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1.
Climate forcing by carbonaceous and sulfate aerosols 总被引：3，自引：0，他引：3
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 相似文献
2.
Impacts of Internally and Externally Mixed Anthropogenic Sulfate and Carbonaceous Aerosols on East Asian Climate 总被引：1，自引：0，他引：1 
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下载免费PDF全文 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. 相似文献
3.
Suresh Tiwari Atul K. Srivastava Deewan S. Bisht Tarannum Bano Sachchidanand Singh Sudhamayee Behura Manoj K. Srivastava D. M. Chate B. Padmanabhamurty 《Journal of Atmospheric Chemistry》2009,62(3):193-209
The concentrations of PM10, PM2.5 and their water-soluble ionic species were determined for the samples collected during January to December, 2007 at New Delhi
(28.63° N, 77.18° E), India. The annual mean PM10 and PM2.5 concentrations (± standard deviation) were about 219 (± 84) and 97 (±56) μgm−3 respectively, about twice the prescribed Indian National Ambient Air Quality Standards values. The monthly average ratio
of PM2.5/PM10 varied between 0.18 (June) and 0.86 (February) with an annual mean of ∼0.48 (±0.2), suggesting the dominance of coarser in
summer and fine size particles in winter. The difference between the concentrations of PM10 and PM2.5, is deemed as the contribution of the coarse fraction (PM10−2.5). The analyzed coarse fractions mainly composed of secondary inorganic aerosols species (16.0 μgm−3, 13.07%), mineral matter (12.32 μgm−3, 10.06%) and salt particles (4.92 μgm−3, 4.02%). PM2.5 are mainly made up of undetermined fractions (39.46 μgm−3, 40.9%), secondary inorganic aerosols (26.15 μgm−3, 27.1%), salt aerosols (22.48 μgm−3, 23.3%) and mineral matter (8.41 μgm−3, 8.7%). The black carbon aerosols concentrations measured at a nearby (∼300 m) location to aerosol sampling site, registered
an annual mean of ∼14 (±12) μgm−3, which is significantly large compared to those observed at other locations in India. The source identifications are made
for the ionic species in PM10 and PM2.5. The results are discussed by way of correlations and factor analyses. The significant correlations of Cl−, SO42−, K+, Na+, Ca2+, NO3− and Mg2+ with PM2.5 on one hand and Mg2+ with PM10 on the other suggest the dominance of anthropogenic and soil origin aerosols in Delhi. 相似文献
4.
Umesh C. Kulshrestha Ramya Sunder Raman Monika J. Kulshrestha T. N. Rao Partha J. Hazarika 《Journal of Atmospheric Chemistry》2009,63(1):33-47
Secondary aerosol formation was studied at Allahabad in the Indo-Gangetic region during a field campaign called Land Campaign-II
in December 2004 (northern winter). Regional source locations of the ionic species in PM10 were identified by using Potential Source Contribution Function (PSCF analysis). On an average, the concentration of water
soluble inorganic ions (sum of anions and cations) was 63.2 μgm−3. Amongst the water soluble ions, average NO3− concentration was the highest (25.0 μgm−3) followed by SO42− (15.8 μgm−3) and NH4+ (13.8 μgm−3) concentrations. These species, contributed 87% of the total mass of water soluble species, indicating that most of the water
soluble PM10 was composed of NH4NO3 and (NH4)2SO4/NH4HSO4 or (NH4)3H(SO4)2 particles. Further, the concentrations of SO42−, NO3−, and NH4+ aerosols increased at high relative humidity levels up to the deliquescence point (∼63% RH) for salts of these species suggesting
that high humidity levels favor the conversion and partitioning of gaseous SO2, NOx, and NH3 to their aerosol phase. Additionally, lowering of ambient temperature as the winter progressed also resulted in an increase
of NO3− and NH4+ concentrations, probably due to the semi volatile nature of ammonium nitrate. PSCF analysis identified regions along the
Indo-Gangetic Plain (IGP) including Northern and Central Uttar Pradesh, Punjab, Haryana, Northern Pakistan, and parts of Rajasthan
as source regions of airborne nitrate. Similar source regions, along with Northeastern Madhya Pradesh were identified for
sulfate. 相似文献
5.
