近地面臭氧研究进展

近地面臭氧是空气中氮氧化物和挥发性有机物发生光化学反应的产物,其浓度与气象条件密切相关。晴天少云、紫外辐射较强、温度较高、相对湿度较低以及风速较小的天气,均有利于臭氧的生成,其中紫外辐射是产生臭氧最关键的因素。臭氧前体物（氮氧化物和挥发性有机物）的浓度及其比值是影响近地面臭氧浓度的另外三个重要因素。我国大多数城市的O3处于VOC控制区,即NOx浓度的增加会引起O3浓度的降低,而VOCs浓度的增加则会使其浓度升高。因而VOC源解析问题成为近年来O3研究的一个热点问题。同时,由于气溶胶可以直接吸收、散射太阳紫外辐射、短波辐射以及大气长波辐射,因此气溶胶的存在会影响大气中光化学反应的进程,从而影响臭氧的光化学生成,气溶胶对近地面臭氧的影响已成为目前大气环境的前沿课题。     

大气气溶胶变化对农业影响的研究进展

随着工业化和城市化的迅速发展,大气气溶胶含量和种类明显增加,它们通过直接吸收和反射太阳辐射以及改变其它辐射强迫因子(云、臭氧)的大小间接影响地气系统的能量收支,从而影响气候。气溶胶变化对气候的影响已有较多的研究,而对植被(农业)的影响是一个相对较新的研究领域,文章简要概述了大气气溶胶辐射强迫效应和大气气溶胶对农业的影响研究现状及国内外主要研究成果,并对气溶胶监测方法及模式评估方面可能存在的问题作了简单的分析。     

青藏高原东北侧臭氧垂直分布与平流层-对流层物质交换

利用臭氧和温度探空廓线,结合NCEP/NCAR资料、TOMS臭氧总量卫星观测资料和NOAAHYSPLIT后向轨迹模式资料,通过个例分析探讨了影响青藏高原(下称高原)附近臭氧垂直分布的因子和过程。结果表明,动力过程是影响高原上空臭氧垂直分布的主要因子,特别是中高纬度高臭氧浓度的空气向南入侵会导致高原上空臭氧浓度的升高,影响高原上空臭氧低谷的范围大小和形态;尽管大气化学过程对高原上空的平流层下层臭氧垂直分布的影响并不显著,但是高原上空的平流层臭氧变化与温度变化具有较好的一致性。同时还发现,对流层上层的强反气旋系统,特别是中高纬度阻塞高压的边缘有明显的平流层空气向对流层入侵,从而导致对流层内臭氧浓度的增加。     

臭氧变化的气候效应——一个回顾

一、引言臭氧-气候问题在近五年内已经引起学者们的广泛注意,其主要原因是人们揭示了这样的可能性:人类活动可以明显地改变现有的大气臭氧浓度。而且,如Ramanathan所总结的,一些研究已经指出:太阳活动可以引起中层大气(即25公里以上的气层)中的臭氧浓度发生较大变化。本文将讨论由于臭氧浓度的波动和变化所能造成对对流层-平流层气候的可能影响。对流层臭氧的变化可以直接通过改变原来的对流层辐射增温率而影响气候,另一方面,平流层中的臭氧变化通过平流层和对流层之间的辐射与动力耦合机制,影响对流层的气候。首先,我们定性阐述这些相关机制的特征;然后,给出臭氧含量变化的各种类型,最后,归纳出考虑了臭氧含量变化之气候效应的模式。     

青藏高原化雪迟早的辐射效应对季节变化的影响

利用大气物理所九层菱形截断１５波大气环流谱模式进行数值试验，研究青藏高原化雪迟早之辐射效应对季节变化的影响。共进行了正常态（ＣＯＮ），化雪迟（ＭＳＮ），化雪早（ＬＳＮ）三个试验。高原第ｉ月积雪状况在ＣＯＮ中取ｉ月气候平均值，在ＭＳＮ中取（ｉ—１）月的气候平均状况，在ＬＳＮ中则取（ｉ＋ｌ）月的气候状况。每个试验都从１月１日气候平均状况出发，积分至１０月。通过比较各试验结果分析化雪迟早的气候效应。结果表明，高原化雪的迟早改变了进入地表的辐射通量，从而改变了地表对大气的加热，由此影响东亚地区的季节变化。化雪迟则高原上春季进入地表的辐射通量减少，导致地表的潜热通量和向外长波辐射减弱。尤其是感热通量的减弱更为严重。一般情况下，高原在冬季为大气的感热汇，３月下旬变为大气的感热源。多雪时，这一变化推迟了近１个月。与之相应，２００ｈＰａ高原上空的南亚高压建立迟，印度西南季风爆发也迟。造成夏季风降水在印度偏少，在中印度半岛和广东沿海偏多。     

