data System (ADS)

    Liu, J.; Li, J.; Liu, D.; Ding, P.; Shen, C.; Mo, Y.; Wang, X.; Luo, C.; Cheng, Z.; Szidat, S.; Zhang, Y.; Chen, Y.; Zhang, G.

    2015-12-01

    Fine carbonaceous aerosols (CAs) is the key factor influencing the currently filthy air in megacities of China, yet seldom study simultaneously focuses on the origins of different CAs species using specific and powerful source tracers. Here, we present a detailed source apportionment for various CAs fractions, including organic carbon (OC), water-soluble OC (WSOC), water-insoluble OC (WIOC), elemental carbon (EC) and secondary OC (SOC) in the largest cities of North (Beijing, BJ) and South China (Guangzhou, GZ), respectively, using the measurements of radiocarbon and anhydrosugars. Results show that non-fossil fuel sources such as biomass burning and biogenic emission make a significant contribution to the total CAs in Chinese megacities: 56 ± 4 % in BJ and 46 ± 5 % in GZ, respectively. The relative contributions of primary fossil carbon from coal and liquid petroleum combustions, primary non-fossil carbon and secondary organic carbon (SOC) to total carbon are 19, 28 and 54 % in BJ, and 40, 15 and 46 % in GZ, respectively. Non-fossil fuel sources account for 52 % in BJ and 71 % in GZ of SOC, respectively. These results suggest that biomass burning has a greater influence on regional particulate air pollution in North China than in South China. We observed an unabridged haze bloom-decay process in South China, which illustrates that both primary and secondary matter from fossil sources played a key role in the blooming phase of the pollution episode, while haze phase is predominantly driven by fossil-derived secondary organic matter and nitrate.

  5. Photochemistry of Secondary Organic Aerosol Components in Water and Ice

    NASA Astrophysics Data System (ADS)

    Epstein, S. A.; Tran, V. T.; Lignell, H.; Nizkorodov, S.; Shemesh, D.; Gerber, R.

    2011-12-01

    Secondary organic aerosol (SOA) can nucleate clouds in the atmosphere and may be scavenged by previously formed cloud droplets. Significant concentrations of dissolved organic matter are typically present in cloud droplets, snow, and ice particles, however the photochemical transformations of these organic components in liquid aqueous solutions and in ice are poorly understood. An apparatus was constructed to measure the absorption spectra of frozen aqueous solutions in the presence of ultra-violet (UV) light. We can monitor the disappearance of the original reactant as a function of UV exposure time with UV-Visible spectroscopy and identify products with gas chromatography-mass spectrometry. Initial experiments with methylhydroperoxide, the simplest organic peroxide, which is readily detectable in solid and liquid cloud particles, reveal no change in the absorption spectra between the liquid and frozen solution. With these photolysis experiments, we can establish quantum yields of methylhydroperoxide photodissociation and allow for the comparison between liquid and ice phase chemistry. Additional experiments with pinonic acid, a significant product formed from alpha-pinene ozonolysis, and a mixture of common SOA constituents will allow us to determine quantum yields and reveal important insight in the understanding of the cloud processing of water soluble SOA by sunlight.

  6. An AeroCom Initial Assessment - Optical Properties in Aerosol Component Modules of Global Models

    SciTech Connect

    Kinne, Stefan; Schulz, M.; Textor, C.; Guibert, S.; Balkanski, Y.; Bauer, S.; Berntsen, T.; Berglen, T.; Boucher, Olivier; Chin, M.; Collins, W.; Dentener, F.; Diehl, T.; Easter, Richard C.; Feichter, H.; Fillmore, D.; Ghan, Steven J.; Ginoux, P.; Gong, S.; Grini, A.; Hendricks, J.; Herzog, M.; Horrowitz, L.; Isaksen, I.; Iversen, T.; Kirkevag, A.; Kloster, S.; Koch, D.; Kristjansson, J. E.; Krol, M.; Lauer, A.; Lamarque, J. F.; Lesins, G.; Liu, Xiaohong; Lohmann, U.; Montanaro, V.; Myhre, G.; Penner, Joyce E.; Pitari, G.; Reddy, S.; Seland, O.; Stier, P.; Takemura, T.; Tie, X.

    2006-05-29

    The AeroCom exercise diagnoses multi-component aerosol modules in global modeling. In an initial assessment global fields for mass and for mid-visible aerosol optical thickness (aot) were compared among aerosol component modules of 21 different global models. There is general agreement among models for the annual global mean of component combined aot. At 0.12 to 0.14, simulated aot values are at the lower end of global averages suggested by remote sensing from ground (AERONET ca 0.14) and space (MODIS-MISR composite ca 0.16). More detailed comparisons, however, reveal that larger differences in regional distribution and significant differences in compositional mixture have remained. Of particular concern is the large model diversity for contributions by dust and carbon, because it leads to significant uncertainty in aerosol absorption (aab). Since not only aot but also aab influence the aerosol impact on the radiative energy-balance, aerosol (direct) forcing uncertainty in modeling is larger than differences in aot might suggest. New diagnostic approaches are proposed to trace model differences in terms of aerosol processing and transport: These include the prescription of common input (e.g. amount, size and injection of aerosol component emissions) and the use of observational capabilities from ground (e.g. measurements networks) and space (e.g. correlations between retrieved aerosol and cloud properties).

