Airborne measurements of savanna fire emissions and the regional distributio of pyrogenic pollutants over Western Africa

We measured CO₂, CO, CH₄, H₂, and NO₂ in air masses polluted by savanna fires over Côte d'Ivoire, western Africa. Elevated concentrations of these trace gases were found in fire plumes and also in extensive haze layers. Trace gas mixing ratios ranged as high as 605 ppmv for CO₂, 14.8 ppmv for CO, 2.7 ppmv for CH₄, 4.2 ppmv for H₂, and 25 ppbv for NO₂. We compare our emission ratios to those obtained in previous field and laboratory studies. The emission ratios, expressed as an average and as a range or as an average only, were: dCO/dCO₂ 5.3×10^–2 (3–18×10^–2); dCH₄/dCO 5.3×10^–2; dH₂/dCO 2.4×10^–1 and dNO₂/dCO₂ 1.8×10^–4 (1.5–2.2×10^–4). The values found match those found during similar measurements, though our results point to rather vigorous burning in the savanna of western Africa.     

Ozone production potential following convective redistribution of biomass burning emissions

The effects of deep convection on the potential for forming ozone (ozone production potential) in the free troposphere have been simulated for regions where the trace gas composition is influenced by biomass burning. Cloud dynamical and photochemical simulations based on observations in 1980 and 1985 Brazilian campaigns form the basis of a sensitivity study of the ozone production potential under differing conditions. The photochemical fate of pollutants actually entrained in a cumulus event of August 1985 during NASA/GTE/ABLE 2A (Case 1) is compared to photochemical ozone production that could have occurred if the same storm had been located closer to regions of savanna burning (Case 2) and forest burning (Case 3). In each case studied, the ozone production potential is calculated for a 24-hour period following convective redistribution of ozone precursors and compared to ozone production in the absence of convection. In all cases there is considerably more ozone formed in the middle and upper troposphere when convection has redistributed NO_x, hydrocarbons and CO compared to the case of no convection.In the August 1985 ABLE 2A event, entrainment of a layer polluted with biomass burning into a convective squall line changes the free tropospheric cloud outflow column (5–13 km) ozone production potential from net destruction to net production. If it is assumed that the same cloud dynamics occur directly over regions of savanna burning, ozone production rates in the middle and upper troposphere are much greater. Diurnally averaged ozone production following convection may reach 7 ppbv/day averaged over the layer from 5–13 km-compared to typical free tropospheric concentrations of 25–30 ppbv O₃ during nonpolluted conditions in ABLE 2A. Convection over a forested region where isoprene as well as hydrocarbons from combustion can be transported into the free troposphere leads to yet higher amounts of ozone production.     

光化学臭氧日变化特征与其前体物关系的探讨

应用大气光化学模式研究了日最大臭氧体积分数及其出现时刻与其前体物NMHC、NOx体积分数及NMHC／NOx比值的关系。结果表明，影响日最大臭氧体积分数（ψ03max）脊线位置（EKMA图，Empirical Kinetic Modeling Approach）的关键因子是NMHC成份组成比例；日臭氧体积分数达到最大值需要的时间（τ03max）与NMHC／NOx比值及NMHC成份组成比例有关，与NMHC、NOx体积分数关系不大。此外，利用该结果解释了近20a北京日最大臭氧体积分数出现时刻具有不断提前的变化趋势的原因。     

Isoprene emissions from vegetation and hydrocarbon emissions from bushfires in tropical Australia

Information from a variety of sources, including an airborne field expedition in November 1985, is used to produce estimates of the annual emissions of some hydrocarbons from bushfires, and isoprene from trees, in tropical Australia. For the continent north of 23° S the annual bushfires (biomass burning) input was estimated, in units of Tg carbon, to be 2 TgC (uncertainty range 0.8–5 TgC), emitted predominantly during the May to October dryseason. Isoprene emissions during this period were estimated also to be 2 TgC (uncertainty range 0.5–8 TgC), but were estimated to be an order of magnitude higher during the November to April wet season, at a level of 23 TgC (uncertainty range 6–100 TgC).The large annual emission of isoprene over the tropical part of the Australian continent yields ppbv levels of isoprene measured at the surface in summertime. Isoprene reactivity with hydroxyl radical is such that at these concentrations isoprene must be a dominant factor in controlling the concentration of OH radical in the convective boundary layer. Simple arguments based on the convective velocity scale suggest that the shape of the isoprene vertical profile in November 1985 would be consistent with available data on the OH-isoprene reaction rate if OH concentration in the boundary layer averaged about 2.5×10⁶ cm^-3 over the middle part of the day.Temporarily at the International Meteorological Institute, Stockholm University, S-106 91, Stockholm, Sweden.     

