Biomass Burning in Southern Africa: Individual Particle Characterization of Atmospheric Aerosols and Savanna Fire Samples

Ambient atmospheric aerosols and savanna fireparticulate emission samples from southern Africa werecharacterised in terms of particle classes and theirnumber abundance by electron probe X-ray microanalysis(EPXMA). About ten particle classes were identifiedfor each sample. The major classes werealuminosilicates and sea salts for ambient coarse(2–10 m equivalent aerodynamic diameter (EAD))samples, and K-S and S-only particles for ambient fine(<2 m EAD) samples. The K-S particles are oneof the major products of biomass burning. The EPXMAresults were found to be consistent with the resultsfrom bulk analyses on a sample by sample basis. Forsavanna fire fine samples, quantitative EPXMA revealedthat many particles had a composition of simple saltssuch as KCl. Some particles had a deviatingcomposition in the sense that more ionic species wereinvolved in sustaining the balance between cations andanions, and they were composite or mixed salts.Because of extensive processing during the atmospherictransport, the composition of the K-S particles in theambient samples was different from K₂SO₄,and such particles were enriched with S. The finepyrogenic KCl particles and the fine sea-saltparticles were much depleted in chlorine.     

Comparison of Measured Ozone Production Efficiencies in the Marine Boundary Layer at Two European Coastal Sites under Different Pollution Regimes

Ozone production efficiencies (E_N), which can be defined as the netnumber of ozone molecules produced per molecule of NO_xoxidised, have been calculated from measurements taken during three intensive field campaigns (one in the spring, EASE 96, and two in the summer, EASE 97 and TIGER 95), at two European coastal sites (Mace Head, Ireland (EASE) and Weybourne, Norfolk (TIGER)) impacted by polluted air masses originating from both the U.K. and continental Europe, as well as relatively clean oceanic air masses from the Arctic and Atlantic. From a detailed wind sector analysis of the EASE 96 and 97 data it is clear that two general types of pollution regime were encountered at Mace Head. The calculated ozone production efficiency in clean oceanic air masses was approximately 65, which contrasted to more polluted air, from the U.K. and the continental European plume, where the efficiency decreased to between 4 and 6. The latter values of E_Nagree well with literature measurements conducted downwind of various urban centres in the U.S. and Europe, which are summarised in a wide-ranging review table. The E_N value calculated for clean oceanic air is effectivelyan upper limit, owing to the relatively rapid deposition of HNO₃ tothe ocean. Consideration of the variation of E_N with NO_x forthe three campaigns suggests that ozone production efficiency is relatively insensitive to both geographical location and season. The measuredE_N values are also compared with values derived from steady-state expressions. An observed anti-correlation between E_N and measured ozone tendencyis briefly discussed.     

Influence of South Asian Biomass Burning on Ozone and Aerosol Concentrations Over the Tibetan Plateau

In this work, the influence of South Asian biomass burning emissions on O₃ and PM_2.5 concentrations over the Tibetan Plateau (TP) is investigated by using the regional climate chemistry transport model WRF-Chem. The simulation is validated by comparing meteorological fields and pollutant concentrations against in situ observations and gridded datasets, providing a clear perspective on the spatiotemporal variations of O₃ and PM_2.5 concentrations across the Indian subcontinent, including the Tibetan Plateau. Further sensitivity simulations and analyses show that emissions from South Asian biomass burning mainly affect local O₃ concentrations. For example, contribution ratios were up to 20% in the Indo-Gangetic Plain during the pre-monsoon season but below 1% over the TP throughout the year 2016. In contrast, South Asian biomass burning emissions contributed more than 60% of PM_2.5 concentration over the TP during the pre-monsoon season via significant contribution of primary PM_2.5 components (black carbon and organic carbon) in western India that were lofted to the TP by westerly winds. Therefore, it is suggested that cutting emissions from South Asian biomass burning is necessary to alleviate aerosol pollution over the TP, especially during the pre-monsoon season.     

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.     

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.     