  7. Study of the carbonaceous aerosol and morphological analysis of fine particles along with their mixing state in Delhi, India: a case study.

    PubMed

    Tiwari, S; Pipal, A S; Hopke, Philip K; Bisht, D S; Srivastava, A K; Tiwari, Shani; Saxena, P N; Khan, A H; Pervez, S

    2015-07-01

    Because of high emissions of anthropogenic as well as natural particles over the Indo-Gangetic Plains (IGP), it is important to study the characteristics of fine (PM2.5) and inhalable particles (PM10), including their morphology, physical and chemical characteristics, etc., in Delhi during winter 2013. The mean mass concentrations of fine (PM2.5) and inhalable (PM10) (continuous) was 117.6 ± 79.1 and 191.0 ± 127.6 μg m(-3), respectively, whereas the coarse mode (PM10-2.5) particle PM mass was 73.38 ± 28.5 μg m(-3). During the same period, offline gravimetric monitoring of PM2.5 was conducted for morphological analysis, and its concentration was ~37 % higher compared to the continuous measurement. Carbonaceous PM such as organic carbon (OC) and elemental carbon (EC) were analyzed on the collected filters, and their mean concentration was respectively 33.8 and 4.0 μg m(-3) during the daytime, while at night it was 41.2 and 10.1 μg m(-3), respectively. The average OC/EC ratio was 8.97 and 3.96 during the day and night, respectively, indicating the formation of secondary organic aerosols during daytime. Effective carbon ratio was studied to see the effect of aerosols on climate, and its mean value was 0.52 and 1.79 during night and day, indicating the dominance of absorbing and scattering types of aerosols respectively into the atmosphere over the study region. Elemental analysis of individual particles indicates that Si is the most abundant element (~37-90 %), followed by O (oxide) and Al. Circularity and aspect ratio was studied, which indicates that particles are not perfectly spherical and not elongated in any direction. Trajectory analysis indicated that in the months of February and March, air masses appear to be transported from the Middle Eastern part along with neighboring countries and over Thar Desert region, while in January it was from the northeast direction which resulted in high concentrations of fine particles. PMID:25758418

  8. A new comprehensive approach to characterizing carbonaceous aerosol with an application to wintertime Fresno, California PM2.5

    USGS Publications Warehouse

    Herckes, P.; Leenheer, J.A.; Collett, J.L., Jr.

    2007-01-01

    Fine particulate matter (PM2.5) samples were collected during a three week winter period in Fresno (CA). A composite sample was characterized by isolating several distinct fractions and characterizing them by infrared and nuclear magnetic resonance (NMR) spectroscopy. More than 80% of the organic matter in the aerosol samples was recovered and characterized. Only 35% of the organic matter was water soluble with another third soluble in dichloromethane and the remainder insoluble. Within the isolated water soluble material, hydrophobic acid and hydrophilic acids plus neutrals fractions contained the largest amounts of carbon. The hydrophobic acids fraction appears to contain significant amounts of lignin type structures, spectra of the hydrophilic acids plus neutrals fraction are indicative of carbohydrates and secondary organic material. The dichloromethane soluble fraction contains a variety of organic compound families typical of many previous studies of organic aerosol speciation, including alkanes, alkanols, alkanals and alkanoic acids. Finally the water and solvent insoluble fraction exhibits a strong aromaticity as one would expect from black or elemental carbon like material; however, these spectra also show a substantial amount of aliphaticity consistent with linear side chains on the aromatic structures.

  9. Characteristics of carbonaceous aerosols emitted from peatland fire in Riau, Sumatra, Indonesia (2): Identification of organic compounds

    NASA Astrophysics Data System (ADS)

    Fujii, Yusuke; Kawamoto, Haruo; Tohno, Susumu; Oda, Masafumi; Iriana, Windy; Lestari, Puji

    2015-06-01

    Smoke emitted from Indonesian peatland fires has caused dense haze and serious air pollution in Southeast Asia such as visibility impairment and adverse health impacts. To mitigate the Indonesian peatland fire aerosol impacts, an effective strategy and international framework based on the latest scientific knowledge needs to be established. Although several attempts have been made, limited data exist regarding the chemical characteristics of peatland fire smoke for the source apportionment. In order to identify the key organic compounds of peatland fire aerosols, we conducted intensive field studies based on ground-based and source-dominated sampling of PM2.5 in Riau Province, Sumatra, Indonesia, during the peatland fire seasons in 2012. Levoglucosan was the most abundant compound among the quantified organic compounds at 8.98 ± 2.28% of the PM2.5 mass, followed by palmitic acid at 0.782 ± 0.163% and mannosan at 0.607 ± 0.0861%. Potassium ion was not appropriate for an indicator of Indonesian peatland fires due to extremely low concentrations associated with smoldering fire at low temperatures. The vanillic/syringic acids ratio was 1.06 ± 0.155 in this study and this may be a useful signature profile for peatland fire emissions. Particulate n-alkanes also have potential for markers to identify impact of Indonesian peatland fire source at a receptor site.

