Source terms and source strengths of the carbonaceous aerosol in the tropics

Atmospheric aerosol samples were collected in the Ivory Coast, primarily at Lamto (6°N, 5°W) between 1979 and 1981. The samples were analysed for total particulate carbon concentration and isotopic composition (¹³C/¹²C) by mass spectrometry. Observed concentrations were found high compared to values reported for temperate regions. Fine particulate carbon in the submicrometersize range accounted for 50 to 80% of the reported concentrations. At Lamto, both particulate carbon concentrations and isotopic ratios exhibit a large temporal variability which is shown to reflect the diversity of sources and their seasonal evolution. Natural emissions from the equatorial forest during the wet season, and biomass burning during the dry season, appear to be the major sources. The latter, though active during only a third of the year, is, on an annual basis, the most important source. Based on the data obtained at Lamto, an attempt has been made to estimate the flux of fine particulate carbon emitted from the tropical regions into the global troposphere. This flux, which is of the order of 20×10¹² g C/yr, appears to be equivalent to the flux of fine particulate carbon emitted from industrial sources. These results suggest that the tropospheric burden of fine particulate carbon in lowlatitude regions is dominated by the long-range transport of carbonaceous aerosols originating from the Tropics.     

Rainwater Chemistry and Wet Deposition over the Wet Savanna Ecosystem of Lamto (Côte d'Ivoire)

From the IGAC-DEBITS Africa network (IDAF), data sets on precipitation chemistry collected from the ‘wet savanna ecosystem’ site of Lamto (Côte d'Ivoire), are analyzed (1995–2002). Inorganic (Ca^{2 +}, Mg^{2 +}, Na⁺, K⁺, NH₄ ⁺, Cl^?, SO₄ ^{2 ?}, NO₃ ^?) and organic (HCOO^?, CH₃COO^?) ions content were determined using Ion Chromatography. The analyzed 631 rainfall events represent 8420.9 mm of rainfall from a 9631.1 mm total. The precipitation chemistry at Lamto is influenced by four main sources: natural biogenic emissions from savanna soils (NO _x and NH₃), biomass burning (savanna and domestic fires), terrigeneous particles emissions from dry savanna soils, and marine compounds embedded in the summer monsoon. The inter-annual variability of the weighted volume mean concentration of chemical species linked with wet deposition fluctuates by ～ 20% over the period. Ammonium concentration is found to be the highest (17.6 μ eq.l^{? 1}) from all IDAF sites belonging to the West Africa ecosystems. Ammonia sources are from domestic animals, fertilizers and biomass burning. In spite of the high potential acidity of 30.5 μ eq.l^{? 1} from NO₃ ^?, SO₄ ^{2 ?}, HCOO^? and CH₃COO^?, a relatively weak acidity is measured: 6.9 μ eq.l^{? 1}. The 40% acid neutralization is explained by the acid gas – alkaline soil particles interaction. The remaining neutralization is from inclusion of gaseous ammonia. When results from Lamto, are compared with those from Banizoumbou (dry savanna) and Zoetele (equatorial forest), a regional view for wet tropospheric chemistry processes is obtained. The high concentration of the particulate phase in precipitation emphasizes the importance of multiphases processes between gases and particles in the atmospheric chemistry of the West Africa ecosystems. For example, the nss Ca^{2 +} precipitation content, main indicator of terrigeneous particles, goes from 30.8 μ eq.l^{? 1} in dry savanna to 9.2 μ eq.l^{? 1} at Lamto and 8.9 μ eq.l^{? 1} in the Cameroon forest. A similar gradient is obtained for rainfall mineral particles precipitation content with contribution of 80% in dry savanna, 40% in wet savanna, and 20% in the equatorial forest.     

Biomass burning in the tropical savannas of Ivory Coast: An overview of the field experiment Fire of Savannas (FOS/DECAFE 91)

