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Available online: http://www.atmos-chem-phys.net/11/issue6.html

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Origin and radiative forcing of black carbon transported to the Himalayas and Tibetan Plateau
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Kopacz M.; Mauzerall D.L.; Wang J.; et al. - Copernicus GmbH, 2011The remote and high elevation regions of central Asia are influenced by black carbon (BC) emissions from a variety of locations. BC deposition contributes to melting of glaciers and questions exist, of both scientific and policy interest, as to the origin of the BC reaching the glaciers. We use the adjoint of the GEOS-Chem model to identify the location from which BC arriving at a variety of locations in the Himalayas and Tibetan Plateau originates. We then calculate its direct and snow-albedo radiative forcing. We analyze the seasonal variation in the origin of BC using an adjoint sensitivity ...
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Available online: http://dx.doi.org/10.5194/acp-11-2837-2011
M. Kopacz ; D.L. Mauzerall ; J. Wang ; E.M. Leibensperger ; D.K. Henze ; K. Singh
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2837-2852The remote and high elevation regions of central Asia are influenced by black carbon (BC) emissions from a variety of locations. BC deposition contributes to melting of glaciers and questions exist, of both scientific and policy interest, as to the origin of the BC reaching the glaciers. We use the adjoint of the GEOS-Chem model to identify the location from which BC arriving at a variety of locations in the Himalayas and Tibetan Plateau originates. We then calculate its direct and snow-albedo radiative forcing. We analyze the seasonal variation in the origin of BC using an adjoint sensitivity analysis, which provides a detailed map of the location of emissions that directly contribute to black carbon concentrations at receptor locations. We find that emissions from northern India and central China contribute the majority of BC to the Himalayas, although the precise location varies with season. The Tibetan Plateau receives most BC from western and central China, as well as from India, Nepal, the Middle East, Pakistan and other countries. The magnitude of contribution from each region varies with season and receptor location. We find that sources as varied as African biomass burning and Middle Eastern fossil fuel combustion can significantly contribute to the BC reaching the Himalayas and Tibetan Plateau. We compute radiative forcing in the snow-covered regions and find the forcing due to the BC induced snow-albedo effect to vary from 5–15 W m−2 within the region, an order of magnitude larger than radiative forcing due to the direct effect, and with significant seasonal variation in the northern Tibetan Plateau. Radiative forcing from reduced snow albedo likely accelerates glacier melting. Our analysis may help inform mitigation efforts to slow the rate of glacial melt by identifying regions that make the largest contributions to BC deposition in the Himalayas and Tibetan Plateau.
Language(s): English
Format: Digital (Free)Tags: Atmosphere ; Atmospheric circulation ; Air pollution ; China ; Himalayas ; Tibet, China
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Comparison of ambient aerosol extinction coefficients obtained from in-situ, MAX-DOAS and LIDAR measurements at Cabauw
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Zieger P.; Weingartner E.; Henzing J.; et al. - Copernicus GmbH, 2011In the field, aerosol in-situ measurements are often performed under dry conditions (relative humidity RH<30–40%). Since ambient aerosol particles experience hygroscopic growth at enhanced RH, their microphysical and optical properties – especially the aerosol light scattering – are also strongly dependent on RH. The knowledge of this RH effect is of crucial importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. Here, we will present results from a four-month campaign which took place in summer 2009 in Cabauw, The Netherlands. The aerosol ...
[article]Comparison of ambient aerosol extinction coefficients obtained from in-situ, MAX-DOAS and LIDAR measurements at Cabauw
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Available online: http://dx.doi.org/10.5194/acp-11-2603-2011
P. Zieger ; E. Weingartner ; J. Henzing ; M. Moerman ; G. de Leeuw ; J. Mikkilä ; M. Ehn ; T. Petäjä ; K. Clémer ; M. van Roozendael ; S. Yilmaz ; U. Frieß ; H. Irie ; T. Wagner ; R. Shaiganfar ; S. Beirle ; A. Apituley ; K. Wilson ; U. Baltensperger
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2603-2624In the field, aerosol in-situ measurements are often performed under dry conditions (relative humidity RH<30–40%). Since ambient aerosol particles experience hygroscopic growth at enhanced RH, their microphysical and optical properties – especially the aerosol light scattering – are also strongly dependent on RH. The knowledge of this RH effect is of crucial importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. Here, we will present results from a four-month campaign which took place in summer 2009 in Cabauw, The Netherlands. The aerosol scattering coefficient σsp(λ) was measured dry and at various, predefined RH conditions between 20 and 95% with a humidified nephelometer. The scattering enhancement factor f(RH,λ) is the key parameter to describe the effect of RH on σsp(λ) and is defined as σsp(RH,λ) measured at a certain RH divided by the dry σsp(dry,λ). The measurement of f(RH,λ) together with the dry absorption measurement (assumed not to change with RH) allows the determination of the actual extinction coefficient σep(RH,λ) at ambient RH. In addition, a wide range of other aerosol properties were measured in parallel. The measurements were used to characterize the effects of RH on the aerosol optical properties. A closure study showed the consistency of the aerosol in-situ measurements. Due to the large variability of air mass origin (and thus aerosol composition) a simple parameterization of f(RH,λ) could not be established. If f(RH,λ) needs to be predicted, the chemical composition and size distribution need to be known. Measurements of four MAX-DOAS (multi-axis differential optical absorption spectroscopy) instruments were used to retrieve vertical profiles of σep(λ). The values of the lowest layer were compared to the in-situ values after conversion of the latter ones to ambient RH. The comparison showed a good correlation of R2 = 0.62–0.78, but the extinction coefficients from MAX-DOAS were a factor of 1.5–3.4 larger than the in-situ values. Best agreement is achieved for a few cases characterized by low aerosol optical depths and low planetary boundary layer heights. Differences were shown to be dependent on the applied MAX-DOAS retrieval algorithm. The comparison of the in-situ extinction data to a Raman LIDAR (light detection and ranging) showed a good correlation and higher values measured by the LIDAR (R2 = 0.82−0.85, slope of 1.69–1.76) if the Raman retrieved profile was used to extrapolate the directly measured extinction coefficient to the ground. The comparison improved if only nighttime measurements were used in the comparison (R2 = 0.96, slope of 1.12).
Language(s): English
Format: Digital (Free)Tags: Aerosols ; Atmosphere ; Air pollution
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Comparison of ambient aerosol extinction coefficients obtained from in-situ, MAX-DOAS and LIDAR measurements at Cabauw
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Zieger P.; Weingartner E.; Henzing J.; et al. - Copernicus GmbH, 2011In the field, aerosol in-situ measurements are often performed under dry conditions (relative humidity RH<30–40%). Since ambient aerosol particles experience hygroscopic growth at enhanced RH, their microphysical and optical properties – especially the aerosol light scattering – are also strongly dependent on RH. The knowledge of this RH effect is of crucial importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. Here, we will present results from a four-month campaign which took place in summer 2009 in Cabauw, The Netherlands. The aerosol ...
[article]Comparison of ambient aerosol extinction coefficients obtained from in-situ, MAX-DOAS and LIDAR measurements at Cabauw
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Available online: http://dx.doi.org/10.5194/acp-11-2603-2011
P. Zieger ; E. Weingartner ; J. Henzing ; M. Moerman ; G. de Leeuw ; J. Mikkilä ; M. Ehn ; T. Petäjä ; K. Clémer ; M. van Roozendael ; S. Yilmaz ; U. Frieß ; H. Irie ; T. Wagner ; R. Shaiganfar ; S. Beirle ; A. Apituley ; K. Wilson ; U. Baltensperger
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2603-2624In the field, aerosol in-situ measurements are often performed under dry conditions (relative humidity RH<30–40%). Since ambient aerosol particles experience hygroscopic growth at enhanced RH, their microphysical and optical properties – especially the aerosol light scattering – are also strongly dependent on RH. The knowledge of this RH effect is of crucial importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. Here, we will present results from a four-month campaign which took place in summer 2009 in Cabauw, The Netherlands. The aerosol scattering coefficient σsp(λ) was measured dry and at various, predefined RH conditions between 20 and 95% with a humidified nephelometer. The scattering enhancement factor f(RH,λ) is the key parameter to describe the effect of RH on σsp(λ) and is defined as σsp(RH,λ) measured at a certain RH divided by the dry σsp(dry,λ). The measurement of f(RH,λ) together with the dry absorption measurement (assumed not to change with RH) allows the determination of the actual extinction coefficient σep(RH,λ) at ambient RH. In addition, a wide range of other aerosol properties were measured in parallel. The measurements were used to characterize the effects of RH on the aerosol optical properties. A closure study showed the consistency of the aerosol in-situ measurements. Due to the large variability of air mass origin (and thus aerosol composition) a simple parameterization of f(RH,λ) could not be established. If f(RH,λ) needs to be predicted, the chemical composition and size distribution need to be known. Measurements of four MAX-DOAS (multi-axis differential optical absorption spectroscopy) instruments were used to retrieve vertical profiles of σep(λ). The values of the lowest layer were compared to the in-situ values after conversion of the latter ones to ambient RH. The comparison showed a good correlation of R2 = 0.62–0.78, but the extinction coefficients from MAX-DOAS were a factor of 1.5–3.4 larger than the in-situ values. Best agreement is achieved for a few cases characterized by low aerosol optical depths and low planetary boundary layer heights. Differences were shown to be dependent on the applied MAX-DOAS retrieval algorithm. The comparison of the in-situ extinction data to a Raman LIDAR (light detection and ranging) showed a good correlation and higher values measured by the LIDAR (R2 = 0.82−0.85, slope of 1.69–1.76) if the Raman retrieved profile was used to extrapolate the directly measured extinction coefficient to the ground. The comparison improved if only nighttime measurements were used in the comparison (R2 = 0.96, slope of 1.12).
Language(s): English
Format: Digital (Free)Tags: Aerosols ; Atmosphere ; Air pollution
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SO2 and BrO observation in the plume of the Eyjafjallajökull volcano 2010: CARIBIC and GOME-2 retrievals
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Heue K.-P.; Brenninkmeijer C.A.M.; Baker A.K.; et al. - Copernicus GmbH, 2011The ash cloud of the Eyjafjallajökull (also referred to as: Eyjafjalla (e.g. Schumann et al., 2011), Eyjafjöll or Eyjafjoll (e.g. Ansmann et al., 2010)) volcano on Iceland caused closure of large parts of European airspace in April and May 2010. For the validation and improvement of the European volcanic ash forecast models several research flights were performed. Also the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) flying laboratory, which routinely measures at cruise altitude (≈11 km) performed three dedicated measurements flights ...