  10. The characteristics and origins of carbonaceous aerosol at a rural site of PRD in summer of 2006

    NASA Astrophysics Data System (ADS)

    Hu, W. W.; Hu, M.; Deng, Z. Q.; Xiao, R.; Kondo, Y.; Takegawa, N.; Zhao, Y. J.; Guo, S.; Zhang, Y. H.

    2012-02-01

    Both organic carbon (OC) and elemental carbon (EC) were measured during PRIDE-PRD 2006 summer campaign by using a semi-continuous thermal-optical carbon analyzer at a rural site, Back Garden (BG), which is located 50 km to the northwest of Guangzhou City. Together with the online EC/OC analyzer, various kinds of instruments related to aerosol chemical properties were employed here, which provided a good opportunity to check data quality. The concentrations of OC correlated well with the mass of organic matter (OM) and water soluble organic carbon (WSOC), implying the reliability of the data measured in this campaign. The average OC concentrations in fine particle for three typical periods during the campaign (local emission influence, typhoon and precipitation and normal days) were 28.1 μgC m-3, 4.0 μgC m-3 and 5.7 μgC m-3, respectively; and EC were 11.6 μgC m-3, 1.8 μgC m-3, and 3.3 μgC m-3, respectively. The diurnal patterns of EC and OC during the campaign were higher at night and in early morning than daytime, which was probably caused by the primary emission and accumulation in the occurrence of low boundary layer. Compared with the constant diurnal enhancement ratios of EC, the enhancement ratio of OC (OC versus (CO-CObackground)) kept in a relative high level in the afternoon, with a similar diurnal profile to oxygenated organic aerosol (OOA), due to the strong photochemical formation of OC. Here, a modified EC tracer method was used to estimate the formation of secondary organic carbon (SOC). These results showed that the average SOC concentration (normal days) at BG site was about 2.0 ± 2.3 μgC m-3, and the SOC fraction in OC could reach up to 80% with the average of 47%. The modified approach in this study proved to be effective and reliable for SOC estimation based on good correlations between estimated SOC versus OOA or WSOC, and estimated POC versus hydrocarbon-like organic aerosol (HOA).

  11. Characteristics and the origins of the carbonaceous aerosol at a rural site of PRD in summer 2006

    NASA Astrophysics Data System (ADS)

    Hu, W. W.; Hu, M.; Deng, Z. Q.; Xiao, R.; Kondo, Y.; Takegawa, N.; Zhao, Y. J.; Guo, S.; Zhang, Y. H.

    2011-07-01

    Both organic carbon (OC) and elemental carbon (EC) were measured at a rural site, Back Garden (BG), 50km northwest of the Guangzhou City, by using a semi-continuous thermal-optical analyzer during PRIDE-PRD 2006 summer intensive campaign. Together with the online EC/OC instrument, multiple instruments were also employed here which provided a good opportunity to check data quality. The regressions between the mass of organic aerosol (OM) and OC, as well as OC and water soluble organic carbon (WSOC) imply reliability of the data measured in this campaign. The average OC concentrations in fine particle for three typical periods during the campaign (local emission influence, typhoon and participation, normal days) were 28.1 μg C m-3, 4.0 μg C m-3 and 5.7 μg C m-3, respectively, and EC were 11.6 μg C m-3, 1.8 μg C m-3, and 3.3 μg C m-3 orderly. Diurnal variations of EC and OC showed that there were two peaks for EC and OC concentrations, i.e. at night and early morning, which were probably caused by the primary emission accumulation when the boundary layer was shallow. Compare to the constant diurnal enhancement ratios of primary EC, the enhancement ratio of OC (OC versus (CO-CObackground)) remained in a relative high level in the afternoon with a similar diurnal variation to oxygenated organic aerosol (OOA), indicating the strong photochemical formation of OC. The traditional EC tracer method was modified to estimate the secondary organic carbon (SOC) formation, which shows that the average SOC concentration in BG site was about 2.0 ± 2.3 μg C m-3.The SOC fraction in OC reached up to 80 % with the average of 47 %. Good correlations between estimated SOC versus measured OOA or WSOC, and estimated POC versus measured hydrocarbon-like organic aerosol (HOA) also proved the reliable results by the modified EC tracer method in this paper.

  12. Historical emissions of carbonaceous aerosols from biomass and fossil fuel burning for the period 1870-2000

    NASA Astrophysics Data System (ADS)

    Ito, Akinori; Penner, Joyce E.

    2005-06-01

    Historical changes of black carbon (BC) and particulate organic matter (POM) emissions from biomass burning (BB) and fossil fuel (FF) burning are estimated from 1870 to 2000. A bottom-up inventory for open vegetation (OV) burning is scaled by a top-down estimate for the year 2000. Monthly and interannual variations are derived over the time period from 1979 to 2000 based on the TOMS satellite aerosol index (AI) and this global map. Prior to 1979, emissions are scaled to a CH4 emissions inventory based on land-use change. Biofuel (BF) emissions from a recent inventory for developing countries are scaled forward and backward in time using population statistics and crop production statistics. In developed countries, wood consumption data together with emission factors for cooking and heating practices are used for biofuel estimates. For fossil fuel use, we use fuel consumption data and specific emission factors for different fuel use categories to develop an inventory over 1950-2000, and emissions are scaled to a CO2 inventory prior to that time. Technology changes for emissions from the diesel transport sector are included. During the last decade of this time period, the BC and POM emissions from biomass burning (i.e., OV + BF) contribute a significant amount to the primary sources of BC and POM and are larger than those from FF. Thus 59% of the NH BC emissions and 90% of the NH POM emissions are from BB in 2000. Fossil fuel consumption technologies are needed prior to 1990 in order to improve estimates of fossil fuel emissions during the twentieth century. These results suggest that the aerosol emissions from biomass burning need to be represented realistically in climate change assessments. The estimated emissions are available on a 1° × 1° grid for global climate modeling studies of climate changes.

