基于CMIP6强迫模拟分析人为气溶胶的气候效应(一)——介绍NUIST模式评估结果

为减少不同气候模式评估气溶胶气候效应的差异,第六次耦合模式比较计划(Coupled Model Intercomparison Project Phase 6,CMIP6)直接给定了人为气溶胶强迫数据。因此,有必要基于此强迫数据重新评估气溶胶气候效应。本研究首先将CMIP6给出的描述人为气溶胶强迫的模块引入南京信息工程大学(Nanjing University of Information Science and Technology,NUIST)的地球系统模式(The NUIST Earth System Model,NESM)。之后,利用NESM模式评估地球辐射收支平衡对此人为气溶胶强迫的响应,并分析模式模拟结果的不确定性。评估给出的人为气溶胶有效辐射强迫为-0. 45(±0. 28) W·m~(-2)。其中,气溶胶直接辐射效应为-0. 34(±0. 01) W·m~(-2),与第二次气溶胶比较计划(The second phase of Aerosol Comparisons between Observations and M odels,Aero ComⅡ)的评估结果基本一致;气溶胶对云辐射强迫的影响(包括半直接效应和间接效应)为-0. 10(±0. 30) W·m~(-2),明显受到模式内部变率的干扰,具有较大的不确定性。     

基于CMIP6强迫模拟分析人为气溶胶的气候效应(二)——诊断方法在分类评估中的重要性

对气溶胶气候效应开展分类评估并探讨诊断方法的合理性。人为气溶胶辐射效应对计算云辐射强迫的影响为0.38 W·m~(-2)。诊断评估气溶胶对云辐射强迫的影响需要排除这个偏差。两种基于不同试验设计诊断得出的半直接效应分别为0.21和0.09 W·m~(-2),存在显著差异。主要原因可能是人为气溶胶影响云辐射强迫的不同机制之间在模式模拟过程中不断地相互交织,不是简单的线性叠加关系。模式诊断得出的Twomey效应不仅包括Twomey效应本身,还包括Twomey效应引起的部分快速调整。总之,利用模式评估分析人为气溶胶气候效应需要注意审查试验设计和诊断方法的合理性。     

The atmospheric sulfur cycle in ECHAM-4 and its impact on the shortwave radiation

 The atmospheric general circulation model ECHAM-4 is coupled to a chemistry model to calculate sulfate mass distribution and the radiative forcing due to sulfate aerosol particles. The model simulates the main components of the hydrological cycle and, hence, it allows an explicit treatment of cloud transformation processes and precipitation scavenging. Two experiments are performed, one with pre-industrial and one with present-day sulfur emissions. In the pre-industrial emission scenario SO₂ is oxidized faster to sulfate and the in-cloud oxidation via the reaction with ozone is more important than in the present-day scenario. The atmospheric sulfate mass due to anthropogenic emissions is estimated as 0.38 Tg sulfur. The radiative forcing due to anthropogenic sulfate aerosols is calculated diagnostically. The backscattering of shortwave radiation (direct effect) as well as the impact of sulfate aerosols on the cloud albedo (indirect effect) is estimated. The model predicts a direct forcing of −0.35 W m^-2 and an indirect forcing of −0.76 W m^-2. Over the continents of the Northern Hemisphere the direct forcing amounts to −0.64 W m^-2. The geographical distribution of the direct and indirect effect is very different. Whereas the direct forcing is strongest over highly polluted continental regions, the indirect forcing over sea exceeds that over land. It is shown that forcing estimates based on monthly averages rather than on instantaneous sulfate pattern overestimate the indirect effect but have little effect on the direct forcing. Received: 16 October 1996/Accepted: 24 October 1996     

Clear-sky aerosol radiative forcing effects based on multi-site AERONET observations over Europe

