Analysis on the impact of aerosol optical depth on surface solar radiation in the Shanghai megacity, China

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Xu J.; Li C.; Shi H.; et al. - Copernicus GmbH, 2011

This study investigated the decadal variation of the direct surface solar radiation (DiSR) and the diffuse surface solar radiation (DfSR) during 1961–2008 in the Shanghai megacity as well as their relationships to Aerosol Optical Depth (AOD) under clear-sky conditions. Three successive periods with unique features of long term variation of DiSR were identified for both clear-sky and all-sky conditions: a "dimming" period from the late 1960s to the mid 1980s, a "stabilization"/"slight brightening" period from the mid 1980s to the mid 1990s, and a "renewed dimming" period thereafter. During the ...

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Analysis on the impact of aerosol optical depth on surface solar radiation in the Shanghai megacity, China

  Available online: http://dx.doi.org/10.5194/acp-11-3281-2011

J. Xu ; C. Li ; H. Shi ; Q. He ; L. Pan

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3281-3289

This study investigated the decadal variation of the direct surface solar radiation (DiSR) and the diffuse surface solar radiation (DfSR) during 1961–2008 in the Shanghai megacity as well as their relationships to Aerosol Optical Depth (AOD) under clear-sky conditions. Three successive periods with unique features of long term variation of DiSR were identified for both clear-sky and all-sky conditions: a "dimming" period from the late 1960s to the mid 1980s, a "stabilization"/"slight brightening" period from the mid 1980s to the mid 1990s, and a "renewed dimming" period thereafter. During the two dimming periods of DiSR, DfSR brightened significantly under clear-sky conditions, indicating that change in atmospheric transparency resulting from aerosol emission has an important role on decadal variation of surface solar radiation (SSR) over this area. The analysis on the relationship between the Moderate-resolution Imaging Spectroradiometer (MODIS) retrieved AOD and the corresponding hourly measurements of DiSR and DfSR under clear-sky conditions clearly revealed that AOD is significantly correlated and anti-correlated with DfSR and DiSR, respectively, both above 99% confidence in all seasons, indicating the great impact of aerosols on SSR through absorption and/or scattering in the atmosphere. In addition, both AOD and the corresponding DiSR and DfSR measured during the satellite passage over Shanghai show obvious weekly cycles. On weekends, AOD is lower than the weekly average, corresponding to higher DiSR and lower DfSR, while the opposite pattern was true for weekdays. Less AOD on weekends due to the reduction of transportation and industrial activities results in enhancement of atmospheric transparency under cloud free conditions so as to increase DiSR and decrease DfSR simultaneously. Results show that aerosol loading from the anthropogenic emissions is an important modulator for the long term variation of SSR in Shanghai.

Language(s): English

Format: Digital (Free)

Tags: Aerosols ; Impact studies ; Urban zone ; Solar radiation ; Research ; China Add tag

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Impact of model grid spacing on regional- and urban- scale air quality predictions of organic aerosol

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Stroud C.A.; Makar P.A.; Moran M.D.; et al. - Copernicus GmbH, 2011

Regional-scale chemical transport model predictions of urban organic aerosol to date tend to be biased low relative to observations, a limitation with important implications for applying such models to human exposure health studies. We used a nested version of Environment Canada's AURAMS model (42- to- 15- to- 2.5-km nested grid spacing) to predict organic aerosol concentrations for a temporal and spatial domain corresponding to the Border Air Quality and Meteorology Study (BAQS-Met), an air-quality field study that took place in the southern Great Lakes region in the summer of 2007. The use o ...