FOS/DECAFE 91 (Fire of Savannas/Dynamique et Chimie Atmosphérique en Forêt Equatoriale) was the first multidisciplinary experiment organized in Africa to determine gas and aerosol emissions by prescribed savanna fires. The humid savanna of Lamto in Ivory Coast was chosen for its ecological characteristics representative of savannas with a high biomass density (900 g m^–2 dry matter). Moreover the vegetation and the climate of Lamto have been studied for more than twenty years. The emission ratios (X/CO₂) of the carbon compounds (CO₂, CO, NMHC, CH₄, PAH, organic acids and aerosols), nitrogen compounds (NO_x, N₂O, NH₃ and soluble aerosols) and sulfur compounds (SO₂, COS and aerosols) were experimentally determined by ground and aircraft measurements. To perform this experiment, 4 small plots (100×100 m) and 2 large areas (10×10 km) were prepared and burnt in January 1991 during the period of maximum occurrence of fires in this type of savanna. The detailed ecological study shows that the carbon content of the vegetation is constant within 1% (42 g C for 100 g of vegetal dry matter), the nitrogen content (0.29 g N for 100 g of dry matter) may vary by 10% and the sulfur content (0.05 g S/100 d.m.) by 20%. These variations of the biomass chemical content do not constitute an important factor in the variation of the gas and particle emission levels. With the emission ratios characteristic of humid savanna and flaming conditions (CO/CO₂ of 6.1% at the ground and 8% for airborne measurements), we propose a set of new emission factors, taking into account the burning efficiency which is about 80%: 74.4% of the carbon content of the savanna biomass is released to the atmosphere in the form of CO₂, 4.6% as CO, 0.2% as CH₄, 0.5% as NMHC and 0.7% as aerosols. 17.2% of the nitrogen content of the biomass is released as NO_x, 3.5% as N₂O, 0.6% as NH₃ and 0.5% as soluble aerosols.     

Emissions of Polycyclic aromatic hydrocarbons by savanna fires

Although Polycyclic aromatic hydrocarbons (PAH) are known as anthropogenic compounds arising from the combustion or the pyrolysis of fossil fuels, they may be also emitted by the combustion of vegetation. A field study was carried out in January 1991 at Lamto (Ivory Coast) as part of the FOS DECAFE experiment (Fire Of Savanna). Some ground samplings were devoted to the qualitative and quantitative characterization of atmospheric emissions by savanna fires during prescribed burns and under background conditions. Specific collections for gaseous and particulate PAHs have shown that the African practice of burning the savanna biomass during the winter months is an important source of PAHs. These compounds are emitted mainly in gaseous form but a significant fraction, essentially heavy PAHs, is associated with fine carbonaceous particles and can therefore represent a hazard for human health, since some of these compounds are mutagenic and carcinogenic. Twelve compounds were identified during the fire episodes and in the atmospheric background. The total concentration in the fires is of the order of 10 ng m^–3 for the gas phase and from 0.1 to 1 ng m^–3 in the aerosols. In the atmospheric background the mean concentrations are regular, 0.15 ng m^–3 and 2 pg m^–3, respectively. These concentrations are comparable with what is observed in European rural zones. The particulate emissions of PAHs by the savanna fires are distinguished by the abundance of some compounds which can be considered as tracers, although they are also slightly emitted by fossil fuel sources. These compounds are essentially pyrene, chrysene and coronene. In the gas phase, although no individual PAH may be considered as specific of the biomass combustion emissions, the relative abundances of the main PAHs are characteristic of the biomass burning. The concentrations of pyrene and fluorene are always predominant; these compounds could be considered as characteristic emission products of smoldering and flaming episodes, respectively. In the background the PAH composition shows that in a tropical region the air consists of a mixture coming from the various sources, but the biomass combustion is by far the most important source.The fluxes of total PAH emitted by savanna biomass burning in Africa were estimated to be of the order of 17 and 600 ton yr^–1, respectively, for the particulate PAHs and the gaseous PAHs, respectively.     

Particulate content of savanna fire emissions

As part of the FOS-DECAFE experiment at Lamto (Ivory Coast) in January 1991, various aerosol samples were collected at ground level near prescribed fires or under local background conditions, to characterize the emissions of particulate matter from the burning of savanna vegetation. This paper deals with total aerosol (TPM) and carbon measurements. Detailed trace element and polycyclic hydrocarbon data are discussed in other papers presented in this issue.Near the fire plumes, the aerosols from biomass burning are primarily of a carbonaceous nature (C%70% of the aerosol mass) and consist predominantly of submicron particles (more than 90% in mass.) They are characterized by their organic nature (black to total carbon ratio Cb/Ct in the range 3–20%) and their high potassium content (K/Cb0.6). These aerosols undergo aging during their first minutes in the atmosphere causing slight alterations in their size distribution and chemical composition. However, they remain enriched in potassium (K/Cb=0.21) and pyrene, a polycyclic aromatic hydrocarbon, such that both of these species may be used as tracers of savanna burning aerosols. We show that during this period of the year, the background atmosphere experiences severe pollution from both terrigenous sources and regional biomass burning (44% of the aerosol). Daynight variations of the background carbon concentrations suggest that fire ignition and spreading occur primarily during the day. Simultaneous TPM and CO₂ real-time measurements point to a temporal and spatial heterogeneity of the burning so that the ratio of the above background concentrations (TPM/CO₂) varies from 2 to 400 g/kg C. Smoldering processes are intense sources of particles but particulate emissions may also be important during the rapidly spreading heading fires in connection with the generation of heavy brown smoke. We propose emission factor values (EF) for aerosols from the savanna biomass burning aerosols: EF (TPM)=11.4±4.6 and 69±25 g/kg C_{dry plant} and EF(Ct)=7.4±3.4 and 56±16 g C/kg C_{dry plant} for flaming and smoldering processes respectively. In these estimates, the range of uncertainty is mostly due to the intra-fire variability. These values are significantly lower than those reported in the literature for the combustion of other types of vegetation. But due to the large amounts of vegetation biomass being burnt in African savannas, the annual flux of particulate carbon into the atmosphere is estimated to be of the order of 8 Tg C, which rivals particulate carbon emissions from anthropogenic activities in temperate regions.     