[article]SO2 and BrO observation in the plume of the Eyjafjallajökull volcano 2010: CARIBIC and GOME-2 retrievals
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Available online: http://dx.doi.org/10.5194/acp-11-2973-2011
K.-P. Heue ; C.A.M. Brenninkmeijer ; A.K. Baker ; A. Rauthe-Schöch ; D. Walter ; T. Wagner ; C. Hörmann ; H. Sihler ; B. Dix ; U. Frieß ; U. Platt ; B.G. Martinsson ; P.F.J. van Velthoven ; A. Zahn ; R. Ebinghaus
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2973-2989The ash cloud of the Eyjafjallajökull (also referred to as: Eyjafjalla (e.g. Schumann et al., 2011), Eyjafjöll or Eyjafjoll (e.g. Ansmann et al., 2010)) volcano on Iceland caused closure of large parts of European airspace in April and May 2010. For the validation and improvement of the European volcanic ash forecast models several research flights were performed. Also the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) flying laboratory, which routinely measures at cruise altitude (≈11 km) performed three dedicated measurements flights through sections of the ash plume. Although the focus of these flights was on the detection and quantification of the volcanic ash, we report here on sulphur dioxide (SO2) and bromine monoxide (BrO) measurements with the CARIBIC DOAS (Differential Optical Absorption Spectroscopy) instrument during the second of these special flights on 16 May 2010. As the BrO and the SO2 observations coincide, we assume the BrO to have been formed inside the volcanic plume. Average SO2 and BrO mixing ratios of ≈40 ppb and ≈5 ppt respectively are retrieved inside the plume. The BrO to SO2 ratio retrieved from the CARIBIC observation is ≈1.3×10−4. Both SO2 and BrO observations agree well with simultaneous satellite (GOME-2) observations. SO2 column densities retrieved from satellite observations are often used as an indicator for volcanic ash. As the CARIBIC O4 column densities changed rapidly during the plume observation, we conclude that the aerosol and the SO2 plume are collocated. For SO2 some additional information on the local distribution can be derived from a comparison of forward and back scan GOME-2 data. More details on the local plume size and position are retrieved by combining CARIBIC and GOME-2 data.
Language(s): English
Format: Digital (Free)Tags: Aviation ; Airborne ash ; Volcanic Eruption ; Natural hazards ; Iceland
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Origin and radiative forcing of black carbon transported to the Himalayas and Tibetan Plateau
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Kopacz M.; Mauzerall D.L.; Wang J.; et al. - Copernicus GmbH, 2011The remote and high elevation regions of central Asia are influenced by black carbon (BC) emissions from a variety of locations. BC deposition contributes to melting of glaciers and questions exist, of both scientific and policy interest, as to the origin of the BC reaching the glaciers. We use the adjoint of the GEOS-Chem model to identify the location from which BC arriving at a variety of locations in the Himalayas and Tibetan Plateau originates. We then calculate its direct and snow-albedo radiative forcing. We analyze the seasonal variation in the origin of BC using an adjoint sensitivity ...
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Available online: http://dx.doi.org/10.5194/acp-11-2837-2011
M. Kopacz ; D.L. Mauzerall ; J. Wang ; E.M. Leibensperger ; D.K. Henze ; K. Singh
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2837-2852The remote and high elevation regions of central Asia are influenced by black carbon (BC) emissions from a variety of locations. BC deposition contributes to melting of glaciers and questions exist, of both scientific and policy interest, as to the origin of the BC reaching the glaciers. We use the adjoint of the GEOS-Chem model to identify the location from which BC arriving at a variety of locations in the Himalayas and Tibetan Plateau originates. We then calculate its direct and snow-albedo radiative forcing. We analyze the seasonal variation in the origin of BC using an adjoint sensitivity analysis, which provides a detailed map of the location of emissions that directly contribute to black carbon concentrations at receptor locations. We find that emissions from northern India and central China contribute the majority of BC to the Himalayas, although the precise location varies with season. The Tibetan Plateau receives most BC from western and central China, as well as from India, Nepal, the Middle East, Pakistan and other countries. The magnitude of contribution from each region varies with season and receptor location. We find that sources as varied as African biomass burning and Middle Eastern fossil fuel combustion can significantly contribute to the BC reaching the Himalayas and Tibetan Plateau. We compute radiative forcing in the snow-covered regions and find the forcing due to the BC induced snow-albedo effect to vary from 5–15 W m−2 within the region, an order of magnitude larger than radiative forcing due to the direct effect, and with significant seasonal variation in the northern Tibetan Plateau. Radiative forcing from reduced snow albedo likely accelerates glacier melting. Our analysis may help inform mitigation efforts to slow the rate of glacial melt by identifying regions that make the largest contributions to BC deposition in the Himalayas and Tibetan Plateau.
Language(s): English
Format: Digital (Free)Tags: Atmosphere ; Atmospheric circulation ; Air pollution ; China ; Himalayas ; Tibet, China
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Size dependence of volume and surface nucleation rates for homogeneous freezing of supercooled water droplets
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Kuhn T.; Earle M.E.; Khalizov A.F.; et al. - Copernicus GmbH, 2011The relative roles of volume and surface nucleation were investigated for the homogeneous freezing of pure water droplets. Experiments were carried out in a cryogenic laminar aerosol flow tube using supercooled water aerosols with maximum volume densities at radii between 1 and 3 μm. Temperature- and size-dependent values of volume- and surface-based homogeneous nucleation rates between 234.8 and 236.2 K were derived using a microphysical model and aerosol phase compositions and size distributions determined from infrared extinction measurements in the flow tube. The results show that the cont ...
[article]Size dependence of volume and surface nucleation rates for homogeneous freezing of supercooled water droplets
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Available online: http://dx.doi.org/10.5194/acp-11-2853-2011
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2853-2861The relative roles of volume and surface nucleation were investigated for the homogeneous freezing of pure water droplets. Experiments were carried out in a cryogenic laminar aerosol flow tube using supercooled water aerosols with maximum volume densities at radii between 1 and 3 μm. Temperature- and size-dependent values of volume- and surface-based homogeneous nucleation rates between 234.8 and 236.2 K were derived using a microphysical model and aerosol phase compositions and size distributions determined from infrared extinction measurements in the flow tube. The results show that the contribution from nucleation at the droplet surface increases with decreasing droplet radius and dominates over nucleation in the bulk droplet volume for droplets with radii smaller than approximately 5 μm. This is interpreted in terms of a lowered free energy of ice germ formation in the surface-based process. The implications of surface nucleation for the parameterization of homogeneous ice nucleation in numerical models are considered.
Language(s): English
Format: Digital (Free)Tags: Aerosols ; Atmosphere ; Glaciology ; Air pollution ; Water pollution
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The effect of H2SO4 – amine clustering on chemical ionization mass spectrometry (CIMS) measurements of gas-phase sulfuric acid
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Kurtén T.; Petäjä T.; Smith J.; et al. - Copernicus GmbH, 2011The state-of-the art method for measuring atmospheric gas-phase sulfuric acid is chemical ionization mass spectrometry (CIMS) based on nitrate reagent ions. We have assessed the possible effect of the sulfuric acid molecules clustering with base molecules on CIMS measurements using computational chemistry. From the computational data, three conclusions can be drawn. First, a significant fraction of the gas-phase sulfuric acid molecules are very likely clustered with amines if the amine concentration is around or above a few ppt. Second, some fraction of these acid-amine clusters may not be cha ...
[article]The effect of H2SO4 – amine clustering on chemical ionization mass spectrometry (CIMS) measurements of gas-phase sulfuric acid
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Available online: http://dx.doi.org/10.5194/acp-11-3007-2011
T. Kurtén ; T. Petäjä ; J. Smith ; I.K. Ortega ; M. Sipilä ; H. Junninen ; M. Ehn ; H. Vehkamäki ; L. Mauldin ; D.R. Worsnop ; M. Kulmala
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.3007-3019The state-of-the art method for measuring atmospheric gas-phase sulfuric acid is chemical ionization mass spectrometry (CIMS) based on nitrate reagent ions. We have assessed the possible effect of the sulfuric acid molecules clustering with base molecules on CIMS measurements using computational chemistry. From the computational data, three conclusions can be drawn. First, a significant fraction of the gas-phase sulfuric acid molecules are very likely clustered with amines if the amine concentration is around or above a few ppt. Second, some fraction of these acid-amine clusters may not be charged by the CIMS instrument, though the most reliable computational methods employed predict this fraction to be small; on the order of ten percent or less. Third, the amine molecules will evaporate practically immediately after charging, thus evading detection. These effects may need to be taken into account in the interpretation of atmospheric measurement data obtained using chemical ionization methods. The purpose of this study is not to criticize the CIMS method, but to help understand the implications of the measured results.
Language(s): English
Format: Digital (Free)Tags: Atmosphere ; Environment and landscape ; Measure ; Observations ; Air pollution ; Research
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A new method for retrieval of the extinction coefficient of water clouds by using the tail of the CALIOP signal
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Li J.; Hu Y.; Huang J.; et al. - Copernicus GmbH, 2011A method is developed based on Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) level 1 attenuated backscatter profile data for deriving the mean extinction coefficient of water droplets close to cloud top. The method is applicable to low level (cloud top <2 km), opaque water clouds in which the lidar signal is completely attenuated beyond about 100 m of penetration into the cloud. The photo multiplier tubes (PMTs) of the 532 nm detectors (parallel and perpendicular polarizations) of the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) both exhibit a non-id ...