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.     

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.     

Ozone Production Efficiency in Savanna and Forested Areas during the EXPRESSO Experiment

NO, NO_x, NO_y and O₃ have been measuredduring the airborne EXPRESSO experiment, November 96,which took place near Bangui (Central Africa) at thebeginning of the dry season. This period correspondsto an intense burning activity. Chemical andphotochemical characteristics of the planetaryboundary layer, which corresponds most of the time tothe monsoon layer, and the Harmattan layer, which issituated above the latter, have been studied forsavanna as well as rain forest areas. These two layersare very different when considering the chemicalcomposition (especially for ozone and NO_z) andthe photochemical age.The relationship of photochemical ozone productionversus photochemical NO_x oxidation products hasbeen investigated. Results indicate an ozoneproduction efficiency (OPE) ranging from 6.3 to 14.8in the planetary boundary layer. Thus, this layer ischaracteristic of a photochemically young and activeair mass. In this layer, the ozone potentialproduction increases with the air mass photochemicalage. On the other hand, the Harmattan layer shows anOPE ranging from 4.6 to 7.4. These values arecharacteristic of photochemically well-aged airmasses. In this layer, the ozone potential productionseems to be exhausted with values around 4.0 (i.e., 4ozone molecules produced for each NO_x moleculeemitted).     

平流层臭氧对地表有机氯排放的多耦合响应

采用一个包含平流层化学、辐射、动力相互作用的二维模式,对地表有机氯排放变化影响平流层的具体过程作出评估,从而确定平流层臭氧对于地表有机氯排放的多耦合响应,也检验了“蒙特利尔议定书”的减排效果。结果表明,以议定书框架协议达成的20世纪90年代地表有机氯排放减少按30％计算,通过输送、扩散和一系列化学反应,导致平流层中上层的各活性化学族的浓度发生变化,稳定后平流层40km到48km经向平均的相对变化率,ClOx减少20％,HOx和NOx增加2％左右,O3恢复5％左右。此外,这些成分变化导致平流层中上层辐射加热率增加,平流层变冷趋势减缓0．6K。     

A Method for Retrieving Vertical Ozone Profiles from Limb Scattered Measurements

A two-step method is employed in this study to retrieve vertical ozone profiles using scattered measure- ments from the limb of the atmosphere. The combination of the Differential Optical Absorption Spectroscopy (DOAS) and the Multiplicative Algebraic Reconstruction Technique (MART) is proposed. First, the limb radiance, measured over a range of tangent heights, is processed using the DOAS technique to recover the effective column densities of atmospheric ozone. Second, these effective column densities along the lines of sight (LOSs) are inverted using the MART coupled with a forward model SCIATRAN (radiative transfer model for SCIAMACHY) to derive the ozone profiles. This method is applied to Optical Spectrograph and Infra Red Imager System (OSIRIS) radiance, using the wavelength windows 571-617 nm. Vertical ozone profiles between 10 and 48 km are derived with a vertical resolution of 1 km. The results illustrate a good agreement with the cloud-free coincident SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) ozone measurements, with deviations less than ± 10% ( ± 5% for altitudes from 17 to 47 km). Furthermore, sensitivities of retrieved ozone to aerosol, cloud parameters and NO 2 concentration are also investigated.     

SWIFT-DASH: Spatial Heterodyne Spectroscopy Approach to Stratospheric Wind and Ozone Measurement