Aging of savanna biomass burning aerosols: Consequences on their optical properties

During the FOS-DECAFE experiment at Lamto, Ivory Coast, in January 1991, various ground studies were undertaken simultaneously in order to investigate the physical and chemical characteristics of smoke emitted by savanna biomass burning. Here we present sunphotometer ground-based results which allow the measurements of the spectral optical depth between 450 and 850 nm, the atmospheric water vapour content and the particle size distribution spectrum. The carbonaceous content of the savanna biomass burning aerosols is also investigated. This is the first time that the physical characteristics of particles emitted by savanna plumes are obtained from ground-field studies. All the results suggest that a rapid aging of the smoke occurs first hundred metres from the savanna fire èmission source. They show a relationship between the optical properties of smoke and the chemical aging of the aerosols primarily due to particle growth and a loss of organic material relative to the black carbon content.     

A global model of changing N2O emissions from natural and perturbed soils

A high resolution global model of the terrestrial biosphere is developed to estimate changes in nitrous oxide (N₂O) emissions from 1860–1990. The model is driven by four anthropogenic perturbations, including land use change and nitrogen inputs from fertilizer, livestock manure, and atmospheric deposition of fossil fuel NO _x . Global soil nitrogen mineralization, volatilization, and leaching fluxes are estimated by the model and converted to N₂O emissions based on broad assumptions about their associated N₂O yields. From 1860–1990, global N₂O emissions associated with soil nitrogen mineralization are estimated to have decreased slightly from 5.9 to 5.7 Tg N/yr, due mainly to land clearing, while N₂O emissions associated with volatilization and leaching of excess mineral nitrogen are estimated to have increased sharply from 0.45 to 3.3 Tg N/yr, due to all four anthropogenic perturbations. Taking into account the impact of each perturbation on soil nitrogen mineralization and on volatilization and leaching of excess mineral nitrogen, global 1990 N₂O emissions of 1.4, 0.7, 0.4 and 0.08 Tg N/yr are attributed to fertilizer, livestock manure, land clearing and atmospheric deposition of fossil fuel NO _x , respectively. Consideration of both the short and long-term fates of fertilizer nitrogen indicates that the N₂O/fertilizer-N yield may be 2% or more.C. NBM Definitions AET _mon (cm H₂O) = monthly actual evapotranspiration - AET _ann (cm H₂O) = annual actual evapotranspiration - age _h (years) = stand age of herbaceous biomass - age _w (years) = stand age of woody biomass - atmblc (gC/m²/month) = net flux of CO₂ from grid - biotoc (gC/g biomass) = 0.50 = convert g biomass to g C - beff _h = 0.8 = fraction of cleared herbaceous litter that is burned - beff _w = 0.4 = fraction of cleared woody litter that is burned - bfmin = 0.5 = fraction of burned N litter that is mineralized or converted to reactive gases which rapidly redeposit. Remainder assumed pyrodenitrified to N₂. + N₂O - bprob = probability that burned litter will be burned - burn _h (gC/m²/month) = herbaceous litter burned after land clearing - burn _w (gC/m²/month) = woody litter burned after land clearing - cbiomsh (gC/m²) = C herbaceous biomass pool - cbiomsw (gC/m²) = C woody biomass pool - clear (gC/m²/month) = woody litter C removed by land clearing - clearn (gN/m²/month) = woody litter N removed by land clearing - cldh (month^–1) = herbaceous litter decomposition coefficient - cldw (month^–1) = woody litter decomposition coefficient - clittrh (gC/m²) = C herbaceous litter pool - clittrw (gC/m²) = C woody litter pool - clph (month^–1) = herbaceous litter production coefficient - clpw (month^–1) = woody litter production coefficient - cnrath (gC/gN) = C/N ratio in herbaceous phytomass - cnrats (gC/gN) = C/N ratio in soil organic matter - cnratt (gC/gN) = average C/N ratio in total phytomass - cnratw (gC/gN) = C/N ratio in woody phytomass - crod (month^–1) = forest clearing coefficient - csocd (month^–1) = actual soil organic matter decompostion coefficient - decmult decomposition coefficient multiplier; natural =1.0; agricultural =1.0 (1.2 in sensitivity test) - fertmin (gN/m²/month) = inorganic fertilizer input - fleach fraction of excess inorganic N that is leached - fligh (g Lignin/ g