[article]A new method for retrieval of the extinction coefficient of water clouds by using the tail of the CALIOP signal
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Available online: http://dx.doi.org/10.5194/acp-11-2903-2011
J. Li ; Y. Hu ; J. Huang ; K. Stamnes ; Y. Yi ; S. Stamnes
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2903-2916A method is developed based on Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) level 1 attenuated backscatter profile data for deriving the mean extinction coefficient of water droplets close to cloud top. The method is applicable to low level (cloud top <2 km), opaque water clouds in which the lidar signal is completely attenuated beyond about 100 m of penetration into the cloud. The photo multiplier tubes (PMTs) of the 532 nm detectors (parallel and perpendicular polarizations) of the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) both exhibit a non-ideal recovery of the lidar signal after striking a strongly backscattering target (such as water cloud or surface). Therefore, the effects of any transient responses of CALIOP on the attenuated backscatter profile of the water cloud must first be removed in order to obtain a reliable (validated) attenuated backscatter profile. Then, the slope of the exponential decay of the validated water cloud attenuated backscatter profile, and the multiple scattering factor are used for deriving the mean extinction coefficient of low-level water cloud droplets close to cloud top. This novel method was evaluated and compared with the previous method which combined the cloud effective radius (3.7-μm) reported by MODIS with the lidar depolarization ratios measured by CALIPSO to estimate the mean extinction coefficient. Statistical results show that the extinction coefficients derived by the new method based on CALIOP alone agree reasonbably well with those obtained in the previous study using combined CALIOP and MODIS data. The mean absolute relative difference in extinction coefficient is about 13.4%. An important advantage of the new method is that it can be used to derive the extinction coefficient also during night time, and it is also applicable when multi-layered clouds are present. Overall, the stratocumulus dominated regions experience larger day-night differences which are all negative and seasonal. However, a contrary tendency consisted in the global mean values. The global mean cloud water extinction coefficients during different seasons range from 26 to 30 km−1, and the differences between day and night time are all positive and small (about 1–2 km−1). In addition, the global mean layer-integrated depolarization ratios of liquid water clouds during different seasons range from 0.2 to 0.23, and the differences between day and night also are small, about 0.01.
Language(s): English
Format: Digital (Free)Tags: Water ; Methodology ; Water cloud ; Research
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Concurrent observations of atomic iodine, molecular iodine and ultrafine particles in a coastal environment
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Mahajan A.S.; Sorribas M.; Gómez Martín J.C.; et al. - Copernicus GmbH, 2011Simultaneous measurements of atomic iodine (I), molecular iodine (I2) and ultrafine particles were made at O Grove, Galicia (42.50° N, 8.87° W), on the northwest coast of Spain. The observations show a strong tidal signature, and indicate that the most probable sources of reactive iodine species are the exposed macroalgae during low tide. For the first time, I2 and I were concurrently measured revealing a high average I2/I ratio of ~32, which is higher than previously inferred by modelling studies. A 1-dimensional photochemical model is employed to simulate the observations showing that the hi ...
[article]Concurrent observations of atomic iodine, molecular iodine and ultrafine particles in a coastal environment
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Available online: http://dx.doi.org/10.5194/acp-11-2545-2011
A.S. Mahajan ; M. Sorribas ; J.C. Gómez Martín ; S.M. MacDonald ; M. Gil ; J.M.C. Plane ; A. Saiz-Lopez
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2545-2555Simultaneous measurements of atomic iodine (I), molecular iodine (I2) and ultrafine particles were made at O Grove, Galicia (42.50° N, 8.87° W), on the northwest coast of Spain. The observations show a strong tidal signature, and indicate that the most probable sources of reactive iodine species are the exposed macroalgae during low tide. For the first time, I2 and I were concurrently measured revealing a high average I2/I ratio of ~32, which is higher than previously inferred by modelling studies. A 1-dimensional photochemical model is employed to simulate the observations showing that the high I2/I ratio can be reproduced in the presence of fast vertical mixing close to the surface, or using an extra chemical loss for I atoms with an unknown species. There is a lack of strong correlation between the I2/I and ultrafine particles, indicating that although they both have macroalgal sources, these were not at the same location. The model simulations also suggest that the source of the observed ultrafine particles is likely not very close to the measurement site, in order for the particles to form and grow, but the source for I and I2 must be local. Finally, the effect of NOx levels on iodine oxides, and the conditions under which iodine particle bursts will be suppressed, are explored.
Language(s): English
Format: DigitalTags: Environment and landscape ; Littoral zone ; Observations ; Air pollution
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Atmospheric emissions from vegetation fires in Portugal (1990–2008): estimates, uncertainty analysis, and sensitivity analysis
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Rosa I.M.D.; Pereira J.M.C.; Tarantola S. - Copernicus GmbH, 2011Atmospheric emissions from wildfires in Portugal were estimated yearly over the period 1990–2008 using Landsat-based burnt area maps and land cover maps, national forest inventory data, biometric models, and literature review data. Emissions were calculated as the product of area burnt, biomass loading per unit area, combustion factor, and emission factor, using land cover specific values for all variables. Uncertainty associated with each input variable was quantified with a probability density function or a standard deviation value. Uncertainty and sensitivity analysis of estimates were perf ...
[article]Atmospheric emissions from vegetation fires in Portugal (1990–2008): estimates, uncertainty analysis, and sensitivity analysis
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Available online: http://dx.doi.org/10.5194/acp-11-2625-2011
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2625-2640Atmospheric emissions from wildfires in Portugal were estimated yearly over the period 1990–2008 using Landsat-based burnt area maps and land cover maps, national forest inventory data, biometric models, and literature review data. Emissions were calculated as the product of area burnt, biomass loading per unit area, combustion factor, and emission factor, using land cover specific values for all variables. Uncertainty associated with each input variable was quantified with a probability density function or a standard deviation value. Uncertainty and sensitivity analysis of estimates were performed with Monte Carlo and variance decomposition techniques. Area burnt varied almost 50-fold during the study period, from about 9000 ha in 2008 to 440 000 ha in 2003. Emissions reach maximum and minimum in the same years, with carbon dioxide equivalent (CO2eq.) values of 159 and 5655 Gg for 2008 and 2003, respectively. Emission factors, and the combustion factor for shrubs were identified as the variables with higher impact on model output variance. There is a very strong correlation between area burnt and emissions, allowing for good emissions estimates once area burnt is quantified. Pyrogenic emissions were compared against those from various economy sectors and found to represent 1% to 9% of the total.
Language(s): English
Format: Digital (Free)Tags: Carbon dioxide (CO2) ; Wildfire ; Observations ; Portugal
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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, 2011Size-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).
[article]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
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Available online: http://dx.doi.org/10.5194/acp-11-2817-2011
D. Rose ; S.S. Gunthe ; H. Su ; R.M. Garland ; H. Yang ; M. Berghof ; Y.F. Cheng ; B. Wehner ; P. Achtert ; A. Nowak ; A. Wiedensohler ; N. Takegawa ; Y. Kondo ; M. Hu ; Y. Zhang ; M.O. Andreae ; U. Pöschl
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2817-2836Size-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).
Language(s): English
Format: Digital (Free)Tags: Aerosols ; Biomass ; Cloud condensation nuclei (CCN) ; Air pollution ; Research
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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, 2011Fast 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 ...
[article]Representation of tropical deep convection in atmospheric models – Part 1: Meteorology and comparison with satellite observations
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Available online: http://dx.doi.org/10.5194/acp-11-2765-2011
M.R. Russo ; V. Marécal ; C.R. Hoyle ; J. Arteta ; C. Chemel ; M.P. Chipperfield ; O. Dessens ; W. Feng ; J.S. Hosking ; P.J. Telford ; O. Wild ; X. Yang ; J.A. Pyle
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2765-2786Fast 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 cycle, land/sea contrast and vertical extent, are analysed using satellite observations as a benchmark for model simulations. The observational datasets used in this work comprise precipitation rates, outgoing longwave radiation, cloud-top pressure, and water vapour from a number of independent sources, including ERA-Interim analyses. Most models are generally able to reproduce the seasonal cycle and strength of precipitation for continental regions but show larger discrepancies with observations for the Maritime Continent region. The frequency distribution of high clouds from models and observations is calculated using highly temporally-resolved (up to 3-hourly) cloud top data. The percentage of clouds above 15 km varies significantly between the models. Vertical profiles of water vapour in the upper troposphere-lower stratosphere (UTLS) show large differences between the models which can only be partly attributed to temperature differences. If a convective plume reaches above the level of zero net radiative heating, which is estimated to be ~15 km in the tropics, the air detrained from it can be transported upwards by radiative heating into the lower stratosphere. In this context, we discuss the role of tropical convection as a precursor for the transport of short-lived species into the lower stratosphere.
Language(s): English
Format: Digital (Free)Tags: Atmospheric circulation ; Chemical model of climate ; Modelling ; Observations ; Numerical weather prediction ; Research ; Satellite
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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, 2011Carbon 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.
[article]Long-term analysis of carbon dioxide and methane column-averaged mole fractions retrieved from SCIAMACHY
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Available online: http://dx.doi.org/10.5194/acp-11-2863-2011
O. Schneising ; M. Buchwitz ; M. Reuter ; J. Heymann ; H. Bovensmann ; J.P. Burrows
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2863-2880Carbon 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.
Language(s): English
Format: Digital (Free)Tags: Carbon dioxide (CO2) ; Methane (CH4) ; Long-range weather forecasting, long-term weather forecasting, long-range meteorological forecasting ; Research
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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, 2011As 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 ...
[article]Photochemical processing of organic aerosol at nearby continental sites: contrast between urban plumes and regional aerosol
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Available online: http://dx.doi.org/10.5194/acp-11-2991-2011
J.G. Slowik ; J. Brook ; R.Y.-W. Chang ; G.J. Evans ; K. Hayden ; C.-H. Jeong ; S.-M. Li ; J. Liggio ; P.S.K. Liu ; M. McGuire ; C. Mihele ; S. Sjostedt ; A. Vlasenko ; J.P.D. Abbatt
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2991-3006As 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 yields factors related to secondary organic aerosol (SOA), direct emissions, and a factor tentatively attributed to the reactive uptake of isoprene and/or condensation of its early generation reaction products. This is the first application of PMF to simultaneous AMS measurements at different sites, an approach which allows for self-consistent, direct comparison of the datasets. Case studies are utilized to investigate processing of SOA from (1) fresh emissions from Detroit/Windsor and (2) regional aerosol during periods of inter-site flow. A strong correlation is observed between SOA/excess CO and photochemical age as represented by the NOx/NOy ratio for Detroit/Windsor outflow. Although this correlation is not evident for more aged air, measurements at the two sites during inter-site transport nevertheless show evidence of continued atmospheric processing by SOA production. However, the rate of SOA production decreases with airmass age from an initial value of ~10.1 μg m−3 ppmvCO−1 h−1 for the first ~10 h of plume processing to near-zero in an aged airmass (i.e. after several days). The initial SOA production rate is comparable to the observed rate in Mexico City over similar timescales.