2017年8—9月湖州市臭氧污染特征及其生成机制研究

近年来近地面臭氧问题日益凸显,成为影响空气质量持续改善的瓶颈.本研究基于2017年8—9月在湖州市城区开展的为期1个月的臭氧及其前体物挥发性有机物（VOCs）和氮氧化物（NO_x）在线观测数据,分析了臭氧及其前体物污染特征,利用正矩阵因子分析（PMF）解析了VOCs来源,并采用基于观测的模型（OBM）对臭氧生成机制进行研究.研究结果表明：1）观测期间湖州市VOCs平均体积分数为（24.78±9.10）×10^-9,其中占比最高的组成为烷烃、含氧VOCs （OVOCs）和卤代烃;2）在臭氧非超标时段,湖州市臭氧生成处于VOCs控制区,而在臭氧重污染期间湖州市处于以VOCs控制为主的过渡区;3）在臭氧超标时段,对臭氧生成潜势（OFP）贡献最大的是芳香烃（39.6%）,其次是烯烃（21.5%）和OVOCs （19.4%）,排名前三的关键组分为甲苯、乙烯和间/对二甲苯;4）源解析结果显示观测期间湖州市VOCs的主要来源是溶剂使用（27.0%）、交通排放（22.7%）、背景+传输（19.3%）、工业排放（16.9%）、汽油挥发（7.7%）和植物排放（6.4%）,重污染过程期间对OFP贡献最大的两类源是交通排放源和溶剂使用源,贡献百分比分别为35.1%和30.5%.因此,对交通排放和溶剂使用方面进行控制管理对湖州市大气臭氧污染防控有重要意义.     

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.     

Photochemistry in the Arctic Free Troposphere: Ozone Budget and Its Dependence on Nitrogen Oxides and the Production Rate of Free Radicals

Local ozone production and loss rates for the arctic free troposphere (58–85° N, 1–6 km, February–May) during the TroposphericOzone Production about the Spring Equinox (TOPSE) campaign were calculated using a constrained photochemical box model. Estimates were made to assess the importance of local photochemical ozone production relative to transport in accounting for the springtime maximum in arctic free tropospheric ozone. Ozone production and loss rates from our diel steady-state box model constrained by median observations were first compared to two point box models, one run to instantaneous steady-state and the other run to diel steady-state. A consistent picture of local ozone photochemistry was derived by all three box models suggesting that differences between the approaches were not critical. Our model-derived ozone production rates increased by a factor of 28 in the 1–3 km layer and a factor of 7 in the 3–6 kmlayer between February and May. The arctic ozone budget required net import of ozone into the arctic free troposphere throughout the campaign; however, the transport term exceeded the photochemical production only in the lower free troposphere (1–3 km) between February and March. Gross ozone production rates were calculated to increase linearly with NO_x mixing ratiosup to 300 pptv in February and for NO_x mixing ratios up to 500 pptv in May. These NO_x limits are an order of magnitude higher thanmedian NO_x levels observed, illustrating the strong dependence ofgross ozone production rates on NO_x mixing ratios for the majority of theobservations. The threshold NO_x mixing ratio needed for netpositive ozone production was also calculated to increase from NO_x 10pptv in February to 25 pptv in May, suggesting that the NO_x levels needed to sustain net ozone production are lower in winter than spring. This lower NO_x threshold explains how wintertime photochemical ozone production can impact the build-up of ozone over winter and early spring. There is also an altitude dependence as the threshold NO_x neededto produce net ozone shifts to higher values at lower altitudes. This partly explains the calculation of net ozone destruction for the 1–3 km layerand net ozone production for the 3–6 km layer throughout the campaign.     

Ground Based Gas Phase Measurements in Surinam during the LBA-Claire 98 Experiment