云的辐射特性

1.引言云对地球的辐射收支起着支配的作用.即云可以使入射到地球的太阳辐射反射到宇宙空间,减少地球接收的太阳辐射量(反射率效应),还可以通过吸收和射出地球(红外)辐射,使地表及云层下的大气保温(温室效应).云的辐射效应由这两种效应的平衡来决定.     

中国地区对流层臭氧变化和分布的数值研究

利用三维中尺度非静力模式ＭＭ５和化学模式,对１９９４年８月１６～１８日,１９９５年１月７～９日冬夏两个不同时期中国大陆大气对流层臭氧及其前体物质的分布进行了数值模拟。同时深入地分析了青藏高原地区夏季对流层臭氧的分布。模拟结果地面臭氧和ＮＯｘ的分布与观测结果基本一致,人类活动和光化过程是决定地面臭氧和ＮＯｘ的主要因子。对流层臭氧浓度的分布与气流的辐合辐散存在较好的对应关系,辐合区臭氧浓度较高,辐散区臭氧浓度较低。夏季,青藏高原中低空存在很强的辐合气流,使周边臭氧向高原辐合;而高原高空,受南亚高压控制存在很强的反气旋环流,臭氧由高原向周边辐散。冬季,受西风气流控制,臭氧分布表征大尺度特征。西风急流区臭氧浓度偏低,而急流两侧臭氧浓度偏高。     

重霾天气气溶胶辐射效应对近地面臭氧峰值的影响

重度灰霾(或重霾)条件下,大气气溶胶颗粒物显著衰减到达地表的太阳紫外辐射,对臭氧O3光化学过程形成产生重要影响。通过对2013年12月1-10日发生在长三角地区的一次重霾过程进行详尽分析,结合对流层紫外和可见光模型(TUV)及NCAR箱式模型(MM),探讨气溶胶辐射效应对地面臭氧形成和浓度峰值的影响。研究表明,区域输送、稳定边界层累积和二次气溶胶过程等是导致本次重霾发生的主要原因;重霾条件下,臭氧光化学反应明显减弱,臭氧日峰值明显降低,但光化学反应仍缓慢进行;受各种因素如区域输送、边界层累积效应及二次气溶胶等过程影响,臭氧浓度随细颗粒物PM10浓度升高而缓慢上升。TUV和MM模拟结果与观测吻合较好,模拟结果进一步显示,当气溶胶光学厚度AOD由0.8增加到2.0时,到达地表的紫外辐射衰减63%,地面臭氧峰值浓度降低近83%,表明随着灰霾污染加重,近地层臭氧浓度有所降低。     

青藏高原那曲夏季云中水成物分布特征的毫米波雷达观测

结合2014年7—8月第三次青藏高原大气科学试验获得的毫米波雷达资料与探空温度资料,利用模糊逻辑法反演了西藏那曲地区夏季云中水成物的相态并对其分布特征开展了研究。首先,分析了层积云、雨层云以及深对流云的典型个例,发现三类云反射率因子、多普勒速度、速度谱宽以及退偏振因子垂直分布均有较大差别,相应的云中水凝物的回波特征与相态分布差别也较大。其次,研究了液相、混合相和冰相云层的云雷达探测特征,发现液相云层在0℃层以下的暖云层和0℃层以上的过冷水云层均具有反射率因子高值中心,混合云层的反射率因子高值中心随高度上升变化不大,冰云层的反射率因子高值主要集中在6 km以上,且随高度上升而趋于集中;三种相态云层出现频率高值分别集中在地面以上1、2～3、3～4 km高度层;液相云层在上午出现频率最高,混合相云层高频率发生在下午,冰相云层在晚上的出现频率最高。三种相态云层出现在上午的高度与下午和晚上相比较低,出现在晚上的高度范围最大;液相云层厚度一般小于0.3 km,冰相云层云顶位于9 km左右高度层时平均厚度最大,中云内的混合相和冰相厚度变化较小。     

利用探空资料计算云层对辐射的影响

本文对两次江淮流域的梅雨天气过程作了辐射特征分析。着重考虑了云层对太阳辐射和大气长波辐射的影响。计算时假设云层随高度的分布由大气的湿度决定,方案考虑了大气中云层随高度的分布,所得结果能反映实际大气中各种云的辐射特征。     