Language(s): English
Format: DigitalTags: Aerosols ; Ecology ; Environment and landscape ; Research ; Canada
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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, 2011A 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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Available online: http://dx.doi.org/10.5194/acp-11-2641-2011
D.L. Wu ; J.H. Chae ; A. Lambert ; F.F. Zhang
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2641-2654A 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 backscatter profiles. This scaling α value is sensitive to errors in the calibrated backscatter and the atmospheric model used. Most of the nighttime 532-nm α values are close to unity, as expected, but an abrupt drop occurred in October 2008 in the daytime 532-nm α, which is likely indicative of a problem in the v2.02 daytime calibrated data. The 1064-nm night α is generally close to 2 while its day α is ~3. The other approach to evaluate the lidar measurement noise is to use the calibrated lidar backscatter data at altitudes above 19 km. With this method, the 532-nm and 1064-nm measurement noises are analyzed and characterized individually for each profile in terms of the mean (μ) and standard deviation (σ), showing larger σ values in general over landmasses or bright surfaces during day and in radiation-hard regions during night. A significant increasing trend is evident in the nighttime 1064-nm σ, which is likely responsible for the increasing difference between the feature occurrence frequencies (532-nm vs. 1064-nm) derived from this study. For feature detection with the research algorithm, we apply a σ–based method to the aggregated L1 data. The derived morphology of feature occurrence frequency is in general agreement with that obtained from the Level 2 (L2) 05 km_CLAY+05 km_ALAY products at 5 km horizontal resolution. Finally, a normalized probability density function (PDF) method is employed to evaluate the day-night backscatter data in which noise levels are largely different. CALIOP observations reveal a higher probability of daytime cloud/aerosol occurrence than nighttime in the tropical UT/LS region for 532-nm total backscatters >0.01 km−1 sr−1.
Language(s): English
Format: Digital (Free)Tags: Aerosols ; Atmosphere ; Observations ; Research
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Dry deposition of reactive nitrogen to European ecosystems: a comparison of inferential models across the NitroEurope network
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Flechard C.R.; Nemitz E.; Smith R.I.; et al. - Copernicus GmbH, 2011Inferential models have long been used to determine pollutant dry deposition to ecosystems from measurements of air concentrations and as part of national and regional atmospheric chemistry and transport models, and yet models still suffer very large uncertainties. An inferential network of 55 sites throughout Europe for atmospheric reactive nitrogen (Nr) was established in 2007, providing ambient concentrations of gaseous NH3, NO2, HNO3 and HONO and aerosol NH4+ and NO3− as part of the NitroEurope Integrated Project.
Network results providing modelled inorganic Nr dry deposition ...
[article]Dry deposition of reactive nitrogen to European ecosystems: a comparison of inferential models across the NitroEurope network
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Available online: http://dx.doi.org/10.5194/acp-11-2703-2011
C.R. Flechard ; E. Nemitz ; R.I. Smith ; D. Fowler ; A.T. Vermeulen ; A. Bleeker ; J.W. Erisman ; D. Simpson ; L. Zhang ; Y.S. Tang ; M.A. Sutton
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2703-2728Inferential models have long been used to determine pollutant dry deposition to ecosystems from measurements of air concentrations and as part of national and regional atmospheric chemistry and transport models, and yet models still suffer very large uncertainties. An inferential network of 55 sites throughout Europe for atmospheric reactive nitrogen (Nr) was established in 2007, providing ambient concentrations of gaseous NH3, NO2, HNO3 and HONO and aerosol NH4+ and NO3− as part of the NitroEurope Integrated Project.
Network results providing modelled inorganic Nr dry deposition to the 55 monitoring sites are presented, using four existing dry deposition routines, revealing inter-model differences and providing ensemble average deposition estimates. Dry deposition is generally largest over forests in regions with large ambient NH3 concentrations, exceeding 30–40 kg N ha−1 yr−1 over parts of the Netherlands and Belgium, while some remote forests in Scandinavia receive less than 2 kg N ha−1 yr−1. Turbulent Nr deposition to short vegetation ecosystems is generally smaller than to forests due to reduced turbulent exchange, but also because NH3 inputs to fertilised, agricultural systems are limited by the presence of a substantial NH3 source in the vegetation, leading to periods of emission as well as deposition.
Differences between models reach a factor 2–3 and are often greater than differences between monitoring sites. For soluble Nr gases such as NH3 and HNO3, the non-stomatal pathways are responsible for most of the annual uptake over many surfaces, especially the non-agricultural land uses, but parameterisations of the sink strength vary considerably among models. For aerosol NH4+ and NO3− discrepancies between theoretical models and field flux measurements lead to much uncertainty in dry deposition rates for fine particles (0.1–0.5 μm). The validation of inferential models at the ecosystem scale is best achieved by comparison with direct long-term micrometeorological Nr flux measurements, but too few such datasets are available, especially for HNO3 and aerosol NH4+ and NO3−.Language(s): English
Format: Digital (Free)Tags: Atmosphere ; Nitrogen (N2) ; Environment and landscape ; Air pollution ; Region VI - Europe
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On the impacts of phytoplankton-derived organic matter on the properties of the primary marine aerosol – Part 2: Composition, hygroscopicity and cloud condensation activity
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Fuentes E.; Coe H.; Green D.; et al. - Copernicus GmbH, 2011The effect of nanogel colloidal and dissolved organic matter <0.2 μm, secreted by marine biota, on the hygroscopic growth and droplet activation behaviour of the primary marine aerosol was studied. Seawater proxies were prepared by the combination of artificial seawater devoid of marine organics and natural seawater enriched in organic exudate released by laboratory-grown phytoplankton cultures, as described in a companion paper. The primary aerosol was produced by bubble bursting, using a plunging multijet system as an aerosol generator.
[article]On the impacts of phytoplankton-derived organic matter on the properties of the primary marine aerosol – Part 2: Composition, hygroscopicity and cloud condensation activity
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Available online: http://dx.doi.org/10.5194/acp-11-2585-2011
E. Fuentes ; H. Coe ; D. Green ; G. McFiggans
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2585-2602The effect of nanogel colloidal and dissolved organic matter <0.2 μm, secreted by marine biota, on the hygroscopic growth and droplet activation behaviour of the primary marine aerosol was studied. Seawater proxies were prepared by the combination of artificial seawater devoid of marine organics and natural seawater enriched in organic exudate released by laboratory-grown phytoplankton cultures, as described in a companion paper. The primary aerosol was produced by bubble bursting, using a plunging multijet system as an aerosol generator.
Language(s): English
Format: Digital (Free)Tags: Aerosols ; Ecosystem ; Environment and landscape ; Ocean-atmosphere interaction ; Cloud condensation nuclei (CCN) ; Oceans
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Sources of carbonaceous aerosol in the Amazon basin
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Gilardoni S.; Vignati E.; Marmer E.; et al. - Copernicus GmbH, 2011The quantification of sources of carbonaceous aerosol is important to understand their atmospheric concentrations and regulating processes and to study possible effects on climate and air quality, in addition to develop mitigation strategies.
In the framework of the European Integrated Project on Aerosol Cloud Climate Interactions (EUCAARI) fine (Dp < 2.5 μm) and coarse (2.5 μm < Dp <10 μm) aerosol particles were sampled from February to June (wet season) and from August to September (dry season) 2008 in the central Amazon basin. The mass of fine particles averaged 2.4 μg m−3 duri ...
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Available online: http://dx.doi.org/10.5194/acp-11-2747-2011
S. Gilardoni ; E. Vignati ; E. Marmer ; F. Cavalli ; C. Belis ; V. Gianelle ; A. Loureiro ; P. Artaxo
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2747-2764The quantification of sources of carbonaceous aerosol is important to understand their atmospheric concentrations and regulating processes and to study possible effects on climate and air quality, in addition to develop mitigation strategies.
In the framework of the European Integrated Project on Aerosol Cloud Climate Interactions (EUCAARI) fine (Dp < 2.5 μm) and coarse (2.5 μm < Dp <10 μm) aerosol particles were sampled from February to June (wet season) and from August to September (dry season) 2008 in the central Amazon basin. The mass of fine particles averaged 2.4 μg m−3 during the wet season and 4.2 μg m−3 during the dry season. The average coarse aerosol mass concentration during wet and dry periods was 7.9 and 7.6 μg m−3, respectively. The overall chemical composition of fine and coarse mass did not show any seasonality with the largest fraction of fine and coarse aerosol mass explained by organic carbon (OC); the average OC to mass ratio was 0.4 and 0.6 in fine and coarse aerosol modes, respectively. The mass absorbing cross section of soot was determined by comparison of elemental carbon and light absorption coefficient measurements and it was equal to 4.7 m2 g−1 at 637 nm. Carbon aerosol sources were identified by Positive Matrix Factorization (PMF) analysis of thermograms: 44% of fine total carbon mass was assigned to biomass burning, 43% to secondary organic aerosol (SOA), and 13% to volatile species that are difficult to apportion. In the coarse mode, primary biogenic aerosol particles (PBAP) dominated the carbonaceous aerosol mass. The results confirmed the importance of PBAP in forested areas.
The source apportionment results were employed to evaluate the ability of global chemistry transport models to simulate carbonaceous aerosol sources in a regional tropical background site. The comparison showed an overestimation of elemental carbon (EC) by the TM5 model during the dry season and OC both during the dry and wet periods. The overestimation was likely due to the overestimation of biomass burning emission inventories and SOA production over tropical areas.Language(s): English
Format: Digital (Free)Tags: Aerosols ; Amazon ; Carbon dioxide (CO2) ; Observations ; Air quality ; Region III - South America
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Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Ebert M.; Worringen A.; Benker N.; et al. - Copernicus GmbH, 2011During an intensive campaign at the high alpine research station Jungfraujoch, Switzerland, in February/March 2006 ice particle residuals within mixed-phase clouds were sampled using the Ice-counterflow virtual impactor (Ice-CVI). Size, morphology, chemical composition, mineralogy and mixing state of the ice residual and the interstitial (i.e., non-activated) aerosol particles were analyzed by scanning and transmission electron microscopy. Ice nuclei (IN) were identified from the significant enrichment of particle groups in the ice residual (IR) samples relative to the interstitial aerosol. In ...
