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At least 703 records · Page 39

Source apportionment of soot particles and aqueous-phase processing of black carbon coatings in an urban environment

Abstract. The impacts of soot particles on climate and human health depend on the concentration of black carbon (BC) as well as the thickness and composition of the coating material, i.e., organic and inorganic compounds internally mixed with BC. In this study, the size-resolved chemical composition of BC-containing aerosol was measured using a high-resolution soot particle aerosol mass spectrometer (SP-AMS) during wintertime in Fresno, California, a location influenced by abundant combustion emissions and frequent fog events. Concurrently, particle optical properties were measured to investigate the BC absorption enhancement. Positive matrix factorization (PMF) analysis was performed on the SP-AMS mass spectral measurements to explore the sources of soot particles and the atmospheric processes affecting the properties of BC coatings. The analysis revealed that residential woodburning and traffic are the dominant sources of soot particles. Alongside primary soot particles originating from biomass burning (BBOABC) and vehicles (HOABC) two distinct types of processed BC-containing aerosol were identified: fog-related oxidized organic aerosol (FOOABC) and winter-background OOABC (WOOABC). Both types of OOABC showed evidence of having undergone aqueous processing, albeit with differences. The concentration of FOOABC was substantially elevated during fog events, indicating the formation of aqueous secondary organic aerosol (aqSOA) within fog droplets. On the other hand, WOOABC was present at a relatively consistent concentration throughout the winter and was likely related to the formation of secondary organic aerosol (SOA) in both the gas phase and aerosol liquid water. By comparing the chemical properties and temporal variations in FOOABC and WOOABC, we gain insights into the key aging processes of BC aerosol. It was found that aqueous-phase reactions facilitated by fog droplets had a significant impact on the thickness and chemical composition of BC coatings, thereby affecting the light absorption and hygroscopic properties of soot particles. These findings underscore the important role of chemical reactions occurring within clouds and fogs and influencing the climate forcing of BC aerosol in the atmosphere.

54 ENVIRONMENTAL SCIENCES↗

MODIS Aerosol Observations used to Constrain Dust Distributions and Lifecycle in the NASA GEOS-5 Model

Approximately 240 Tg of mineral dust aerosol are transported annually from Saharan Africa to the Atlantic Ocean. Dust affects the Earth radiation budget, and plays direct (through scattering and absorption of radiation) and indirect (through modification of cloud properties and environment) roles in climate. Deposition of dust to the surface provides an important nutrient source to terrestrial and oceanic ecosystems. Dust is additionally a contributor to adverse air quality. Among the tools toward understanding the lifecycle and impacts of mineral dust aerosols are numerical models. Important constraints on these models come from quantitative satellite observations, like those from the space-based Moderate Resolution Imaging Spectroradiometer (MODIS). In particular, Kauhan et al. [2005] used MODIS aerosol observations to infer transport and deposition fluxes of Saharan dust over the Atlantic, Caribbean, and Amazonian basins. Those observations are used here to constrain the transport of dust and its interannual variability simulated in the NASA GEOS-5 general circulation model and data assimilation system. Significant uncertainty exists in the MODIS-derived fluxes, however, due to uncertainty in the wind fields provided by meteorological analyses in this region. That same uncertainty in the wind fields is manifest in our GEOS-5 simulations of dust distributions. Here we use MODIS observations to investigate the seasonality and location of the Saharan dust plume and explore through sensitivity analysis of our model the meteorological controls on the dust distribution, including dust direct radiative effects and sub-gridscale source and sink processes.

Colarco, P.↗

Limits on the diurnal variation of H2 quadrupole features in Neptune

Spectral profiles of the H2 S4(0) and S4(1) lines are presented for Neptune on three consecutive nights; no variation is detected in the equivalent widths of the H2 4-0 features to within an observational uncertainty of about 20 percent. Comparisons with previous H2 quadrupole observations indicate that no secular trends have been detected over about 15 yr. The equivalent-width error limits are interpreted in terms of the maximum variability of Neptunian tropospheric aerosols. Specifically, the error bars for the globally averaged equivalent widths of the two H2 quadrupole absorption features constrain the bottom of the visible atmosphere, as defined by a bright optically infinite isotropically scattering cloud, to be 2.9 + or - 0.6 bars, while the methane haze opacity is constrained to be 0.30 + or - 0.25.

