Intercomparison of height assignment methods for opaque clouds over the tropics

Several methods of determining the height of opaque clouds over the tropics were compared using geostationary satellite measurements. The possible use of ozone channel measurements around the 9.7-μm ozone absorption band was examined in conjunction with the infrared window (IRW; 10.8 μm), H₂O (6.3 μm), and CO₂ (13.4 μm) channels, which are generally used for the assignment of cloud heights. Cloud top heights were retrieved from Meteosat-8 measurements with the aid of radiative transfer calculations using reanalysis data from the National Centers for Environmental Prediction/National Center for Atmospheric Research (NCEP/NCAR) as inputs. By using cloud top heights from collocated CloudSat observations as a reference, cloud top heights were determined from the one-channel radiance, two-channel brightness temperature difference (BTD), and two-channel radiance ratio methods, and the respective results were then compared for clouds with geometrical thicknesses of > 4 km. Overall, the retrievals from the CO₂-IRW ratio and O₃-CO₂ ratio methods are in substantial agreement with CloudSat observations, while the other methods either underestimate cloud top heights or demonstrate a lower ratio of successful height assignment. The O₃-CO₂ ratio method appears to be less practical than the CO₂-IRW ratio method because it requires two absorption channels. Our comparison also shows that the BTD between the ozone and IRW channels yields information that is similar to that of the IRW channel alone. It further shows that the O₃-IRW combination is not appropriate for the two-channel radiance ratio method. These results suggest that the inclusion of the ozone channel in BTD and ratio methods may not offer any significant improvement in convective cloud height retrieval over the tropics. In conclusion, the CO₂-IRW ratio method appears to provide the most accurate retrievals for opaque clouds.     

Exploration of the remote sounding of infrared cooling rates due to water vapor

Summary We explore the feasibility of deriving atmospheric infrared cooling rates by direct inversion of radiances observed by satellites from space. In order to convert radiances to fluxes and achieve vertical profiling at the same time, we show that it is necessary to combine radiances from narrow channels with radiances averaged over spectral bands. We demonstrate that the vertical integral of the cooling rate in the spectral band, convolved with a kernel function associated with the narrow channel, can be related to a weighted sum of the channel and band radiances. The band radiance must be evaluated at a specific zenith angle, which is a result of use of the mean value theorem. With known kernel functions, the combined radiances may be inverted to obtain the cooling rate profile. These results are derived from use of a random model for the transmittance in its strong-and weak-line limits. The results are similar in the two limits leading us to conclude that there are expressions that are approximately valid over the entire range of transmittance. We show by numerical methods that this conclusion is correct and apply the retrieval technique successfully to get the cooling rate profile in the rotational band of water vapor.With 3 Figures     

Stratospheric response to chemical perturbations

The paper presents a coupled chemical-radiative one-dimensional model which is used to assess the steady-state and time-dependent composition and temperature changes in relation to the release in the atmosphere of chemicals such as CO₂, N₂O, CH₄, NO _x and chlorofluorocarbons.The model indicates that a doubling in CO₂ leads to an increase in temperature of 12.7 K near the stratopause and to an increase in total ozone of 3.3% with a local enhancement of 17% at 40 km altitude. Additional release of N₂O leads to an ozone reduction in the middle stratosphere. The reduction in the ozone column is predicted to be equal to 8.8% when the amount of N₂O is doubled. The chemical effect of CH₄ on ozone is particularly important in the troposphere. A doubling in the mixing ratio of this gas enhances the O₃ concentration by 11% at 5 km. The predicted increase of the ozone column is equal to 1.4%. A constant emission of CFCl₃ (230 kT/yr) and CF₂Cl₂ (300 kT/yr) leads to a steady-state reduction in the ozone column of 1.9% compared to the present-day situation. The effect of some uncertainties in the chemical scheme as well as the impact of a high chlorine perturbation are briefly discussed.Finally the results of a time dependent calculation assuming a realistic scenario for the emission of chemical species are presented and analyzed.     

Development of the new CCC/GCM longwave radiation model for extension into the middle atmosphere

Abstract

A new infrared (IR) radiation scheme for extending the CCC/GCM (Canadian Climate Center General Circulation Model) into the middle atmosphere is proposed. It combines the previous CCC/GCM radiation scheme including the effects of H₂O, CO₂, O₃, CH₄, N₂O, CFC11 and CFC12, clouds and aerosols, with a new computationally efficient matrix parameterization for the cooling rate in the middle atmosphere for both LTE (local thermodynamic equilibrium) and non‐LTE layers. The matrix parameterization includes the effects of both the 15 μm CO₂ and the 9.6 μm O₃ bands and provides a proper lower boundary condition for the non‐LTE recurrence formula. The new scheme shows satisfactory agreement with line‐by‐line calculations. The absolute error does not exceed 0.8 ? day^‐1 for vastly different atmospheric conditions. Introducing the new radiation module into the CCC/GCM results in deviations of the simulated temperature from the CIRA‐1986 model of not more than 10 ? throughout most of the altitude‐latitude domain.     