Abstract

Passive wind measurements using Doppler shifts from atmospheric emissions were well demonstrated by the Wind Imaging Interferometer (WINDII) and the High Resolution Doppler Imager (HRDI) instruments on the National Aeronautics and Space Administration's (NASA's) Upper Atmosphere Research Satellite, operated from 1991 to 2005. For WINDII these emissions were from visible region upper atmospheric airglow in the altitude range from 80 to 300?km. Application of the same technique in the stratosphere requires using thermal emission from a minor constituent, and an ozone line near 1133?cm^?1 (about 8.8?μm) has been identified as a suitable target line. The WINDII method employed a Doppler Michelson Interferometer, in which the wind is measured from phase shifts of a single spectral line. Isolating a single ozone spectral line is a major challenge but using Spatial Heterodyne Spectroscopy (SHS) offers a way to resolve a number of interferogram spectral components (fringes) within a narrow spectral range. The instrument is a Michelson interferometer similar to WINDII but one in which the two mirrors are replaced by diffraction gratings. A developmental instrument capable of measuring the phase shifts from several ozone lines within a spectral range of 4?cm^?1 has been designed, built, and operated in the laboratory. Simulated retrievals using the measurement parameters of this instrument demonstrate the capability of wind measurement with an accuracy better than 3?m?s^?1 over an altitude range of 24 to 60?km. The retrieval employs four spectral lines for wind and three fringe frequencies for ozone concentration (of about 30 possible), each of which provides an optimal measurement for a particular altitude range. Ozone concentrations are also provided with an accuracy better than 10% from 20 to 50?km. Further detailed tests of this instrument are planned for the future. This work is supported by the Canadian Space Agency.     

地基与星载仪器观测大气臭氧总量分析

本文选取多个臭氧总量观测站点,采用"三重制约法"分别对下列3组仪器观测臭氧总量数据进行统计分析,解算出不同观测资料的误差标准差,进而对比研究各种仪器的精度特征:1)1996~2003年期间地基WOUDC(World Ozone and Ultraviolet Radiation Data Centre)观测网络仪器(包括Brewer、Dobson和Filter臭氧测量仪)与星载TOMS(Total Ozone Mapping Spectrometer)和GOME(The Global Ozone Monitoring Experiment)仪器;2)2004~2013年期间WOUDC与星载OMI(ozone monitoring instrument)和SCIAMACHY(scanning imaging absorption spectrometer for atmospheric chartography)仪器;3)2004~2013年期间地基SAOZ(Système D’Analyse par Observations Zénithales)与星载OMI和SCIAMACHY仪器。结果表明,1996~2003年期间TOMS V8和GOME观测精度相当,分别为7.6±2.8 DU/46(其中,7.6±2.8 DU为所分析站点观测资料的平均精度及其标准差,46为站点数目)和7.6±1.5 DU/46。TOMS V8观测精度优于TOMS V7(8.5±3.0 DU/46),验证了前者对后者有所改进。2004~2013年期间OMI和SCIAMACHY在WOUDC地基站点观测精度接近,分别为6.6±1.4 DU/21和6.0±1.6 DU/21。SAOZ地基仪器精度为8.4±3.6 DU/8。对于3类WOUDC地基仪器,Brewer站点观测资料的平均精度最优(7.9±3.3 DU/12),Dobson次之(8.7±2.3 DU/19),Filter最差(14.7±4.0 DU/15)。相比于卫星,3种地面仪器观测平均精度较差(10.5±4.3 DU/46),这主要是由于Filter精度较差引起。中国境内的瓦里关(Brewer)、香河(Dobson)和昆明(Dobson)3个地基站点仪器观测精度均较优,分别为7.8 DU、6.7 DU和6.6 DU。尽管不同站点之间存在一定差异,但整体来说,地基与卫星仪器在中国境内3个站点观测臭氧总量吻合较好。     

区域酸性沉降的数值研究：Ⅱ.个例模拟和试验

利用建立的区域酸性污染物沉降模式，配合中尺度模式ＭＭ４预报的气象场，以１９９１年６月１２￣１４日淮河流域的一次降雨过程作为实例，对我国东半部及其相邻地区的酸沉降进行了数值模拟和试验研究。结果表明，模式基本上能够模拟出区域酸性沉降的特征，具有良好的综合模拟性能和广阔的应用前景。     

Sensitivity Studies for Monitoring Tropospheric Ozone from Space Using the Ultraviolet,Visible,and Polarization Bands

The authors analyzed the retrieval sensitivity of tropospheric ozone using simulated the Global Ozone Monitoring Experiment-2 （GOME-2） measurements. The retrieval sensitivity was evaluated by the degree of free- dom for signal （DFS）. The combination of the ultraviolet （UV）, UV polarization （UVPOL）, and visible （VIS） bands enhances DFS of tropospheric ozone and improves the vertical resolution of the retrieved ozone profile. UVPOL reduces the dependence on solar zenith angle, mainly in- creases the sensitivity in upper troposphere. Polarization increased the DFS by 20% on the eastern side of the GOME-2 orbit, with little improvement on the western side because the increase in DFS due to polarization is depend- ent on the relative azimuth angle. The inclusion of the visi- ble band reduces significantly the dependence on viewing geometry, and mainly increases the DFS in the lower tro- posphere （0-6 kin） by a factor of two. It was possible to retrieve several independent pieces of tropospheric ozone information from GOME-2 UV/UVPOL/VIS measure- ments, especially in the lower troposphere.     

