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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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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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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

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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

Format: Digital (Free)

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

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Saharan and Asian dust: similarities and differences determined by CALIPSO, AERONET, and a coupled climate-aerosol microphysical model

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Su L.; Toon O.B. - Copernicus GmbH, 2011

This study compares the properties of atmospheric dust from the Saharan deserts and the Asian deserts using data from CALIPSO and AERONET during 2006 and 2007 along with simulations using a coupled climate-microphysical sectional model. Saharan deserts are largely south of 30° N, while Asian ones are primarily north of 30° N, hence they experience different meteorological regimes. Saharan dust lifting occurs all year long, primarily due to subtropical weather systems. However, Asian dust is lifted mostly in spring when mid-latitude frontal systems lead to high winds. Rainfall is more abundant ...

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Saharan and Asian dust: similarities and differences determined by CALIPSO, AERONET, and a coupled climate-aerosol microphysical model

  Available online: http://dx.doi.org/10.5194/acp-11-3263-2011

L. Su ; O.B. Toon

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3263-3280

This study compares the properties of atmospheric dust from the Saharan deserts and the Asian deserts using data from CALIPSO and AERONET during 2006 and 2007 along with simulations using a coupled climate-microphysical sectional model. Saharan deserts are largely south of 30° N, while Asian ones are primarily north of 30° N, hence they experience different meteorological regimes. Saharan dust lifting occurs all year long, primarily due to subtropical weather systems. However, Asian dust is lifted mostly in spring when mid-latitude frontal systems lead to high winds. Rainfall is more abundant over Asia during the dust lifting events, leading to greater local dust removal than over the Sahara. However, most dust removal is due to sedimentation. Despite the different meteorological regimes, the same dust lifting schemes work in models for Asian and Saharan dust. The magnitudes of dust lifted in Africa and Asia differ significantly over the year. In our model the yearly horizontal dust flux just downwind of the African dust source is about 1088 Tg (10° S–40° N, 10° W) and from the Asian dust source it is about 355 Tg (25° N–55° N, 105° E) in 2007, which is comparable to previous studies. We find the difference in dust flux is mainly due to the larger area over which dust is lifted in Africa than Asia. However, Africa also has stronger winds in some seasons. Once lifted, the Saharan dust layers generally move toward the west and descend in altitude from about 7 km to the surface over several days in the cases studied. Asian dust often has multiple layers (two layers in the cases studied) during transport largely to the east. One layer stays well above boundary layer during transport and shows little descent, while the other, lower, layer descends with time. This observation contrasts with studies suggesting the descent of Saharan dust is due to sedimentation of the particles, and suggests instead it is dominated by meteorology. We find the size distributions of Asian and African dust are similar when the dust is lifted, but the mode size can differ and secondary size modes can develop probably due to differences in vertical wind velocities during transport. The single scattering albedo of African and Asian dust does differ, due primarily to the imaginary parts of the refractive indexes being different, which in turn is likely due to different dust composition. This study is a step towards a global understanding of dust and its properties.

Language(s): English

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Tags: Aerosols ; Climate model ; Atmospheric circulation ; Climate ; Modelling ; Dust plume ; Region II - Asia ; Sahara Add tag

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Atmospheric degradation of 3-methylfuran: kinetic and products study

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Tapia A.; Villanueva F.; Salgado M.S.; et al. - Copernicus GmbH, 2011

A study of the kinetics and products obtained from the reactions of 3-methylfuran with the main atmospheric oxidants has been performed. The rate coefficients for the gas-phase reaction of 3-methylfuran with OH and NO3 radicals have been determined at room temperature and atmospheric pressure (air and N2 as bath gases), using a relative method with different experimental techniques. The rate coefficients obtained for these reactions were (in units cm3 molecule−1 s−1) kOH = (1.13 ± 0.22) × 10−10 and kNO3 = (1.26 ± 0.18) × 10−11. Products from the reaction of 3-methylfuran with OH, NO3 and Cl at ...

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Atmospheric degradation of 3-methylfuran: kinetic and products study

  Available online: http://dx.doi.org/10.5194/acp-11-3227-2011

A. Tapia ; F. Villanueva ; M.S. Salgado ; B. Cabañas ; E. Martínez ; P. Martín

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3227-3241

A study of the kinetics and products obtained from the reactions of 3-methylfuran with the main atmospheric oxidants has been performed. The rate coefficients for the gas-phase reaction of 3-methylfuran with OH and NO3 radicals have been determined at room temperature and atmospheric pressure (air and N2 as bath gases), using a relative method with different experimental techniques. The rate coefficients obtained for these reactions were (in units cm3 molecule−1 s−1) kOH = (1.13 ± 0.22) × 10−10 and kNO3 = (1.26 ± 0.18) × 10−11. Products from the reaction of 3-methylfuran with OH, NO3 and Cl atoms in the absence and in the presence of NO have also been determined. The main reaction products obtained were chlorinated methylfuranones and hydroxy-methylfuranones in the reaction of 3-methylfuran with Cl atoms, 2-methylbutenedial, 3-methyl-2,5-furanodione and hydroxy-methylfuranones in the reaction of 3-methylfuran with OH and NO3 radicals and also nitrated compounds in the reaction with NO3 radicals. The results indicate that, in all cases, the main reaction path is the addition to the double bond of the aromatic ring followed by ring opening in the case of OH and NO3 radicals. The formation of 3-furaldehyde and hydroxy-methylfuranones (in the reactions of 3-methylfuran with Cl atoms and NO3 radicals) confirmed the H-atom abstraction from the methyl group and from the aromatic ring, respectively. This study represents the first product determination for Cl atoms and NO3 radicals in reactions with 3-methylfuran. The reaction mechanisms and atmospheric implications of the reactions under consideration are also discussed.