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Impact of model grid spacing on regional- and urban- scale air quality predictions of organic aerosol

  Available online: http://dx.doi.org/10.5194/acp-11-3107-2011

C.A. Stroud ; P.A. Makar ; M.D. Moran ; W. Gong ; S. Gong ; J. Zhang ; K. Hayden ; C. Mihele ; J.R. Brook ; J.P.D. Abbatt ; J.G. Slowik

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3107-3118

Regional-scale chemical transport model predictions of urban organic aerosol to date tend to be biased low relative to observations, a limitation with important implications for applying such models to human exposure health studies. We used a nested version of Environment Canada's AURAMS model (42- to- 15- to- 2.5-km nested grid spacing) to predict organic aerosol concentrations for a temporal and spatial domain corresponding to the Border Air Quality and Meteorology Study (BAQS-Met), an air-quality field study that took place in the southern Great Lakes region in the summer of 2007. The use of three different horizontal grid spacings allowed the influence of this parameter to be examined. A domain-wide average for the 2.5-km domain and a matching 15-km subdomain yielded very similar organic aerosol averages (4.8 vs. 4.3 μg m−3, respectively). On regional scales, secondary organic aerosol dominated the organic aerosol composition and was adequately resolved by the 15-km model simulation. However, the shape of the organic aerosol concentration histogram for the Windsor urban station improved for the 2.5-km simulation relative to those from the 42- and 15-km simulations. The model histograms for the Bear Creek and Harrow rural stations were also improved in the high concentration "tail" region. As well the highest-resolution model results captured the midday 4 July organic-aerosol plume at Bear Creek with very good temporal correlation. These results suggest that accurate simulation of urban and large industrial plumes in the Great Lakes region requires the use of a high-resolution model in order to represent urban primary organic aerosol emissions, urban VOC emissions, and the secondary organic aerosol production rates properly. The positive feedback between the secondary organic aerosol production rate and existing organic mass concentration is also represented more accurately with the highest-resolution model. Not being able to capture these finer-scale features may partly explain the consistent negative bias reported in the literature when urban-scale organic aerosol evaluations are made using coarser-scale chemical transport models.

Language(s): English

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Tags: Aerosols ; Methodology ; Urban zone ; Weather forecasting ; Air quality ; Research Add tag

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Pseudo steady states of HONO measured in the nocturnal marine boundary layer: a conceptual model for HONO formation on aqueous surfaces

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Wojtal P.; Halla J.D.; McLaren R. - Copernicus GmbH, 2011

A complete understanding of the formation mechanism of nitrous acid (HONO) in the ambient atmosphere is complicated by a lack of understanding of processes occurring when aqueous water is present. We report nocturnal measurements of HONO, SO2 and NO2 by differential optical absorption spectroscopy over the ocean surface in a polluted marine environment. In this aqueous environment, we observed reproducible pseudo steady states (PSS) of HONO every night, that are fully formed shortly after sunset, much faster than seen in urban environments. During the PSS period, HONO is constant with time, in ...

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Pseudo steady states of HONO measured in the nocturnal marine boundary layer: a conceptual model for HONO formation on aqueous surfaces

  Available online: http://dx.doi.org/10.5194/acp-11-3243-2011

P. Wojtal ; J.D. Halla ; R. McLaren

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3243-3261

A complete understanding of the formation mechanism of nitrous acid (HONO) in the ambient atmosphere is complicated by a lack of understanding of processes occurring when aqueous water is present. We report nocturnal measurements of HONO, SO2 and NO2 by differential optical absorption spectroscopy over the ocean surface in a polluted marine environment. In this aqueous environment, we observed reproducible pseudo steady states (PSS) of HONO every night, that are fully formed shortly after sunset, much faster than seen in urban environments. During the PSS period, HONO is constant with time, independent of air mass source and independent of the concentration of NO2. The independence of HONO on the concentration of NO2 implies a 0° order formation process, likely on a saturated surface, with reversible partitioning of HONO to the gas phase, through vaporization and deposition to the surface. We observed median HONO/NO2 ratios starting at 0.13 at the beginning of the PSS period (with an apparent lower bound of 0.03), rising to median levels of ~0.30 at the end of the PSS period (with an upper bound >1.0). The implication of these numbers is that they suggest a common surface mechanism of HONO formation on terrestrial and aqueous surfaces, with an increase in the HONO/NO2 ratio with the amount of water available at the surface. The levels of HONO during the nocturnal PSS period are positively correlated with temperature, consistent with a partitioning of HONO from the surface to the gas phase with an apparent enthalpy of vaporization of ΔHSNL (HONO)=55.5±5.4 kJ mol−1. The formation mechanism on aqueous surfaces is independent of relative humidity (RH), despite observation of a negative HONO-RH correlation. A conceptual model for HONO formation on ambient aqueous surfaces is presented, with the main elements being the presence of a surface nanolayer (SNL), highly acidic and saturated with N(IV) precursors, production of HNO3, that diffuses to underlying water layers, and HONO, which partitions reversibly between the SNL and the gas phase. Implications of the conceptual model are discussed.