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Available online: http://dx.doi.org/10.5194/acp-11-2805-2011
M. Ebert ; A. Worringen ; N. Benker ; S. Mertes ; E. Weingartner ; S. Weinbruch
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2805-2816During an intensive campaign at the high alpine research station Jungfraujoch, Switzerland, in February/March 2006 ice particle residuals within mixed-phase clouds were sampled using the Ice-counterflow virtual impactor (Ice-CVI). Size, morphology, chemical composition, mineralogy and mixing state of the ice residual and the interstitial (i.e., non-activated) aerosol particles were analyzed by scanning and transmission electron microscopy. Ice nuclei (IN) were identified from the significant enrichment of particle groups in the ice residual (IR) samples relative to the interstitial aerosol. In terms of number lead-bearing particles are enriched by a factor of approximately 25, complex internal mixtures with silicates or metal oxides as major components by a factor of 11, and mixtures of secondary aerosol and carbonaceous material (C-O-S particles) by a factor of 2. Other particle groups (sulfates, sea salt, Ca-rich particles, external silicates) observed in the ice-residual samples cannot be assigned unambiguously as IN. Between 9 and 24% of all IR are Pb-bearing particles. Pb was found as major component in around 10% of these particles (PbO, PbCl2). In the other particles, Pb was found as some 100 nm sized agglomerates consisting of 3–8 nm sized primary particles (PbS, elemental Pb). C-O-S particles are present in the IR at an abundance of 17–27%. The soot component within these particles is strongly aged. Complex internal mixtures occur in the IR at an abundance of 9–15%. Most IN identified at the Jungfraujoch station are internal mixtures containing anthropogenic components (either as main or minor constituent), and it is concluded that admixture of the anthropogenic component is responsible for the increased IN efficiency within mixed phase clouds. The mixing state appears to be a key parameter for the ice nucleation behaviour that cannot be predicted from the sole knowledge of the main component of an individual particle.
Language(s): English
Format: Digital (Free)Tags: Aerosols ; Atmosphere ; Glaciology ; Cloud ; Observations ; Air pollution ; Alps, the ; Region VI - Europe
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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, 2011We 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 ...
[article]Evaluating a 3-D transport model of atmospheric CO2 using ground-based, aircraft, and space-borne data
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Available online: http://dx.doi.org/10.5194/acp-11-2789-2011
L. Feng ; P.I. Palmer ; Y. Yang ; R.M. Yantosca ; S.R. Kawa ; J.-D. Paris ; H. Matsueda ; T. Machida
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2789-2803We 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 GEOS-4 (GEOS-5) meteorology are −4.4 ± 0.9 (−4.2 ± 0.9), −3.9 ± 0.9 (−4.5 ± 0.9), and −5.2 ± 0.9 (−4.9 ± 0.9) PgC yr−1, respectively. After taking into account anthropogenic fossil fuel and bio-fuel emissions, the global annual net CO2 emissions for 2004–2006 are estimated to be 4.0 ± 0.9 (4.2 ± 0.9), 4.8 ± 0.9 (4.2 ± 0.9), and 3.8 ± 0.9 (4.1 ± 0.9) PgC yr−1, respectively. The estimated 3-yr total net emission for GEOS-4 (GEOS-5) meteorology is equal to 12.5 (12.4) PgC, agreeing with other recent top-down estimates (12–13 PgC). The regional a posteriori fluxes are broadly consistent in the sign and magnitude of the TransCom-3 study for 1992–1996, but we find larger net sinks over northern and southern continents. We find large departures from our a priori over Europe during summer 2003, over temperate Eurasia during 2004, and over North America during 2005, reflecting an incomplete description of terrestrial carbon dynamics. We find GEOS-4 (GEOS-5) a posteriori CO2 concentrations reproduce the observed surface trend of 1.91–2.43 ppm yr−1 (parts per million per year), depending on latitude, within 0.15 ppm yr−1 (0.2 ppm yr−1) and the seasonal cycle within 0.2 ppm (0.2 ppm) at all latitudes. We find the a posteriori model reproduces the aircraft vertical profile measurements of CO2 over North America and Siberia generally within 1.5 ppm in the free and upper troposphere but can be biased by up to 4–5 ppm in the boundary layer at the start and end of the growing season. The model has a small negative bias in the free troposphere CO2 trend (1.95–2.19 ppm yr−1) compared to AIRS data which has a trend of 2.21–2.63 ppm yr−1 during 2004–2006, consistent with surface data. Model CO2 concentrations in the upper troposphere, evaluated using CONTRAIL (Comprehensive Observation Network for TRace gases by AIrLiner) aircraft measurements, reproduce the magnitude and phase of the seasonal cycle of CO2 in both hemispheres. We generally find that the GEOS meteorology reproduces much of the observed tropospheric CO2 variability, suggesting that these meteorological fields will help make significant progress in understanding carbon fluxes as more data become available.
Language(s): English
Format: Digital (Free)Tags: Atmosphere ; Atmospheric circulation ; Carbon dioxide (CO2) ; Modelling ; Research ; Satellite ; Aircraft ascent, aircraft sounding
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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, 2011Mesoscale 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 ...
[article]Sensitivity of mesoscale model urban boundary layer meteorology to the scale of urban representation
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Available online: http://dx.doi.org/10.5194/acp-11-2951-2011
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2951-2972Mesoscale 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 Forecasting (WRF) model with its coupled single-layer urban canopy model. Some model verification is presented using measurements from the Border Air Quality and Meteorology Study (BAQS-Met) 2007 field campaign and additional sources. Case studies span from "neighborhood" (10 s ~308 m) to very coarse (120 s ~3.7 km) resolution. Small changes in scale can affect the classification of the surface, affecting both the local and grid-average meteorology. Results indicate high sensitivity in turbulent latent heat flux from the natural surface and sensible heat flux from the urban canopy. Small scale change is also shown to delay timing of a lake-breeze front passage and can affect the timing of local transition in static stability.
Language(s): English
Format: Digital (Free)Tags: Meteorology ; Modelling ; Weather forecasting ; Research
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Distribution and air-sea exchange of mercury (Hg) in the Yellow Sea
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Ci Z.J.; Zhang X.S.; Wang Z.W.; et al. - Copernicus GmbH, 2011The Yellow Sea, surrounded by East China and the Korea Peninsula, is a potentially important receptor for anthropogenic mercury (Hg) emissions from East Asia. However, there is little documentation about the distribution and cycle of Hg in this marine system. During the cruise covering the Yellow Sea in July 2010, gaseous elemental mercury (GEM or Hg(0)) in the atmosphere, total Hg (THg), reactive Hg (RHg) and dissolved gaseous mercury (DGM, largely Hg(0)) in the waters were measured aboard the R/V Kexue III. The mean (±SD) concentration of GEM over the entire cruise was 2.61 ± 0.50 ng m−3 (ra ...
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Available online: http://dx.doi.org/10.5194/acp-11-2881-2011
Z.J. Ci ; X.S. Zhang ; Z.W. Wang ; Z.C. Niu ; X.Y. Diao ; S.W. Wang
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2881-2892The Yellow Sea, surrounded by East China and the Korea Peninsula, is a potentially important receptor for anthropogenic mercury (Hg) emissions from East Asia. However, there is little documentation about the distribution and cycle of Hg in this marine system. During the cruise covering the Yellow Sea in July 2010, gaseous elemental mercury (GEM or Hg(0)) in the atmosphere, total Hg (THg), reactive Hg (RHg) and dissolved gaseous mercury (DGM, largely Hg(0)) in the waters were measured aboard the R/V Kexue III. The mean (±SD) concentration of GEM over the entire cruise was 2.61 ± 0.50 ng m−3 (range: 1.68 to 4.34 ng m−3), which were generally higher than other open oceans. The spatial distribution of GEM generally reflected a clear gradient with high levels near the coast of East China and low levels in open waters, suggesting the significant atmospheric Hg outflow from East China. The mean concentration of THg in the surface waters was 1.69 ± 0.35 ng l−1 and the RHg accounted for a considerable fraction of THg (RHg: 1.08 ± 0.28 ng l−1, %RHg/THg = 63.9%). The mean concentration of DGM in the surface waters was 63.9 ± 13.7 pg l−1 and always suggested the supersaturation of Hg(0) in the surface waters with respect to Hg(0) in the atmosphere (the degree of saturation: 7.8 ± 2.3 with a range of 3.6–14.0). The mean Hg(0) flux at the air-sea interface was estimated to be 18.3 ± 11.8 ng m−2 h−1 based on a two-layer exchange model. The high wind speed and DGM levels induced the extremely high Hg(0) emission rates. Measurements at three stations showed no clear vertical patterns of DGM, RHg and THg in the water column. Overall, the elevated Hg levels in the Yellow Sea compared with other open oceans suggested that the human activity has influenced the oceanic Hg cycle downwind of East Asia.
Language(s): English
Format: Digital (Free)Tags: Region II - Asia ; China ; Republic of Korea ; Yellow Sea ; Atmosphere ; Ocean-atmosphere interaction ; Metals ; Observations ; Air pollution
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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, 2011Means, 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% ...
[article]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
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Available online: http://dx.doi.org/10.5194/acp-11-2893-2011
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2893-2901Means, 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% for cloud fraction, 7% for liquid water path, and 0.2% for cloud particle effective radius. These scale dependences contribute to the uncertainties in their global budgets. Scale dependence for standard deviations and generalized flatness are compared to predictions for turbulent systems. Analytical expressions are identified that fit best to each observed PDF. While the best analytical PDF fit to each variable differs, all PDFs are well described by log-normal PDFs when the mean is normalized by the standard deviation inside each averaging domain. Importantly, log-normal distributions yield significantly better fits to the observations than gaussians at all scales. This suggests a possible approach for both sub-grid and unified stochastic modeling of these variables at all scales. The results also highlight the need to establish an adequate spatial resolution for two-stream radiative studies of cloud-climate interactions.
Language(s): English
Format: Digital (Free)Tags: Cloud ; Research ; Turbulence
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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, 2011The 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 ...