Language(s): English

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Tags: Aerosols ; Atmosphere ; Environmental degradation ; Research Add tag

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The Smithsonian solar constant data revisited: no evidence for a strong effect of solar activity in ground-based insolation data

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Feulner G. - Copernicus GmbH, 2011

Apparent evidence for a strong signature of solar activity in ground-based insolation data was recently reported. In particular, a strong increase of the irradiance of the direct solar beam with sunspot number as well as a decline of the brightness of the solar aureole and the measured precipitable water content of the atmosphere with solar activity were presented. The latter effect was interpreted as evidence for cosmic-ray-induced aerosol formation. Here I show that these spurious results are due to a failure to correct for seasonal variations and the effects of volcanic eruptions and local ...

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The Smithsonian solar constant data revisited: no evidence for a strong effect of solar activity in ground-based insolation data

  Available online: http://dx.doi.org/10.5194/acp-11-3291-2011

G. Feulner

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3291-3301

Apparent evidence for a strong signature of solar activity in ground-based insolation data was recently reported. In particular, a strong increase of the irradiance of the direct solar beam with sunspot number as well as a decline of the brightness of the solar aureole and the measured precipitable water content of the atmosphere with solar activity were presented. The latter effect was interpreted as evidence for cosmic-ray-induced aerosol formation. Here I show that these spurious results are due to a failure to correct for seasonal variations and the effects of volcanic eruptions and local pollution in the data. After correcting for these biases, neither the atmospheric water content nor the brightness of the solar aureole show any significant change with solar activity, and the variations of the solar-beam irradiance with sunspot number are in agreement with previous estimates. Hence there is no evidence for the influence of solar activity on the climate being stronger than currently thought.

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Tags: Sunniness ; Meteorological instrument ; Solar radiation ; Research Add tag

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Latitudinal distributions of organic nitrogen and organic carbon in marine aerosols over the western North Pacific

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Miyazaki Y.; Kawamura K.; Jung J.; et al. - Copernicus GmbH, 2011

Marine aerosol samples were collected over the western North Pacific along the latitudinal transect from 44° N to 10° N in late summer 2008 for measurements of organic nitrogen (ON) and organic carbon (OC) as well as isotopic ratios of total nitrogen (TN) and total carbon (TC). Increased concentrations of methanesulfonic acid (MSA) and diethylammonium (DEA+) at 40–44° N and subtropical regions (10–20° N) together with averaged satellite chlorophyll-a data and 5-day back trajectories suggest a significant influence of marine biological activities on aerosols in these regions. ON exhibited incre ...

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Latitudinal distributions of organic nitrogen and organic carbon in marine aerosols over the western North Pacific

  Available online: http://dx.doi.org/10.5194/acp-11-3037-2011

Y. Miyazaki ; K. Kawamura ; J. Jung ; H. Furutani ; M. Uematsu

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3037-3049

Marine aerosol samples were collected over the western North Pacific along the latitudinal transect from 44° N to 10° N in late summer 2008 for measurements of organic nitrogen (ON) and organic carbon (OC) as well as isotopic ratios of total nitrogen (TN) and total carbon (TC). Increased concentrations of methanesulfonic acid (MSA) and diethylammonium (DEA+) at 40–44° N and subtropical regions (10–20° N) together with averaged satellite chlorophyll-a data and 5-day back trajectories suggest a significant influence of marine biological activities on aerosols in these regions. ON exhibited increased concentrations up to 260 ngN m−3 in these marine biologically influenced aerosols. Water-insoluble organic nitrogen (WION) was found to be the most abundant nitrogen in the aerosols, accounting for 55 ± 16% of total aerosol nitrogen. In particular, the average WION/ON ratio was as high as 0.93 ± 0.07 at 40–44° N. These results suggest that marine biological sources significantly contributed to ON, a majority of which is composed of water-insoluble fractions in the study region. Analysis of the stable carbon isotopic ratios (δ13C) indicated that, on average, marine-derived carbon accounted for ~88 ± 12% of total carbon in the aerosols. In addition, the δ13C showed higher values (from −22 to −20‰) when ON/OC ratios increased from 0.15 to 0.35 in marine biologically influenced aerosols. These results clearly show that organic nitrogen is enriched in organic aerosols originated from an oceanic region with high biological productivity, indicating a preferential transfer of nitrogen-containing organic compounds from the sea surface to the marine atmosphere. Both WION concentrations and WION/water-insoluble organic carbon (WIOC) ratios tended to increase with increasing local wind speeds, indicating that sea-to-air emissions of ON via sea spray contribute significantly to the marine organic aerosols over the study region.

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Tags: Aerosols ; Nitrogen ; Ocean-atmosphere interaction ; Observations ; Pacific Ocean ; Region V - South-West Pacific Add tag

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The effect of meteorological and chemical factors on the agreement between observations and predictions of fine aerosol composition in southwestern Ontario during BAQS-Met

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Markovic M.Z.; Hayden K.L.; Murphy J.G.; et al. - Copernicus GmbH, 2011

The Border Air Quality and Meteorology Study (BAQS-Met) was an intensive, collaborative field campaign during the summer of 2007 that investigated the effects of transboundary pollution, local pollution, and local meteorology on air quality in southwestern Ontario. This analysis focuses on the measurements of the inorganic constituents of particulate matter with diameter of less than 1 μm (PM1), with a specific emphasis on nitrate. We evaluate the ability of AURAMS, Environment Canada's chemical transport model, to represent regional air pollution in SW Ontario by comparing modelled aerosol in ...

