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.     

CALIOP对一次秸秆焚烧后气溶胶光学特性的探测分析

采用星载激光雷达(Cloud - Aerosol LIdar with Orthogonal Polarization,CALIOP)资料研究了2008年6月2日华东秸秆焚烧排放气溶胶的光学特性,并与2006～2008年统计结果进行了对比.结果表明:1)CALIOP能够有效探测到气溶胶层,探测结果符合生物质燃烧气溶胶的...     

生物质燃烧输送对青藏高原气溶胶光学辐射特性的影响研究

利用青藏高原拉萨(Lhasa)和珠峰(QOMS_CAS)站点地基CE 318太阳光度计观测数据，研究了2012年4月2日至4月5日一次生物质燃烧输送对青藏高原气溶胶光学和辐射特性的影响；并结合卫星遥感产品以及后向轨迹模式分析了本次生物质燃烧输送的可能来源。结果表明：本次气溶胶污染期间Lhasa和QOMS_CAS站点的主要气溶胶类型变为生物质燃烧气溶胶，气溶胶粒子的消光性增大(气溶胶光学厚度(AOD)增大，Lhasa和QOMS_CAS站点AOD最大值分别为0.4和0.29)，尺度减小(消光波长指数(EAE)>1.5)，吸收性增大(吸收波长指数(AAE)>1.3)，细模态粒子体积浓度增大，而细模态粒子峰值半径减小。气溶胶辐射强迫表明此次输送过程使得Lhasa和QOMS_CAS站点的气溶胶对大气顶和地表的降温作用增强，对大气的增温作用也增强。生物质燃烧输送的可能来源为南亚的印度东北部，尼泊尔与不丹地区。     

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.     

2004年北京秋季大气颗粒物的化学组分和来源特征

2004年9月在北京城区进行了大气颗粒物采样,样品用PIXE方法进行了分析,得到了20种元素的浓度及其谱分布。并对北京颗粒物的谱分布、富集因子和来源进行了分析研究。发现K元素浓度分布呈细粒态单峰谱分布,细粒态K富集因子较高,表明了生物质燃烧的主要贡献。因子分析结果还表明,土壤尘、生物质燃烧、煤烟尘、工业源和汽车尾气排放源对秋季北京局地排放源有明显贡献。     

Influence of natural and anthropogenic activities on UV Index variations – a study over tropical urban region using ground based observations and satellite data

Measurements of total ozone column and solar UV radiation under different atmospheric conditions are needed to define variations of both UV and ozone and to study the impact of ozone depletion at the Earth’s surface. In this study, spectral and broadband measurements of UV-B irradiance were obtained along with total ozone observations and aerosol optical depth measurements in the tropical urban region of Hyderabad, south India. We specifically used an Ultra-Violet Multifilter Rotating Shadow band Radiometer (UVMFR-SR), to measure UV irradiance in time and space. To assess the aerosol and O₃ effects on ground-reaching UV irradiance, we used measurements from a Microtops II sun photometer in addition to the Tropospheric Ultraviolet Visible radiation (TUV) model. We also assessed the Defense Meteorological Satellite Program – Operational Line Scanner (DMSP-OLS) night time satellite data for inferring biomass burning fires during the study period. Results clearly suggested a negative correlation between the DMSP-OLS satellite derived fire count data and UVMFR-SR data suggesting that aerosols from biomass burning are directly attenuating UV irradiance in the study region. Also, correlation analysis between UV index and ozone measurements from sun photometer and TOMS-Ozone Mapping Instrument (OMI) indicated a clear decrease in ground reaching UV-B irradiance during higher ozone conditions. The higher levels are attributed to photochemical production of O₃ during the oxidation of trace gases emitted from biomass burning. Results also suggested a relatively high attenuation in UV irradiance (~6% higher) from smoke particles than dust. We also found a relatively good agreement between the modeled (TUV) and measured UV irradiance spectra for different atmospheric conditions. Our results highlight the factors affecting UV irradiance in a tropical urban environment, south India.     

CALIOP对一次秸秆焚烧后气溶胶光学特性的探测分析

采用星载激光雷达(Cloud-Aerosol LIdar with Orthogonal Polarization,CALIOP)资料研究了2008年6月2日华东秸秆焚烧排放气溶胶的光学特性,并与2006~2008年统计结果进行了对比。结果表明:1)CALIOP能够有效探测到气溶胶层,探测结果符合生物质燃烧气溶胶的典型特征;气溶胶分布及廓线特点可以由火点分布及大气环流形势做出解释。2)个例中气溶胶光学特性廓线与该地区2006~2008年全年平均和夏季平均都存在一定差异。个例中后向散射系数廓线的峰值显示出气溶胶垂直分布结构,对应高度上的退偏振率比平均偏大而双波长比则偏小,表明秸秆焚烧源气溶胶层由大量非球形的细粒子组成。3)个例中气溶胶粒子谱特征与3年夏季平均接近而与3年平均差别很大,显示出个例的季节特征。更多个例的统计分析和地基观测的验证有助于了解秸秆焚烧源气溶胶的普遍规律。     