  13. MODELS-3 COMMUNITY MULTISCALE AIR QUALITY (CMAQ) MODEL AEROSOL COMPONENT 1: MODEL DESCRIPTION

    EPA Science Inventory

    The aerosol component of the Community Multiscale Air Quality (CMAQ) model is designed to be an efficient and economical depiction of aerosol dynamics in the atmosphere. The approach taken represents the particle size distribution as the superposition of three lognormal subdis...

  14. Organic Aerosol Component (OACOMP) Value-Added Product

    SciTech Connect

    Fast, J; Zhang, Q; tilp, A; Shippert, T; Parworth, C; Mei, F

    2013-08-23

    Organic aerosol (OA, i.e., the organic fraction of particles) accounts for 10–90% of the fine aerosol mass globally and is a key determinant of aerosol radiative forcing. But atmospheric OA is poorly characterized and its life cycle insufficiently represented in models. As a result, current models are unable to simulate OA concentrations and properties accurately. This deficiency represents a large source of uncertainty in quantification of aerosol effects and prediction of future climate change. Evaluation and development of aerosol models require data products generated from field observations. Real-time, quantitative data acquired with aerosol mass spectrometers (AMS) (Canagaratna et al. 2007) are critical to this need. The AMS determines size-resolved concentrations of non-refractory (NR) species in submicrometer particles (PM1) with fast time resolution suitable for both ground-based and aircraft deployments. The high-resolution AMS (HR-AMS), which is equipped with a high mass resolution time-of-flight mass spectrometer, can be used to determine the elemental composition and oxidation degrees of OA (DeCarlo et al. 2006).

  15. Size distribution characteristics of carbonaceous aerosol in Xishuangbanna, southwest China: a sign for biomass burning in Asia.

    PubMed

    Guo, Yuhong

    2016-03-01

    In 2012, size-segregated aerosol samples were collected in Xishuangbanna, a forest station in southwest China. The concentrations of organic and elemental carbon (OC and EC for short) were quantified with thermal/optical carbon analyzer in the filter samples. OC and EC exhibited similar seasonal patterns, with the highest concentrations in spring, possibly due to the influence of biomass burning in south and southeast Asia. The mass size distributions of OC and EC were bimodal in all the sampling seasons, each with a dominant peak in the fine mode of 0.4-0.7 μm and a coarse peak in the size range of 2.1-4.7 μm. In fine mode, OC and EC showed smaller geometric mean diameters (GMDs) during winter. OC and EC were prone to be more concentrated in fine particles in spring and winter than in summer and autumn. Furthermore, EC was more abundant in fine particles than OC. Good correlations (R(2) = 0.75-0.82) between OC and EC indicated that they had common dominant sources of combustion such as biomass burning and fossil fuel combustion emissions. The daily average OC/EC ratios ranged from 2.1 to 9.1, more elevated OC/EC ratios being found in the winter. PMID:26851952

  16. Online coupling of pure O2 thermo-optical methods - 14C AMS for source apportionment of carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Agrios, Konstantinos; Salazar, Gary; Zhang, Yan-Lin; Uglietti, Chiara; Battaglia, Michael; Luginbühl, Marc; Ciobanu, Viorela Gabriela; Vonwiller, Matthias; Szidat, Sönke

    2015-10-01

    This paper reports on novel separation methods developed for the direct determination of 14C in organic carbon (OC) and elemental carbon (EC), two sub-fractions of total carbon (TC) of atmospheric air particulate matter. Until recently, separation of OC and EC has been performed off-line by manual and time-consuming techniques that relied on the collection of massive CO2 fractions. We present here two on-line hyphenated techniques between a Sunset OC/EC analyzer and a MICADAS (MIni radioCArbon DAting System) accelerator mass spectrometer (AMS) equipped with a gas ion source. The first implementation facilitates the direct measurement in the low sample size range (<10 μg C) with high throughput on a routine basis, while the second explores the potential for a continuous-flow real-time CO2 gas feed into the ion source. The performance achieved with reference materials and real atmospheric samples will be discussed to draw conclusions on the improvement offered in the field of 14C aerosol source apportionment.