Summary One of the great unknowns in climate research is the contribution of aerosols to climate forcing and climate perturbation. In this study, retrievals from AERONET are used to estimate the direct clear-sky aerosol top-of-atmosphere and surface radiative forcing effects for 12 multi-site observing stations in Europe. The radiative transfer code sdisort in the libRadtran environment is applied to accomplish these estimations. Most of the calculations in this study rely on observations which have been made for the years 1999, 2000, and 2001. Some stations do have observations dating back to the year of 1995. The calculations rely on a pre-compiled aerosol optical properties database for Europe. Aerosol radiative forcing effects are calculated with monthly mean aerosol optical properties retrievals and calculations are presented for three different surface albedo scenarios. Two of the surface albedo scenarios are generic by nature bare soil and green vegetation and the third relies on the ISCCP (International Satellite Cloud Climatology Project) data product. The ISCCP database has also been used to obtain clear-sky weighting fractions over AERONET stations. The AERONET stations cover the area 0° to 30° E and 42° to 52° N. AERONET retrievals are column integrated and this study does not make any seperation between the contribution of natural and anthropogenic components. For the 12 AERONET stations, median clear-sky top-of-atmosphere aerosol radiative forcing effect values for different surface albedo scenarios are calculated to be in the range of −4 to −2 W/m². High median radiative forcing effect values of about −6 W/m² were found to occur mainly in the summer months while lower values of about −1 W/m² occur in the winter months. The aerosol surface forcing also increases in summer months and can reach values of −8 W/m². Individual stations often have much higher values by a factor of 2. The median top-of-atmosphere aerosol radiative forcing effect efficiency is estimated to be about −25 W/m² and their respective surface efficiency is around −35 W/m². The fractional absorption coefficient is estimated to be 1.7, but deviates significantly from station to station. In addition, it is found that the well known peak of the aerosol radiative forcing effect at a solar zenith angle of about 75° is in fact the average of the peaks occurring at shorter and longer wavelengths. According to estimations for Central Europe, based on mean aerosol optical properties retrievals from 12 stations, the critical threshold of the aerosol single scattering albedo, between cooling and heating in the presence of an aerosol layer, is close between 0.6 and 0.76.     

A Review of Aerosol Optical Properties and Radiative Effects

Atmospheric aerosols influence the earth's radiative balance directly through scattering and absorbing solar radiation, and indirectly through affecting cloud properties. An understanding of aerosol optical properties is fundamental to studies of aerosol effects on climate. Although many such studies have been undertaken, large uncertainties in describing aerosol optical characteristics remain, especially regarding the absorption properties of different aerosols. Aerosol radiative effects are considered as either positive or negative perturbations to the radiation balance, and they include direct, indirect (albedo effect and cloud lifetime effect), and semi-direct effects. The total direct effect of anthropogenic aerosols is negative (cooling), although some components may contribute a positive effect (warming). Both the albedo effect and cloud lifetime effect cool the atmosphere by increasing cloud optical depth and cloud cover, respectively. Absorbing aerosols, such as carbonaceous aerosols and dust, exert a positive forcing at the top of atmosphere and a negative forcing at the surface, and they can directly warm the atmosphere. Internally mixed black carbon aerosols produce a stronger warming effect than externally mixed black carbon particles do. The semi-direct effect of absorbing aerosols could amplify this warming effect. Based on observational (ground-and satellite-based) and simulation studies, this paper reviews current progress in research regarding the optical properties and radiative effects of aerosols and also discusses several important issues to be addressed in future studies.     