As part of the LBA-CLAIRE-98 experiment, ground level atmosphericconcentrations of O₃, CO, hydroperoxides and organic acids weremeasured in the rainforest region in Surinam. Measurements of CO andO₃ were also made at a coastal site.The results suggest that a significant consumption of `boundary layer' ozoneoccurs over the forested region of Surinam, with an estimated net ozoneconsumption of about 5% hr^–1 during daytime. Thiswould be mainly explained by a low photochemical production and high drydeposition to the forest vegetation. Compared to other tropical sites, lowerlevels of H₂O₂ were observed at the rainforest site,with an average boundary layer concentration of 0.55± 0.2 nmolmol^–1. Also acetic and formic acids showed relatively lowaverage boundary layer mixing ratios; 1.1± 0.4 nmolmol^–1 and 1.4± 0.5 nmol mol^–1,respectively. Significant correlations were found between both acids andbetween the acids and hydrogen peroxide, suggesting an atmospheric source forthe acids.From the available observations we discuss possible implications of ourmeasurements for the O₃, HO₂, and NO_x budgetsand concentrations in the boundary layer. We conclude that, despite the highsolar irradiation, relatively low levels of O₃,H₂O₂, HCOOH and CH₃COOH are observed in theboundary layer of the rainforest of Surinam, probably due to low levels ofNO_x and high levels of VOCs, which leads to loss of OH andHO₂ radicals. Additionally, high deposition rates of these gasesoccur to the forest vegetation.     

鼎湖山森林地区臭氧及其前体物的变化特征和分析

通过对鼎湖山森林地区近地面O3和NOx浓度、太阳辐射、气象参数等为期一年的观测和资料分析,给出了地面O3和NOx浓度、太阳辐射的变化规律及其相互之间的关系.地面O3、NOx、CO、SO2浓度以及紫外辐射、太阳总辐射等有明显的日变化和季节变化.不同因子对O3的敏感性试验结果表明,晴天和实际天气,O3浓度对NO、NO2浓度的变化最为敏感,其次是水汽、气溶胶,最后是紫外辐射.所有因子的变化均引起O3在湿季比干季更大的变化率,因此在研究臭氧化学和光化学时,应该考虑水汽以及OH自由基的重要作用.对于晴天和实际天气的逐时值和日平均值而言,O3浓度与NO2/NO之间存在很好的正相关关系,比值NO2/NO可以作为判断O3峰值出现的一个指标.O3极值的出现既受NO和NOx影响,也受气象因素(温湿度、云、风、雾、降雨)和辐射的影响.周末O3、NOx浓度及NO2/NO有规律的增大,表明实验地点的大气受到人为污染源的影响.     

Methane,carbon monoxide and light non-methane hydrocarbon emissions from African savanna burnings during the FOS/DECAFE experiment

Atmospheric samples from savanna burnings were collected in the Ivory Coast during two campaigns in January 1989 and January 1991. About 30 nonmethane hydrocarbons from C₂ to C₆, carbon monoxide, carbon dioxide and methane were measured from the background and also at various distances from the burning. Concentrations in the fire plume reached ppmv levels for C₂-C₄ hydrocarbons, and 5300, 500 and 93 ppmv for CO₂, CO and CH₄ respectively. The excess in the mixing ratios of these gases above their background level is used to derive emission factors relative to CO and CO₂. For the samples collected immediately in the fire plume, a differentiation between high and low combustion efficiency conditions is made by considering the CO/CO₂ ratio. Ethene (C₂H₄), acetylene (C₂H₂), ethane (C₂H₆) and propene (C₃H₆) are the major NMHC produced in the flaming stage, whereas a different pattern with an increasing contribution of alkanes is observed in samples typical of post flaming processes. A strong correlation between methane and carbon monoxide suggests that these compounds are produced during the same stage of the combustion. In samples collected at a distance from the fire and integrated over a period of 30 minutes, the composition is very similar to that of flaming. NMHC/CO₂ is of the order of 0.7%, CH₄/CO₂ of the order of 0.4% and CO/CO₂ of the order of 6.3%. From this study, a global production by African savanna fires is derived: 65 Tg of CO-C, 4.2 Tg of CH₄-C and 6.7 Tg of NMHC-C. Whereas acetylene can be used as a conservative tracer of the fire plumes, only ethene, propene and butenes can be considered in terms of their direct photochemical impact.     