  17. Concentrations and light absorption characteristics of carbonaceous aerosol in PM2.5 and PM10 of Lhasa city, the Tibetan Plateau

    NASA Astrophysics Data System (ADS)

    Li, Chaoliu; Chen, Pengfei; Kang, Shichang; Yan, Fangping; Hu, Zhaofu; Qu, Bin; Sillanpää, Mika

    2016-02-01

    Light absorption properties of carbonaceous aerosol strongly influence the Earth's radiative balance, yet the related knowledge is limited for the Tibetan Plateau (TP), the highest and largest plateau in the world. In this study, organic carbon (OC), elemental carbon (EC) and water soluble organic carbon (WSOC) of PM2.5 and PM10 of Lhasa collected from May 2013 to March 2014 were studied. It showed that daily-average concentrations of OC, EC and WSOC of PM2.5 and PM10 were lower than those of other megacities. Lhasa PM2.5 was characterized by low OC/EC ratio (1.46 ± 0.55), which was similar to that of Lhasa roadside PM2.5 (1.25 ± 0.45), reflecting mainly direct influence of primary emissions and less secondary formation. Hence, although Lhasa atmosphere is relatively clean, it is intensively influenced by local vehicle emissions. Mass absorption cross-section of EC (MACEC) for both PM2.5 and PM10 at 632 nm were 7.19 ± 1.19 m2 g-1 and 7.98 ± 2.32 m2 g-1, respectively, both of which had similar variation patterns to OC/EC and secondary OC (SOC)/OC, indicating that the increase of MACEC might be caused by coating with organic aerosol. Additionally, the loading of EC for both PM2.5 and PM10 showed logarithmic relationships with those of optical attenuation (ATN) of EC, implying that the shadowing effect enhanced logarithmic with increased EC concentration. MAC of WSOC at 365 nm for PM2.5 (0.74 ± 0.22 m2 g-1) and PM10 (0.78 ± 0.21 m2 g-1) were also close to reported values of other cities mainly influenced by fossil combustion. Additionally, attenuation at 365 nm of WSOC of both PM2.5 and PM10 showed the same relationship with their WSOC concentrations, implying no difference for light absorption properties of WSOC for these two grain sizes.

  18. Ensemble projections of wildfire activity and carbonaceous aerosol concentrations over the western United States in the mid-21st century

    PubMed Central

    Yue, Xu; Mickley, Loretta J.; Logan, Jennifer A.; Kaplan, Jed O.

    2013-01-01

    We estimate future wildfire activity over the western United States during the mid-21st century (2046–2065), based on results from 15 climate models following the A1B scenario. We develop fire prediction models by regressing meteorological variables from the current and previous years together with fire indexes onto observed regional area burned. The regressions explain 0.25–0.60 of the variance in observed annual area burned during 1980–2004, depending on the ecoregion. We also parameterize daily area burned with temperature, precipitation, and relative humidity. This approach explains ~0.5 of the variance in observed area burned over forest ecoregions but shows no predictive capability in the semi-arid regions of Nevada and California. By applying the meteorological fields from 15 climate models to our fire prediction models, we quantify the robustness of our wildfire projections at mid-century. We calculate increases of 24–124% in area burned using regressions and 63–169% with the parameterization. Our projections are most robust in the southwestern desert, where all GCMs predict significant (p<0.05) meteorological changes. For forested ecoregions, more GCMs predict significant increases in future area burned with the parameterization than with the regressions, because the latter approach is sensitive to hydrological variables that show large inter-model variability in the climate projections. The parameterization predicts that the fire season lengthens by 23 days in the warmer and drier climate at mid-century. Using a chemical transport model, we find that wildfire emissions will increase summertime surface organic carbon aerosol over the western United States by 46–70% and black carbon by 20–27% at midcentury, relative to the present day. The pollution is most enhanced during extreme episodes: above the 84th percentile of concentrations, OC increases by ~90% and BC by ~50%, while visibility decreases from 130 km to 100 km in 32 Federal Class 1

  19. Ensemble projections of wildfire activity and carbonaceous aerosol concentrations over the western United States in the mid-21st century

    NASA Astrophysics Data System (ADS)

    Yue, Xu; Mickley, Loretta J.; Logan, Jennifer A.; Kaplan, Jed O.

    2013-10-01

    We estimate future wildfire activity over the western United States during the mid-21st century (2046-2065), based on results from 15 climate models following the A1B scenario. We develop fire prediction models by regressing meteorological variables from the current and previous years together with fire indexes onto observed regional area burned. The regressions explain 0.25-0.60 of the variance in observed annual area burned during 1980-2004, depending on the ecoregion. We also parameterize daily area burned with temperature, precipitation, and relative humidity. This approach explains ˜0.5 of the variance in observed area burned over forest ecoregions but shows no predictive capability in the semi-arid regions of Nevada and California. By applying the meteorological fields from 15 climate models to our fire prediction models, we quantify the robustness of our wildfire projections at midcentury. We calculate increases of 24-124% in area burned using regressions and 63-169% with the parameterization. Our projections are most robust in the southwestern desert, where all GCMs predict significant (p < 0.05) meteorological changes. For forested ecoregions, more GCMs predict significant increases in future area burned with the parameterization than with the regressions, because the latter approach is sensitive to hydrological variables that show large inter-model variability in the climate projections. The parameterization predicts that the fire season lengthens by 23 days in the warmer and drier climate at midcentury. Using a chemical transport model, we find that wildfire emissions will increase summertime surface organic carbon aerosol over the western United States by 46-70% and black carbon by 20-27% at midcentury, relative to the present day. The pollution is most enhanced during extreme episodes: above the 84th percentile of concentrations, OC increases by ˜90% and BC by ˜50%, while visibility decreases from 130 km to 100 km in 32 Federal Class 1 areas in

  20. Ensemble projections of wildfire activity and carbonaceous aerosol concentrations over the western United States in the mid-21st century.