C) = lignin fraction of herbaceous litter C - fligw (g Lignin/ g C) = 0.3 = lignin fraction of woody litter C - fln2o = .01–.02 = fraction of leached N emitted as N₂O - fnav = 0.95 = fraction of mineral N available to plants - fosdep (gN/m²/month) = wet and dry atmospheric deposition of fossil fuel NO _x - fresph = 0.5 = fraction of herbaceous litter decomposition that goes to CO₂ respiration - fresps = 0.51 + .068 ^* sand = fraction of soil organic matter decomposition that goes to CO₂ respiration - frespw = 0.3 ^* (^* see comments in Section 2.3 under decomposition) = fraction of woody litter decomposition that goes to CO₂ respiration - fsoil = ratio of NPP measured on given FAO soil type to NPF_miami - fstruct = 0.15 + 0.018 ^* ligton = fraction of herbaceous litter going to structural/woody pool - fvn2o = .05–.10 = fraction of excess volatilized mineral N emitted as N₂O - fvol = .02 = fraction of gross mineralization flux and excess mineral N volatilized - fyield ratio of total agricultural NPP in a given country in 1980 to total NPP_miami of all displaced natural grids in that country - gimmob _h (gN/m²/month) = gross immobilization of inorganic N into microbial biomass due to decomposition of herbaceous litter - gimmob _s (gN/m²/month) = gross immobilization of inorganic N into microbial biomass due to decomposition of soil organic matter - gimmob _w (gN/m²/month) = gross immobilization of inorganic N into microbial biomass due to decomposition of woody litter - graze (gC/m²/month) = C herbaceous biomass grazed by livestock - grazen (gN/m²/month) = N herbaceous biomass grazed by livestock - growth _h (gC/m²/month) = herbaceous litter incorporated into microbial biomass - growth _w (gC/m²/month) = woody litter incorporated into microbial biomass - gromin _h (gN/m²/month) = gross N mineralization due to decomposition and burning of herbaceous litter - gromin _s (gN/m²/month) = gross N mineralization due to decomposition of soil organic matter - gromin _w (gN/m²/month) = gross N mineralization due to decomposition and burning of woody litter - herb herbaceous fraction by weight of total biomass - leach (gN/m²/month) = leaching (& volatilization) losses of excess inorganic N - ligton (g lignin-C/gN) = lignin/N ratio in fresh herbaceous litter - LP _h (gC/m²/month)= C herbaceous litter production - LP (gC/m²/month) = C woody litter production - LPN _h (gN/m²/month) = N herbaceous litter production - LPN _W (gN/m²/month) = N woody litter production - manco2 (gC/m²/month) = grazed C respired by livestock - manlit (gC/m²/month) = C manure input (feces + urine) - n2oint (gN/m²/month) = intercept of N₂O flux vs gromin regression - n2oleach (gN/m²/month) = N₂O flux associated with leaching and volatilization of excess inorganic N - n2onat (gN/m²/month) = natural N₂O flux from soils - n2oslope slope of N₂O flux vs gromin regression - nbiomsh (gN/m²) = N herbaceous biomass pool - nbiomsw (gN/m²) = N woody biomass pool - nfix (gN/m²/month) = N₂ fixation + natural atmospheric deposition - nlittrh (gN/m²) = N herbaceous litter pool - nlittrw (gN/m²) = N woody litter pool - nmanlit (gN/m²/month) = organic N manure input (feces) - nmanmin (gN/m²/month) = inorganic N manure input (urine) - nmin (gN/m²) = inorganic N pool - NPP _acth (gC/m²/month)= actual herbaceous net primary productivity - NPP _actw (gC/m²/month) = actual woody net primary productivity - nvol (gN/m²/month) = volatilization losses from inorganic N pool - plntnav (gN/m²/month)= mineral N available to plants - plntup _h (gN/m²/month) = inorganic N incorporated into herbaceous biomass - plntup _w (gN/m²/month) = inorganic N incorporated into woody biomass - precip _ann (mm) = mean annual precipitation - precip _mon (mm) = mean monthly precipitation - pyroden _h (gN/m²/month) = burned herbaceous litter N that is pyrodenitrified to N₂ - pyroden _w (gN/m²/month) = burned woody litter N that is pyrodenitrified to N₂ - recyc fraction of N that is retranslocated before senescence - resp _h (gC/m²/month) = herbaceous litter CO₂ respiration - resp _s (gC/m²/month) = soil organic carbon CO₂ respiration - resp _w (gC/m²/month) = woody litter CO₂ respiration - sand sand fraction of soil - satrat ratio of maximum NPP to N-limited NPP - soiloc (gC/m²) = soil organic C pool - soilon (gN/m²) = soil organic N pool - temp _ann (°C) = mean annual temperature - temp _mon (°C) = mean monthly temperature Now at the NOAA Aeronomy Laboratory, Boulder, Colorado.     