黄土高原半干旱区典型日吸收性气溶胶综合观测分析

利用兰州大学半干旱气候与环境观测站的太阳光度计、激光雷达、微波辐射计综合观测资料,结合辐射传输模式分析了该地区秋季典型日2012年9月3~4日、21日和28日气溶胶物理特性、垂直分布特征,及其与气象条件的关系。研究时期的气溶胶主要为局地沙尘与人为污染混合气溶胶,吸收性明显,尺度较小。其中,4日西北风增强,远距离传输沙尘气溶胶,气溶胶光学厚度最大,粒子尺度明显增大。尝试利用灰色关联度法确定参考高度,分别为7.41 km、8.47 km、7.13 km和7.66 km,反演气溶胶消光系数,由此积分得到的光学厚度与太阳光度计观测值相关性可达0.975,反演效果较好。研究时期气溶胶的抬升主要受白天热力湍流作用,边界层发展,气溶胶向上传输,每日12时（当地时间,下同）至14时传输至最大高度,气溶胶抬升的高度对应大气加热率的高值区,低层加热率可达1 K d-1。气溶胶在大气层顶和地面造成负辐射强迫,分别为-12.707 W m-2、-25.398 W m-2,大气中表现为正辐射强迫,为12.692 W m-2,大气层顶的辐射强迫对气溶胶的物理特性最为敏感,当气溶胶吸收性明显时,大气层顶的瞬时辐射强迫会出现正值。     

Direct Radiative Forcing of Anthropogenic Aerosols over Oceans from Satellite Observations

Anthropogenic aerosols play an important role in the atmospheric energy balance. Anthropogenic aerosol optical depth (AOD) and its accompanying shortwave radiative forcing (RF) are usually simulated by nu- merical models. Recently, with the development of space-borne instruments and sophisticated retrieval algorithms, it has become possible to estimate aerosol radiative forcing based on satellite observations. In this study, we have estimated shortwave direct radiative forcing due to anthropogenic aerosols over oceans in all-sky conditions by combining clouds and the Single Scanner Footprint data of the Clouds and Earth’s Radiant Energy System (CERES/SSF) experiment, which provide measurements of upward shortwave fluxes at the top of atmosphere, with Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol and cloud products. We found that globally averaged aerosol radiative forcing over oceans in the clear-sky conditions and all-sky conditions were -1.03±0.48 W m-2 and -0.34 ±0.16 W m-2, respectively. Direct radiative forcing by anthropogenic aerosols shows large regional and seasonal variations. In some regions and in particular seasons, the magnitude of direct forcing by anthropogenic aerosols can be comparable to the forcing of greenhouse gases. However, it shows that aerosols caused the cooling effect, rather than warming effect from global scale, which is different from greenhouse gases.     

Effects of increasing surface reflectivity on aerosol,radiation, and cloud interactions in the urban atmosphere

The online Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is used to simulate the effects of albedo enhancement on aerosol, radiation, and cloud interactions in the Greater Montreal Area during the 2011 heat wave period. We used a 2-way nested approach to capture the full impacts of meteorological and photochemical reactions in the urban atmosphere. We conducted four sets of simulations with and without aerosol estimations and convective parameterizations to explore the aerosol interactions with radiation and cloud in the urban atmosphere. The direct, semi-direct, and indirect effects of aerosols are analyzed. The meteorological performance of the model indicates that the model slightly underpredicts air temperature, overpredicts wind speed, and underpredicts relative humidity. The chemical component of the model indicates that the model tends to underpredict fine particulate matters and overpredict ozone and nitrogen dioxide concentrations. The surface reflectivity of roofs, walls, and grounds is increased from 0.2 to 0.65, 0.60, and 0.45, respectively. Albedo enhancement led to a net decrease in radiative balance at solar noon by 25 W/m2, a decrease in daily air temperature by 0.5 °C, a reduction in water mixing ratio to 0.5 g/kg, and a decline in cloud coverage by 3% in the center part of the domain. Increasing urban albedo caused a decrease in planetary boundary layer height by 25 m. Albedo enhancement affords a decrease in temperature-sensitive photochemical reaction rates and thus reduces daily ozone concentrations by 3 ppb across the entire domain. The concentration of daily fine particulate matters decreased by 3 μg/m3 in the center part of the GMA during the 2011 heat wave period.     