Anthropogenic Direct Radiative Forcing of Tropospheric Ozone and Aerosols from 1850 to 2000 Estimated with IPCC AR5 Emissions Inventories

This study estimates direct radiative forcing by tropospheric ozone and all aerosols between the years 1850 and 2000, using the new IPCC AR5 （the Intergovernmental Panel on Climate Change Fifth Assessment Report） emissions inventories and a fully coupled chemistry-aerosol general circulation model. As compared to the previous Global Emissions Inventory Activity （GEIA） data, that have been commonly used for forcing estimates since 1990, the IPCC AR5 emissions inventories report lower anthropogenic emissions of organic carbon and black carbon aerosols and higher sulfur and NOx emissions. The simulated global and annual mean burdens of sulfate, nitrate, black carbon （BC）, primary organic aerosol （POA）, secondary organic aerosol （SOA）, and ozone were 0.79, 0.35, 0.05, 0.49, 0.34, and 269 Tg, respectively, in the year 1850, and 1.90, 0.90, 0.11, 0.71, 0.32, and 377 Tg, respectively, in the year 2000. The estimated annual mean top of the atmosphere （TOA） direct radiative forcing of all anthropogenic aerosols based on the AR5 emissions inventories is -0.60 W m^-2 on a global mean basis from 1850 to 2000. However, this is -2.40 W m-2 when forcing values are averaged over eastern China （18-45°N and 95-125°E）. The value for tropospheric ozone is 0.17 W m^-1 on a global mean basis and 0.24 W m^-2 over eastern China. Forcing values indicate that the climatic effect of aerosols over eastern China is much more significant than the globally averaged effect.     

新冠肺炎疫情期间中国人为碳排放和大气污染物的变化

利用行业经济活动数据、1 580个地面监测站和6套卫星反演数据,分析了我国新冠肺炎疫情期间人为碳排放和主要大气污染物的变化。与2019年第一季度相比,2020年同期我国碳排放降低9.8%,其中交通部门降幅最大达到43.4%。与2019年2-3月相比,疫情期间全国地表臭氧浓度同比升高1.9 nL/L(5%),其中华北平原以降低为主,东南部地区以上升为主。PM2.5浓度同比下降12.6μg·m^-3(24.9%),其中长三角降幅最大。二氧化氮(NO2)的地面浓度和对流层柱浓度在京津冀、珠三角和长三角都降低20%~30%,体现了高低层的一致性。地面一氧化碳(CO)浓度同比降低17%,而对流层CO柱浓度升高2.5%,可能原因是境外生物质燃烧输送提升了我国南方高层大气的CO浓度。中东部地区气溶胶光学厚度显著降低,导致地表晴空短波辐射同比升高11.6 W·m^-2(9.6%)。     

Atmospheric Circulation Changes in Response to an Observed Stratospheric Zonal Ozone Anomaly

Abstract

In a sensitivity study, the influence of an observed stratospheric zonal ozone anomaly on the atmospheric circulation was investigated using the Fifth Generation European Centre Hamburg Model (ECHAM5) which is a general circulation model. The model was run from 1960 to 1999 (40 years) with a mean seasonal cycle of zonally symmetric ozone. In order to isolate the induced dynamical influence of the observed zonally asymmetric part of the three-dimensional stratospheric ozone, a second run was performed for the boreal extratropics using prescribed monthly means from the 40-year reanalysis dataset from the European Centre for Medium-range Weather Forecasts (ERA-40). The main findings are the interdecadal westward shift of the polar vortex at about 65°N and a significant increase in the number of stratospheric sudden warmings during the 1980–99 period. Under the action of zonally asymmetric ozone a decrease in the Arctic Oscillation was identified between the mid-1980s and the mid-1990s. The lag correlation between the mean Arctic Oscillation at the surface and the daily stratospheric northern annular mode increased in mid-winter. Furthermore, we examined the influence of the stratospheric zonal ozone anomaly on Rossby wave breaking in the upper troposphere and found a significant westward shift of poleward Rossby wave breaking events over western Europe in the winter. By this we show that the stratospheric zonal ozone anomaly has a strong influence on the tropospheric circulation as a result of enhanced dynamical coupling processes.     