NUMERICAL MODELING OF CUMULUS CLOUD CHEMISTRY—PART Ⅰ.MODEL DEVELOPMENT

A one-dimensional cumulus cloud chemistry model(1CCCM)is developed to simulate cloudphysical processes and chemical processes during the evolution of a convective cloud.The cloudphysical submodel includes a detailed microphysical parameterized scheme of 20 processes.Thechemistry submodel is composed of three parts:gas phase chemistry,aqueous phase chemistry andscavenging of soluble gases.The gas phase reaction mechanism contains 85 reactions among 45species including 13 organics.The aqueous phase reaction mechanism contains 54 reactions among40 species and 12 ion equilibria.Mass of 19 gases is transported between the gas phase and theaqueous phase.With this model,studies may be made to analyze the interactions among processesduring lifetime of a cumulus cloud.     

NUMERICAL MODELING OF CUMULUS CLOUD CHEMISTRY—PART Ⅰ.MODEL DEVELOPMENT*

A one-dimensional cumulus cloud chemistry model(ICCCM) is developed to simulate cloud physical processes and chemical processes during the evolution of a convective cloud.The cloud physical submodel includes a detailed microphysical parameterized scheme of 20 processes.The chemistry submodel is composed of three parts:gas phase chemistry,aqueous phase chemistry and scavenging of soluble gases.The gas phase reaction mechanism contains 85 reactions among 45 species including 13 organics.The aqueous phase reaction mechanism contains 54 reactions among 40 species and 12 ion equilibria.Mass of 19 gases is transported between the gas phase and the aqueous phase.With this model,studies may be made to analyze the interactions among processes during lifetime of a cumulus cloud.     

Tropospheric ozone chemistry. The impact of cloud chemistry

The effect of clouds and cloud chemistry on tropospheric ozone chemistry is tested out in a two-dimensional channel model covering a latitudinal band from 30 to 60° N. Three different methods describing how clouds affect gaseous species are applied, and the results are compared. The three methods are:

?A first order parameterization scheme for the removal of sulphur and other soluble gases by liquid droplets.

?A parameterization scheme for SO₂, O₃, and H₂O₂ removal is constructed. The scheme is based on the solubility of gases in liquid droplets, cycling times of air masses between clouds and cloud free areas and on the chemical interaction of SO₂ with H₂O₂ and O₃ in the liquid phase.

?Gas-aqueous-phase interactions and aqueous-phase chemical reactions are included in the reaction scheme for a number of components in areas where clouds are present.

In all three methods, a full gas-phase chemistry scheme is used. Particular emphasis is given to the study of how the ozone and hydrogen peroxide levels are affected. Significant changes in the distributions are found when aqueous-phase chemical reactions are included. The result is loss of ozone in the aqueous phase, with pronounced reductions in ozone levels in the middle and lower troposphere. Ozone levels are reduced by 10 to 30% with the largest reductions in the remote middle troposphere, bringing the values in better agreement with observations. Changes in H₂O₂ are harder to predict. Although, in one case study, hydrogen peroxide is produced within the aqueous phase, concentrations are mostly comparable or even lower than in the other cases. Hydrogen peroxide levels are, however, shown to be very pH sensitive. pH values around 5 seem to favour high H₂O₂ levels. High H₂O₂ concentrations may be found particularly in the upper part of the clouds under favourable conditions.     

Impact of cloud dynamics on tropospheric chemistry: Advances in modeling the interactions between microphysical and chemical processes

A chemical module describing the tropospheric photochemistry of ozone precursors in both gaseous and aqueous phases for a remote continental atmosphere has been developed within the framework of a two-dimensional cloud model. Dynamical, microphysical and chemical processes are fully interacting in order to study the influence of clouds on ozone chemistry and to quantify the relative importance of the different processes on the budget and evolution of 12 chemical species. Whereas the concentrations of highly soluble species are strongly affected by evaporation and sedimentation, less soluble species are affected primarily by accretion. The model reproduces previously observed chemical phenomena such as the enrichment of formic acid at the top of the cloud.     