Sensitivity Study of Anthropogenic Aerosol Indirect Forcing through Cirrus Clouds with CAM5 Using Three Ice Nucleation Parameterizations

Quantifying the radiative forcing due to aerosol–cloud interactions especially through cirrus clouds remains challenging because of our limited understanding of aerosol and cloud processes. In this study, we investigate the anthropogenic aerosol indirect forcing (AIF) through cirrus clouds using the Community Atmosphere Model version 5 (CAM5) with a state-of-the-art treatment of ice nucleation. We adopt a new approach to isolate anthropogenic AIF through cirrus clouds in which ice nucleation parameterization is driven by prescribed pre-industrial (PI) and presentday (PD) aerosols, respectively. Sensitivities of anthropogenic ice AIF (i.e., anthropogenic AIF through cirrus clouds) to different ice nucleation parameterizations, homogeneous freezing occurrence, and uncertainties in the cloud microphysics scheme are investigated. Results of sensitivity experiments show that the change (PD minus PI) in global annual mean longwave cloud forcing (i.e., longwave anthropogenic ice AIF) ranges from 0.14 to 0.35 W m^–2, the change in global annual mean shortwave cloud forcing (i.e., shortwave anthropogenic ice AIF) from–0.47 to–0.20 W m^–2, and the change in net cloud forcing from–0.12 to 0.05 W m^–2. Our results suggest that different ice nucleation parameterizations are an important factor for the large uncertainty of anthropogenic ice AIF. Furthermore, improved understanding of the spatial and temporal occurrence characteristics of homogeneous freezing events and the mean states of cirrus cloud properties are also important for constraining anthropogenic ice AIF.     

Impacts of Internally and Externally Mixed Anthropogenic Sulfate and Carbonaceous Aerosols on East Asian Climate

A coupled regional climate and aerosol-chemistry model, RIEMS 2.0 (Regional Integrated Environmental Model System for Asia), in which anthropogenic sulfate, black carbon, and organic carbon were assumed to be externally mixed (EM), internally mixed (IM) or partially internally mixed (IEM), was used to simulate the impacts of these anthropogenic aerosols on East Asian climate for the entire year of 2006. The distributions of aerosol mass concentration, radiative forcing and hence the surface air temperature and precipitation variations under three mixing assumptions of aerosols were analyzed. The results indicated that the mass concentration of sulfate was sensitive to mixing assumptions, but carbonaceous aerosols were much less sensitive to the mixing types. Modeled results were compared with observations in a variety of sites in East Asia. It was found that the simulated concentrations of sulfate and carbonaceous aerosols were in accord with the observations in terms of magnitude. The simulated aerosol concentrations in IM case were closest to observation results. The regional average column burdens of sulfate, black carbon, and organic carbon, if internally mixed, were 11.49, 0.47, and 2.17 mg m⁻², respectively. The radiative forcing of anthropogenic aerosols at the top of the atmosphere increased from −1.27 (EM) to −1.97 W m⁻² (IM) while the normalized radiative forcing (NRF) decreased from −0.145 (EM) to −0.139 W mg⁻¹ (IM). The radiative forcing and NRF were −1.82 W m⁻² and −0.141 W mg⁻¹ for IEM, respectively. The surface air temperature changes over the domain due to the anthropogenic sulfate and carbonaceous aerosols were −0.067, −0.078, and −0.072 K, with maxima of −0.47, −0.50, and −0.49 K, for EM, IM, and IEM, respectively. Meanwhile, the annual precipitation variations were −8.0 (EM), −20.6 (IM), and −21.9 mm (IEM), with maxima of 148, 122, and 102 mm, respectively, indicating that the climate effects were stronger if the sulfate and carbonaceous aerosols were internally mixed.     