Production of N2O,CH4, and CO2 from soils in the tropical savanna during the dry season

Emissions of N₂O, CH₄, and CO₂ from soils at two sites in the tropical savanna of central Venezuela were determined during the dry season in February 1987. Measured arithmetic mean fluxes of N₂O, CH₄, and CO₂ from undisturbed soil plots to the atmosphere were 2.5×10⁹, 4.3×10¹⁰, and 3.0×10¹³ molecules cm^-2 s^-1, respectively. These fluxes were not significantly affected by burning the grass layer. Emissions of N₂O increased fourfold after simulated rainfall, suggesting that production of N₂O in savanna soils during the rainy season may be an important source for atmospheric N₂O. The CH₄ flux measurements indicate that these savanna soils were not a sink, but a small source, for atmospheric methane. Fluxes of CO₂ from savanna soils increased ninefold two hours after simulated rainfall, and remained three times higher than normal after 16 hours. More research is needed to clarify the significance of savannas in the global cycles of N₂O, CH₄, CO₂, and other trace gases, especially during the rainy season.     

Carbonyl sulfide emissions from biomass burning in the tropics

Carbonyl sulfide emissions from biomass burning have been studied during field experiments conducted both in an African savanna area (Ivory Coast) and rice fields, central highland pine forest and savanna areas in Viet-Nam. During these experiments CO₂, CO and C₂H₂ or CH₄ have also been also monitored. COS values range from 0.6 ppbv outside the fires to 73 ppbv in the plumes. Significant correlations have been observed between concentrations of COS and CO (R ²=0.92,n=25) and COS and C₂H₂ (R ²=0.79,n=26) indicating a COS production during the smoldering combustion. COS/CO₂ emission factors (COS/CO₂) during field experiments ranged from 1.2 to 61×10^–6 (11.4×10^–6 mean value). COS emission by biomass burning was estimated to be up to 0.05 Tg S/yr in tropics and up to 0.07 Tg S/yr on a global basis, contributing thus about 10% to the global COS flux. Based on the S/C ratio measured in the dry plant biomass and the COS/CO₂ emission factor, COS can account for only about 7% of the sulfur emitted in the atmosphere by biomass burning.     

An Examination of the Atmospheric Chemistry of Mercury Using 210Pb and 7Be

Measurements of Hg (total gas-phase, precipitation-phase andparticulate-phase), aerosol mass, particulate ²¹⁰Pb and⁷Be and precipitation ²¹⁰Pb were made at an atmosphericcollection station located in a near remote area of northcentral Wisconsin,U.S.A. (46°10N, 89°50W) during the summers of 1993, 1994and 1995. Total Hg and ²¹⁰Pb were observed to correlate strongly(slope = 0.06 ± 0.03 ng mBq^-1; r ² =0.72) in rainwater. Mercury to ²¹⁰Pb ratios in particulate matter(0.03 ± 0.02 ng mBq^-1; r ² = 0.06) wereconsistent with the ratio in rain. Enrichment of the Hg/mass ratio (approx.5–50×) relative to soil and primary pollutant aerosols indicatedthat gas-to-particle conversion had taken place during transport. Comparisonof these results with models for the incorporation of Hg into precipitationindicates that atmospheric particles deliver more Hg to precipitation than canbe explained by the presence of soot. A lack of correlation between totalgas-phase Hg (TGM) and a ⁷Be/²¹⁰Pb function suggests novertical concentration gradient within the troposphere, and allows an estimateof TGM residence time of 1.5 ± 0.6 yr be made based on surface airsamples.     

Field studies of methane emission from termite nests into the atmosphere and measurements of methane uptake by tropical soils

The flux of CH₄ and CO₂ from termite nests into the atmosphere has been measured in a broad-leafed-type savannah in South Africa. Measurements were carried out on nests of species of six genera, i.e., Hodotermes, Macrotermes, Odontotermes, Trinervitermes, Cubitermes, and Amitermes. The flux rates of CH₄ relative to the flux rate of CO₂ in terms of carbon obtained for the individual species showed ratios of 2.9×10^-3, 7.0×10^-4, 6.7×10^-5, 8.7×10^-3, 2.0×10^-3 and 4.2×10^-3, respectively. Using data published on the assimulation efficiencies of termites, the flux of carbon as CH₄ accounts for 6.0×10^-5 to 2.6×10^-3 of the carbon ingested which results in a global CH₄ emission by termites of 2 to 5×10¹² g/yr. Methane is decomposed in the soil with average decomposition rates of 52 g/m²/h. The annual CH₄ consumption in the tropics and subtropics is estimated to be 21×10¹² g which exceeds the CH₄ emission rate by termites.     