Precipitation Chemistry in Semi-Arid Areas of Southern Africa: A Case Study of a Rural and an Industrial Site

Experimental data on the precipitation chemistry in the semi-arid savanna of South Africa is presented in this paper. A total of 901 rainwater samples were collected with automatic wet-only samplers at a rural site, Louis Trichardt, and at an industrial site, Amersfoort, from July 1986 to June 1999. The chemical composition of precipitation was analysed for seven inorganic and two organic ions, using ion chromatography. The most abundant ion was SO₄ ^{2 –} and a large proportion of theprecipitation is acidic, with 98% of samples at Amersfoort and 94% at LouisTrichardt having a pH below 5.6 (average pH of 4.4 and 4.9, respectively). This acidity results from a mixture of mineral and organic acids, with mineral acids being the primary contributors to the precipitation acidity in Amersfoort, while at Louis Trichardt, organic and mineral acids contribute equal amounts of acidity. It was found that the composition of rainwater is controlled by five sources: marine, terrigenous, nitrogenous, biomass burning and anthropogenic sources. The relative contributions of these sources at the two sites were calculated. Anthropogenic sources dominate at Amersfoort and biomass burning at Louis Trichardt. Most ions exhibit a seasonal pattern at Louis Trichardt, with the highest concentrations occurring during the austral spring as a result of agricultural activities and biomass combustion, while at Amersfoort it is less pronounced due to the dominance of relatively constant industrial emissions. The results are compared to observations from other African regions.     

Tropospheric chemical composition measurements in Brazil during the dry season

Field measurement programs in Brazil during the dry seasons in August and September 1979 and 1980 have demonstrated the large importance of the continental tropics in global air chemistry. Many important trace gases are produced in large amounts over the continents. During the dry season, much biomass burning takes place, especially in the cerrado regions, leading to a substantial emission of air pollutants, such as CO, NO _x , N₂O, CH₄ and other hydrocarbons. Ozone concentrations are enhanced due to photochemical reactions. The large biogenic organic emissions from tropical forests play an important role in the photochemistry of the atmosphere and explain why CO is present in such high concentrations in the boundary layer of the tropical forest. Carbon monoxide production may represent more than 3% of the net primary productivity of the tropical forests. Ozone concentrations in the boundary layer of the tropical forests indicate strong removal processes. Due to atmospheric supply of NO _x by lightning, there is probably a large production of O₃ in the free troposphere over the Amazon tropical forests. This is transported to the marine-free troposphere and to the forest boundary layer.     

In Situ Trace Gas and Particle Measurements in the Summer Lower Stratosphere during STREAM II: Implications for O3 Production

In situ aircraft measurements of O₃, CO,HNO₃, and aerosol particles are presented,performed over the North Sea region in the summerlower stratosphere during the STREAM II campaign(Stratosphere Troposphere Experiments by AircraftMeasurements) in July 1994. Occasionally, high COconcentrations of 200-300 pbbv were measured in thelowermost stratosphere, together with relatively highHNO₃ concentrations up to 1.6 ppbv. The particlenumber concentration (at standard pressure andtemperature) between 0.018-1 m decreased acrossthe tropopause, from >1000 cm^-3 in the uppertroposphere to <500 cm^-3 in the lowermoststratosphere. Since the CO sources are found in thetroposphere, the elevated CO mixing ratios areattributed to mixing of polluted tropospheric air intothe lowermost extratropical stratosphere. Further wehave used a chemical model to illustrate that nitrogenoxide reservoir species (mainly HNO₃) determinethe availability of NO_x (=NO + NO₂) andtherefore largely control the total net O₃production in the lower kilometers of thestratosphere. Model simulations, applying additionalNO_x perturbations from aircraft, show that theO₃ production efficiency of NO_x is smallerthan previously assumed, under conditions withrelatively high HNO₃ mixing ratios, as observedduring STREAM II. The model simulations furthersuggest a relatively high O₃ productionefficiency from CO oxidation, as a result of therelatively high ambient HNO₃ and NO_xconcentrations, implying that upward transport of COrich air enhances O₃ production in the lowermoststratosphere. Analysis of the measurements and themodel calculations suggest that the lowermoststratosphere is a transition region in which thechemistry deviates from both the upper troposphere andlower stratosphere.     