On radiative forcing of sulphate aerosol produced from ion-promoted nucleation mechanisms in an atmospheric global model

A significant fraction of the total number of particles present in the atmosphere is formed by nucleation in the gas phase. Nucleation and the subsequent growth process influence both number concentration of particles and their size distribution besides chemical and optical properties of atmospheric aerosols. Sulphate aerosol nucleation mechanisms promoted by ions have been evaluated here in a tropospheric interactive chemistry-aerosol module for mass and number concentration in a global atmospheric model. The indirect radiative forcing of sulphate particles is assessed in this model; indirect radiative forcing is different for ion-induced (IIN) and ion-mediated (IMN) mechanisms. The indirect radiative forcing in 10-year simulation runs has been calculated as ?1.42?W/m² (IIN) and ?1.54?W/m² (IMN). The 5% emission of primary sulphate particles in simulations changes the indirect radiative forcing from ?1.42 to ?1.44?W/m² for IIN case, and from ?1.54 to ?1.55 W/m² for the IMN case. More precisely, owing to greater nucleation rates, IMN mechanisms produces greater cooling than the IIN mechanisms in the backdrop that both mechanisms produce almost identical distribution of CDNC in their pre-industrial runs. The inclusion of primary particles in simulations with IIN and IMN mechanisms increases both CDNC and the indirect radiative forcing.     

Assessment of the first indirect radiative effect of ammonium-sulfate-nitrate aerosols in East Asia

A physically based cloud nucleation parameterization was introduced into an optical properties/radiative transfer module incorporated with the off-line air quality modeling system Regional Atmospheric Modeling System (RAMS)-Models-3 Community Multi Scale Air Quality (CMAQ) to investigate the distribution features of the first indirect radiative effects of sulfate, nitrate, and ammonium-sulfate-nitrate (ASN) over East Asia for the years of 2005, 2010, and 2013. The relationship between aerosol particles and cloud droplet number concentration could be properly described by this parameterization because the simulated cloud fraction and cloud liquid water path were generally reliable compared with Moderate Resolution Imaging Spectroradiometer (MODIS) retrieved data. Simulation results showed that the strong effect of indirect forcing was mainly concentrated in Southeast China, the East China Sea, the Yellow Sea, and the Sea of Japan. The highest indirect radiative forcing of ASN reached ?3.47 W m^?2 over Southeast China and was obviously larger than the global mean of the indirect forcing of all anthropogenic aerosols. In addition, sulfate provided about half of the contribution to the ASN indirect forcing effect. However, the effect caused by nitrate was weak because the mass burden of nitrate was very low during summer, whereas the cloud fraction was the highest. The analysis indicated that even though the interannual variation of indirect forcing magnitude generally followed the trend of aerosol mass burden from 2005 to 2013, the cloud fraction was an important factor that determined the distribution pattern of indirect forcing. The heaviest aerosol loading in North China did not cause a strong radiative effect because of the low cloud fraction over this region.     

硫酸盐气溶胶辐射强迫的数值模拟研究

利用IAP/LASG GOALS 4.0海气耦合模式,"显式"考虑了硫酸盐气溶胶的直接作用,并且引入德国马普气象研究所的三维浓度分布资料,模拟计算了硫酸盐气溶胶的辐射强迫.主要结果为:全球气溶胶年平均的辐射强迫为-0.29 W m-2,在IPCC TAR给定的范围内,空间分布上具有明显的地域性,几个大值地区分别为东亚、西欧和北美,它们的中心值均超过-1.5 W m-2,南美、澳大利亚以及非洲南部的辐射强迫介于-0.2～-0.4 W m-2之间,而海洋和偏远的大陆地区,则基本上不受人为硫酸盐气溶胶的影响;计算的东亚地区硫酸盐气溶胶的平均辐射强迫为-0.75 W m-2,约为全球平均的2.5倍,为北半球平均的1.6倍.文中还讨论了全球硫酸盐气溶胶对温室气体辐射强迫的减缓作用.     