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The effect of meteorological and chemical factors on the agreement between observations and predictions of fine aerosol composition in southwestern Ontario during BAQS-Met

  Available online: http://dx.doi.org/10.5194/acp-11-3195-2011

M.Z. Markovic ; K.L. Hayden ; J.G. Murphy ; P.A. Makar ; R.A. Ellis ; R.Y.-W. Chang ; J.G. Slowik ; C. Mihele ; J. Brook

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3195-3210

The Border Air Quality and Meteorology Study (BAQS-Met) was an intensive, collaborative field campaign during the summer of 2007 that investigated the effects of transboundary pollution, local pollution, and local meteorology on air quality in southwestern Ontario. This analysis focuses on the measurements of the inorganic constituents of particulate matter with diameter of less than 1 μm (PM1), with a specific emphasis on nitrate. We evaluate the ability of AURAMS, Environment Canada's chemical transport model, to represent regional air pollution in SW Ontario by comparing modelled aerosol inorganic chemical composition with measurements from Aerosol Mass Spectrometers (AMS) onboard the National Research Council (NRC) of Canada Twin Otter aircraft and at a ground site in Harrow, ON. The agreement between modelled and measured pNO3− at the ground site (observed mean (Mobs) = 0.50 μg m−3; modelled mean (Mmod) = 0.58 μg m−3; root mean square error (RSME) = 1.27 μg m−3) was better than aloft (Mobs = 0.32 μg m−3; Mmod = 0.09 μg m−3; RSME = 0.48 μg m−3). Possible reasons for discrepancies include errors in (i) emission inventories, (ii) atmospheric chemistry, (iii) predicted meteorological parameters, or (iv) gas/particle thermodynamics in the model framework. Using the inorganic thermodynamics model, ISORROPIA, in an offline mode, we find that the assumption of thermodynamic equilibrium is consistent with observations of gas and particle composition at Harrow. We develop a framework to assess the sensitivity of PM1 nitrate to meteorological and chemical parameters and find that errors in both the predictions of relative humidity and free ammonia (FA ≡ NH3(g) + pNH4+ − 2 · pSO42-) are responsible for the poor agreement between modelled and measured values.

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Tags: Aerosols ; Atmosphere ; Meteorology ; Observations ; Weather forecasting ; Research ; Canada Add tag

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Global distribution of sea salt aerosols: new constraints from in situ and remote sensing observations

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Jaeglé L.; Quinn P.K.; Bates T.S.; et al. - Copernicus GmbH, 2011

We combine in situ measurements of sea salt aerosols (SS) from open ocean cruises and ground-based stations together with aerosol optical depth (AOD) observations from MODIS and AERONET, and the GEOS-Chem global chemical transport model to provide new constraints on SS emissions over the world's oceans. We find that the GEOS-Chem model using the Gong (2003) source function overestimates cruise observations of coarse mode SS mass concentrations by factors of 2–3 at high wind speeds over the cold waters of the Southern, North Pacific and North Atlantic Oceans. Furthermore, the model systematical ...

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Global distribution of sea salt aerosols: new constraints from in situ and remote sensing observations

  Available online: http://dx.doi.org/10.5194/acp-11-3137-2011

L. Jaeglé ; P.K. Quinn ; T.S. Bates ; B. Alexander ; J.-T. Lin

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3137-3157

We combine in situ measurements of sea salt aerosols (SS) from open ocean cruises and ground-based stations together with aerosol optical depth (AOD) observations from MODIS and AERONET, and the GEOS-Chem global chemical transport model to provide new constraints on SS emissions over the world's oceans. We find that the GEOS-Chem model using the Gong (2003) source function overestimates cruise observations of coarse mode SS mass concentrations by factors of 2–3 at high wind speeds over the cold waters of the Southern, North Pacific and North Atlantic Oceans. Furthermore, the model systematically underestimates SS over the warm tropical waters of the Central Pacific, Atlantic, and Indian Oceans. This pattern is confirmed by SS measurements from a global network of 15 island and coastal stations. The model discrepancy at high wind speeds (>6 m s −1) has a clear dependence on sea surface temperature (SST). We use the cruise observations to derive an empirical SS source function depending on both wind speed and SST. Implementing this new source function in GEOS-Chem results in improved agreement with in situ observations, with a decrease in the model bias from +64% to +33% for the cruises and from +32% to −5% for the ground-based sites. We also show that the wind speed-SST source function significantly improves agreement with MODIS and AERONET AOD, and provides an explanation for the high AOD observed over the tropical oceans. With the wind speed-SST formulation, global SS emissions show a small decrease from 5200 Mg yr−1 to 4600 Mg yr−1, while the SS burden decreases from 9.1 to 8.5 mg m−2. The spatial distribution of SS, however, is greatly affected, with the SS burden increasing by 50% in the tropics and decreasing by 40% at mid- and high-latitudes. Our results imply a stronger than expected halogen source from SS in the tropical marine boundary layer. They also imply stronger radiative forcing of SS in the tropics and a larger response of SS emissions to climate change than previously thought.

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Tags: Aerosols ; Methodology ; Observations Add tag

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Multi-scale modeling study of the source contributions to near-surface ozone and sulfur oxides levels over California during the ARCTAS-CARB period

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Huang M.; Carmichael Gregory R.; Spak S.N.; et al. - Copernicus GmbH, 2011

Chronic high surface ozone (O3) levels and the increasing sulfur oxides (SOx = SO2+SO4) ambient concentrations over South Coast (SC) and other areas of California (CA) are affected by both local emissions and long-range transport. In this paper, multi-scale tracer, full-chemistry and adjoint simulations using the STEM atmospheric chemistry model are conducted to assess the contribution of local emission sourcesto SC O3 and to evaluate the impacts of transported sulfur and local emissions on the SC sulfur budgetduring the ARCTAS-CARB experiment period in 2008. Sensitivity simulations quantify c ...