    PubMed

    Yue, Xu; Mickley, Loretta J; Logan, Jennifer A; Kaplan, Jed O

    2013-10-01

    We estimate future wildfire activity over the western United States during the mid-21(st) century (2046-2065), based on results from 15 climate models following the A1B scenario. We develop fire prediction models by regressing meteorological variables from the current and previous years together with fire indexes onto observed regional area burned. The regressions explain 0.25-0.60 of the variance in observed annual area burned during 1980-2004, depending on the ecoregion. We also parameterize daily area burned with temperature, precipitation, and relative humidity. This approach explains ~0.5 of the variance in observed area burned over forest ecoregions but shows no predictive capability in the semi-arid regions of Nevada and California. By applying the meteorological fields from 15 climate models to our fire prediction models, we quantify the robustness of our wildfire projections at mid-century. We calculate increases of 24-124% in area burned using regressions and 63-169% with the parameterization. Our projections are most robust in the southwestern desert, where all GCMs predict significant (p<0.05) meteorological changes. For forested ecoregions, more GCMs predict significant increases in future area burned with the parameterization than with the regressions, because the latter approach is sensitive to hydrological variables that show large inter-model variability in the climate projections. The parameterization predicts that the fire season lengthens by 23 days in the warmer and drier climate at mid-century. Using a chemical transport model, we find that wildfire emissions will increase summertime surface organic carbon aerosol over the western United States by 46-70% and black carbon by 20-27% at midcentury, relative to the present day. The pollution is most enhanced during extreme episodes: above the 84(th) percentile of concentrations, OC increases by ~90% and BC by ~50%, while visibility decreases from 130 km to 100 km in 32 Federal Class 1 areas in

  1. Radiative properties of the background aerosol: absorption component of extinction.

    PubMed

    Clarke, A D; Charlson, R J

    1985-07-19

    The light-scattering and light-absorption coefficients of the global background aerosol define its single-scatter albedo. Continuous, simultaneous measurements of these optical coefficients were made on a daily basis for the remote marine mid-troposphere; such measurements are essential for assessment of the effects of aerosol on atmospheric radiative transfer. Measurements of light-absorption coefficients made at the Mauna Loa Observatory in Hawaii were higher than expected, and the single-scatter albedo was lower than the value often used in radiative transfer models. Soot appears to be the most likely primary absorber, and hemispheric dispersal of this combustion-derived material is suggested. PMID:17759145

  2. Changes in chemical components of aerosol particles in different haze regions in China from 2006 to 2013 and contribution of meteorological factors

    NASA Astrophysics Data System (ADS)

    Zhang, X. Y.; Wang, J. Z.; Wang, Y. Q.; Liu, H. L.; Sun, J. Y.; Zhang, Y. M.

    2015-11-01

    Since there have been individual reports of persistent haze-fog events in January 2013 in central-eastern China, questions on factors causing the drastic differences in changes in 2013 from changes in adjacent years have been raised. Changes in major chemical components of aerosol particles over the years also remain unclear. The extent of meteorological factors contributing to such changes is yet to be determined. The study intends to present the changes in daily based major water-soluble constituents, carbonaceous species, and mineral aerosol in PM10 at 13 stations within different haze regions in China from 2006 to 2013, which are associated with specific meteorological conditions that are highly related to aerosol pollution (parameterized as an index called Parameter Linking Aerosol Pollution and Meteorological Elements - PLAM). No obvious changes were found in annual mean concentrations of these various chemical components and PM10 in 2013, relative to 2012. By contrast, wintertime mass of these components was quite different. In Hua Bei Plain (HBP), sulfate, organic carbon (OC), nitrate, ammonium, element carbon (EC), and mineral dust concentrations in winter were approximately 43, 55, 28, 23, 21, and 130 μg m-3, respectively; these masses were approximately 2 to 4 times higher than those in background mass, which also exhibited a decline during 2006 to 2010 and then a rise till 2013. The mass of these concentrations and PM10, except minerals, respectively, increased by approximately 28 to 117 % and 25 % in January 2013 compared with that in January 2012. Thus, persistent haze-fog events occurred in January 2013, and approximately 60 % of this increase in component concentrations from 2012 to 2013 can be attributed to severe meteorological conditions in the winter of 2013. In the Yangtze River Delta (YRD) area, winter masses of these components, unlike HBP, have not significantly increase since 2010; PLAM were also maintained at a similar level without

  3. Production-based emissions, consumption-based emissions and consumption-based health impacts of PM2.5 carbonaceous aerosols in Asia

    NASA Astrophysics Data System (ADS)

    Takahashi, Kei; Nansai, Keisuke; Tohno, Susumu; Nishizawa, Masato; Kurokawa, Jun-ichi; Ohara, Toshimasa