[article]Evaluating the effects of microphysical complexity in idealised simulations of trade wind cumulus using the Factorial Method
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Available online: http://dx.doi.org/10.5194/acp-11-2729-2011
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2729-2746The 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 effect of additional microphysical complexity in terms of the impact on surface precipitation. At relatively low updraught speeds, the sensitivity of the bulk schemes was found to depend on the assumptions made with regards the treatment of droplet activation. It was possible to achieve a much closer agreement between the single and dual moment bulk schemes by tuning the specified droplet number concentration in the single moment scheme, suggesting that a diagnostic representation of droplet number may be an acceptable alternative to the more expensive prognostic option. However the effect of changes in CCN concentration were found to produce a relatively stronger effect on precipitation in the bulk schemes compared to the bin scheme; this is believed to be a consequence of differences in the treatment of drop growth by collision and coalescence. Collectively, these results demonstrate the usefulness of the Factorial Method as a model development tool for quantitatively comparing and contrasting the behaviour of microphysics schemes of differing levels of complexity within a specified parameter space.
Language(s): English
Format: Digital (Free)Tags: Trade wind ; Impact studies ; Warm cloud ; Research ; Wind
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Size and time-resolved roadside enrichment of atmospheric particulate pollutants
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Amato F.; Viana M.; Richard A.; et al. - Copernicus GmbH, 2011Size and time-resolved roadside enrichments of atmospheric particulate pollutants in PM10 were detected and quantified in a Mediterranean urban environment (Barcelona, Spain). Simultaneous data from one urban background (UB), one traffic (T) and one heavy traffic (HT) location were analysed, and roadside PM10 enrichments (RE) in a number of elements arising from vehicular emissions were calculated. Tracers of primary traffic emissions (EC, Fe, Ba, Cu, Sb, Cr, Sn) showed the largest REs (>70%). Other traffic tracers (Zr, Cd) showed lower but still consistent REs (25–40%), similar to those obtai ...
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Available online: http://dx.doi.org/10.5194/acp-11-2917-2011
F. Amato ; M. Viana ; A. Richard ; M. Furger ; A.S.H. Prévôt ; S. Nava ; F. Lucarelli ; N. Bukowiecki ; A. Alastuey ; C. Reche ; T. Moreno ; M. Pandolfi ; J. Pey ; X. Querol
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2917-2931Size and time-resolved roadside enrichments of atmospheric particulate pollutants in PM10 were detected and quantified in a Mediterranean urban environment (Barcelona, Spain). Simultaneous data from one urban background (UB), one traffic (T) and one heavy traffic (HT) location were analysed, and roadside PM10 enrichments (RE) in a number of elements arising from vehicular emissions were calculated. Tracers of primary traffic emissions (EC, Fe, Ba, Cu, Sb, Cr, Sn) showed the largest REs (>70%). Other traffic tracers (Zr, Cd) showed lower but still consistent REs (25–40%), similar to those obtained for mineral matter resulting from road dust resuspension (Ca, La, Ce, Ti, Ga, Sr, 30–40%). The sum of primary and secondary organic carbon showed a RE of 41%, with contributions of secondary OC (SOC) to total OC ranging from 46% at the HT site, 63% at the T site, and 78% in the UB. Finally, other trace elements (As, Co, Bi) showed unexpected but consistent roadside enrichments (23% up to 69%), suggesting a link to traffic emissions even though the emission process is unclear.
Language(s): English
Format: Digital (Free)Tags: Atmosphere ; Urban zone ; Air pollution ; Region VI - Europe
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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, 2011Stratospheric 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 ...
[article]Impact of deep convection and dehydration on bromine loading in the upper troposphere and lower stratosphere
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Available online: http://dx.doi.org/10.5194/acp-11-2671-2011
J. Aschmann ; B.-M. Sinnhuber ; M.P. Chipperfield ; R. Hossaini
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2671-2687Stratospheric 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), assuming a uniform convective detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach.
Language(s): English
Format: Digital (Free)Tags: Environment and landscape ; Air pollution ; Research ; Stratosphere ; Troposphere ; Region VI - Europe
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Measurements of volatile organic compounds at a suburban ground site (T1) in Mexico City during the MILAGRO 2006 campaign: measurement comparison, emission ratios, and source attribution
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Bon D.M.; Ulbrich I.M.; de Gouw J.A.; et al. - Copernicus GmbH, 2011Volatile organic compound (VOC) mixing ratios were measured with two different instruments at the T1 ground site in Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO) campaign in March of 2006. A gas chromatograph with flame ionization detector (GC-FID) quantified 18 light alkanes, alkenes and acetylene while a proton-transfer-reaction ion-trap mass spectrometer (PIT-MS) quantified 12 VOC species including oxygenated VOCs (OVOCs) and aromatics. A GC separation system was used in conjunction with the PIT-MS (GC-PIT-MS) to evaluate PIT-MS measurements an ...
[article]Measurements of volatile organic compounds at a suburban ground site (T1) in Mexico City during the MILAGRO 2006 campaign: measurement comparison, emission ratios, and source attribution
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Available online: http://dx.doi.org/10.5194/acp-11-2399-2011
D.M. Bon ; I.M. Ulbrich ; J.A. de Gouw ; C. Warneke ; W.C. Kuster ; M.L. Alexander ; A. Baker ; A.J. Beyersdorf ; D. Blake ; R. Fall ; J.L. Jimenez ; S.C. Herndon ; L.G. Huey ; W.B. Knighton ; J. Ortega ; S. Springston ; O. Vargas
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2399-2421Volatile organic compound (VOC) mixing ratios were measured with two different instruments at the T1 ground site in Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO) campaign in March of 2006. A gas chromatograph with flame ionization detector (GC-FID) quantified 18 light alkanes, alkenes and acetylene while a proton-transfer-reaction ion-trap mass spectrometer (PIT-MS) quantified 12 VOC species including oxygenated VOCs (OVOCs) and aromatics. A GC separation system was used in conjunction with the PIT-MS (GC-PIT-MS) to evaluate PIT-MS measurements and to aid in the identification of unknown VOCs. The VOC measurements are also compared to simultaneous canister samples and to two independent proton-transfer-reaction mass spectrometers (PTR-MS) deployed on a mobile and an airborne platform during MILAGRO. VOC diurnal cycles demonstrate the large influence of vehicle traffic and liquid propane gas (LPG) emissions during the night and photochemical processing during the afternoon. Emission ratios for VOCs and OVOCs relative to CO are derived from early-morning measurements. Average emission ratios for non-oxygenated species relative to CO are on average a factor of ~2 higher than measured for US cities. Emission ratios for OVOCs are estimated and compared to literature values the northeastern US and to tunnel studies in California. Positive matrix factorization analysis (PMF) is used to provide insight into VOC sources and processing. Three PMF factors were distinguished by the analysis including the emissions from vehicles, the use of liquid propane gas and the production of secondary VOCs + long-lived species. Emission ratios to CO calculated from the results of PMF analysis are compared to emission ratios calculated directly from measurements. The total PIT-MS signal is summed to estimate the fraction of identified versus unidentified VOC species.
Language(s): English
Format: Digital (Free)Tags: Atmosphere ; Volatile Organic Compounds (VOCs) ; Measure ; Urban zone ; Observations ; Mexico
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Investigations of aerosol impacts on hurricanes: virtual seeding flights
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Carrio G.G.; Cotton William R. - Copernicus GmbH, 2011This paper examines the feasibility of mitigating the intensity of hurricanes by enhancing the CCN concentrations in the outer rainband region. Increasing CCN concentrations would cause a reduced collision and coalescence, resulting in more supercooled liquid water to be transported aloft which then freezes and enhances convection via enhanced latent heat of freezing. The intensified convection would condense more water ultimately enhancing precipitation in the outer rainbands. Enhanced evaporative cooling from the increased precipitation in the outer rainbands would produce stronger and more ...
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Available online: http://dx.doi.org/10.5194/acp-11-2557-2011
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2557-2567This paper examines the feasibility of mitigating the intensity of hurricanes by enhancing the CCN concentrations in the outer rainband region. Increasing CCN concentrations would cause a reduced collision and coalescence, resulting in more supercooled liquid water to be transported aloft which then freezes and enhances convection via enhanced latent heat of freezing. The intensified convection would condense more water ultimately enhancing precipitation in the outer rainbands. Enhanced evaporative cooling from the increased precipitation in the outer rainbands would produce stronger and more widespread areal cold pools which block the flow of energy into the storm core, ultimately inhibiting the intensification of the tropical cyclone.
We designed a series of multi-grid for which the time of the "virtual flights" as well as the aerosol release rates are varied. A code that simulates the flight of a plane is used to increase the CCN concentrations as an aircraft flies. Results show a significant sensitivity to both the seeding time and the aerosol release rates and support the aforementioned hypothesis.Language(s): English
Format: Digital (Free)Tags: Aerosols ; Impact studies ; Hurricane ; Natural hazards ; United States of America
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Measurement and simulation of the 16/17 April 2010 Eyjafjallajökull volcanic ash layer dispersion in the northern Alpine region
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Emeis S.; Forkel R.; Junkermann W.; et al. - Copernicus GmbH, 2011The spatial structure and the progression speed of the first ash layer from the Icelandic Eyjafjallajökull volcano which reached Germany on 16/17 April is investigated from remote sensing data and numerical simulations. The ceilometer network of the German Meteorological Service was able to follow the progression of the ash layer over the whole of Germany. This first ash layer turned out to be a rather shallow layer of only several hundreds of metres thickness which was oriented slantwise in the middle troposphere and which was brought downward by large-scale sinking motion over Southern Germa ...