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Multi-scale modeling study of the source contributions to near-surface ozone and sulfur oxides levels over California during the ARCTAS-CARB period

  Available online: http://dx.doi.org/10.5194/acp-11-3173-2011

M. Huang ; Gregory R. Carmichael ; S.N. Spak ; B. Adhikary ; S. Kulkarni ; Y. Cheng ; C. Wei ; Y. Tang ; A. D'Allura ; P.O. Wennberg ; G.L. Huey ; J.E. Dibb ; J.L. Jimenez ; M.J. Cubison ; A.J. Weinheimer ; A. Kaduwela ; C. Cai ; M. Wong ; R. Bradley Pierce ; J.A. Al-Saadi ; D.G. Streets ; Q. Zhang

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3173-3194

Chronic high surface ozone (O3) levels and the increasing sulfur oxides (SOx = SO2+SO4) ambient concentrations over South Coast (SC) and other areas of California (CA) are affected by both local emissions and long-range transport. In this paper, multi-scale tracer, full-chemistry and adjoint simulations using the STEM atmospheric chemistry model are conducted to assess the contribution of local emission sourcesto SC O3 and to evaluate the impacts of transported sulfur and local emissions on the SC sulfur budgetduring the ARCTAS-CARB experiment period in 2008. Sensitivity simulations quantify contributions of biogenic and fire emissions to SC O3 levels. California biogenic and fire emissions contribute 3–4 ppb to near-surface O3 over SC, with larger contributions to other regions in CA. During a long-range transport event from Asia starting from 22 June, high SOx levels (up to ~0.7 ppb of SO2 and ~1.3 ppb of SO4) is observed above ~6 km, but they did not affect CA surface air quality. The elevated SOx observed at 1–4 km is estimated to enhance surface SOx over SC by ~0.25 ppb (upper limit) on ~24 June. The near-surface SOx levels over SC during the flight week are attributed mostly to local emissions. Two anthropogenic SOx emission inventories (EIs) from the California Air Resources Board (CARB) and the US Environmental Protection Agency (EPA) are compared and applied in 60 km and 12 km chemical transport simulations, and the results are compared withobservations. The CARB EI shows improvements over the National Emission Inventory (NEI) by EPA, but generally underestimates surface SC SOx by about a factor of two. Adjoint sensitivity analysis indicated that SO2 levels at 00:00 UTC (17:00 local time) at six SC surface sites were influenced by previous day maritime emissions over the ocean, the terrestrial emissions over nearby urban areas, and by transported SO2 from the north through both terrestrial and maritime areas. Overall maritime emissions contribute 10–70% of SO2 and 20–60% fine SO4 on-shore and over the most terrestrial areas, with contributions decreasing with in-land distance from the coast. Maritime emissions also modify the photochemical environment, shifting O3 production over coastal SC to more VOC-limited conditions. These suggest an important role for shipping emission controls in reducing fine particle and O3 concentrations in SC.

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Tags: Ozone depletion ; Modelling ; Ozone ; Research ; United States of America Add tag

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On the potential contribution of open lead particle emissions to the central Arctic aerosol concentration

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Held A.; Brooks I.M.; Leck C.; et al. - Copernicus GmbH, 2011

We present direct eddy covariance measurements of aerosol number fluxes, dominated by sub-50 nm particles, at the edge of an ice floe drifting in the central Arctic Ocean. The measurements were made during the ice-breaker borne ASCOS (Arctic Summer Cloud Ocean Study) expedition in August 2008 between 2°–10° W longitude and 87°–87.5° N latitude. The median aerosol transfer velocities over different surface types (open water leads, ice ridges, snow and ice surfaces) ranged from 0.27 to 0.68 mm s−1 during deposition-dominated episodes. Emission periods were observed more frequently over the open ...

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On the potential contribution of open lead particle emissions to the central Arctic aerosol concentration

  Available online: http://dx.doi.org/10.5194/acp-11-3093-2011

A. Held ; I.M. Brooks ; C. Leck ; M. Tjernström

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3093-3105

We present direct eddy covariance measurements of aerosol number fluxes, dominated by sub-50 nm particles, at the edge of an ice floe drifting in the central Arctic Ocean. The measurements were made during the ice-breaker borne ASCOS (Arctic Summer Cloud Ocean Study) expedition in August 2008 between 2°–10° W longitude and 87°–87.5° N latitude. The median aerosol transfer velocities over different surface types (open water leads, ice ridges, snow and ice surfaces) ranged from 0.27 to 0.68 mm s−1 during deposition-dominated episodes. Emission periods were observed more frequently over the open lead, while the snow behaved primarily as a deposition surface. Directly measured aerosol fluxes were compared with particle deposition parameterizations in order to estimate the emission flux from the observed net aerosol flux. Finally, the contribution of the open lead particle source to atmospheric variations in particle number concentration was evaluated and compared with the observed temporal evolution of particle number. The direct emission of aerosol particles from the open lead can explain only 5–10% of the observed particle number variation in the mixing layer close to the surface.

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Tags: Aerosols ; Atmosphere ; Research ; Arctic Add tag

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African biomass burning plumes over the Atlantic: aircraft based measurements and implications for H2SO4 and HNO3 mediated smoke particle activation

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Fiedler V.; Arnold F.; Ludmann S.; et al. - Copernicus GmbH, 2011

Airborne measurements of trace gases and aerosol particles have been made in two aged biomass burning (BB) plumes over the East Atlantic (Gulf of Guinea). The plumes originated from BB in the Southern-Hemisphere African savanna belt. On the day of our measurements (13 August 2006), the plumes had ages of about 10 days and were respectively located in the middle troposphere (MT) at 3900–5500 m altitude and in the upper troposphere (UT) at 10 800–11 200 m. Probably, the MT plume was lifted by dry convection and the UT plume was lifted by wet convection. In the more polluted MT-plume, numerous me ...