Smith, Wm. Hayden↗

Retrieval and molecule sensitivity studies for the global ozone monitoring experiment and the scanning imaging absorption spectrometer for atmospheric chartography

The Global Ozone Monitoring Experiment (GOME) and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) are diode based spectrometers that will make atmospheric constituent and aerosol measurements from European satellite platforms beginning in the mid 1990's. GOME measures the atmosphere in the UV and visible in nadir scanning, while SCIAMACHY performs a combination of nadir, limb, and occultation measurements in the UV, visible, and infrared. A summary is presented of the sensitivity studies that were performed for SCIAMACHY measurements. As the GOME measurement capability is a subset of the SCIAMACHY measurement capability, the nadir, UV, and visible portion of the studies is shown to apply to GOME as well.

Chance, Kelly V.↗

The effect of the Mt. Pinatubo aerosol on the NHO3 column over Mauna Loa, Hawaii

A very high resolution infrared solar spectrometer system for the Network for Detection of Stratospheric Change has been routinely operated at the Mauna Loa Observatory in Hawaii since November, 1991. Solar absorption spectra are normally taken one day a week at sunrise. We report the analysis of these spectra for the vertical column amount of nitric acid (HNO3) vapor. The observations began four months after the arrival of volcanic aerosols from Mt. Pinatubo over the site. Although quite variable, total HNO3 columns were initially about 7 x 10(exp 15) molecules/sq cm and have decreased about 30% in the following two years.

David, Shelle J.↗

Identifying Chemical Aerosol Signatures Using Optical Suborbital Observations: How Much Can Optical Properties Tell us about Aerosol Composition?

Improvements in air quality and Earth’s climate predictions require improvements of the aerosol speciation in chemical transport models, using observational constraints. Aerosol speciation (e.g., organic aerosols, black carbon, sulfate, nitrate, ammonium, dust or sea salt) is typically determined using in situ instrumentation. Continuous, routine surface network aerosol composition measurements are not uniformly widespread over the globe. Satellites, on the other hand, can provide a maximum coverage of the horizontal and vertical atmosphere but observe aerosol optical properties (and not aerosol speciation) based on remote sensing instrumentation. Combinations of satellite-derived aerosol optical properties can inform on air mass aerosol types (AMTs e.g., clean marine, dust, polluted continental). However, these AMTs are subjectively defined, might often be misclassified and are hard to relate to the critical parameters that need to be refined in models. In this paper, we derive AMTs that are more directly related to sources and hence to speciation. They are defined, characterized, and derived using simultaneous in situ gas-phase, chemical and optical instruments on the same aircraft during the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS, US, summer of 2013). First, we prescribe well-informed AMTs that display distinct aerosol chemical and optical signatures to act as a training AMT dataset. These in situ observations reduce the errors and ambiguities in the selection of the AMT training dataset. We also investigate the relative skill of various combinations of aerosol optical properties to define AMTs and how much these optical properties can capture dominant aerosol speciation. We find distinct optical signatures for biomass burning (from agricultural or wildfires), biogenic and dust-influence AMTs. Useful aerosol optical properties to characterize these signatures are the extinction angstrom exponent (EAE), the single scattering albedo, the difference of single scattering albedo in two wavelengths, the absorption coefficient, the absorption angstrom exponent (AAE), and the real part of the refractive index (RRI). We find that all four AMTs studied when prescribed using mostly airborne in situ gas measurements, can be successfully extracted from at least three combinations of airborne in situ aerosol optical properties (e.g., EAE, AAE and RRI) over the US during SEAC4RS. However, we find that the optically based classifications for BB from agricultural fires and polluted dust include a large percentage of misclassifications that limit the usefulness of results relating to those classes. The technique and results presented in this study are suitable to develop a representative, robust and diverse source-based AMT database. This database could then be used for widespread retrievals of AMTs using existing and future remote sensing suborbital instruments/networks. Ultimately, it has the potential to provide a much broader observational aerosol data set to evaluate chemical transport and air quality models than is currently available by direct in situ measurements. This study illustrates how essential it is to explore existing airborne datasets to bridge chemical and optical signatures of different AMTs, before the implementation of future spaceborne missions (e.g., the next generation of Earth Observing System (EOS) satellites addressing Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables).