Impact of increasing stratospheric water vapor on ozone depletion and temperature change

Using a detailed, fully coupled chemistry climate model (CCM), the effect of increasing stratospheric H_{2O on ozone and temperature is investigated. Different CCM time-slice runs have been performed to investigate the chemical and radiative impacts of an assumed 2 ppmv increase in H2O. The chemical effects of this H2O increase lead to an overall decrease of the total column ozone (TCO) by ～1% in the tropics and by a maximum of 12% at southern high latitudes. At northern high latitudes, the TCO is increased by only up to 5% due to stronger transport in the Arctic. A 2-ppmv H2O increase in the model's radiation scheme causes a cooling of the tropical stratosphere of no more than 2 K, but a cooling of more than 4 K at high latitudes. Consequently, the TCO is increased by about 2%--6%. Increasing stratospheric H2O, therefore, cools the stratosphere both directly and indirectly, except in the polar regions where the temperature responds differently due to feedbacks between ozone and H2O changes. The combined chemical and radiative effects of increasing H2O may give rise to more cooling in the tropics and middle latitudes but less cooling in the polar stratosphere. The combined effects of H2O increases on ozone tend to offset each other, except in the Arctic stratosphere where both the radiative and chemical impacts give rise to increased ozone. The chemical and radiative effects of increasing H2O cause dynamical responses in the stratosphere with an evident hemispheric asymmetry. In terms of ozone recovery, increasing the stratospheric H2O is likely to accelerate the recovery in the northern high latitudes and delay it in the southern high latitudes. The modeled ozone recovery is more significant between 2000--2050 than between 2050--2100, driven mainly by the larger relative change in chlorine in the earlier period.}     

Preliminary Retrieval of Aerosol Optical Depth from All-sky Images

The relationship between the radiance ratio (radiance at wavelength 450 nm to 650 nm) and aerosol optical depth (AOD) is analyzed in this paper by numerical simulation and a "LUT" (look-up table) approach is then presented for the retrieval of AOD from the radiance ratio. In this LUT approach, the AOD retrieval error depends mainly on the assumption of aerosol types. From the preliminary simulation, a typical error of 15%–20% in AOD obtained from the radiance ratio is estimated, due to neglecting changes in...     

污染源反演对重点城市群夏季O3模拟的改进效果评估

在嵌套网格空气质量预报模式系统(NAQPMS)的基础上,采用污染源反演方法优化以中国多尺度排放清单(MEIC)为主的先验排放清单中臭氧(O₃)前体物排放量估计。分析时段为2019年6～8月,重点评估了污染源反演对我国“2+26”城市、长三角、珠三角、成渝4个重点城市群O₃模拟的改进效果。评估结果表明,污染源反演获得的“2+26”城市、长三角、珠三角的氮氧化物(NO_x)排放速率整体低于先验清单的排放速率约0.6μg m_-2 s_-1,但反演的挥发性有机物(VOCs)排放速率在“2+26”城市整体上高于先验清单的排放速率约0.5μg m_-2 s_-1。利用反演的NO_x和VOCs排放量和NAQPMS模式对4个城市群O₃进行模拟,发现反演排放数据可以显著改进夏季O₃模拟性能,使得O₃日最大8小时平均值(MDA8-O₃)模拟的均方根误差(R...     

MEASUREMENTS AND MODEL SIMULATIONS OF SURFACE OZONE VARIATIONS AT DIFFERENT BACKGROUND CONCENTRATIONS OF THE PRECURSORS*

Ozone photochemical production and loss in very different environments at Waliguan baseline station and Lin'an background station were simulated by using the measurement data and photochemical box model.The results show that net ozone photochemical production rate is negative,about 0.5 ppb/d,at Waliguan baseline sation,because of very low precursor concentrations.But at Lin'an background station,the net photochemical ozone production is positive,about 2-3 ppb/h.which is very closed with the measurement at Lin'an.That means ozone production was controlled by photochemical reactions at Lin'an background station,because of the higher precursor concentrations.The net destruction rate,at Waliguan Mt.,is not large,so that future increase in anthropogenic emission of reactive nitrogen will lead to larger production rates of steady-state O₃ concentration.     

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.     