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African biomass burning plumes over the Atlantic: aircraft based measurements and implications for H2SO4 and HNO3 mediated smoke particle activation

  Available online: http://dx.doi.org/10.5194/acp-11-3211-2011

V. Fiedler ; F. Arnold ; S. Ludmann ; A. Minikin ; T. Hamburger ; L. Pirjola ; A. Dörnbrack ; H. Schlager

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3211-3225

Airborne measurements of trace gases and aerosol particles have been made in two aged biomass burning (BB) plumes over the East Atlantic (Gulf of Guinea). The plumes originated from BB in the Southern-Hemisphere African savanna belt. On the day of our measurements (13 August 2006), the plumes had ages of about 10 days and were respectively located in the middle troposphere (MT) at 3900–5500 m altitude and in the upper troposphere (UT) at 10 800–11 200 m. Probably, the MT plume was lifted by dry convection and the UT plume was lifted by wet convection. In the more polluted MT-plume, numerous measured trace species had markedly elevated abundances, particularly SO2 (up to 1400 pmol mol−1), HNO3 (5000–8000 pmol mol−1) and smoke particles with diameters larger than 270 nm (up to 2000 cm−3). Our MT-plume measurements indicate that SO2 released by BB had not experienced significant loss by deposition and cloud processes but rather had experienced OH-induced conversion to gas-phase sulfuric acid. By contrast, a significant fraction of the released NOy had experienced loss, most likely as HNO3 by deposition. In the UT-plume, loss of NOy and SO2 was more pronounced compared to the MT-plume, probably due to cloud processes. Building on our measurements and accompanying model simulations, we have investigated trace gas transformations in the ageing and diluting plumes and their role in smoke particle processing and activation. Emphasis was placed upon the formation of sulfuric acid and ammonium nitrate, and their influence on the activation potential of smoke particles. Our model simulations reveal that, after 13 August, the lower plume traveled across the Atlantic and descended to 1300 m and hereafter ascended again. During the travel across the Atlantic, the soluble mass fraction of smoke particles and their mean diameter increased sufficiently to allow the processed smoke particles to act as water vapor condensation nuclei already at very low water vapor supersaturations of only about 0.04%. Thereby, aged smoke particles had developed a potential to act as water vapor condensation nuclei in the formation of maritime clouds.

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Tags: Region I - Africa ; Atlantic Ocean ; Atmospheric circulation ; Biomass burning experiment ; Plume ; Aircraft ascent, aircraft sounding Add tag

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A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Donahue N.M.; Epstein S.A.; Pandis S.N.; et al. - Copernicus GmbH, 2011

We develop the thermodynamic underpinnings of a two-dimensional volatility basis set (2D-VBS) employing saturation mass concentration (Co) and the oxygen content (O:C) to describe volatility, mixing thermodynamics, and chemical evolution of organic aerosol. The work addresses a simple question: "Can we reasonably constrain organic-aerosol composition in the atmosphere based on only two measurable organic properties, volatility and the extent of oxygenation?" This is an extension of our earlier one-dimensional approach employing volatility only (C* = γ Co, where γ is an activity coefficient). U ...

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A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics

  Available online: http://dx.doi.org/10.5194/acp-11-3303-2011

N.M. Donahue ; S.A. Epstein ; S.N. Pandis ; A.L. Robinson

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3303-3318

We develop the thermodynamic underpinnings of a two-dimensional volatility basis set (2D-VBS) employing saturation mass concentration (Co) and the oxygen content (O:C) to describe volatility, mixing thermodynamics, and chemical evolution of organic aerosol. The work addresses a simple question: "Can we reasonably constrain organic-aerosol composition in the atmosphere based on only two measurable organic properties, volatility and the extent of oxygenation?" This is an extension of our earlier one-dimensional approach employing volatility only (C* = γ Co, where γ is an activity coefficient). Using available constraints on bulk organic-aerosol composition, we argue that one can reasonably predict the composition of organics (carbon, oxygen and hydrogen numbers) given a location in the Co – O:C space. Further, we argue that we can constrain the activity coefficients at various locations in this space based on the O:C of the organic aerosol.

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Synergetic monitoring of Saharan dust plumes and potential impact on surface: a case study of dust transport from Canary Islands to Iberian Peninsula

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Córdoba-Jabonero C.; Sorribas M.; Guerrero-Rascado J.L.; et al. - Copernicus GmbH, 2011

The synergetic use of meteorological information, remote sensing both ground-based active (lidar) and passive (sun-photometry) techniques together with backtrajectory analysis and in-situ measurements is devoted to the characterization of dust intrusions. A case study of air masses advected from the Saharan region to the Canary Islands and the Iberian Peninsula, located relatively close and far away from the dust sources, respectively, was considered for this purpose. The observations were performed over three Spanish geographically strategic stations within the dust-influenced area along a co ...

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Synergetic monitoring of Saharan dust plumes and potential impact on surface: a case study of dust transport from Canary Islands to Iberian Peninsula

  Available online: http://dx.doi.org/10.5194/acp-11-3067-2011

C. Córdoba-Jabonero ; M. Sorribas ; J.L. Guerrero-Rascado ; J.A. Adame ; Y. Hernández ; H. Lyamani ; V. Cachorro ; M. Gil ; L. Alados-Arboledas ; E. Cuevas ; B. de la Morena

