Measurements of submicron aerosol composition, light scattering, and size distribution were made from 17 October to 15 November 2008 at the elevated Paposo site (25° 0.4' S, 70° 27.01' W, 690 m ...a.s.l.) on the Chilean coast as part of the VOCALS* Regional Experiment (REx). Based on the chemical composition measurements, a receptor modeling analysis using Positive Matrix Factorization (PMF) was carried out, yielding four broad source categories of the aerosol mass, light scattering coefficient, and a proxy for cloud condensation nucleus (CCN) concentration at 0.4% supersaturation derived from the size distribution measurements assuming an observed soluble mass fraction of 0.53. The sources resolved were biomass burning, marine, an urban-biofuels mix and a somewhat ambiguous mix of smelter emissions and mineral dust. The urban-biofuels mix is the most dominant aerosol mass component (52%) followed by biomass burning (25%), smelter/soil dust (12%) and marine (9%) sources. The average (mean±std) submicron aerosol mass concentration, aerosol light scattering coefficient and proxy CCN concentration were, 8.77±5.40 μg m−3, 21.9±11.0 Mm−1 and 548±210 cm−3, respectively. Sulfate is the dominant identified submicron species constituting roughly 40% of the dry mass (3.64±2.30 μg m−3), although the indentified soluble species constitute only 53% of the mass. Much of the unidentified mass is likely organic in nature. The relative importance of each aerosol source category is different depending upon whether mass, light scattering, or CCN concentration is being considered, indicating that the mean size of aerosols associated with each source are different. Marine aerosols do not appear to contribute to more than 10% to either mass, light scattering, or CCN concentration at this site. Back trajectory cluster analysis proved consistent with the PMF source attribution. *VOCALS: VAMOS** Ocean-Cloud-Atmosphere-Land Study (VOCALS) **VAMOS: Variability of American Monsoon System
During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. ...These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.
The Community Atmosphere Model (CAM5), equipped with a technique to tag black carbon (BC) emissions by source regions and types, has been employed to establish source–receptor relationships for ...atmospheric BC and its deposition to snow over western North America. The CAM5 simulation was conducted with meteorological fields constrained by reanalysis for year 2013 when measurements of BC in both near-surface air and snow are available for model evaluation. We find that CAM5 has a significant low bias in predicted mixing ratios of BC in snow but only a small low bias in predicted atmospheric concentrations over northwestern USA and western Canada. Even with a strong low bias in snow mixing ratios, radiative transfer calculations show that the BC-in-snow darkening effect is substantially larger than the BC dimming effect at the surface by atmospheric BC. Local sources contribute more to near-surface atmospheric BC and to deposition than distant sources, while the latter are more important in the middle and upper troposphere where wet removal is relatively weak. Fossil fuel (FF) is the dominant source type for total column BC burden over the two regions. FF is also the dominant local source type for BC column burden, deposition, and near-surface BC, while for all distant source regions combined the contribution of biomass/biofuel (BB) is larger than FF. An observationally based positive matrix factorization (PMF) analysis of the snow-impurity chemistry is conducted to quantitatively evaluate the CAM5 BC source-type attribution. While CAM5 is qualitatively consistent with the PMF analysis with respect to partitioning of BC originating from BB and FF emissions, it significantly underestimates the relative contribution of BB. In addition to a possible low bias in BB emissions used in the simulation, the model is likely missing a significant source of snow darkening from local soil found in the observations.
Nucleation in the atmosphere Hegg, D A; Baker, M B
Reports on progress in physics,
05/2009, Letnik:
72, Številka:
5
Journal Article
Recenzirano
Small particles play major roles in modulating radiative and hydrological fluxes in the atmosphere and thus they impact both climate (IPCC 2007) and weather. Most atmospheric particles outside clouds ...are created in situ through nucleation from gas phase precursors and most ice particles within clouds are formed by nucleation, usually from the liquid. Thus, the nucleation process is of great significance in the Earth's atmosphere.
While stand alone satellite and model aerosol products see wide utilization, there is a significant need in numerous atmospheric and climate applications for a fused product on a regular grid. ...Aerosol data assimilation is an operational reality at numerous centers, and like meteorological reanalyses, aerosol reanalyses will see significant use in the near future. Here we present a standardized 2003–2013 global 1 × 1° and 6-hourly modal aerosol optical thickness (AOT) reanalysis product. This data set can be applied to basic and applied Earth system science studies of significant aerosol events, aerosol impacts on numerical weather prediction, and electro-optical propagation and sensor performance, among other uses. This paper describes the science of how to develop and score an aerosol reanalysis product. This reanalysis utilizes a modified Navy Aerosol Analysis and Prediction System (NAAPS) at its core and assimilates quality controlled retrievals of AOT from the Moderate Resolution Imaging Spectroradiometer (MODIS) on Terra and Aqua and the Multi-angle Imaging SpectroRadiometer (MISR) on Terra. The aerosol source functions, including dust and smoke, were regionally tuned to obtain the best match between the model fine- and coarse-mode AOTs and the Aerosol Robotic Network (AERONET) AOTs. Other model processes, including deposition, were tuned to minimize the AOT difference between the model and satellite AOT. Aerosol wet deposition in the tropics is driven with satellite-retrieved precipitation, rather than the model field. The final reanalyzed fine- and coarse-mode AOT at 550 nm is shown to have good agreement with AERONET observations, with global mean root mean square error around 0.1 for both fine- and coarse-mode AOTs. This paper includes a discussion of issues particular to aerosol reanalyses that make them distinct from standard meteorological reanalyses, considerations for extending such a reanalysis outside of the NASA A-Train era, and examples of how the aerosol reanalysis can be applied or fused with other model or remote sensing products. Finally, the reanalysis is evaluated in comparison with other available studies of aerosol trends, and the implications of this comparison are discussed.