气溶胶辐射效应在华东地区一次雾霾过程中的作用

利用WRF/Chem(Weather Research and Forecasting Model coupled with Chemistry)模拟了2013年12月华东地区一次雾、霾事件气溶胶辐射反馈效应对气象场和大气质量的影响。通过3个不同气溶胶浓度设置的试验区分气溶胶浓度不同辐射效应的影响。比较不同试验得出,本次雾、霾过程中,不论是气溶胶直接、半直接辐射效应还是间接效应均使污染地区短波辐射减少、2 m气温下降、大气边界层高度降低,不利于水汽与污染物的扩散,空气污染进一步加重,雾结构进一步稳定,并使雾的持续时间延长,发展高度更高;对于化学场来说,气溶胶直接、半直接辐射效应使污染地区PM_(2.5)浓度增大、消光系数增大、氮氧化物浓度增大,臭氧浓度降低;间接辐射效应使PM_(2.5)浓度和消光系数进一步增大,氮氧化物、臭氧浓度降低。综上所述,气溶胶辐射效应能使大气污染加重,并利于雾的发生、发展。     

Investigation on semi-direct and indirect climate effects of fossil fuel black carbon aerosol over China

A Regional Climate Chemistry Modeling System that employed empirical parameterizations of aerosol-cloud microphysics was applied to investigate the spatial distribution, radiative forcing (RF), and climate effects of black carbon (BC) over China. Results showed high levels of BC in Southwest, Central, and East China, with maximum surface concentrations, column burden, and optical depth (AOD) up to 14 μg?m^?3, 8 mg?m^?2, and 0.11, respectively. Black carbon was found to result in a positive RF at the top of the atmosphere (TOA) due to its direct effect while a negative RF due to its indirect effect. The regional-averaged direct and indirect RF of BC in China was about +0.81 and ?0.95 W?m^?2, respectively, leading to a net RF of ?0.15 W?m^?2 at the TOA. The BC indirect RF was larger than its direct RF in South China. Due to BC absorption of solar radiation, cloudiness was decreased by 1.33 %, further resulting in an increase of solar radiation and subsequently a surface warming over most parts of China, which was opposite to BC’s indirect effect. Further, the net effect of BC might cause a decrease of precipitation of ?7.39 % over China. Investigations also suggested large uncertainties and non-linearity in BC’s indirect effect on regional climate. Results suggested that: (a) changes in cloud cover might be more affected by BC’s direct effect, while changes in surface air temperature and precipitation might be influenced by BC’s indirect effect; and (b) BC second indirect effect might have more influence on cloud cover and water content compared to first indirect effect. This study highlighted a substantial role of BC on regional climate changes.     

A Study of Shallow Cumulus Cloud Droplet Dispersion by Large Eddy Simulations

Cloud droplet dispersion is an important parameter in estimating aerosol indirect effect on climate in general circulation models (GCMs). This study investigates droplet dispersion in shallow cumulus clouds under different aerosol conditions using three-dimensional large eddy simulations (LES). It is found that cloud droplet mean radius, standard deviation, and relative dispersion generally decrease as aerosol mixing ratio increases from 25 mg⁻¹ (clean case) to 100 mg⁻¹ (moderate case), and to 2000 mg⁻¹ (polluted case). Under all the three simulated aerosol conditions, cloud droplet mean radius and standard deviation increase with height. However, droplet relative dispersion increases with height only in the polluted case, and does not vary with height in the clean and moderate cases.     

A numerical investigation of the impacts of anthropogenic sulfate aerosol on regional climate in East Asia

Aerosol and its effects, especially its indirect effects, on climate have drawn more and more attention in recent years. In this study, the first indirect radiative forcing (RF) of sulfate aerosol and its impacts on the regional climate in East Asia during the period from December 2008 to November 2009 were investigated. Affected by the general circulation and the conversion efficiency from SO₂ to SO₄ ^2? in aqueous phase, a remarkable seasonal variation of sulfate was found. The results show that the highest sulfate concentration as large as 24 g m^?2 appears in the summer. The indirect RF due to sulfate aerosol at the top of atmosphere (TOA) and the surface is negative, which leads to a cooling effect on the surface by 0.12°C and a reduction of precipitation by 0.01 mm d^?1. The tendencies of temperature and rainfall have significant diversity in space and time. The cloud feedback, associated with the hydrologic cycle and energy budget, is responsible for this discordant distribution. The variation of low cloud dominates the change of surface temperature. The subsidence due to the cooling effect in the mid atmosphere restrained and reduced the low clouds, leading to an apparent warm effect on the surface in Northeast Mongolia.     