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3067-3091

The synergetic use of meteorological information, remote sensing both ground-based active (lidar) and passive (sun-photometry) techniques together with backtrajectory analysis and in-situ measurements is devoted to the characterization of dust intrusions. A case study of air masses advected from the Saharan region to the Canary Islands and the Iberian Peninsula, located relatively close and far away from the dust sources, respectively, was considered for this purpose. The observations were performed over three Spanish geographically strategic stations within the dust-influenced area along a common dust plume pathway monitored from 11 to 19 of March 2008. A 4-day long dust event (13–16 March) over the Santa Cruz de Tenerife Observatory (SCO), and a linked short 1-day dust episode (14 March) in the Southern Iberian Peninsula over the Atmospheric Sounding Station "El Arenosillo" (ARN) and the Granada station (GRA) were detected. Meteorological conditions favoured the dust plume transport over the area under study. Backtrajectory analysis clearly revealed the Saharan region as the source of the dust intrusion. Under the Saharan air masses influence, AERONET Aerosol Optical Depth at 500 nm (AOD500) ranged from 0.3 to 0.6 and Ångström Exponent at 440/675 nm wavelength pair (AE440/675) was lower than 0.5, indicating a high loading and predominance of coarse particles during those dusty events. Lidar observations characterized their vertical layering structure, identifying different aerosol contributions depending on altitude. In particular, the 3-km height dust layer transported from the Saharan region and observed over SCO site was later on detected at ARN and GRA stations. No significant differences were found in the lidar (extinction-to-backscatter) ratio (LR) estimation for that dust plume over all stations when a suitable aerosol scenario for lidar data retrieval is selected. Lidar-retrieved LR values of 60–70 sr were obtained during the main dust episodes. These similar LR values found in all the stations suggest that dust properties were kept nearly unchanged in the course of its medium-range transport. In addition, the potential impact on surface of that Saharan dust intrusion over the Iberian Peninsula was evaluated by means of ground-level in-situ measurements for particle deposition assessment together with backtrajectory analysis. However, no connection between those dust plumes and the particle sedimentation registered at ground level is found. Differences on particle deposition processes observed in both Southern Iberian Peninsula sites are due to the particular dust transport pattern occurred over each station. Discrepancies between columnar-integrated and ground-level in-situ measurements show a clear dependence on height of the dust particle size distribution. Then, further vertical size-resolved observations are needed for evaluation of the impact on surface of the Saharan dust arrival to the Iberian Peninsula

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Tags: Region I - Africa ; Spain ; Region VI - Europe ; Sahara ; Atmospheric circulation ; Observations ; Dust plume Add tag

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Projections of air pollutant emissions and its impacts on regional air quality in China in 2020

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Xing J.; Wang S.X.; Chatani S.; et al. - Copernicus GmbH, 2011

Anthropogenic emissions of air pollutants in China influence not only local and regional environments but also the global atmospheric environment; therefore, it is important to understand how China's air pollutant emissions will change and how they will affect regional air quality in the future. Emission scenarios in 2020 were projected using forecasts of energy consumption and emission control strategies based on emissions in 2005, and on recent development plans for key industries in China. We developed four emission scenarios: REF[0] (current control legislations and implementation status), ...

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Projections of air pollutant emissions and its impacts on regional air quality in China in 2020

  Available online: http://dx.doi.org/10.5194/acp-11-3119-2011

J. Xing ; S.X. Wang ; S. Chatani ; C.Y. Zhang ; W. Wei ; J.M. Hao ; Z. Klimont ; J. Cofala ; M. Amann

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3119-3136

Anthropogenic emissions of air pollutants in China influence not only local and regional environments but also the global atmospheric environment; therefore, it is important to understand how China's air pollutant emissions will change and how they will affect regional air quality in the future. Emission scenarios in 2020 were projected using forecasts of energy consumption and emission control strategies based on emissions in 2005, and on recent development plans for key industries in China. We developed four emission scenarios: REF[0] (current control legislations and implementation status), PC[0] (improvement of energy efficiencies and current environmental legislation), PC[1] (improvement of energy efficiencies and better implementation of environmental legislation), and PC[2] (improvement of energy efficiencies and strict environmental legislation). Under the REF[0] scenario, the emission of SO2, NOx, VOC and NH3 will increase by 17%, 50%, 49% and 18% in 2020, while PM10 emissions will be reduced by 10% over East China, compared to that in 2005. In PC[2], sustainable energy polices will reduce SO2, NOx and PM10 emissions by 4.1 Tg, 2.6 Tg and 1.8 Tg, respectively; better implementation of current control policies will reduce SO2, NOx and PM10 emission by 2.9 Tg, 1.8 Tg, and 1.4 Tg, respectively; strict emission standards will reduce SO2, NOx and PM10 emissions by 3.2 Tg, 3.9 Tg, and 1.7 Tg, respectively. Under the PC[2] scenario, SO2 and PM10 emissions will decrease by 18% and 38%, while NOx and VOC emissions will increase by 3% and 8%, compared to that in 2005. Future air quality in China was simulated using the Community Multi-scale Air Quality Model (CMAQ). Under REF[0] emissions, compared to 2005, the surface concentrations of SO2, NO2, hourly maximum ozone in summer, PM2.5, total sulfur and nitrogen depositions will increase by 28%, 41%, 8%, 8%, 19% and 25%, respectively, over east China. Under the PC[2] emission scenario, the surface concentrations of SO2, PM2.5, total sulfur depositions will decrease by 18%, 16% and 15%, respectively, and the surface concentrations of NO2, nitrate, hourly maximum ozone in summer, total nitrogen depositions will be kept as 2005 level, over east China. The individual impacts of SO2, NOx, NH3, NMVOC and primary PM emission changes on ozone and PM2.5 concentrations have been analyzed using sensitivity analysis. The results suggest that NOx emission control need to be enhanced during the summertime to obtain both ozone and PM2.5 reduction benefits. NH3 emission controls should also be considered in order to reduce both nitrate concentration and total nitrogen deposition in the future.