Direct Radiative Effect of Aerosols on Net Ecosystem Carbon Exchange in the Pearl River Delta Region

The environmental impact of aerosols is currently a hot issue that has received worldwide attention. Lacking simultaneous observations of aerosols and carbon flux, the understanding of the aerosol radiative effect of urban agglomeration on the net ecosystem carbon exchange(NEE) is restricted. In 2009-2010, an observation of the aerosol optical property and CO_2 flux was carried out at the Dongguan Meteorological Bureau Station(DMBS) using a sun photometer and eddy covariance systems. The different components of photosynthetically active radiation(PAR),including global PAR(GPAR), direct PAR(DPAR), and scattered PAR(FPAR), were calculated using the Santa Barbara DISORT Atmospheric Radiative Transfer(SBDART) model. The effects of PAR on the NEE between land-atmosphere systems were investigated. The results demonstrated that during the study period the aerosol optical depth(AOD)reduced the DPAR by 519.28±232.89 μmol photons · m~(-2)s~(-1);, but increased the FPAR by 324.93±169.85μmol photons ·m~(-2)s~(-1);, ultimately leading to 194.34±92.62 μmol photons · m~(-2)s~(-1); decrease in the GPAR. All the PARs(including GPAR,DPAR, and FPAR) resulted in increases in the NEE(improved carbon absorption), but the FPAR has the strongest effect with the light use efficiency(LUE) being 1.12 times the values for the DPAR. The absorption of DPAR by the vegetation exhibited photo-inhibition in the radiation intensity 600 photons · m~(-2)s~(-1); in contrast, the absorptions of FPAR did not exhibit apparent photo-inhibition. Compared with the FPAR caused by aerosols, the DPAR was not the primary factor affecting the NEE. On the contrary, the increase in AOD significantly increased the FPAR, enhancing the LUE of vegetation ecosystems and finally promoting the photosynthetic CO_2 absorption.     

Aerosol characteristics during winter fog at Agra,North India

Simultaneous measurements on physical, chemical and optical properties of aerosols over a tropical semi-arid location, Agra in north India, were undertaken during December 2004. The average concentration of total suspended particulates (TSP) increased by about 1.4 times during intense foggy/hazy days. Concentrations of SO₄ ²⁻, NO₃ ⁻, NH₄ ⁺ and Black Carbon (BC) aerosols increased by 4, 2, 3.5 and 1.7 times, respectively during that period. Aerosols were acidic during intense foggy/hazy days but the fog water showed alkaline nature, mainly due to the neutralizing capacity of NH₄ aerosols. Trajectory analyses showed that air masses were predominantly from NW direction, which might be responsible for transport of BC from distant and surrounding local sources. Diurnal variation of BC on all days showed a morning and an evening peak that were related to domestic cooking and vehicular emissions, apart from boundary layer changes. OPAC (Optical properties of aerosols and clouds) model was used to compute the optical properties of aerosols. Both OPAC-derived and observed aerosol optical depth (AOD) values showed spectral variation with high loadings in the short wavelengths (<1 μm). AOD value at 0.5 μm wavelength was significantly high during intense foggy/hazy days (1.22) than during clear sky or less foggy/hazy days (0.63). OPAC-derived Single scattering albedo (SSA) was 0.84 during the observational period, indicating significant contribution of absorbing aerosols. However, the BC mass fraction to TSP increased by only 1% during intense foggy/hazy days and thereby did not show any impact on SSA during that period. A large increase was observed in the shortwave (SW) atmospheric (ATM) forcing during intense foggy/hazy days (+75.8 W/m²) than that during clear sky or less foggy/hazy days (+38 W/m²), mainly due to increase in absorbing aerosols. Whereas SW forcing at surface (SUF) increased from −40 W/m² during clear sky or less foggy/hazy days to −76 W/m² during intense foggy/hazy days, mainly due to the scattering aerosols like SO₄ ^2-.     