南极春季臭氧的TOVS反演及其与BREWER观测的比较

通过改进臭氧的统计反演算法，从NOAA卫星的TOVS资料中提取了1993年南极臭氧洞期间中山站上空大气臭氧含量的资料。本文的结果与NOAA的TOVS臭氧产品以及中山站的Brewer观测进行了比较。尽管3种资料对在臭氧洞期间臭氧含量的显著减少这一特征上相当一致，但此项结果相对于Brewer观测，其均方根误差29 DU，优于NOAA的业务反演产品。此外，还初步讨论了这两种反演的误差特征。     

东亚地区陆地植被净初级生产力与夏季气候的模拟

利用中国科学院大气物理研究所(IAP)一个海洋-大气-动态植被耦合模式(GOALS-AVIM),进行了100年模拟积分.基于模拟结果,对东亚地区的植被净初级生产力(NPP)、降水、地面气温和短波辐射的季节变化进行了标准化对比,分析了NPP的时空格局与气候因子(气温、短波辐射和降水)的关系;利用奇异值分解(SVD)对东亚夏季降水场和NPP的关系进行分解.结果表明,夏季东亚地区植被NPP及相关气候因子的时空变化规律明显,耦合模式可以很好地模拟出观测存在的降水及NPP、LAI(叶面积指数)大值区随季节北移南退的形态;由于耦合模式中AVIM的双向特点,模式模拟的NPP与其他物理场的季节变化有很强的对应关系,而且在不同时间和地区,NPP与降水、地面气温、短波辐射表现出不同的对应关系,其中植被NPP时间变化与气温和降水的相关性都较高;从NPP场和降水场夏季逐月标准化距平奇异值分解的空间分布模态来看.NPP与降水在时空场上表现出很强的耦合性,NPP的空间格局与降水存在较好的相关性,不同地理位置的相关性强弱不同,分解出的降水场异常相关模态也再现了东亚夏季降水移动的时空特征,同时东亚雨带随季节变化与NPP的气候变率表现出不同的对应模态.     

应用查表法模拟区域对流层O3、Nox分布和演化的研究

应用STEM-II气相光化学模式探讨了影响对流层O3、NOx气相光化学转化率的各物理、化学因子。表明在我国多数地区光化学污染物特征(NMHC/NOx较高)下,光辐射强度、温度、初始O3浓度和NOx浓度是影响O3、NOx气相光化学转化率的主要因子。将以上因子分档组合,计算并建立了各种情况下O3、NOx气相光化学转化率的查算表,并将之用于模拟区域O3、NOx的演化和分布。结果表明,与光化学模式直接耦合计算法相比,该方法既能显著缩短计算时间,又能基本反映大气化学反应的非线性过程,并与直接耦合法符合得较好。     

香河地基观测臭氧柱总量数据分析及臭氧变化趋势研究

大气臭氧变化在全球气候和环境中具有重要作用,是当今大气科学领域的重要研究对象之一。对比分析了中国科学院大气物理研究所河北香河大气综合观测试验站2014～2016年Dobson和Brewer两种臭氧总量观测仪器探测结果的一致性,并使用1979～2016年Dobson观测数据分析了香河地区臭氧总量的长期变化趋势。结果表明:进行有效温度修正后,两种臭氧总量仪器观测结果一致性较好,平均偏差仅为-0.14DU(多布森单位),平均绝对偏差为8.00 DU,标准差为36.09 DU,相关系数达0.964。整体来说,两类仪器观测臭氧总量吻合较好。SO2浓度对Dobson仪器数据精度有一定影响,两组仪器数据在SO2浓度为0～0.2DU、0.2～0.4DU和0.4DU大气条件情况下的平均偏差分别为4.8 DU、7.0 DU和8.0 DU,平均偏差随SO2浓度升高而增大。过去38年香河地区的臭氧总量季节差异性强,春、冬两季臭氧总量高,夏、秋两季臭氧总量相对低,季节变化趋势差异明显。从长期变化上看,臭氧总量变化波动有不同的周期,在4个大的时间段变化趋势不同,2000～2010年臭氧层有显著恢复,但最近几年又有变薄的趋势。