    2014-11-01

    This study determined the production-based emissions, the consumption-based emissions, and the consumption-based health impact of primary carbonaceous aerosols (black carbon: BC, organic carbon: OC) in nine countries and regions in Asia (Indonesia, Malaysia, the Philippines, Singapore, Thailand, China, Taiwan, South Korea, and Japan) in 2008. For the production-based emissions, sectoral emissions inventory of BC and OC for the year of 2008 based on the Asian international input-output tables (AIIOT) was compiled including direct emissions from households. Then, a multiregional environmental input-output analysis with the 2008 AIIOT which was originally developed by updating the table of 2000 was applied for calculating the consumption-based emissions for each country and region. For the production-based emissions, China had the highest BC and OC emissions of 4520 Gg-C in total, which accounted for 75% of the total emissions in the nine countries and regions. For consumption-based emissions, China was estimated to have had a total of 4849 Gg-C of BC and OC emissions, which accounted for 77% of the total emissions in the Asia studied. We also quantified how much countries and regions induced emissions in other countries and regions. Furthermore, taking account of the source-receptor relationships of BC and OC among the countries and regions, we converted their consumption-based emissions into the consumption-based health impact of each country and region. China showed the highest consumption-based health impact of BC and OC totaling 111 × 103 premature deaths, followed by Indonesia, Japan, Thailand and South Korea. China accounted for 87% of the sum total of the consumption-based health impacts of the countries/regions, indicating that China's contribution to consumption-based health impact in Asia was greater than its consumption-based emissions. By elucidating the health impacts that each country and region had on other countries and from which country the impacts

  4. Emission factors of fine particles, carbonaceous aerosols and traces gases from road vehicles: Recent tests in an urban tunnel in the Pearl River Delta, China

    NASA Astrophysics Data System (ADS)

    Zhang, Yanli; Wang, Xinming; Li, Guanghui; Yang, Weiqiang; Huang, Zhonghui; Zhang, Zhou; Huang, Xinyu; Deng, Wei; Liu, Tengyu; Huang, Zuzhao; Zhang, Zhanyi

    2015-12-01

    Motor vehicles contribute primarily and secondarily to air quality problems due to fine particle (PM2.5) and ozone (O3) pollution in China's megacities. Characterizing vehicle emission with the rapid change of vehicle numbers and fleet compositions is vital for both bottom-up emission survey and top-down source apportioning. To obtain emission factors (EFs) of PM2.5, carbonaceous aerosols and trace gases for road vehicles, in urban Guangzhou we conducted a field campaign in 2014 in the Zhujiang Tunnel, a heavily burdened tunnel with about 40,000 motor vehicles passing through each of its two separated bores per day. PM2.5 and volatile organic compounds (VOCs) were sampled for offline analysis while trace gases including SO2, NOx and CO were measured online and in situ. An eddy covariance system with an integrated 3-D sonic anemometer was also adopted to measure CO2 and winds inside the tunnel. We recorded an average fleet composition of 61% light-duty gasoline vehicles (LDVs) + 12% heavy-duty diesel vehicles (HDVs) + 27% liquefied petroleum gas vehicles (LPGVs), and EFs of 82.7 ± 28.3, 19.3 ± 4.7 and 13.3 ± 3.3 mg veh-1 km-1, respectively, for PM2.5, organic carbon (OC) and elemental carbon (EC). These EFs were respectively 23.4%, 18.3% and 72.3% lower when compared to that measured in the same tunnel in 2004. EFs of PM2.5, OC and EC were higher at night time (148 ± 126, 29 ± 24 and 21 ± 18 mg veh-1 km-1, respectively) due to significantly elevated fractions of HDVs in the traffic fleets. An average ratio of OC to EC 1.45 from this tunnel study was much higher than that of ∼0.5 in previous tunnel studies. The EFs of SO2, NOx, CO, CO2 and NMHCs for road traffic were also obtained from our tunnel tests, and they were 20.7 ± 2.9, (1.29 ± 0.2)E+03, (3.10 ± 0.68)E+03, (3.90 ± 0.49)E+05, and 448 ± 39 mg veh-1 km-1, respectively.

  5. Satellite-Based Evidence of Wavelength-Dependent Aerosol Absorption in Biomass Burning Smoke Inferred from Ozone Monitoring Instrument

    NASA Technical Reports Server (NTRS)

    Jethva, H.; Torres, O.

    2012-01-01

    We provide satellite-based evidence of the spectral dependence of absorption in biomass burning aerosols over South America using near-UV measurements made by the Ozone Monitoring Instrument (OMI) during 2005-2007. In the current near-UV OMI aerosol algorithm (OMAERUV), it is implicitly assumed that the only absorbing component in carbonaceous aerosols is black carbon whose imaginary component of the refractive index is wavelength independent. With this assumption, OMI-derived aerosol optical depth (AOD) is found to be significantly over-estimated compared to that of AERONET at several sites during intense biomass burning events (August-September). Other well-known sources of error affecting the near-UV method of aerosol retrieval do not explain the large observed AOD discrepancies between the satellite and the ground-based observations. A number of studies have revealed strong spectral dependence in carbonaceous aerosol absorption in the near-UV region suggesting the presence of organic carbon in biomass burning generated aerosols. A sensitivity analysis examining the importance of accounting for the presence of wavelength-dependent aerosol absorption in carbonaceous particles in satellite-based remote sensing was carried out in this work. The results convincingly show that the inclusion of spectrally-dependent aerosol absorption in the radiative transfer calculations leads to a more accurate characterization of the atmospheric load of carbonaceous aerosols.