非洲地区大气气溶胶光学厚度时空变化及亚速尔高压对沙尘越大西洋传输的影响

研究了非洲地区大气气溶胶光学厚度（AOD）的时空变化及沙尘气溶胶越大西洋海区的传输。结果表明：1）源于撒哈拉沙漠的沙尘及其随赤道东风向西输送使得沙尘气溶胶成为非洲沙漠地区和紧邻的大西洋海区的主要气溶胶组分;AOD高值区和沙尘气溶胶光学厚度高值区在1—7月随赤道辐合带北移同步向北移动,而在8—12月则向南回撤。2）刚果盆地大气气溶胶主要为热带雨林和稀树草原排放的有机碳（OC）和黑碳（BC）气溶胶;其中与生物质燃烧源排放有关的OC、BC高值主要集中在干季（6—9月）的后半段（8—9月）;而生物源OC排放全年连续,其排放峰值出现于雨季开始时;生物质燃烧排放高值期与生物源排放高值期前后相继,形成干季（尤其是后半段）时期的OC、BC光学厚度高值。3）亚马逊河入海口地区主要气溶胶组分为海盐气溶胶,9—11月该区风力输送增强,风向由东南风转变为东风,海盐进入亚马逊河入海口处,形成AOD和海盐气溶胶光学厚度高值区。4）撒哈拉沙漠沙尘气溶胶向大西洋传输的偏北月份为7—9月、偏南月份为1—3月;2000—2016年海区沙尘气溶胶的传输路径存在向南移动的变化趋势,与同期亚速尔高压的增强和沙尘传输路径以北北风分量的增强以及赤道辐合带的移动一致。上述研究结果揭示了利用大气气溶胶时空变化特征反映区域大气环流和气候变化的可能性。     

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.     

Aerosol Properties and Their Impacts on Surface CCN at the ARM Southern Great Plains Site during the 2011 Midlatitude Continental Convective Clouds Experiment

Aerosol particles are of particular importance because of their impacts on cloud development and precipitation processes over land and ocean. Aerosol properties as well as meteorological observations from the Department of Energy Atmospheric Radiation Measurement(ARM) platform situated in the Southern Great Plains(SGP) are utilized in this study to illustrate the dependence of continental cloud condensation nuclei(CCN) number concentration(NCCN) on aerosol type and transport pathways. ARM-SGP observations from the 2011 Midlatitude Continental Convective Clouds Experiment field campaign are presented in this study and compared with our previous work during the 2009–10 Clouds, Aerosol, and Precipitation in the Marine Boundary Layer field campaign over the current ARM Eastern North Atlantic site. Northerly winds over the SGP reflect clean, continental conditions with aerosol scattering coefficient(σ_(sp)) values less than 20 Mm~(-1) and NCCNvalues less than 100 cm~(-3). However, southerly winds over the SGP are responsible for the observed moderate to high correlation(R)among aerosol loading(σ_(sp) 60 Mm~(-1)) and NCCN, carbonaceous chemical species(biomass burning smoke), and precipitable water vapor. This suggests a common transport mechanism for smoke aerosols and moisture via the Gulf of Mexico,indicating a strong dependence on air mass type. NASA MERRA~(-2) reanalysis aerosol and chemical data are moderately to highly correlated with surface ARM-SGP data, suggesting that this facility can represent surface aerosol conditions in the SGP, especially during strong aerosol loading events that transport via the Gulf of Mexico. Future long-term investigations will help to understand the seasonal influences of air masses on aerosol, CCN, and cloud properties over land in comparison to over ocean.     

Characteristics of biomass burning aerosol and its impact on regional air quality in the summer of 2003 at Gwangju, Korea

The main objective of this study is to investigate the chemical characteristics of biomass burning aerosol and its impact on regional air quality during an agricultural waste burning period in early summer in the rural areas of Korea. A 12-h integrated intensive sampling of biomass burning aerosol in the fine and coarse modes was conducted on 2–20 June 2003 in Gwangju, Korea. The collected samples were analyzed for concentrations of mass, ionic, elemental, and carbonaceous species. Average concentrations of fine and coarse mass were measured to be 67.9 and 18.7 μg m^− 3 during the biomass burning period, 41.9 and 18.8 μg m^− 3 during the haze period, and 35.6 and 13.3 μg m^− 3 during the normal period, respectively. An exceptionally high PM_2.5 concentration of 110.3 μg m^− 3 with a PM_2.5/PM₁₀ ratio of 0.79 was observed on 6 June 2003 during the biomass burning period. The potassium ratio method was used to identify biomass burning samples. The average ratio of potassium in the fine mode to the coarse mode (FK/CK) was 23.8 during the biomass burning period, 6.0 during the haze period, and 4.7 during the normal period, respectively. A FK/CK ratio above 9.2 was considered a criterion for biomass burning event in this study. Particulate matter from the open field burning of agricultural waste has an adverse impact on visibility, human health, and regional air quality.     