Chemical characteristics and deposition fluxes of dust-carbon mixed coarse aerosols at three sites of Delhi,NCR

The present paper reports chemistry and fluxes of dust-carbon mixed coarse particles. For the purpose of this study, different carbonaceous fractions i.e. organic carbon ((OC), elemental carbon (EC) and carbonate carbon (CC) of atmospheric dust and their respective local soils were quantified at three sites of National Capital Region (NCR) of Delhi viz. Jawaharlal Nehru University campus (JNU), Connaught Place (CP) and Vishali area of Ghaziabad (GB). It has been observed that the OC and EC levels were approximately five to nine times higher in urban atmospheric dust than their corresponding soils, whereas CC levels were about three times higher than the corresponding soils. Average dustfall fluxes were significantly different at all the sites due to their different land-use patterns. At urban background site (JNU), the dust flux was lowest (172 mg/m²/day) followed by CP, a commercial site, (192 mg/m²/day) and GB, an industrial/residential area, (302 mg/m²/day). Similar to the dustfall pattern, the mean values of OC, EC and CC deposition fluxes were also observed to be lowest at JNU (9.2, 0.8 and 1.0 mg/m²/day, respectively) as compared to CP (12.2, 1.2 and 1.3 mg/m²/day, respectively) and GB sites (11.1, 1.1 and 1.4 mg/m²/day, respectively). Interestingly, unlike fine mode, different correlation pattern of OC and EC in coarse mode dust aerosols at three sites has suggested their independent deposition processes and source contribution. Fluxes of major water soluble inorganic ions (Na⁺, NH₄ ⁺, K⁺, Ca²⁺, Mg²⁺, F^?, Cl^?, NO₃ ^? and SO₄ ^2?) were also determined. Ca²⁺, Cl^? and SO₄ ^2? were found to be the major ionic species of water soluble fraction of the urban dust at all the sites. These interactions are corroborated by the morphology of the mixed aerosols. High levels of measured chemical species and their spatial distribution revealed close correspondence with the local emissions from transport, industries, biomass burning, road dust and construction activities etc.     

The Variability of Air-sea O2 Flux in CMIP6: Implications for Estimating Terrestrial and Oceanic Carbon Sinks

The measurement of atmospheric O₂ concentrations and related oxygen budget have been used to estimate terrestrial and oceanic carbon uptake. However, a discrepancy remains in assessments of O₂ exchange between ocean and atmosphere (i.e. air-sea O₂ flux), which is one of the major contributors to uncertainties in the O₂-based estimations of the carbon uptake. Here, we explore the variability of air-sea O₂ flux with the use of outputs from Coupled Model Intercomparison Project phase 6 (CMIP6). The simulated air-sea O₂ flux exhibits an obvious warming-induced upward trend (~1.49 Tmol yr^?2) since the mid-1980s, accompanied by a strong decadal variability dominated by oceanic climate modes. We subsequently revise the O₂-based carbon uptakes in response to this changing air-sea O₂ flux. Our results show that, for the 1990?2000 period, the averaged net ocean and land sinks are 2.10±0.43 and 1.14±0.52 GtC yr^?1 respectively, overall consistent with estimates derived by the Global Carbon Project (GCP). An enhanced carbon uptake is found in both land and ocean after year 2000, reflecting the modification of carbon cycle under human activities. Results derived from CMIP5 simulations also investigated in the study allow for comparisons from which we can see the vital importance of oxygen dataset on carbon uptake estimations.     

Nitrogen compound emission from biomass burning in tropical African savanna FOS/DECAFE 1991 experiment (Lamto,Ivory Coast)

Gaseous nitrogen compounds (NO _x , NO _y , NH₃, N₂O) were measured at ground level in smoke plumes of prescribed savanna fires in Lamto, in the southern Ivory Coast, during the FOS/DECAFE experiment in January 1991. During the flaming phase, the linear regression between [NO _x ] and [CO₂] (differences in concentration between smoke plumes and atmosheric background) results volumic emission ratio [NO _x ]/[CO₂]=1.37×10^–3 with only slight differences between heading and backing fires. Nearly 90% of the nitrogen oxides are emitted as NO. Average emission ratios of other compounds are: 1.91, 0.047, and 0.145×10^–3 for NO _y , NH₃ and N₂O, respectively. The emission ratios obtained during this field experiment are compred with corresponding values measured during former experiments with the same plant species in combustion chambers. An accurate determination of both the biomass actually burned and of the plant nitrogen content, allows an assessment of emission fluxes of N-compounds from Guinean savanna burns. Preliminary results dealing with the influence of fire on biogenic emissions from soils are also reported.     