[article]Measurement and simulation of the 16/17 April 2010 Eyjafjallajökull volcanic ash layer dispersion in the northern Alpine region
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Available online: http://dx.doi.org/10.5194/acp-11-2689-2011
S. Emeis ; R. Forkel ; W. Junkermann ; K. Schäfer ; H. Flentje ; S. Gilge ; W. Fricke ; M. Wiegner ; V. Freudenthaler ; S. Groβ ; L. Ries ; F. Meinhardt ; W. Birmili ; C. Münkel ; F. Obleitner ; P. Suppan
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2689-2701The spatial structure and the progression speed of the first ash layer from the Icelandic Eyjafjallajökull volcano which reached Germany on 16/17 April is investigated from remote sensing data and numerical simulations. The ceilometer network of the German Meteorological Service was able to follow the progression of the ash layer over the whole of Germany. This first ash layer turned out to be a rather shallow layer of only several hundreds of metres thickness which was oriented slantwise in the middle troposphere and which was brought downward by large-scale sinking motion over Southern Germany and the Alps. Special Raman lidar measurements, trajectory analyses and in-situ observations from mountain observatories helped to confirm the volcanic origin of the detected aerosol layer. Ultralight aircraft measurements permitted the detection of the arrival of a second major flush of volcanic material in Southern Germany. Numerical simulations with the Eulerian meso-scale model MCCM were able to reproduce the temporal and spatial structure of the ash layer. Comparisons of the model results with the ceilometer network data on 17 April and with the ultralight aircraft data on 19 April were satisfying. This is the first example of a model validation study from this ceilometer network data.
Language(s): English
Format: Digital (Free)Tags: Alps, the ; Region VI - Europe ; Atmosphere ; Airborne ash ; Volcanic Eruption ; Natural hazards
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Carbon dioxide atmospheric vertical profiles retrieved from space observation using ACE-FTS solar occultation instrument
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Foucher P.Y.; Chédin A.; Armante R.; et al. - Copernicus GmbH, 2011Major limitations of our present knowledge of the global distribution of CO2 in the atmosphere are the uncertainty in atmospheric transport and the sparseness of in situ concentration measurements. Limb viewing spaceborne sounders such as the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) offer a vertical resolution of a few kilometres for profiles, which is much better than currently flying or planned nadir sounding instruments can achieve. After having demonstrated the feasibility of obtaining CO2 vertical profiles in the 5–25 km altitude range with an accuracy of ...
[article]Carbon dioxide atmospheric vertical profiles retrieved from space observation using ACE-FTS solar occultation instrument
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Available online: http://dx.doi.org/10.5194/acp-11-2455-2011
P.Y. Foucher ; A. Chédin ; R. Armante ; C. Boone ; C. Crevoisier ; P. Bernath
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2455-2470Major limitations of our present knowledge of the global distribution of CO2 in the atmosphere are the uncertainty in atmospheric transport and the sparseness of in situ concentration measurements. Limb viewing spaceborne sounders such as the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) offer a vertical resolution of a few kilometres for profiles, which is much better than currently flying or planned nadir sounding instruments can achieve. After having demonstrated the feasibility of obtaining CO2 vertical profiles in the 5–25 km altitude range with an accuracy of about 2 ppm in a previous study, we present here the results of five years of ACE-FTS observations in terms of monthly mean profiles of CO2 averaged over 10° latitude bands for northern mid-latitudes. These results are compared with in-situ aircraft measurements and with simulations from two different air transport models. Key features of the measured altitude distribution of CO2 are shown to be accurately reproduced by the ACE-FTS retrievals: variation in altitude of the seasonal cycle amplitude and extrema, seasonal change of the vertical gradient, and mean growth rate. We show that small but significant differences from model simulations could result from an over estimation of the model circulation strength during the northern hemisphere spring. Coupled with column measurements from a nadir viewing instrument, it is expected that occultation measurements will bring useful constraints to the surface carbon flux determination.
Language(s): English
Format: Digital (Free)Tags: Atmosphere ; Carbon dioxide (CO2) ; Greenhouse gas (GHG)
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Optical properties of pristine ice crystals in mid-latitude cirrus clouds: a case study during CIRCLE-2 experiment
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Gayet J.-F.; Mioche G.; Shcherbakov V.; et al. - Copernicus GmbH, 2011In this paper, we describe in situ observations of mid-latitude cirrus cloud band carried out on 16 May 2007 during the CIRCLE-2 experiment. The Polar Nephelometer and the Cloud Particle Imager (CPI) instruments with PMS FSSP-300 and 2D-C probes were used for the description of the optical and microphysical cloud properties. Two selected cloud regions are compared and discussed in detail. Significant differences in optical properties are evidenced in terms of 22° halo occurrences even though prevalent planar-plate ice crystals are observed in both cloud regions. Featureless scattering phase fu ...
[article]Optical properties of pristine ice crystals in mid-latitude cirrus clouds: a case study during CIRCLE-2 experiment
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Available online: http://dx.doi.org/10.5194/acp-11-2537-2011
J.-F. Gayet ; G. Mioche ; V. Shcherbakov ; C. Gourbeyre ; R. Busen ; A. Minikin
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2537-2544In this paper, we describe in situ observations of mid-latitude cirrus cloud band carried out on 16 May 2007 during the CIRCLE-2 experiment. The Polar Nephelometer and the Cloud Particle Imager (CPI) instruments with PMS FSSP-300 and 2D-C probes were used for the description of the optical and microphysical cloud properties. Two selected cloud regions are compared and discussed in detail. Significant differences in optical properties are evidenced in terms of 22° halo occurrences even though prevalent planar-plate ice crystals are observed in both cloud regions. Featureless scattering phase functions are measured in the first cloud region located near the trailing edge of the cirrus-band at about 11 800 m/−57 °C. In contrast, well pronounced 22° halo peaks are observed with predominant similar-shaped ice crystals near the cirrus-band leading edge at 7100 m/−27 °C. CPI ice crystal images with Polar Nephelometer observations are carefully analysed and interpreted from a theoretical light scattering model in order to explain occurrence and non-occurrence of the 22° halo feature. The results highlight that the halo peaks are inherent only in perfect plate ice crystals (or pristine crystals). On the basis of previous datasets in mid-latitude cirrus, it is found that simple pristine crystals are uncommon whereas particles with imperfect or complex shapes are prevalent. As a result, phase functions that are smooth and featureless best represent cirrus scattering properties.
Language(s): English
Format: Digital (Free)Tags: Cirrus (Ci) ; Cloud ; Observations
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Transport analysis of ozone enhancement in Southern Ontario during BAQS-Met
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. He H.; Tarasick D.W.; Hocking W.K.; et al. - Copernicus GmbH, 2011Twice-daily ozonesondes were launched from Harrow, in southwestern Ontario, Canada, during the BAQS-Met (Border Air Quality and Meteorology Study) field campaign in June and July of 2007. A co-located radar windprofiler measured tropopause height continuously. These data, in combination with continuous surface ozone measurements and geo-statistical interpolation of satellite ozone observations, present a consistent picture and indicate that a number of significant ozone enhancements in the troposphere were observed that were the result of stratospheric intrusion events. The combined observatio ...
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Available online: http://dx.doi.org/10.5194/acp-11-2569-2011
H. He ; D.W. Tarasick ; W.K. Hocking ; T.K. Carey-Smith ; Y. Rochon ; J. Zhang ; P.A. Makar ; M. Osman ; J. Brook ; M.D. Moran ; D.B.A. Jones ; C. Mihele ; J.C. Wei ; G. Osterman ; P.S. Argall ; J. McConnell ; M.S. Bourqui
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2569-2583Twice-daily ozonesondes were launched from Harrow, in southwestern Ontario, Canada, during the BAQS-Met (Border Air Quality and Meteorology Study) field campaign in June and July of 2007. A co-located radar windprofiler measured tropopause height continuously. These data, in combination with continuous surface ozone measurements and geo-statistical interpolation of satellite ozone observations, present a consistent picture and indicate that a number of significant ozone enhancements in the troposphere were observed that were the result of stratospheric intrusion events. The combined observations have also been compared with results from two Environment Canada numerical models, the operational weather prediction model GEM (as input to FLEXPART), and a new version of the regional air quality model AURAMS, in order to examine the ability of these models to accurately represent sporadic cross-tropopause ozone transport events. The models appear to reproduce intrusion events with some skill, implying that GEM dynamics (which also drive AURAMS) are able to represent such events well. There are important differences in the quantitative comparison, however; in particular, the poor vertical resolution of AURAMS around the tropopause causes it to bring down too much ozone in individual intrusions.
Language(s): English
Format: Digital (Free)Tags: Canada ; Measure ; Observations ; Ozone ; Troposphere
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Mesoscale convective systems observed during AMMA and their impact on the NOx and O3 budget over West Africa
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Huntrieser H.; Schlager H.; Lichtenstern M.; et al. - Copernicus GmbH, 2011During the "African Monsoon Multidisciplinary Analysis" (AMMA) field phase in August 2006, a variety of measurements focusing on deep convection were performed over West Africa. The German research aircraft Falcon based in Ouagadougou (Burkina Faso) investigated the chemical composition in the outflow of large mesoscale convective systems (MCS). Here we analyse two different types of MCS originating north and south of the intertropical convergence zone (ITCZ, ~10° N), respectively. In addition to the airborne trace gas measurements, stroke measurements from the Lightning Location Network (LINE ...
[article]Mesoscale convective systems observed during AMMA and their impact on the NOx and O3 budget over West Africa
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Available online: http://dx.doi.org/10.5194/acp-11-2503-2011
H. Huntrieser ; H. Schlager ; M. Lichtenstern ; P. Stock ; T. Hamburger ; H. Höller ; K. Schmidt ; H.-D. Betz ; A. Ulanovsky ; F. Ravegnani
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2503-2536During the "African Monsoon Multidisciplinary Analysis" (AMMA) field phase in August 2006, a variety of measurements focusing on deep convection were performed over West Africa. The German research aircraft Falcon based in Ouagadougou (Burkina Faso) investigated the chemical composition in the outflow of large mesoscale convective systems (MCS). Here we analyse two different types of MCS originating north and south of the intertropical convergence zone (ITCZ, ~10° N), respectively. In addition to the airborne trace gas measurements, stroke measurements from the Lightning Location Network (LINET), set up in Northern Benin, are analysed. The main focus of the present study is (1) to analyse the trace gas composition (CO, O3, NO, NOx, NOy, and HCHO) in the convective outflow as a function of distance from the convective core, (2) to investigate how different trace gas compositions in the boundary layer (BL) and ambient air may influence the O3 concentration in the convective outflow, and (3) to estimate the rate of lightning-produced nitrogen oxides per flash in selected thunderstorms and compare it to our previous results for the tropics. The MCS outflow was probed at different altitudes (~10–12 km) and distances from the convective core (<500 km). Trace gas signatures similar to the conditions in the MCS inflow region were observed in the outflow close to the convective core, due to efficient vertical transport. In the fresh MCS outflow, low O3 mixing ratios in the range of 35–40 nmol mol−1 were observed. Further downwind, O3 mixing ratios in the outflow rapidly increased with distance, due to mixing with the ambient O3-rich air. After 2–3 h, O3 mixing ratios in the range of ~65 nmol mol−1 were observed in the aged outflow. Within the fresh MCS outflow, mean NOx (=NO+NO2) mixing ratios were in the range of ~0.3–0.4 nmol mol−1 (peaks ~1 nmol mol−1) and only slightly enhanced compared to the background. Both lightning-produced NOx (LNOx) and NOx transported upward from the BL contributed about equally to this enhancement. On the basis of Falcon measurements, the mass flux of LNOx in the investigated MCS was estimated to be ~100 g(N) s−1. The average stroke rate of the probed thunderstorms was 0.04–0.07 strokes s−1 (here only strokes with peak currents ≥10 kA contributing to LNOx were considered). The LNOx mass flux and the stroke rate were combined to estimate the LNOx production rate. For a better comparison with other published results, LNOx estimates per LINET stroke were scaled to Lightning Imaging Sensor (LIS) flashes. The LNOx production rate per LIS flash was estimated to 1.0 and 2.5 kg(N) for the MCS located south and north of the ITCZ, respectively. If we assume, that these different types of MCS are typical thunderstorms occurring globally (LIS flash rate ~44 s−1), the annual global LNOx production rate was estimated to be ~1.4 and 3.5 Tg(N) a−1.