Formation and chemical composition of atmospheric aerosols in an equatorial forest area

The physical properties and the chemical composition of atmospheric aerosols have been studied in an equatorial region in the southern Congo (Africa). Field experiments were conducted between 1978 and 1983 in the equatorial forest of the Mayombe during periods where the influence of biomass burning was minimum. The results indicate that the forest is a net source of both fine particles resulting primarily from gas-to-particle conversion and coarse particles produced by mechanical processes. Carbonaceous matter is the major component of these biogenic particles but the forest is also a significant source of sulfate, nitrate, ammonium and potassium. Half of this carbon is attached to submicron particles and likely derives from organic gaseous precursors naturally emitted by the local biosphere.Presented at the international Symposium Influence of marine and terrestrial biosphere on the chemical composition of the atmosphere, held in Mainz, F.R.G., on 16–22 March 1986.     

Remote sensing-modelisation approach for diurnal estimation of burnt biomass in the Central African Republic Savanna

Experimental studies and mesoscale modeling of atmospheric chemistry require a good knowledge of the sources of the atmospheric constituent, at a temporal scale of about one hour and at a spatial scale corresponding to the model grid. A combined remote sensing/modeling approach for the estimation of the diurnal distribution of the amount of biomass burning in Central African Republic (C.A.R.) savanna fires is proposed. The fire propagation model (BEHAVE) developed by Rothermel was adapted to the fuel characteristics encountered in C.A.R. Ground and airborne measurements with satellite images (NOAA/AVHRR) were used to predict an accurate estimate of the burnt biomass. This combination allows the calculation of the distribution of the number of fires during the day providing an evaluation of the instantaneous fluxes of the compounds emitted in the atmosphere by these fires.     

生物质燃烧颗粒物中有机质及源解析研究进展

对近年来有关生物质燃烧排放的颗粒物中有机化合物和有机示踪物的研究进展进行了综述,分析了各国学者根据有机示踪物研究城市大气颗粒物中生物质燃烧和其他排放源对空气污染的贡献,对以后的相关研究具有借鉴意义．     

Observed changes in aerosol physical and optical properties before and after precipitation events

Precipitation scavenging of aerosol particles is an important removal process in the atmosphere that can change aerosol physical and optical properties. This paper analyzes the changes in aerosol physical and optical properties before and after four rain events using in situ observations of mass concentration, number concentration, particle size distribution, scattering and absorption coefficients of aerosols in June and July 2013 at the Xianghe comprehensive atmospheric observation station in China. The results show the effect of rain scavenging is related to the rain intensity and duration, the wind speed and direction. During the rain events, the temporal variation of aerosol number concentration was consistent with the variation in mass concentration, but their size-resolved scavenging ratios were different. After the rain events, the increase in aerosol mass concentration began with an increase in particles with diameter 0.8 μm [measured using an aerodynamic particle sizer(APS)], and fine particles with diameter 0.1 μm [measured using a scanning mobility particle sizer(SMPS)]. Rainfall was most efficient at removing particles with diameter ～0.6 μm and greater than 3.5 μm. The changes in peak values of the particle number distribution(measured using the SMPS) before and after the rain events reflect the strong scavenging effect on particles within the 100–120 nm size range. The variation patterns of aerosol scattering and absorption coefficients before and after the rain events were similar, but their scavenging ratios differed, which may have been related to the aerosol particle size distribution and chemical composition.     

