An instrument for measuring size-resolved aerosol hygroscopicity at both sub- and super-micron sizes

The article of record as published may be found at http://dx.doi.org/10.1080/02786820701506955A new instrument to measure the size-resolved hygroscopic growth of both sub- and super-micron atmospheric aerosol is described. It consists of two white-light optical particle counters measuring the same sample aerosol simultaneously at two different controlled relative humidities. Calibration with aerosols of different refractive index confirms the expected relative insensitivity of the instrument to index of refraction. Data obtained in the field from airborne sampling support the utility of the instrument in measuring differences in size-resolved hygroscopicity in the marine boundary layer and also in addressing the issue of kinetic limitations to aerosol condensational growth.Office of Naval ResearchGrant no. N0014-97-1-013

Sources of light-absorbing aerosol in arctic snow and their seasonal variation

Two data sets consisting of measurements of light absorbing aerosols (LAA) in arctic snow together with suites of other corresponding chemical constituents are presented; the first from Siberia, Greenland and near the North Pole obtained in 2008, and the second from the Canadian arctic obtained in 2009. A preliminary differentiation of the LAA into black carbon (BC) and non-BC LAA is done. Source attribution of the light absorbing aerosols was done using a positive matrix factorization (PMF) model. Four sources were found for each data set (crop and grass burning, boreal biomass burning, pollution and marine). For both data sets, the crops and grass biomass burning was the main source of both LAA species, suggesting the non-BC LAA was brown carbon. Depth profiles at most of the sites allowed assessment of the seasonal variation in the source strengths. The biomass burning sources dominated in the spring but pollution played a more significant (though rarely dominant) role in the fall, winter and, for Greenland, summer. The PMF analysis is consistent with trajectory analysis and satellite fire maps

Water-Soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution, and Distribution

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

Aerosol Properties and Chemical Apportionment of Aerosol Optical Depth at Locations off the U.S. East Coast in July and August 2001

Airborne in situ measurements of vertical profiles of the aerosol light scattering coefficient, light absorption coefficient, and single scattering albedo (ω0) are presented for locations off the East Coast of the United States in July–August 2001. The profiles were obtained in relatively clean air, dominated by airflows that had passed over Canada and the Atlantic Ocean. Comparisons of aerosol optical depths (AODs) at 550 nm derived from airborne in situ and sun-photometer measurements agree, on average, to within 0.034 ± 0.021. A frequency distribution of ω0 measured in the atmospheric boundary layer off the coast yields an average value of ω0 = 0.96 ± 0.03 at 550 nm. Values for the mass scattering efficiencies of sulfate and total carbon (organic and black carbon) derived from a multiple linear regression are 6.0 ± 1.0 m2 (g SO=4)−1 and 2.6 ± 0.9 m2 (g C)−1, respectively. Measurements of sulfate and total carbon mass concentrations are used to estimate the contributions of these two major components of the submicron aerosol to the AOD. Mean percentage contributions to the AOD from sulfate, total carbon, condensed water, and absorbing aerosols are 38% ± 8%, 26% ± 9%, 32% ± 9%, and 4% ± 2%, respectively. The sensitivity of the above results to the assumed values of the hygroscopic growth factors for the particles are examined and it is found that, although the AOD derived from the in situ measurements can vary by as much as 20%, the average value of ω0 is not changed significantly. The results are compared with those obtained in the same region in 1996 under more polluted conditions

Clear-Column Radiative Closure During ACE-Asia: Comparison of Multiwavelength Extinction Derived from Particle Size and Composition with Results from Sun Photometry