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Tags: China ; Air pollution ; Air quality ; Scenario Add tag

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Microphysical and radiative effects of aerosols on warm clouds during the Amazon biomass burning season as observed by MODIS: impacts of water vapor and land cover

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Ten Hoeve J.E.; Remer L.A.; Jacobson M.Z. - Copernicus GmbH, 2011

Aerosol, cloud, water vapor, and temperature profile data from the Moderate Resolution Imaging Spectroradiometer (MODIS) are utilized to examine the impact of aerosols on clouds during the Amazonian biomass burning season in Rondônia, Brazil. It is found that increasing background column water vapor (CWV) throughout this transition season between the Amazon dry and wet seasons likely exerts a strong effect on cloud properties. As a result, proper analysis of aerosol-cloud relationships requires that data be stratified by CWV to account better for the influence of background meteorological vari ...

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Microphysical and radiative effects of aerosols on warm clouds during the Amazon biomass burning season as observed by MODIS: impacts of water vapor and land cover

  Available online: http://dx.doi.org/10.5194/acp-11-3021-2011

J.E. Ten Hoeve ; L.A. Remer ; M.Z. Jacobson

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3021-3036

Aerosol, cloud, water vapor, and temperature profile data from the Moderate Resolution Imaging Spectroradiometer (MODIS) are utilized to examine the impact of aerosols on clouds during the Amazonian biomass burning season in Rondônia, Brazil. It is found that increasing background column water vapor (CWV) throughout this transition season between the Amazon dry and wet seasons likely exerts a strong effect on cloud properties. As a result, proper analysis of aerosol-cloud relationships requires that data be stratified by CWV to account better for the influence of background meteorological variation. Many previous studies of aerosol-cloud interactions over Amazonia have ignored the systematic changes to meteorological factors during the transition season, leading to possible misinterpretation of their results. Cloud fraction (CF) is shown to increase or remain constant with aerosol optical depth (AOD), depending on the value of CWV, whereas the relationship between cloud optical depth (COD) and AOD is quite different. COD increases with AOD until AOD ~ 0.3, which is assumed to be due to the first indirect (microphysical) effect. At higher values of AOD, COD is found to decrease with increasing AOD, which may be due to: (1) the inhibition of cloud development by absorbing aerosols (radiative effect/semi-direct effect) and/or (2) a possible retrieval artifact in which the measured reflectance in the visible is less than expected from a cloud top either from the darkening of clouds through the addition of carbonaceous biomass burning aerosols within or above clouds or subpixel dark surface contamination in the measured cloud reflectance. If (1) is a contributing mechanism, as we suspect, then an empirically-derived increasing function between cloud drop number and aerosol concentration, assumed in a majority of global climate models, is inaccurate since these models do not include treatment of aerosol absorption in and around clouds. The relationship between aerosols and both CWV and clouds over varying land surface types is also analyzed. The study finds that the difference in CWV between forested and deforested land is not correlated with aerosol loading, supporting the assumption that temporal variation of CWV is primarily a function of the larger-scale meteorology. However, a difference in the response of CF to increasing AOD is observed between forested and deforested land. This suggests that dissimilarities between other meteorological factors, such as atmospheric stability, may have an impact on aerosol-cloud correlations between different land cover types.

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Tags: Aerosols ; Amazon ; Biomass ; Warm cloud ; Observations ; Water vapour ; Region III - South America Add tag

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Dependence of the single-scattering properties of small ice crystals on idealized shape models

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Um J.; McFarquhar G.M. - Copernicus GmbH, 2011

The projections of small ice crystals (with maximum dimension <50 μm) appear quasi-circular when imaged by probes on aircraft flying through cloud. Therefore, idealized models constructed to calculate their single-scattering properties have included quasi-spherical models such as Chebyshev particles, Gaussian random spheres, and droxtals. Recently, an ice analogue grown from sodium fluorosilicate solution on a glass substrate, with several columns emanating from a common center of mass, was shown to be quasi-circular when imaged by state-of-the-art cloud probes. In this study, a new idealized ...

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Dependence of the single-scattering properties of small ice crystals on idealized shape models

  Available online: http://dx.doi.org/10.5194/acp-11-3159-2011

J. Um ; G.M. McFarquhar

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3159-3171

The projections of small ice crystals (with maximum dimension <50 μm) appear quasi-circular when imaged by probes on aircraft flying through cloud. Therefore, idealized models constructed to calculate their single-scattering properties have included quasi-spherical models such as Chebyshev particles, Gaussian random spheres, and droxtals. Recently, an ice analogue grown from sodium fluorosilicate solution on a glass substrate, with several columns emanating from a common center of mass, was shown to be quasi-circular when imaged by state-of-the-art cloud probes. In this study, a new idealized model, called the budding Bucky ball (3B) that resembles the shape of the small ice analogue is developed. The corresponding single-scattering properties (scattering phase function P11 and asymmetry parameter g) are computed by a ray-tracing code. Compared with previously used models, 3B scatters less light in the forward and more light in the lateral and backward directions. The Chebyshev particles and Gaussian random spheres show smooth and featureless P11, whereas droxtals and 3Bs, which have a faceted structure, show several peaks in P11 associated with angles of minimum deviation. Overall, the difference in the forward (lateral; backward) scattering between models are up to 22% (994%; 132%), 20% (510%; 101%), and 16% (146%; 156%) for small ice crystals with respective area ratios of 0.85, 0.77, and 0.69. The g for different models varies by up to 25%, 23%, and 19% for particles with area ratios of 0.85, 0.77, and 0.69, respectively. Because the single-scattering properties of small ice crystals depend both on the choice of the idealized model and the area ratios used to characterize the small ice crystals, higher resolution observations of small ice crystals or direct observations of their single-scattering properties are required.