  6. Development of ATLID-MSI synergy for retrieving the vertical profiles of aerosol components

    NASA Astrophysics Data System (ADS)

    Kudo, R.; Nishizawa, T.; Higurashi, A.; Sugimoto, N.; Oikawa, E.

    2014-12-01

    EarthCARE is an earth observation satellite and will be launched in 2016. Using its two sensors, ATLID (High spectral resolution lidar) and MSI (Multi-spectral imager), we are developing the synergy algorithm to retrieve the vertical profiles of extinction coefficients at 355 nm of four aerosol components (Water-soluble, black carbon, dust, and sea-salt particles), and the column mean of mode radii of water-soluble and dust particles. The ATLID data are extinction coefficient, backscatter coefficient, and depolarization ratio for total aerosols at 355 nm. The MSI data are radiances at 670 and 865 nm. The dry volume concentrations of four aerosol components at each altitude and the mode radii of water-soluble and dust particles in the column are simultaneously optimized to ATLID and MSI data by the gauss newton method. After the optimization, the vertical profiles of the extinction coefficient at 355 nm of four aerosol components are obtained. The size distributions of four aerosol components are assumed to be a lognormal distribution. The refractive indices of four aerosol components are given from previously observational studies. The humidity growth is considered for water-soluble and sea-salt particles. The volume concentration and the mode radius of the sea-salt particle are parameterized using the surface wind speed on the ocean. We assumed that the shape of the water-soluble, black carbon, and sea-salt particles are spherical, and the shape of the dust particle is spheroidal. We tested the algorithm using the ATLID and MSI data simulated using clean, dust-transported, and smoke-transported aerosols. The extinction coefficients of each component at 355 nm are retrieved well. The mode radius of water-soluble and dust particles were somehow overestimated.

  7. Extraction of Aerosol and Rayleigh Components from Doppler Lidar Return Signal

    NASA Technical Reports Server (NTRS)

    Barnes, John E.; Fischer, Ken W.; Abreu, Vincent J.; Skinner, Wilbert R.

    1992-01-01

    One of the most significant problems which limits the applicability of lidar systems for pressure and density profile measurements below 30 km altitude is the presence of atmospheric aerosols which contaminate the molecular or Rayleigh return signal. A new technique is described which allows for the separation of the return signal into aerosol and molecular scattered components. The technique was applied to data from the University of Michigan's High Resolution Doppler Lidar (HRDL).

  8. Beyond the Alphabet Soup: Molecular Properties of Aerosol Components Influence Optics. (Invited)

    NASA Astrophysics Data System (ADS)

    Thompson, J. E.

    2013-12-01

    Components within atmospheric aerosols exhibit almost every imaginable model of chemical bonding and physical diversity. The materials run the spectrum from crystalline to amorphous, covalent to ionic, and have varying viscosities, phase, and hygroscopicity. This seminar will focus on the molecular properties of materials that influence the optical behavior of aerosols. Special focus will be placed on the polarizability of materials, hygroscopic growth, and particle phase.

  9. CARBON CONTAINING COMPONENT OF THE LOS ANGELES AEROSOL: SOURCE APPORTIONMENT AND CONTRIBUTIONS TO THE VISIBILITY BUDGET

    EPA Science Inventory

    Source resolution of the organic component of the fine fraction of the ambient aerosol (d(sub p) < 3.5 micrometers) has been carried out by combining source information from the organic component with thermal analysis and local emission inventories. The primary and secondary carb...

  10. Improving Pharmaceutical Aerosol Delivery During Noninvasive Ventilation: Effects of Streamlined Components

    PubMed Central

    Longest, P. Worth; Golshahi, Laleh; Hindle, Michael

    2013-01-01

    Aerosol delivery efficiency during noninvasive ventilation (NIV) is known to be low (~10%) and is associated with poor outcomes of aerosol therapy. The objective of this study was to demonstrate the benefit of redesigning ventilation circuit components using a streamlining approach to improve aerosol delivery during nasal high flow therapy in adults with a conventional-sized aerosol from a mesh nebulizer. The ventilation circuit consisted of a humidifier, mesh nebulizer, mixing T-connector (with 90° angle), 10 mm tubing, and nasal cannula interface. In vitro experiments and computational fluid dynamics analyses were used to evaluate depositional losses in a system of existing components and a newly proposed streamlined T-connector and cannula at flow rates of 30 and 45 LPM. Streamlined designs reduced deposition in the T-connector by a factor of 4. In the nasal cannula, the streamlined designs reduced depositional losses by factors of 1.25–2.0. With the streamlined designs, the highest emitted dose achieved was >40% for a conventional-sized aerosol at 30 LPM. Streamlined geometries offer an effective method to significantly improve the delivery of aerosols through components of NIV systems. This increase in delivery efficiency is important for new inhaled medications with narrow therapeutic windows, increased costs, or long delivery times. PMID:23423706