Meloe S F Kacenelenbogen↗

An attribution of the low single-scattering albedo of biomass burning aerosol over the southeastern Atlantic

Abstract. Aerosol over the remote southeastern Atlantic is some of the most sunlight-absorbing aerosol on the planet: the in situ free-tropospheric single-scattering albedo at the 530 nm wavelength (SSA530 nm) ranges from 0.83 to 0.89 within ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) aircraft flights from late August–September. Here we seek to explain the low SSA. The SSA depends strongly on the black carbon (BC) number fraction, which ranges from 0.15 to 0.4. Low organic aerosol (OA)-to-BC mass ratios of 8–14 and modified combustion efficiency values >0.975 point indirectly to the dry, flame-efficient combustion of primarily grass fuels, with back trajectories ending in the miombo woodlands of Angola. The youngest aerosol, aged 4–5 d since emission, occupied the top half of a 5 km thick plume sampled directly west of Angola with a vertically consistent BC:ΔCO (carbon monoxide) ratio, indicating a homogenization of the source emissions. The younger aerosol, transported more quickly off of the continent by stronger winds, overlaid older, slower-moving aerosol with a larger mean particle size and fraction of BC-containing particles. This is consistent with ongoing gas condensation and the coagulation of smaller non-BC particles upon the BC-containing particles. The particle volumes and OA:BC mass ratios of the older aerosol were smaller, attributed primarily to evaporation following fragmentation, instead of dilution or thermodynamics. The CLARIFY (CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017) aircraft campaign sampled aerosols that had traveled further to reach the more remote Ascension Island. CLARIFY reported higher BC number fractions, lower OA:BC mass ratios, and lower SSA yet larger mass absorption coefficients compared to this study's. Values from one ORACLES 2017 flight, held midway to Ascension Island, are intermediate, confirming the long-range changes. Overall the data are most consistent with continuing oxidation through fragmentation releasing aerosols that subsequently enter the gas phase, reducing the OA mass, rather than evaporation through dilution or thermodynamics. The data support the following best fit: SSA530nm=0.801+0055⋅(OA:BC) (r=0.84). The fires of southern Africa emit approximately one-third of the world's carbon; the emitted aerosols are distinct from other regional smoke emissions, and their composition needs to be represented appropriately to realistically depict regional aerosol radiative effects.

54 ENVIRONMENTAL SCIENCES↗

Determination of the ground albedo and the index of absorption of atmospheric particulates by remote sensing. I - Theory

A statistical technique is developed for inferring the optimum values of the ground albedo and the effective imaginary term of the complex refractive index of atmospheric particulates. The procedure compares measurements of the ratio of the hemispheric diffuse to directly transmitted solar flux density at the earth's surface with radiative transfer computations of the same as suggested by Herman et al. (1975). A detailed study is presented which shows the extent to which the ratio of diffuse to direct solar radiation is sensitive to many of the radiative transfer parameters. Results indicate that the optical depth and size distribution of atmospheric aerosol particles are the two parameters which uniquely specify the radiation field to the point where ground albedo and index of absorption can be inferred. Varying the real part of the complex refractive index of atmospheric particulates as well as their vertical distribution is found to have a negligible effect on the diffuse-direct ratio. The statistical procedure utilizes a semi-analytic gradient search method from least-squares theory and includes a detailed error analysis.