强对流天气对O3和CO的垂直输送作用

利用ACTIVE（aerosol and chemical transport in tropical convection）试验资料,取2006年1月20日澳大利亚北部达尔文岛附近发生的一次飑线强对流天气的AE17航次和2006年1月27日无对流天气的AE21航次飞行路径中的探测资料,对澳大利亚达尔文地区夏季风盛行期间发生的有无强对流发生时O₃和CO浓度垂直分布变化进行对比,考察强对流性天气发生对O₃和CO浓度垂直输送作用。深对流云内强烈的垂直上升运动将O₃和CO等化学气体携带输送至对流层上部并在对流层顶堆积,从而在对流层上部产生浓度峰值。当有强对流发生,飞机进入对流云上层时,O₃浓度和CO浓度升高,O₃和CO浓度变率增大,在对流层上部浓度出现峰值;当飞机飞出对流云时,O₃和CO浓度相对较低,在对流云外出现谷值。在无对流发生的条件下O₃和CO浓度相对较小,浓度变率也较小,无峰值产生。分析表明:O₃和CO浓度分布不仅与强对流的垂直输送作用关系密切,且与气象要素垂直和水平分布以及动力输送过程密切相关。     

气溶胶核化清除的化学效应 I：云滴化学非均匀性的研究

本文将水汽在云滴上凝结增长的物理过程与气溶胶、气体的化学过程相结合，对气溶胶核化清除的化学效应进行了研究。 计算结果表明:气溶胶的核化清除造成了云滴化学成分随云滴大小分布的非均匀性，这种非均匀性又对云滴内发生的气体吸收、液相氧化产生影响。 本文还比较了不同污染状况下，不同大小的云滴内气溶胶核化清除与液相氧化对云滴化学的相对贡献的差异。 因此，这种云滴化学的非均匀性(云微化学)的研究对于云化学的野外观测及数值模拟都是重要的。     

Cloud model experiments of the effect of iron and copper on tropospheric ozone under marine and continental conditions

Summary We have used a multi-phase cloud photochemistry model to investigate the influence of dissolved iron (Fe) and copper (Cu) on the in-cloud production and loss of ozone and ozone-related species. Comparison of the results of our simulations with and without Fe and Cu reactions for three different photochemical scenarios (marine, averaged continental and polluted continental) indicate that Fe and Cu reactions, depending upon the scenario considered, can either increase or decrease the predicted rate of loss of ozone and ozone related species. For the marine and averaged continental scenarios the rate of loss of ozone in the aqueous-phase was decreased by as much as 45% and 70%, respectively, when Fe and Cu reactions were considered. For polluted continental conditions, the rate of loss of ozone in the aqueous phase increased with a factor 2 for low metal concentrations up to a factor 20 for high metal concentrations. In all three scenarios inclusion of the Fe and Cu reactions results in cloud droplets becoming more efficient sinks for gas-phase HO₂ and also enhances OH production. The net effect of the decreased losses of ozone from the aqueous phase and the effect of the cloud droplets on HO₂ and OH determine the overall impact on ozone and ozone related species, for each of the situations considered. Overall, when Fe and Cu reactions were included the marine cloud was found to be a less efficient sink for ozone, and averaged continental and polluted continental clouds were more efficient sinks for ozone (O₃ losses doubled in the averaged continental scenario). The higher OH flux in the aqueous phase also enhances the rate at which organic compounds, such as formaldehyde and formic acid, are oxidized in the cloud.With 4 Figures     

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.     

NUMERICAL SIMULATION OF ACIDIFICATION PROCESSES IN COLD CUMULUS CLOUDS

In this paper, a 1-D time dependent cold cumulus chemistry model is presented. In the coldcumulus model, 4 categories of hydrometeors: cloud drops, raindrops, cloud ice crystals, graupelparticles, and 18 microphysical interactions are considered, In the chemical model, the source andsink terms for pollutants include: the complicated interactions between pollutants (gases andaerosol particles) and the hydrometeors (especially ice crystals and graupel particles), the ex-changes of chemical compounds between two hydrometeors accompanying microphysical processesand the aqueous oxidations of S (IV) to S (VI). The two models are combined to study the acidifi-cation processes in cold cumulus clouds.     

欧拉型区域硫沉降模式研究

建立了一个三维硫沉降欧拉模式，模式中比较全面地考虑了硫沉降过程中的物理、化学机制。包括平流、扩散、干湿沉降和积云的垂直输送作用等物理过程，气相化学、液相化学和气溶胶表面的非均相化学等化学过程。其中非均相化学和积云的垂直输送参数化在国内外同类模式中尚不多见。模式结果与实测及其他模式结果的对比表明，该模式能够较好地模拟出SO2的水平和垂直分布及SO2-4在降水中的浓度。