漠河地区臭氧的观测和计算

1997年3月上旬,在黑龙江漠河地区对地面和整层臭氧、太阳辐射等进行了短期观测,以初步了解该地区臭氧和辐射的变化规律以及它们之间的相互关系.研究发现,漠河地区近地面臭氧日变化明显,其峰值出现在每日10:00(北京时间)左右,并早于紫外辐射(UV)峰值出现时间.整层大气臭氧总量的日变化特征不明显.基于UV能量守恒,建立了臭氧与其影响因子-光化学、散射、UV等因子之间较好的定量关系和经验模式,并将其用于计算地面、整层大气臭氧小时值和日平均值.结果表明,计算值与观测值吻合的都比较好,它们相对偏差的平均值分别为:地面臭氧小时值(11.9%)和日平均值(9.0%);整层大气臭氧小时值和日平均值-7.4%、1.8%.因此,地面和整层臭氧的经验算法是合理和可行的.利用散射辐射/直接辐射(D/S)和散射辐射/总辐射(D/Q)可以描述大气中的物质如气溶胶、云等的散射作用.采用D/Q表示散射作用可以提高地面臭氧和整层大气臭氧计算的准确度,特别是对云量较大的情况.       

Emission of nitric oxide from soils and termite nests in a Trachypogon savanna of the Orinoco basin

Nitric oxide fluxes from soils in the Trachypogon savanna of the Orinoco basin were determined during the dry season using the static chamber method. The emission from dry soils fluctuated from 0.4 to 3 ng N m^–2 s^–1 and increased up to 25 ng N m^–2 s^–1 after moderate watering or light rain-falls (1 to 5 mm). The mean emission values are up to 6 times lower than one observed earlier at the Chaguaramas site, but up to 10 times higher than one recorded at the Guri site, indicating an important spatial variability in NO fluxes of the Venezuelan savanna region. The changes observed after the addition of nitrogen to the soil, in the form of ammonium and/or nitrate, indicate a high denitrification potential in this acidic soil. Burning of the surface vegetation produced an increase by a factor of 10 in the emission rate of NO, but the effect was relatively short in time, about 5 days. It was estimated for the savanna region that burning increases the total NO soil emission during the dry season by 15% compared to the unburnt case. Soils with termite nests emit 10 times more NO than soil without nests, but the contribution from this source is less than 2% of the total savanna soil flux.     

The Role of Ozone Depletion in the Lack of Cooling in the Antarctic Upper Stratosphere during Austral Winter

Temperature trends in the upper stratosphere are investigated using satellite measurements from Stratospheric Sounding Unit(SSU) outputs and simulations from chemistry–climate models(CCMs) and the Coupled Model Intercomparison Project Phase 6(CMIP6). Observational evidence shows a lack of cooling in the Antarctic, in contrast to strong cooling at other latitudes, during austral winter over 1979–97. Analysis of CCM simulations for a longer period of1961–97 also shows a significant contrast in the...     

Observations of Streamers in the Troposphere and Stratosphere Using Ozone Lidar

We describe here a DIAL lidar system for atmospheric ozone measurements atAberystwyth, Wales, together witha method for deriving a stratospheric ozone profile from a single laserwavelength. Lidar measurements are used todepict the passage of three mesoscale ozone disturbances in the troposphereand stratosphere. In the troposphere, twosmall fold-like structures are shown beneath and at the edge of streamers ofhigh potential vorticity in ECMWFanalyses. MST radar measurements at the same time show that one of these foldswas actively turbulent, causingmixing of stratospheric and tropospheric air. In the stratosphere, a streamerof low-latitude air drawn into a filamentby a breaking Rossby wave event was observed crossing the lidar site.     

青藏高原夏季臭氧低谷形成的机理-臭氧输送和化学过程

利用三维化学输送模式(OSLO CTM2)模拟青藏高原夏季臭氧低谷。结果表明：在青藏高原夏季臭氧低谷的形成和变化过程中，动力输送过程起着最主要作用，化学过程部分补偿了输送过程引起的臭氧减少。在动力输送过程中，水平输送在5月份是造成臭氧减少的主要原因，可在6月和7月成为使臭氧增加；垂直平流的作用不断增强，在6月和7月成为臭氧减少的主要因素；对流输送的作用在7月份大幅增加，其引起的臭氧减少可以与净的变化相比，其作用也不可忽视。气相的化学过程引起的臭氧增加的量值有时超过了臭氧的净变化的大小，因此它也起着重要作用。