Aircraft-based measurements of aerosol light-scattering coefficient, cloud condensation nuclei (CCN) measured directly or by proxy, and aerosol chemical composition are reported for three different ...years in the region of the large stratocumulus deck off the California coast. Receptor modeling is used to differentiate the contributions of the main aerosol sources to the light scattering and CCN activity. The contribution of anthropogenic sources to the two climatically important aerosol parameters (for direct and indirect forcing) varied from year to year but, on average, was found to be 67% in the case of CCN concentration and 57% in the case of light-scattering coefficient.
Aerosol column optical depths derived from airborne Sun photometer and in situ measurements of aerosol properties in 14 vertical profiles off the mid‐Atlantic coast of the United States in June show ...excellent agreement. Simultaneous measurements of the chemical compositions of the aerosol allows an assessment of the chemical apportionment of the aerosol column optical depths. The optical depths had essentially three chemical components, which, in order of descending average contributions, were condensed water, carbonaceous species, and sulfate. These results do not support the common assumption that sulfate dominates aerosol optical depths in polluted regions.
In this paper we report results of aircraft measurements of mass concentrations of carbonaceous aerosols, total aerosol mass, and simultaneously determined light scattering and absorption ...coefficients onshore and offshore of the eastern coast of the United States. We describe the sampling and analytical methodology used to derive spatially resolved aerosol carbon concentrations and discuss these in the context of other concurrently collected data. The carbon mass was, on average, 50% of the total dry aerosol mass. The carbon mass fraction tended to increase with altitude, suggesting that ground‐based measurements can significantly underestimate the importance of carbon species in the column aerosol mass budget. The aerosol carbon mass was significantly correlated with aerosol light absorption, suggesting that the black and organic carbon components have, at least in part, common combustion sources. A regression of the light absorption coefficient onto carbon mass suggests that ∼10% of the carbon mass is in the form of black (light‐absorbing) carbon.
Aerosol samples were collected and cloud condensation nuclei (CCN) concentrations at five supersaturations were measured along and off the central California coast within the cloud-topped, marine ...boundary layer from aircraft flights during August 2007. Receptor modelling has been applied to estimate the natural versus anthropogenic source contribution of cloud condensation nuclei in this region, a region of climatically important marine stratocumulus. The results suggest that anthropogenic CCN accounted for about 50% of the CCN active at 0.3% supersaturation in this region during the measurement period.
We assess the consistency (closure) between solar beam attenuation by aerosols and water vapor measured by airborne Sun photometry and derived from airborne in situ and ship‐based lidar measurements ...during the April 2001 Asian Pacific Regional Aerosol Characterization Experiment (ACE‐Asia). The airborne data presented here were obtained aboard the Twin Otter aircraft. Comparing aerosol extinction σep(550 nm) from four different techniques shows good agreement for the vertical distribution of aerosol layers. However, the level of agreement in absolute magnitude of the derived aerosol extinction varied among the aerosol layers sampled. The σep(550 nm) computed from airborne in situ size distribution and composition measurements shows good agreement with airborne Sun photometry in the marine boundary layer but is considerably lower in layers dominated by dust if the particles are assumed to be spherical. The σep(550 nm) from airborne in situ scattering and absorption measurements are about ∼13% lower than those obtained from airborne Sun photometry during 14 vertical profiles. Combining lidar and the airborne Sun photometer measurements reveals the prevalence of dust layers at altitudes up to 10 km with layer aerosol optical depth (from 3.5 to 10 km altitude) of ∼0.1 to 0.2 (500 nm) and extinction‐to‐backscatter ratios of 59–71 sr (523 nm). The airborne Sun photometer aboard the Twin Otter reveals a relatively dry atmosphere during ACE‐Asia with all water vapor columns <1.5 cm and water vapor densities ρw < 12 g/m3. Comparing layer water vapor amounts and ρw from the airborne Sun photometer to the same quantities measured with aircraft in situ sensors leads to a high correlation (r2 = 0.96), but the Sun photometer tends to underestimate ρw by 7%.
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