An Investigation into the Ionic Chemical Composition and Mixing State of Biomass Burning Particles Recorded During TRACE-P P3B Flight#10

In this study bulk airborne aerosol composition measured by the PILS-IC (integration time of 3 min 24 s) during TRACE-P P3B Flight 10 are used to investigate the ionic chemical composition and mixing state of biomass burning particles. A biomass burning plume, roughly 3–4 days old, moderately influenced by urban pollution aerosols recorded in the Philippine Sea is investigated. Focusing on the fine particle NO₃⁻, SO₄²⁻, K⁺, NH₄⁺, and water-soluble organics, the observed correlations and nearly 1-to-1 molar ratios between K⁺ and NO₃⁻ and between NH₄⁺ and (SO₄²⁻+ inferred Organics) suggest the presence of fine-mode KNO₃, (NH₄)₂SO₄, and NH₄(Organics) aerosols. Under the assumption that these ion pairs existed, and because KNO₃ is thermodynamically less favored than K₂SO₄ in a mixture of NO₃⁻, SO₄²⁻, K⁺, NH₄⁺, and Organic anions, the measurements suggest that aerosols could be composed of biomass burning particles (KNO₃) mixed to a large degree externally with the (NH₄)₂SO₄ aerosols. A “closed-mode” thermodynamic aerosol simulation predicts that a degree of external mixing (by SO₄²⁻ mass) of 60 to 100% is necessary to achieve the observed ionic associations in terms of the existence of KNO₃. However, the degree of external mixing is most likely larger than 90%, based on both the presence of KNO₃ and the amounts of NH₄NO₃. Calculations are also shown that the aerosol mixing state significantly impacts particle growth by water condensation/evaporation. In the case of P3B Flight #10, the internal mixture is generally more hygroscopic than the external mixture. This method for estimating particle mixing state from bulk aerosol data is less definitive than single particle analysis, but because the data are quantitative, it may provide a complementary method to single particle chemical analysis.     

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.     

Oligomerization of levoglucosan by Fenton chemistry in proxies of biomass burning aerosols

Reactions of levoglucosan with produced from Fenton chemistry were studied in solution serving as a proxy for biomass burning aerosols. Two modes of oligomerization (≤2000 u) were observed for reaction times between 1 and 7 days using matrix-assisted laser desorption time-of-flight mass spectrometry (MALDI-TOF-MS) and laser desorption ionization time-of-flight mass spectrometry (LDI-TOF-MS). Single-mass unit continuum mass distributions with dominant −2 u patterns were measured and superimposed by a +176/+162 u oligomer series. This latter oligomer pattern was attributed to a Criegee rearrangement (+14 u) of levoglucosan, initiated by , forming a lactone (176 u). The acid-catalyzed reaction of any ROH from levoglucosan (+162 u) forms an ester through transesterification of the lactone functionality, whereupon propagation forms polyesters. Proposed products and chemical mechanisms are suggested as sources and precursors of humic-like substances (HULIS), which are known to possess a large saccharic component and are possibly formed from biomass burning aerosols (Andreae, Global Biomass Burning, MIT Press, Cambridge, Massachusetts, 3–21, 1991).     

A Closure Study of Aerosol Hygroscopic Growth Factor during the 2006 Pearl River Delta Campaign

Measurements of aerosol physical, chemical and optical parameters were carried out in Guangzhou, China from 1 July to 31 July 2006 during the Pearl River Delta Campaign. The dry aerosol scattering coefficient was measured using an integrating nephelometer and the aerosol scattering coefficient for wet conditions was determined by subtracting the sum of the aerosol absorption coefficient, gas scattering coefficient and gas absorption coefficient from the atmospheric extinction coefficient. Following this, the aerosol hygroscopic growth factor, f(RH), was calculated as the ratio of wet and dry aerosol scattering coefficients. Measurements of size-resolved chemical composition, relative humidity (RH), and published functional relationships between particle chemical composition and water uptake were likewise used to find the aerosol scattering coefficients in wet and dry conditions using Mie theory for internally- or externally-mixed particle species [(NH₄)₂SO₄, NH₄NO₃, NaCl, POM, EC and residue]. Closure was obtained by comparing the measured f(RH) values from the nephelometer and other in situ optical instruments with those computed from chemical composition and thermodynamics. Results show that the model can represent the observed f(RH) and is appropriate for use as a component in other higher-order models.     

Intercomparison of Two Box Models of the Chemical Evolution in Biomass-Burning Smoke Plumes

Results from two independently developed biomass-burning smoke plume models are compared. Model results were obtained for the temporal evolution of two nascent smoke plumes originating from significantly different fire environments (an Alaskan boreal forest and an African savanna). The two smoke plume models differed by 1%–10% for [O₃], with similar differences for NO _x and formaldehyde (relative percent differences). Smaller intermodel differences were observed for the African savanna smoke plume as compared to the plume from the Alaskan boreal fire. Mechanistic differences between the models are heightened for the Alaskan smoke plume due to the higher VOC emission ratios as compared to the African savanna fire. The largest deviations result from the differences in oxidative photochemical mechanisms, with a smaller contribution attributable to the calculation of photolysis frequencies. The differences between the two smoke plume models are significantly smaller than the uncertainties of available photokinetic data or field measurements. Model accuracy depends most significantly on having the fullest possible VOC data, a requirement that is constrained by currently available instrumentation.