Man-Ting Cheng Wei-Chun Chou Chia-Pin Chio Shih-Chieh Hsu Yi-Ru Su Pei-Hsuan Kuo Ben-Jei Tsuang Shuen-Hsin Lin Charles C.-K. Chou 《Journal of Atmospheric Chemistry》2008,61(2):155-173
A study has been carried out on water soluble ions, trace elements, as well as PM2.5 and PM2.5–10 elemental and organic carbon samples collected daily from Central Taiwan over a one year period in 2005. A source apportionment
study was performed, employing a Gaussian trajectory transfer coefficient model (GTx) to the results from 141 sets of PM2.5 and PM2.5–10 samples. Two different types of PM10 episodes, local pollution (LOP) and Asian dust storm (ADS) were observed in this study. The results revealed that relative
high concentrations of secondary aerosols (NO3−, SO42− and NH4+) and the elements Cu, Zn, Cd, Pb and As were observed in PM2.5 during LOP periods. However, sea salt species (Na+ and Cl−) and crustal elements (e.g., Al, Fe, Mg, K, Ca and Ti) of PM2.5–10 showed a sharp increase during ADS periods. Anthropogenic source metals, Cu, Zn, Cd, Pb and As, as well as coarse nitrate
also increased with ADS episodes. Moreover, reconstruction of aerosol compositions revealed that soil of PM2.5–10 elevated approximately 12–14% in ADS periods than LOP and Clear periods. A significantly high ratio of non-sea salt sulfate
to elemental carbon (NSS-SO42−/EC) of PM2.5–10 during ADS periods was associated with higher concentrations of non-sea-salt sulfates from the industrial regions of China.
Source apportionment analysis showed that 39% of PM10, 25% of PM2.5, 50% of PM2.5–10, 42% of sulfate and 30% of nitrate were attributable to the long range transport during ADS periods, respectively. 相似文献
6.
In this study, a regional air quality model system (RAQMS) was
applied to investigate the spatial distributions and seasonal variations of
atmospheric aerosols in 2006 over East Asia. Model validations demonstrated
that RAQMS was able to reproduce the evolution processes of aerosol components
reasonably well. Ground-level PM10 (particles with aerodynamic diameter
≤10 μm) concentrations were highest in spring and lowest in
summer and were characterized by three maximum centers: the Taklimakan Desert
(～1000 μg m-3), the Gobi Desert (～400 μg m-3), and
the Huabei Plain (～300 μm-3) of China. Vertically, high
PM10 concentrations ranging from 100 μg m-3 to 250 μg
m-3 occurred from the surface to an altitude of 6000 m at
30o--45oN in spring. In winter, the vertical gradient was so
large that most aerosols were restricted in the boundary layer. Both sulfate
and ammonium reached their highest concentrations in autumn, while nitrate
reached its maximum level in winter. Black carbon and organic carbon aerosol
concentrations reached maximums in winter. Soil dust were strongest in spring,
whereas sea salt exerted the strongest influence on the coastal regions of
eastern China in summer. The estimated burden of anthropogenic aerosols was
largest in winter (1621 Gg) and smallest in summer (1040 Gg). The sulfate
burden accounted for ～42% of the total anthropogenic aerosol burden. The
dust burden was about twice the anthropogenic aerosol burden, implying the
potentially important impacts of the natural aerosols on air quality and
climate over East Asia. 相似文献
7.
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 相似文献
8.
黄土高原半干旱区典型日吸收性气溶胶综合观测分析 总被引：2，自引：0，他引：2
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。 相似文献
9.