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Tags: Atmosphere ; Glaciology ; Modelling ; Observations Add tag

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Analysis of number size distributions of tropical free tropospheric aerosol particles observed at Pico Espejo (4765 m a.s.l.), Venezuela

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Schmeissner T.; Krejci R.; Ström J.; et al. - Copernicus GmbH, 2011

The first long-term measurements of aerosol number and size distributions in South-American tropical free troposphere (FT) were performed from March 2007 until March 2009. The measurements took place at the high altitude Atmospheric Research Station Alexander von Humboldt. The station is located on top of the Sierra Nevada mountain ridge at 4765 m a.s.l. nearby the city of Mérida, Venezuela. Aerosol size distribution and number concentration data was obtained with a custom-built Differential Mobility Particle Sizer (DMPS) system and a Condensational Particle Counter (CPC). The analysis of the ...

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Analysis of number size distributions of tropical free tropospheric aerosol particles observed at Pico Espejo (4765 m a.s.l.), Venezuela

  Available online: http://dx.doi.org/10.5194/acp-11-3319-2011

T. Schmeissner ; R. Krejci ; J. Ström ; W. Birmili ; A. Wiedensohler ; G. Hochschild ; J. Gross ; P. Hoffmann ; S. Calderon

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3319-3332

The first long-term measurements of aerosol number and size distributions in South-American tropical free troposphere (FT) were performed from March 2007 until March 2009. The measurements took place at the high altitude Atmospheric Research Station Alexander von Humboldt. The station is located on top of the Sierra Nevada mountain ridge at 4765 m a.s.l. nearby the city of Mérida, Venezuela. Aerosol size distribution and number concentration data was obtained with a custom-built Differential Mobility Particle Sizer (DMPS) system and a Condensational Particle Counter (CPC). The analysis of the annual and diurnal variability of the tropical FT aerosol focused mainly on possible links to the atmospheric general circulation in the tropics. Considerable annual and diurnal cycles of the particle number concentration were observed. Highest total particle number concentrations were measured during the dry season (January–March, 519 ± 613 cm−3), lowest during the wet season (July–September, 318 ± 194 cm−3). The more humid FT (relative humidity (RH) range 50–95 %) contained generally higher aerosol particle number concentrations (573 ± 768 cm−3 during dry season, 320 ± 195 cm−3 during wet season) than the dry FT (RH < 50 %, 454 ± 332 cm−3 during dry season, 275 ± 172 cm−3 during wet season), indicating the importance of convection for aerosol distributions in the tropical FT. The diurnal cycle in the variability of the particle number concentration was mainly driven by local orography.

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Tags: Aerosols ; Observations ; Troposphere ; Venezuela, Bolivarian Republic of Add tag

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Evaluation of the accuracy of analysis tools for atmospheric new particle formation

Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 7. Korhonen H.; Sihto S.-L.; Kerminen V.-M.; et al. - Copernicus GmbH, 2011

Several mathematical tools have been developed in recent years to analyze new particle formation rates and to estimate nucleation rates and mechanisms at sub-3 nm sizes from atmospheric aerosol data. Here we evaluate these analysis tools using 1239 numerical nucleation events for which the nucleation mechanism and formation rates were known exactly. The accuracy of the estimates of particle formation rate at 3 nm (J3) showed significant sensitivity to the details of the analysis, i.e. form of equations used and assumptions made about the initial size of nucleating clusters, with the fraction o ...

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Evaluation of the accuracy of analysis tools for atmospheric new particle formation

  Available online: http://dx.doi.org/10.5194/acp-11-3051-2011

H. Korhonen ; S.-L. Sihto ; V.-M. Kerminen ; K.E.J. Lehtinen

in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 7 [04/01/2011] . - p.3051-3066

Several mathematical tools have been developed in recent years to analyze new particle formation rates and to estimate nucleation rates and mechanisms at sub-3 nm sizes from atmospheric aerosol data. Here we evaluate these analysis tools using 1239 numerical nucleation events for which the nucleation mechanism and formation rates were known exactly. The accuracy of the estimates of particle formation rate at 3 nm (J3) showed significant sensitivity to the details of the analysis, i.e. form of equations used and assumptions made about the initial size of nucleating clusters, with the fraction of events within a factor-of-two accuracy ranging from 43–97%. In general, the estimates of the actual nucleation rate at 1.5 nm (J1.5) were less accurate, and even the most accurate analysis set-up estimated only 59% of the events within a factor of two of the simulated mean nucleation rate. The J1.5 estimates were deteriorated mainly by the size dependence of the cluster growth rate below 3 nm, which the analysis tools do not take into account, but also by possible erroneous assumptions about the initial cluster size. The poor estimates of J1.5 can lead to large uncertainties in the nucleation prefactors (i.e. constant P in nucleation equation J1.5 = P × [H2SO4]k). Large uncertainties were found also in the procedures that are used to determine the nucleation mechanism. When applied to individual events, the analysis tools clearly overestimated the number of H2SO4 molecules in a critical cluster for most events, and thus associated them with a wrong nucleation mechanism. However, in some conditions the number of H2SO4 molecules in a critical cluster was underestimated. This indicates that analysis of field data that implies a maximum of 2 H2SO4 molecules in a cluster does not automatically rule out a higher number of molecules in the actual nucleating cluster. Our analysis also suggests that combining data from several new particle formation events to scatter plots of H2SO4 vs formation rates (J1.5 or J3) and determining the slope of the regression line may not give reliable information about the nucleation mechanism. Overall, while the analysis tools for new particle formation are useful for getting order-of-magnitude estimates of parameters related to atmospheric nucleation, one should be very cautious in interpreting the results. It is, for example, possible that the tools may have misdirected our theoretical understanding of the nucleation mechanism.

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Tags: Aerosols ; Atmosphere ; Hydrometeorological instrument ; Research Add tag

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