The characterization and distribution of aerosol and gaseous species in the winter monsoon over the western pacific ocean

In order to obtain a better understanding of the behavior of aerosols and SO₂ in the longrange transport through a marine boundary layer, a simple box-model is applied to the evaluation of the residence times of the species from the concentrations of gases and aerosols measured simulataneously on two islands in the West Pacific Ocean in the north-west monsoon. For Aitken and large particles, the residence time is varied from 3.7 to 7.4 days depending on the particle size, and their flux to the sea is equal to or slightly smaller than that of the free atmosphere. The residence time of giant particles is about one day and their flux to the sea is three times larger than that of the free atmosphere. The residence time of SO₂ is 15 hr, and the relative SO₂ mass flows of the deposition to the sea, of the diffusion to the free atmosphere and of the transformation to SO₄ ^2- are approximately 4, 1 and 1, respectively.     

Impacts of greenhouse gases and aerosol direct and indirect effects on clouds and radiation in atmospheric GCM simulations of the 1930–1989 period

Among anthropogenic perturbations of the Earths atmosphere, greenhouse gases and aerosols are considered to have a major impact on the energy budget through their impact on radiative fluxes. We use three ensembles of simulations with the LMDZ general circulation model to investigate the radiative impacts of five species of greenhouse gases (CO₂, CH₄, N₂O, CFC-11 and CFC-12) and sulfate aerosols for the period 1930–1989. Since our focus is on the atmospheric changes in clouds and radiation from greenhouse gases and aerosols, we prescribed sea-surface temperatures in these simulations. Besides the direct impact on radiation through the greenhouse effect and scattering of sunlight by aerosols, strong radiative impacts of both perturbations through changes in cloudiness are analysed. The increase in greenhouse gas concentration leads to a reduction of clouds at all atmospheric levels, thus decreasing the total greenhouse effect in the longwave spectrum and increasing absorption of solar radiation by reduction of cloud albedo. Increasing anthropogenic aerosol burden results in a decrease in high-level cloud cover through a cooling of the atmosphere, and an increase in the low-level cloud cover through the second aerosol indirect effect. The trend in low-level cloud lifetime due to aerosols is quantified to 0.5 min day^–1 decade^–1 for the simulation period. The different changes in high (decrease) and low-level (increase) cloudiness due to the response of cloud processes to aerosols impact shortwave radiation in a contrariwise manner, and the net effect is slightly positive. The total aerosol effect including the aerosol direct and first indirect effects remains strongly negative.     

A multifunctional HTDMA system with a robust temperature control

The hygroscopicity of atmospheric aerosols significantly influences their size distribution, cloud condensation nuclei ability, atmospheric residence time, and climate forcing. In order to investigate the hygroscopic behavior of aerosol particles and serious haze in China, a Hygroscopic Tandem Differential Mobility Analyzers (HTDMA) system was designed and constructed at Fudan University. It can function as a scanning mobility particle sizing system to measure particle size distribution in the range of 20--1000 nm in diameter, as well as a hygroscopicity analyzer for aerosol particles with diameters between 20--400 nm in the range of 20%--90% RH (relative humidity). It can also measure the effect of uptake of inorganic acids or semi-VOCs on the hygroscopic behavior of aerosols, such as typical inorganic salts in atmospheric dust or their mixtures. The performance tests show that the system measured particle size of the standard polystyrene latex spheres (PSLs) is 197 nm, which is in excellent agreement with the certified diameter D=199±6 nm, as well as a standard deviation of the repeated runs SD=8.9x10^-4. In addition, the measured hygroscopic growth factors of the model compounds, (NH₄)₂SO₄ and NaNO₃, agree with the Kohler theoretical curves. The results indicate that the HTDMA system is an excellent and powerful tool for studying the hygroscopic behavior of submicron aerosols and meets the demand required for laboratory research and fieldwork on atmospheric aerosols in China.     

The flux of charcoal to the troposphere during the period of agricultural burning in Panama

Although extensive areas of forests and grasslands are burned in the tropics, relatively little scientific attention has been focused on this phenomenon. In order to determine the land area burned and estimate the charcoal (elemental or graphitic carbon) produced, I monitored agricultural burning in a 1145 km² area in central Panama during the 1981 dry season. Over 10% of the land surface was burned in that year. Charcoal concentrations in the aerosol were also measured and reached values of 3.1 gC/m³ during the peak in burning. Off-peak values of aerosol charcoal are less than 1 gC/m³. The high charcoal concentration reflects the massive amounts of vegetational burning occurring in the area.The charcoal advected by the air mass flowing over the area has been estimated using a box model. Assuming an average aerosol concentration of charcoal of 1 gC/m³ for a three-month burning period, a 2 km atmospheric mixed layer, a 14 km/h wind velocity to the south, and a 150 km wide zone across the western Gulf of Panama watershed, I estimate that, during the dry season, 9×10⁹ g charcoal are mobilized by the troposphere. If 4.1×10¹² g phytomass are annually burned in this region, then the charcoal emission factor to the troposphere is 2.2×10^–3.