近红外CO2高光谱探测仪通道选择

近红外波段 (1.6 μm) 遥感可探测大气CO₂含量信息,应用于碳循环研究中。宽波段、高分辨率不但对仪器研制是一个挑战,而且巨大的数据量对观测的正演、反演也是一个挑战性课题。该文应用自由度及信息量分析法,对近红外高光谱波段中探测通道进行CO₂信息量分析,选择前20~100个高信息量的CO₂探测通道,并进行了反演模拟测试。结果表明:前20个高信息量通道占所有通道总信息量的76.4%,仅用所选的前20个通道进行反演,与所有通道参加反演的结果相比,误差增加0.3×10-6;通道数增至60时,信息量增加,通道数再增加,信息量则增加不显著;CO₂反演误差存在相似的关系。在高CO₂信息量分布上,弱吸收性质的1.6 μm波段和强吸收性质的2.06 μm波段表现出不同特点。     

北京地区严重大气污染的气象和化学因子

利用北京３２５ ｍ 气象塔进行了大气污染物臭氧、氮氧化物、一氧化碳和气象要素的同步观测, 对影响大气污染的气象和化学因子进行了分析,探讨大气污染物变化的规律, 为城市空气污染预报提供理论基础。     

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。     

NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript> change over China and its influences

A 3-D chemical transport model (OSLO CTM2) is used to investigate the impact of the increase of NOx emission over China. The model is capable to reproduce basically the seasonal variation of surface NOx and ozone over eastern China. NOx emission data and observations reveal that NOx over eastern China increases quite quickly with the economic development of China. Model results indicate that NOx concentration over eastern China increasingly rises with the increase of NOx emission over China, and accelerates to increase in winter. When the NOx emission increases from 1995 to its double, the ratio of NO2/NOx abruptly drops in winter over northern China. Ozone at the surface decreases in winter with the continual enhancement of the NOx level over eastern China, but increases over southern China in summertime. It is noticeable that peak ozone over northern China increases in summer although mean ozone changes little. In summer, ozone increases in the free troposphere dominantly below 500 hPa.Moreover, the increases of total ozone over eastern China are proportional to the increases of NOx emission.In a word, the model results suggest that the relationship between NOx and ozone at the surface would change with NOx increase.     

Fog detection using geostationary satellite data: Temporally continuous algorithm

A fog detection algorithm that uses geostationary satellite data has been developed and tested. This algorithm focuses on continuous fog detection since temporal discontinuities, especially at dawn and dusk, are a major problem with current fog detection algorithms that use satellite imagery data. This is because the spectral radiance at 3.7 μm contains overlapping emissive and reflectance components. In order to determine the radiance at 3.7 μm under fog conditions, radiative transfer model simulations were performed. The results showed that the radiance at 3.7 μm obviously varies with the solar zenith angle, and the brightness temperature differences between 3.7 μm and 10.8 μm are completely dissimilar between day and night (positive and varying with the angle during the daytime, but negative and constant at night). In this algorithm, a dynamic threshold is used as a function of the solar zenith angle. Moreover, additional criteria such as infrared, split-window channels, and a water vapor channel are used to remove high-level clouds. Also, the visible reflectance (0.67 μm) channel is used in the daytime algorithm because visible channel images are very practical for confirming a fog area with the high reflectivity and the smooth texture. The clear-sky visible reflectance for the previous 15 days was also employed to eliminate the surface effect that appeared during dawn and dusk. As the results, fog areas were estimated continuously, allowing the lifecycle of the fog system, from its development to decline, to appear obviously in the resulting images. Moreover, the estimated fog areas matched well with surface observations, except in a high latitude region that was covered by thin cirrus clouds.     

太原冬季PM2.5中有机碳和元素碳的变化特征

2005年12月—2006年2月在太原市区持续观测了气溶胶细粒子PM_2.5, 并应用Sunset碳分析仪进行了有机碳 (organic carbon, OC) 和元素碳 (elemental carbon, EC) 的测定。结果表明:太原冬季PM_2.5, OC和EC浓度均较高, 其中PM_2.5日平均浓度变化范围为25.4~419.0 μg/m3, 日平均浓度为193.4±102.3 μg/m3, OC平均浓度为28.9±14.8 μg/m3, EC平均浓度为4.8±2.2 μg/m3, OC/EC平均比值是7.0±3.9, 即太原市冬季PM_2.5和碳气溶胶污染严重。OC在PM _2.5中占18.6%, EC占2.9%, 这表明碳气溶胶是太原大气细粒子污染控制的关键组分。在太原市冬季, 采暖燃烧的煤是OC和EC的主要贡献源, 造成OC大大高于EC, 从而使OC/EC比值增大。各种气象条件对PM_2.5, OC, EC和OC/EC比值的变化都有不同程度的影响, 特别是大雾天气、相对湿度、风速和降雪是影响碳气溶胶浓度变化的重要因素。     