Language(s): English
Format: Digital (Free)Tags: Region I - Africa ; West Africa ; Atmosphere ; Atmospheric circulation ; Monsoon
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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, 2011We 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 ...
[article]Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic Climate (ARCPAC) Project
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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.2423-2453We 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
Format: Digital (Free)Tags: Aerosols ; Atmospheric circulation ; Climate ; Impact studies ; Cloud formation ; Research ; Arctic
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HFC-152a and HFC-134a emission estimates and characterization of CFCs, CFC replacements, and other halogenated solvents measured during the 2008 ARCTAS campaign (CARB phase) over the South Coast Air Basin of California
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Barletta B.; Nissenson P.; Meinardi S.; et al. - Copernicus GmbH, 2011This work presents results from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) study. Whole air samples were obtained on board research flights that flew over California during June 2008 and analyzed for selected volatile organic compounds, including several halogenated species. Samples collected over the South Coast Air Basin of California (SoCAB), which includes much of Los Angeles (LA) County, were compared with samples from inflow air masses over the Pacific Ocean. The levels of many halocarbon species were enhanced significantly over t ...
[article]HFC-152a and HFC-134a emission estimates and characterization of CFCs, CFC replacements, and other halogenated solvents measured during the 2008 ARCTAS campaign (CARB phase) over the South Coast Air Basin of California
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Available online: http://dx.doi.org/10.5194/acp-11-2655-2011
B. Barletta ; P. Nissenson ; S. Meinardi ; D. Dabdub ; F. Sherwood Rowland ; R.A. VanCuren ; J. Pederson ; G.S. Diskin ; D.R. Blake
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2655-2669This work presents results from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) study. Whole air samples were obtained on board research flights that flew over California during June 2008 and analyzed for selected volatile organic compounds, including several halogenated species. Samples collected over the South Coast Air Basin of California (SoCAB), which includes much of Los Angeles (LA) County, were compared with samples from inflow air masses over the Pacific Ocean. The levels of many halocarbon species were enhanced significantly over the SoCAB, including compounds regulated by the Montreal Protocol and subsequent amendments. Emissions estimates of HFC-152a (1,1-difluoroethane, CH3CHF2; 0.82 ± 0.11 Gg) and HFC-134a (1,1,1,2-tetrafluoroethane, CH2FCF3; 1.16 ± 0.22 Gg) in LA County for 2008 were obtained using the observed HFC:carbon monoxide (CO) enhancement ratio. Emission rates also were calculated for the SoCAB (1.60 ± 0.22 Gg yr−1 for HFC-152a and 2.12 ± 0.28 Gg yr−1 for HFC-134a) and then extrapolated to the United States (32 ± 4 Gg yr−1 for HFC-152a and 43 ± 6 Gg yr−1 for HFC-134a) using population data. In addition, emission rates of the two HFCs in LA County and SoCAB were calculated by a second method that utilizes air quality modeling. Emissions estimates obtained using both methods differ by less than 25% for the LA County and less than 45% for the SoCAB.
Language(s): English
Format: Digital (Free)Tags: Aerosols ; Atmosphere ; Air pollution ; United States of America
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Ozone production in remote oceanic and industrial areas derived from ship based measurements of peroxy radicals during TexAQS 2006
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Sommariva R.; Brown S.S.; Roberts J.M.; et al. - Copernicus GmbH, 2011During the Texas Air Quality Study II (TexAQS 2006) campaign, a PEroxy Radical Chemical Amplifier (PERCA) was deployed on the NOAA research vessel R/V Brown to measure total peroxy radicals (HO2+Σ RO2). Day-time mixing ratios of HO2+Σ RO2 between 25 and 110 ppt were observed throughout the study area – the Houston/Galveston region and the Gulf coast of the US – and analyzed in relation to measurements of nitrogen oxides, volatile organic compounds (VOC) and photolysis rates to assess radical sources and sinks in the region.
[article]Ozone production in remote oceanic and industrial areas derived from ship based measurements of peroxy radicals during TexAQS 2006
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Available online: http://dx.doi.org/10.5194/acp-11-2471-2011
R. Sommariva ; S.S. Brown ; J.M. Roberts ; D.M. Brookes ; A.E. Parker ; P.S. Monks ; T.S. Bates ; D. Bon ; J.A. de Gouw ; G.J. Frost ; J.B. Gilman ; P.D. Goldan ; S.C. Herndon ; W.C. Kuster ; B.M. Lerner ; H.D. Osthoff ; S.C. Tucker ; C. Warneke ; E.J. Williams ; M.S. Zahniser
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2471-2485During the Texas Air Quality Study II (TexAQS 2006) campaign, a PEroxy Radical Chemical Amplifier (PERCA) was deployed on the NOAA research vessel R/V Brown to measure total peroxy radicals (HO2+Σ RO2). Day-time mixing ratios of HO2+Σ RO2 between 25 and 110 ppt were observed throughout the study area – the Houston/Galveston region and the Gulf coast of the US – and analyzed in relation to measurements of nitrogen oxides, volatile organic compounds (VOC) and photolysis rates to assess radical sources and sinks in the region.
Language(s): English
Format: Digital (Free)Tags: United States of America ; Ocean-atmosphere interaction ; Observations ; Ozone
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Understanding the transport of Patagonian dust and its influence on marine biological activity in the South Atlantic Ocean
Atmospheric Chemistry and Physics (ACP), Vol. 11. N° 3. Johnson M.S.; Meskhidze N.; Kiliyanpilakkil V.P.; et al. - Copernicus GmbH, 2011The supply of bioavailable iron to the high-nitrate low-chlorophyll (HNLC) waters of the Southern Ocean through atmospheric pathways could stimulate phytoplankton blooms and have major implications for the global carbon cycle. In this study, model results and remotely-sensed data are analyzed to examine the horizontal and vertical transport pathways of Patagonian dust and quantify the effect of iron-laden mineral dust deposition on marine biological productivity in the surface waters of the South Atlantic Ocean (SAO). Model simulations for the atmospheric transport and deposition of mineral du ...
[article]Understanding the transport of Patagonian dust and its influence on marine biological activity in the South Atlantic Ocean
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Available online: http://dx.doi.org/10.5194/acp-11-2487-2011
M.S. Johnson ; N. Meskhidze ; V.P. Kiliyanpilakkil ; S. Gassó
in Atmospheric Chemistry and Physics (ACP) > Vol. 11. N° 3 [03/01/2011] . - p.2487-2502The supply of bioavailable iron to the high-nitrate low-chlorophyll (HNLC) waters of the Southern Ocean through atmospheric pathways could stimulate phytoplankton blooms and have major implications for the global carbon cycle. In this study, model results and remotely-sensed data are analyzed to examine the horizontal and vertical transport pathways of Patagonian dust and quantify the effect of iron-laden mineral dust deposition on marine biological productivity in the surface waters of the South Atlantic Ocean (SAO). Model simulations for the atmospheric transport and deposition of mineral dust and bioavailable iron are carried out for two large dust outbreaks originated at the source regions of northern Patagonia during the austral summer of 2009. Model-simulated horizontal and vertical transport pathways of Patagonian dust plumes are in reasonable agreement with remotely-sensed data. Simulations indicate that the synoptic meteorological patterns of high and low pressure systems are largely accountable for dust transport trajectories over the SAO. According to model results and retrievals from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO), synoptic flows caused by opposing pressure systems (a high pressure system located to the east or north-east of a low pressure system) elevate the South American dust plumes well above the marine boundary layer. Under such conditions, the bulk concentration of mineral dust can quickly be transported around the low pressure system in a clockwise manner, follow the southeasterly advection pathway, and reach the HNLC waters of the SAO and Antarctica in ~3–4 days after emission from the source regions of northern Patagonia. Two different mechanisms for dust-iron mobilization into a bioavailable form are considered in this study. A global 3-D chemical transport model (GEOS-Chem), implemented with an iron dissolution scheme, is employed to estimate the atmospheric fluxes of soluble iron, while a dust/biota assessment tool (Boyd et al., 2010) is applied to evaluate the amount of bioavailable iron formed through the slow and sustained leaching of dust in the ocean mixed layer. The effect of iron-laden mineral dust supply on surface ocean biomass is investigated by comparing predicted surface chlorophyll-a concentration ([Chl-a]) to remotely-sensed data. As the dust transport episodes examined here represent large summertime outflows of mineral dust from South American continental sources, this study suggests that (1) atmospheric fluxes of mineral dust from Patagonia are not likely to be the major source of bioavailable iron to ocean regions characterized by high primary productivity; (2) even if Patagonian dust plumes may not cause visible algae blooms, they could still influence background [Chl-a] in the South Atlantic sector of the Southern Ocean.
Language(s): English
Format: Digital (Free)Tags: Argentina ; Atlantic Ocean ; Atmosphere ; Atmospheric circulation ; Thermohaline circulation ; Ocean-atmosphere interaction ; Oceans
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