King, M. D.↗

Characterizing the Vertical Profile of Aerosol Particle Extinction and Linear Depolarization over Southeast Asia and the Maritime Continent: The 2007-2009 View from CALIOP

Vertical profiles of 0.532 μm aerosol particle extinction coefficient and linear volume depolarization ratio are described for Southeast Asia and the Maritime Continent. Quality-screened and cloud-cleared Version 3.01 Level 2 NASA Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) 5-km Aerosol Profile datasets are analyzed from 2007 to 2009. Numerical simulations from the U.S. Naval Aerosol Analysis and Predictive System (NAAPS), featuring two-dimensional variational assimilation of NASA Moderate Resolution Imaging Spectroradiometer and Multi-angle Imaging Spectro- Radiometer quality-assured datasets, combined with regional ground-based lidar measurements, are considered for assessing CALIOP retrieval performance, identifying bias, and evaluating regional representativeness. CALIOP retrievals of aerosol particle extinction coefficient and aerosol optical depth (AOD) are high over land and low over open waters relative to NAAPS (0.412/0.312 over land for all data points inclusive, 0.310/0.235 when the per bin average is used and each is treated as single data points; 0.102/0.151 and 0.086/0.124, respectively, over ocean). Regional means, however, are very similar (0.180/0.193 for all data points and 0.155/0.159 when averaged per normalized bin), as the two factors offset one another. The land/ocean offset is investigated, and discrepancies attributed to interpretation of particle composition and a-priori assignment of the extinction-to-backscatter ratio ("lidar ratio") necessary for retrieving the extinction coefficient from CALIOP signals. Over land, NAAPS indicates more dust present than CALIOP algorithms are identifying, indicating a likely assignment of a higher lidar ratio representative of more absorptive particles. NAAPS resolvesmore smoke overwater than identified with CALIOP, indicating likely usage of a lidar ratio characteristic of less absorptive particles to be applied that biases low AOD there. Over open waters except within the Bay of Bengal, aerosol particle scattering is largely capped below 1.5 km MSL, though ground-based lidar measurements at Singapore differ slightly from this finding. Significant aerosol particle presence over land is similarly capped near 3.0 km MSL over most regions. Particle presence at low levels regionally, except over India, is dominated by relatively non-depolarizing particles. Industrial haze, sea salt droplets and fresh smoke are thus most likely present.

linear volume depolarization ratio↗

An improved Venus cloud model

An inhomogeneous cloud model for Venus is presented in which a (transparent) sulfuric acid aerosol extends above the tropopause, but an (absorbing) sulfur aerosol consisting of much larger particles does not. It is shown that the temperature dependence of the absorption spectrum of sulfur, combined with the lapse rate in the planet's atmosphere, can explain the color of Venus. A simple 'black-white' radiative-transfer model is developed, the spectral reflectance of the cloud model is computed for the 60-km level in Marov's (1972) model atmosphere, and strong evidence is obtained that sulfur is the UV absorber on Venus. The wavelength variation of contrast in UV cloud features is analyzed, and absorption is found to increase with depth at every wavelength due to the inward increase in temperature. The black-white model is applied to CO2 absorption, variations in CO2 and UV absorption with phase angle are compared, and line profiles are calculated for pressure-broadened CO2 lines. The theoretical results are compared with Venera 9 and 10 data.

Young, A. T.↗

Inference of the aerosol Angstrom coefficient from SAGE short-wavelength data

SAGE four-channel transmission profiles are inverted to retrieve the extinction profiles from which the aerosol Angstrom coefficient alpha is obtained. The procedure allows one to check the influence of the NO2 absorption profile, which is small below 25 km. The results compare well with those obtained by a completely different procedure at NASA Langley Research Center, and the main features of the alpha profiles seem to be significant, even considering the rather large error bars. The relation between the retrieved Angstrom coefficient, the particle effective radius and the asymmetry factor is considered.