P. D. Safai S. Kewat G. Pandithurai P. S. Praveen K. Ali S. Tiwari P. S. P. Rao K. B. Budhawant S. K. Saha P. C. S. Devara 《Journal of Atmospheric Chemistry》2008,61(2):101-118
Simultaneous measurements on physical, chemical and optical properties of aerosols over a tropical semi-arid location, Agra
in north India, were undertaken during December 2004. The average concentration of total suspended particulates (TSP) increased
by about 1.4 times during intense foggy/hazy days. Concentrations of SO4
2−, NO3
−, NH4
+ and Black Carbon (BC) aerosols increased by 4, 2, 3.5 and 1.7 times, respectively during that period. Aerosols were acidic
during intense foggy/hazy days but the fog water showed alkaline nature, mainly due to the neutralizing capacity of NH4 aerosols. Trajectory analyses showed that air masses were predominantly from NW direction, which might be responsible for
transport of BC from distant and surrounding local sources. Diurnal variation of BC on all days showed a morning and an evening
peak that were related to domestic cooking and vehicular emissions, apart from boundary layer changes. OPAC (Optical properties
of aerosols and clouds) model was used to compute the optical properties of aerosols. Both OPAC-derived and observed aerosol
optical depth (AOD) values showed spectral variation with high loadings in the short wavelengths (<1 μm). AOD value at 0.5 μm
wavelength was significantly high during intense foggy/hazy days (1.22) than during clear sky or less foggy/hazy days (0.63).
OPAC-derived Single scattering albedo (SSA) was 0.84 during the observational period, indicating significant contribution
of absorbing aerosols. However, the BC mass fraction to TSP increased by only 1% during intense foggy/hazy days and thereby
did not show any impact on SSA during that period. A large increase was observed in the shortwave (SW) atmospheric (ATM) forcing
during intense foggy/hazy days (+75.8 W/m2) than that during clear sky or less foggy/hazy days (+38 W/m2), mainly due to increase in absorbing aerosols. Whereas SW forcing at surface (SUF) increased from −40 W/m2 during clear sky or less foggy/hazy days to −76 W/m2 during intense foggy/hazy days, mainly due to the scattering aerosols like SO4
2-. 相似文献
10.
Cloud/fog water samples were collected at Daekwanreung (840 m msl), a ridge site, in South Korea, from March 2002 to September 2003, by using a Caltech type, self fabricated active strand cloud water collector. The pH, electrical conductivity and major ion concentrations were analyzed. The cloud water pH ranged from 3.6 to 6.8 with an average of 5.2, which was close to the atmospheric neutral point. However, the pH calculated from average concentrations of H+ was 4.7, indicating the cloud/fog water was weakly acidified. SO4
2−, NO3
− and NH4
+ are predominant ions of which average concentrations were 203.1, 128.1, and 211.7 μeq⋅L−1, respectively. Samples were categorized into four groups by applying 48-hour back trajectory analysis, using the HYbrid Single-Particle Largrangian Integrated Trajectory (HYSPLIT) model. Chemical compositions for the four cases significantly differed from each other. For air masses transported from the East Sea (group E), sea salt concentrations, including Na+, Cl− Mg2+, were relatively high. Principal acidifying pollutants, such as NO3
− and nss-SO4
2−, significantly increased in the case of air masses transported from the Northeast Asian continent through North Korea (group N) and air masses from the Seoul metropolitan area (group W). However, the mean pH of group N was the highest while the mean pH of group W was the lowest. This suggests that most NO3
− and nss-SO4
2− in cloud/fog water was neutralized by ammonia and calcium compounds under the influence of air masses transported from Northeast Asia. N/S ratio for the group W was significantly higher than those for the other three groups, suggesting nitrogen species transported from the Seoul metropolitan area contributed to acidification of cloud/fog water at Daekwanreung. Principle Component analysis (PCA) was applied to the cloud/fog water data for presenting characteristics in the four different categories. 相似文献