From March to May 2001, aerosol size distributions and chemical compositions were measured using differential mobility analyzers (DMA), an aerodynamic particle sizer (APS), Micro-Orifice Uniform Deposit Impactors (MOUDI), and denuder samplers onboard the Twin Otter aircraft as part of the Aerosol Characterization Experiment (ACE)-Asia campaign. Of the 19 research flights, measurements on four flights that represented different aerosol characteristics are analyzed in detail. Clear-column radiative closure is studied by comparing aerosol extinctions predicted using in situ aerosol size distribution and chemical composition measurements to those derived from the 14-wavelength NASA Ames Airborne Tracking Sun photometer (AATS-14). In the boundary layer, pollution layers, and free troposphere with no significant mineral dust present, aerosol extinction closure was achieved within the estimated uncertainties over the full range of wavelengths of AATS-14. Aerosol extinctions predicted based on measured size distributions also reproduce the wavelength dependence derived from AATS-14 data. Considering all four flights, the best fit lines yield Predicted/Observed ratios in boundary and pollution layers of 0.97 ± 0.24 and 1.07 ± 0.08 at λ = 525 nm and 0.96 ± 0.21 and 1.08 ± 0.08 at λ = 1059 nm, respectively. In free troposphere dust layers, aerosol extinctions predicted from the measured size distributions were generally smaller than those derived from the AATS-14 data, with Predicted/Observed ratios of 0.65 ± 0.06 and 0.66 ± 0.05 at 525 and 1059 nm, respectively. A detailed analysis suggests that the discrepancy is likely a result of the lack of the knowledge of mineral dust shape as well as variations in aerosol extinction derived from AATS-14 data when viewing through horizontally inhomogeneous layers

An 11-Year Global Gridded Aerosol Optical Thickness Reanalysis (v1.0) for Atmospheric and Climate Sciences

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

Clear-sky closure studies of lower tropospheric aerosol and water vapor during ACE-2 using airborne sunphotometer, airborne in-situ, space-borne, and ground-based measurements

We report on clear-sky column closure experiments (CLEARCOLUMN) performed in the Canary Islands during the second Aerosol Characterization Experiment (ACE-2) in June/July 1997. We present CLEARCOLUMN results obtained by combining airborne sunphotometer and in-situ (optical particle counter, nephelometer, and absorption photometer) measurements taken aboard the Pelican aircraft, space-borne NOAA/AVHRR data and ground-based lidar and sunphotometer measurements. During both days discussed here, vertical profiles flown in cloud-free air masses revealed 3 distinctly different layers: a marine boundary layer (MBL) with varying pollution levels, an elevated dust layer, and a very clean layer between the MBL and the dust layer. A key result of this study is the achievement of closure between extinction or layer aerosol optical depth (AOD) computed from continuous in-situ aerosol size-distributions and composition and those measured with the airborne sunphotometer. In the dust, the agreement in layer AOD (λ=380–1060 nm) is 3–8%. In the MBL there is a tendency for the in-situ results to be slightly lower than the sunphotometer measurements (10–17% at λ=525 nm), but these differences are within the combined error bars of the measurements and computations

Experimental and Modeling Studies of Secondary Organic Aerosol Formation and Some Applications to the Marine Boundary Layer

A series of controlled experiments were carried out in the Calspan Corporation\u27s 600 m3environmental chamber to study some secondary organic aerosol formation processes. Three precursor-ozone systems were studied: cyclopentene-ozone, cyclohexene-ozone, and α-pineneozone. Additionally, SO2 was added to the initial gas mixture in several instances and was likely present at trace levels in the ostensibly organic-only experiments. It was found that all three systems readily formed new submicron aerosols at very low reactant levels. The chemical composition of formed aerosols was consistent with some previous studies, but the yields of organic products were found to be lower in the Calspan experiments. A three-step procedure is proposed to explain the observed particle nucleation behavior: HO · production → H2SO4 formation → H2SO4-H2O (perhaps together with NH3) homogeneous nucleation. It is also proposed that some soluble organic products would partition into the newly formed H2SO4-H2O nuclei, enhance water condensation, and quickly grow these nuclei into a larger size range. While the observations in the two cycloolefin-ozone systems could be well explained by these proposed mechanisms, the exact nature of the nucleation process in the α-pinene-ozone system remains rather opaque and could be the result of nucleation involving certain organics. The results from three simple modeling studies further support these proposals. Their applicability to the marine boundary layer (MBL) is also discussed in some detail. Particularly, such a particle nucleation and growth process could play an important role in secondary aerosol formation and, quite likely, CCN formation as well in certain MBL regions