Influence of atmospheric relative humidity on ultraviolet flux and aerosol direct radiative forcing: Observation and simulation

The atmospheric aerosols can absorb moisture from the environment due to their hydrophilicity and thus affect atmospheric radiation fluxes. In this article, the ultraviolet radiation and relative humidity (RH) data from ground observations and a radiative transfer model were used to examine the influence of RH on ultraviolet radiation flux and aerosol direct radiative forcing under the clear-sky conditions. The results show that RH has a significant influence on ultraviolet radiation because of aerosol hygroscopicity. The relationship between attenuation rate and RH can be fitted logarithmically and all of the R² of the 4 sets of samples are high, i.e. 0.87, 0.96, 0.9, and 0.9, respectively. When the RH is 60%, 70%, 80% and 90%, the mean aerosol direct radiative forcing in ultraviolet is ?4.22W m^?2, ?4.5W m^?2, ?4.82W m^?2 and ?5.4W m^?2, respectively. For the selected polluted air samples the growth factor for computing aerosol direct radiative forcing in the ultraviolet for the RH of 80% varies from 1.19 to 1.53, with an average of 1.31.     

Cloud radiative forcing of subtropical low level clouds in global models

Simulations of subtropical marine low clouds and their radiative properties by nine coupled ocean-atmosphere climate models participating in the fourth assesment report (AR4) of the intergovernmental panel on climate change (IPCC) are analyzed. Satellite observations of cloudiness and radiative fluxes at the top of the atmosphere (TOA) are utilized for comparison. The analysis is confined to the marine subtropics in an attempt to isolate low cloudiness from tropical convective systems. All analyzed models have a negative bias in the low cloud fraction (model mean bias of −15%). On the other hand, the models show an excess of cloud radiative cooling in the region (model mean excess of 13 W m⁻²). The latter bias is shown to mainly originate from too much shortwave reflection by the models clouds rather than biases in the clear-sky fluxes. These results confirm earlier studies, thus no major progress in simulating the marine subtropical clouds is noted. As a consequence of the combination of these two biases, this study suggests that all investigated models are likely to overestimate the radiative response to changes in low level subtropical cloudiness.     

Climate forcing by carbonaceous and sulfate aerosols

 An atmospheric general circulation model is coupled to an atmospheric chemistry model to calculate the radiative forcing by anthropogenic sulfate and carbonaceous aerosols. The latter aerosols result from biomass burning as well as fossil fuel burning. The black carbon associated with carbonaceous aerosols is absorbant and can decrease the amount of reflected radiation at the top-of-the-atmosphere. In contrast, sulfate aerosols are reflectant and the amount of reflected radiation depends nonlinearly on the relative humidity. We examine the importance of treating the range of optical properties associated with sulfate aerosol at high relative humidities and find that the direct forcing by anthropogenic sulfate aerosols can decrease from −0.81 W m^-2 to −0.55 Wm^-2 if grid box average relative humidity is not allowed to increase above 90%. The climate forcing associated with fossil fuel emissions of carbonaceous aerosols is calculated to range from +0.16 to +0.20 Wm^-2, depending on how much organic carbon is associated with the black carbon from fossil fuel burning. The direct forcing of carbonaceous aerosols associated with biomass burning is calculated to range from −0.23 to −0.16 Wm^-2. The pattern of forcing by carbonaceous aerosols depends on both the surface albedo and the presence of clouds. Multiple scattering associated with clouds and high surface albedos can change the forcing from negative to positive. Received: 29 September 1997 / Accepted: 10 June 1998