Language(s): English

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Tags: Ocean-atmosphere interaction ; Oceans ; Water pollution ; Research Add tag

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New particle formation events in semi-clean South African savannah

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Vakkari V.; Laakso H.; Kulmala M.; et al. - Copernicus GmbH, 2011

This study is based on 18 months (20 July 2006–5 February 2008) of continuous measurements of aerosol particle size distributions, air ion size distributions, trace gas concentrations and basic meteorology in a semi-clean savannah environment in Republic of South Africa. New particle formation and growth was observed on 69% of the days and bursts of non-growing ions/sub-10 nm particles on additional 14% of the days. This new particle formation frequency is the highest reported from boundary layer so far. Also the new particle formation and growth rates were among the highest reported in the li ...

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New particle formation events in semi-clean South African savannah

  Available online: http://dx.doi.org/10.5194/acp-11-3333-2011

V. Vakkari ; H. Laakso ; M. Kulmala ; A. Laaksonen ; D. Mabaso ; M. Molefe ; N. Kgabi ; L. Laakso

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3333-3346

This study is based on 18 months (20 July 2006–5 February 2008) of continuous measurements of aerosol particle size distributions, air ion size distributions, trace gas concentrations and basic meteorology in a semi-clean savannah environment in Republic of South Africa. New particle formation and growth was observed on 69% of the days and bursts of non-growing ions/sub-10 nm particles on additional 14% of the days. This new particle formation frequency is the highest reported from boundary layer so far. Also the new particle formation and growth rates were among the highest reported in the literature for continental boundary layer locations; median 10 nm formation rate was 2.2 cm−3 s−1 and median 10–30 nm growth rate 8.9 nm h−1. The median 2 nm ion formation rate was 0.5 cm−3 s−1 and the median ion growth rates were 6.2, 8.0 and 8.1 nm h−1 for size ranges 1.5–3 nm, 3–7 nm and 7–20 nm, respectively. The growth rates had a clear seasonal dependency with minimum during winter and maxima in spring and late summer. The relative contribution of estimated sulphuric acid to the growth rate was decreasing with increasing particle size and could explain more than 20% of the observed growth rate only for the 1.5–3 nm size range. Also the air mass history analysis indicated the highest formation and growth rates to be associated with the area of highest VOC (Volatile Organic Compounds) emissions following from biological activity rather than the highest estimated sulphuric acid concentrations. The frequency of new particle formation, however, increased nearly monotonously with the estimated sulphuric acid reaching 100% at H2SO4 concentration of 6 · 107 cm−3, which suggests the formation and growth to be independent of each other.

Language(s): English

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Tags: Aerosols ; Atmosphere ; Research ; Region I - Africa ; Sahara Add tag

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Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic Climate (ARCPAC) Project

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Brock C.A.; Cozic J.; Bahreini R.; et al. - Copernicus GmbH, 2011

We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea ...