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。     

外来输送对江苏冬季PM2.5贡献的数值模拟研究

利用WRF-Chem模式对2016年12月中下旬的两次重污染过程进行模拟,定量研究外来污染输送对江苏省PM_2.5的污染贡献。15—17日和22—23日两次过程都存在明显的上游污染输送特征:宿迁、扬州、无锡(自西北向东南)的PM_2.5浓度先后出现峰值,峰值均出现在西北风场中,当风向转为偏北风时峰值逐渐减弱。第二次过程中地面风力更大,高空形势更有利于远距离输送,高值区范围强度明显强于第一次,重度污染层厚度达到900~1 500 m,且持续时间较长。第一次过程中江苏省内排放源贡献率为23%~79%(第二次为5%~32%),苏南仍以本地排放源污染为主,苏北外来输送贡献率超过50%。第二次过程中宿迁、扬州、无锡的PM_2.5外来输送贡献分别为105.9 μg/m3、83.1 μg/m3、64.8 μg/m3(第一次为40.2 μg/m3、20.9 μg/m3、11.1 μg/m3),山东省和京津冀地区排放源是主要污染输送来源,二者贡献之和在44%~70%。两次过程中,外来输送贡献均是自北向南递减,山东省贡献率高于京津冀地区,而其余周边省份的贡献率相对较低;安徽省对江苏西部城市的贡献率较高。      

Ozone and PAN Formation Inside and Outside of the Berlin Plume – Process Analysis and Numerical Process Simulation

During the BERLIOZ field phase on 20 July 1998 a 40 km wide ozone-plume 30 to 70 km north of Berlin in the lee of the city was detected. The ozone mixing ratio inside the plume was app. 15 ppb higher than outside, mainly caused by high ozone precursor emissions in Berlin, resulting in a net chemical ozone production of 6.5 ppb h^–1, which overcompensates ozone advection of –3.6 ppb h^–1 andturbulent diffusion of –1.1 ppb h^–1. That means, although moreozone leaves the control volume far in the lee of Berlin than enters it at the leeside cityborder and although turbulent diffusion causes a loss of ozone in the leeside control volume the chemical production inside the volume leads to a net ozone increase. Using a semi-Lagrangian mass budget method to estimate the net ozone production, 5.0 ppb h^–1 are calculated for theplume. This means a fraction of about 20% of ozone in the plume is producedby local emissions, therefore called `home made' by the Berlin emissions. For the same area KAMM/DRAIS simulations using an observation based initialisation, results in a net production rate between 4.0 and 6.5 ppbh^–1, while the threefold nested EURAD model gives 6.0 ppbh^–1. The process analysis indicates in many cases goodagreement (10% or better) between measurements and simulations not only in the ozone concentrations but also with respect to the physical and chemical processes governing the total change. Remaining differences are caused by different resolution in time and space of the models and measurements as well as by errors in the emission calculation.The upwind-downwind differences in PAN concentrations are partly similar to those of ozone, because in the BERLIOZ case they are governed mainly by photochemical production. While in the stable boundary layer at night and windward of Berlin 0.1 to 0.3 ppb are detected, in the centre of the plume at noon concentrations between 0.75 ppb and 1.0 ppb are measured. The O₃/PAN ratio is about 80 to 120 and thus due to the relatively lowPAN concentrations significantly higher than found in previous studies. The low PAN formation on 20 July, was mainly restricted by the moderate nonmethane hydrocarbon levels, whereas high PAN concentrations of 3.0 ppb on 21 July, are caused by local production in the boundary layer and by large scale advection aloft.     

Interannual and Decadal Changes in Tropospheric Ozone in China and the Associated Chemistry–Climate Interactions: A Review

China has been experiencing widespread air pollution due to rapid industrialization and urbanization in recent decades.The two major concerns of ambient air quality in China are particulate matter(PM) and tropospheric ozone(O_3). With the implementation of air pollution prevention and control actions in the last five years, the PM pollution in China has been substantially reduced. In contrast, under the conditions of the urban air pollution complex, the elevated O_3 levels in city clusters of eastern China, especially in warm seasons, have drawn increasing attention. Emissions of air pollutants and their precursors not only contribute to regional air quality, but also alter climate. Climate change in turn can change chemical processes, long-range transport, and local meteorology that influence air pollution. Compared to PM, less is known about O_3 pollution and its climate effects over China. Here, we present a review of the main findings from the literature over the period 2011–18 with regard to the characteristics of O_3 concentrations in China and the mechanisms that drive its interannual to decadal variations, aiming to identify robust conclusions that may guide decision-making for emissions control and to highlight critical knowledge gaps. We also review regional and global modeling studies that have investigated the impacts of tropospheric O_3 on climate, as well as the projections of future tropospheric O_3 owing to climate and/or emission changes.