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Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic Climate (ARCPAC) Project

  Available online: http://dx.doi.org/10.5194/acp-11-2423-2011

C.A. Brock ; J. Cozic ; R. Bahreini ; K.D. Froyd ; A.M. Middlebrook ; A. McComiskey ; J. Brioude ; O.R. Cooper ; A. Stohl ; K.C. Aikin ; J.A. de Gouw ; D.W. Fahey ; R.A. Ferrare ; R.-S. Gao ; W. Gore ; J.S. Holloway ; G. Hübler ; A. Jefferson ; D.A. Lack ; S. Lance ; R.H. Moore ; D.M. Murphy ; A. Nenes ; P.C. Novelli ; J.B. Nowak ; J.A. Ogren ; J. Peischl ; R.B. Pierce ; P. Pilewskie ; P.K. Quinn ; T.B. Ryerson ; K.S. Schmidt ; J.P. Schwarz ; H. Sodemann ; J.R. Spackman ; H. Stark ; D.S. Thomson ; T. Thornberry ; P. Veres ; L.A. Watts ; C. Warneke ; A.G. Wollny

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2423-2453

We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background) aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in southern Russia and southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion.
Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB) and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day−1 between 3 and 7 km and a slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO) in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of the BB particles between the time they were emitted and the time they were observed in dense layers above the sea-ice inversion layer.

Language(s): English

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Tags: Aerosols ; Atmospheric circulation ; Climate ; Impact studies ; Cloud formation ; Research ; Arctic Add tag

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Impact of deep convection and dehydration on bromine loading in the upper troposphere and lower stratosphere

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Aschmann J.; Sinnhuber B.-M.; Chipperfield M.P.; et al. - Copernicus GmbH, 2011

Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assumin ...

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Evaluating the effects of microphysical complexity in idealised simulations of trade wind cumulus using the Factorial Method

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Dearden C.; Connolly P.J.; Choularton T.W.; et al. - Copernicus GmbH, 2011

The effect of microphysical and environmental factors on the development of precipitation in warm idealised cloud is explored using a kinematic modelling framework. A simple one-dimensional column model is used to drive a suite of microphysics schemes including a flexible multi-moment bulk scheme (including both single and dual moment cloud liquid water) and a state-of-the-art bin-resolved scheme with explicit treatments of liquid and aerosol. The Factorial Method is employed to quantify and compare the sensitivities of each scheme under a set of controlled conditions, in order to isolate the ...

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Scale-by-scale analysis of probability distributions for global MODIS-AQUA cloud properties: how the large scale signature of turbulence may impact statistical analyses of clouds

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. de la Torre Juárez M.; Davis A.B.; Fetzer E.J. - Copernicus GmbH, 2011

Means, standard deviations, homogeneity parameters used in models based on their ratio, and the probability distribution functions (PDFs) of cloud properties from the MODerate resolution Infrared Spectrometer (MODIS) are estimated globally as function of averaging scale varying from 5 to 500 km. The properties – cloud fraction, droplet effective radius, and liquid water path – all matter for cloud-climate uncertainty quantification and reduction efforts. Global means and standard deviations are confirmed to change with scale. For the range of scales considered, global means vary only within 3% ...

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Evaluating a 3-D transport model of atmospheric CO2 using ground-based, aircraft, and space-borne data

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Feng L.; Palmer P.I.; Yang Y.; et al. - Copernicus GmbH, 2011

We evaluate the GEOS-Chem atmospheric transport model (v8-02-01) of CO2 over 2003–2006, driven by GEOS-4 and GEOS-5 meteorology from the NASA Goddard Global Modeling and Assimilation Office, using surface, aircraft and space-borne concentration measurements of CO2. We use an established ensemble Kalman Filter to estimate a posteriori biospheric+biomass burning (BS + BB) and oceanic (OC) CO2 fluxes from 22 geographical regions, following the TransCom-3 protocol, using boundary layer CO2 data from a subset of GLOBALVIEW surface sites. Global annual net BS + BB + OC CO2 fluxes over 2004–2006 for ...

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Sensitivity of mesoscale model urban boundary layer meteorology to the scale of urban representation

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Flagg D.D.; Taylor P.A. - Copernicus GmbH, 2011

Mesoscale modeling of the urban boundary layer requires careful parameterization of the surface due to its heterogeneous morphology. Model estimated meteorological quantities, including the surface energy budget and canopy layer variables, will respond accordingly to the scale of representation. This study examines the sensitivity of the surface energy balance, canopy layer and boundary layer meteorology to the scale of urban surface representation in a real urban area (Detroit-Windsor (USA-Canada)) during several dry, cloud-free summer periods. The model used is the Weather Research and Forec ...

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Characteristics of CALIOP attenuated backscatter noise: implication for cloud/aerosol detection

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Wu D.L.; Chae J.H.; Lambert A.; et al. - Copernicus GmbH, 2011

A research algorithm is developed for noise evaluation and feature detection of the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) Level 1 (L1) backscatter data with an emphasis on cloud/aerosol features in the upper troposphere and lower stratosphere (UT/LS). CALIOP measurement noise of the version v2.01 and v2.02 L1 backscatter data aggregated to (5 km) horizontal resolution is analyzed with two approaches in this study. One is to compare the observed and modeled molecular scatter profiles by scaling the modeled profile (with a fitted scaling factor α) to the observed clear-sky ba ...

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Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 2: Size-resolved aerosol chemical composition, diurnal cycles, and externally mixed weakly CCN-active soot particles

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Rose D.; Gunthe S.S.; Su H.; et al. - Copernicus GmbH, 2011

Size-resolved chemical composition, mixing state, and cloud condensation nucleus (CCN) activity of aerosol particles in polluted mega-city air and biomass burning smoke were measured during the PRIDE-PRD2006 campaign near Guangzhou, China, using an aerosol mass spectrometer (AMS), a volatility tandem differential mobility analyzer (VTDMA), and a continuous-flow CCN counter (DMT-CCNC).

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Long-term analysis of carbon dioxide and methane column-averaged mole fractions retrieved from SCIAMACHY

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Schneising O.; Buchwitz M.; Reuter M.; et al. - Copernicus GmbH, 2011

Carbon dioxide (CO2) and methane (CH4) are the two most important anthropogenic greenhouse gases contributing to global climate change. SCIAMACHY onboard ENVISAT (launch 2002) was the first and is now with TANSO onboard GOSAT (launch 2009) one of only two satellite instruments currently in space whose measurements are sensitive to CO2 and CH4 concentration changes in the lowest atmospheric layers where the variability due to sources and sinks is largest.

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Photochemical processing of organic aerosol at nearby continental sites: contrast between urban plumes and regional aerosol

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Slowik J.G.; Brook J.; Chang R.Y.-W.; et al. - Copernicus GmbH, 2011

As part of the BAQS-Met 2007 field campaign, Aerodyne time-of-flight aerosol mass spectrometers (ToF-AMS) were deployed at two sites in southwestern Ontario from 17 June to 11 July 2007. One instrument was located at Harrow, ON, a rural, agriculture-dominated area approximately 40 km southeast of the Detroit/Windsor/Windsor urban area and 5 km north of Lake Erie. The second instrument was located at Bear Creek, ON, a rural site approximately 70 km northeast of the Harrow site and 50 km east of Detroit/Windsor. Positive matrix factorization analysis of the combined organic mass spectral dataset ...

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Representation of tropical deep convection in atmospheric models – Part 1: Meteorology and comparison with satellite observations

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Russo M.R.; Marécal V.; Hoyle C.R.; et al. - Copernicus GmbH, 2011

Fast convective transport in the tropics can efficiently redistribute water vapour and pollutants up to the upper troposphere. In this study we compare tropical convection characteristics for the year 2005 in a range of atmospheric models, including numerical weather prediction (NWP) models, chemistry transport models (CTMs), and chemistry-climate models (CCMs). The model runs have been performed within the framework of the SCOUT-O3 (Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere) project. The characteristics of tropical convection, such as seasonal c ...

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