Lenoble, J.↗

Pole-to-Pole Distribution of Stratospheric Black Carbon (Soot) Aerosol from Aircraft

The distribution of black carbon (soot) aerosol (BCA) in the atmosphere is of interest for several reasons: (1) Because BCA has the highest absorption cross section of any compound known, it can absorb solar radiation to cause atmospheric warming. (2) Because it is a strong adsorber of gases, it can catalyze heterogeneous reactions to change the chemical composition of the atmosphere.(3) If aircraft are a major source of BCA, it is an important tracer of aircraft emissions. Analysis for BCA of impactor samples from Arctic and Antarctic deployments, utilizing particle morphology of scanning electron microscopy images, permits the following conclusions: (1) The BCA concentration in the northern stratosphere varies between 0 and 2.6 ng m-3 averaging 0.6 ng/cu m. (2) This BCA loading is commensurate with estimated fuel consumptions in the stratosphere by the current commercial fleet and an emission index E=0.03 g BCA per kg fuel burnt which was measured in jet exhaust at al titude.Thus, most stratospheric BCA in the northern stratosphere results from aircraft emissions. The background BCA concentration in the southern stratosphere varies between 0 and 0.6 ng cu m averaging 0.1 ng/cu m. This strong meridional gradient implies that stratospheric BCA residence time- is shorter than are mixing times between hemispheres. Projected annual fuel consumption of a future supersonic commercial fleet is 7E13 g. This fleet would increase stratospheric BCA loadings by a factor of 2-3, because almost all fuel would be burnt above the tropopause. An improved EI(BCA) by a factor of ten would result in an increase of stratospheric BCA loadings by approximately 50 %.

Pueschel, R. F.↗

Dispersion of the Volcanic Sulfate Cloud from the Mount Pinatubo Eruption

We simulate the transport of the volcanic cloud from the 1991 eruption of Mount Pinatubo with the GEOS-5 general circulation model. Our simulations are in good agreement with observational data. We tested the importance of initial condition corresponding to the specific meteorological situation at the time of the eruption by employing reanalysis from MERRA. We found no significant difference in the transport of the cloud. We show how the inclusion of the interaction between volcanic sulfate aerosol and radiation is essential for a reliable simulation of the transport of the volcanic cloud. The absorption of long wave radiation by the volcanic sulfate induces a rising of the volcanic cloud up to the middle stratosphere, combined with divergent motion from the latitude of the eruption to the tropics. Our simulations indicate that the cloud diffuses to the northern hemisphere through a lower stratospheric pathway, and to mid- and high latitudes of the southern hemisphere through a middle stratospheric pathway, centered at about 30 hPa. The direction of the middle stratospheric pathway depends on the season. We did not detect any significant change of the mixing between tropics and mid- and high latitudes in the southern hemisphere.

Aquila, Valentina↗

Comparison of Aerosol Single Scattering Albedos Derived by Diverse Techniques In Two North Atlantic Experiments

Aerosol single scattering albedo omega (the ratio of scattering to extinction) is important in determining aerosol climatic effects, in explaining relationships between calculated and measured radiative fluxes, and in retrieving aerosol optical depths from satellite radiances. Recently, two experiments in the North Atlantic region, the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the Second Aerosol Characterization Experiment (ACE-2), determined aerosol omega by a variety of techniques. The techniques included fitting of calculated to measured radiative fluxes; retrievals of omega from skylight radiances; best fits of complex refractive index to profiles of backscatter extinction, and size distribution; and in situ measurements of scattering and absorption at the surface and aloft. Both TARFOX and ACE-2 found a fairly wide range of values for omega at midvisable wavelengths approx. 550 nm, with omega(sub midvis) greater than or equal to 0.85 and less than or equal to 0.99 for the marine aerosol impacted by continental pollution. Frequency distributions of omega could usually be approximated by lognormals in omega(sub max) - omega, with some occurrence of bimodality, suggesting the influence of different aerosol sources or processing. In both TARFOX and ACE-2, closure tests between measured and calculated radiative fluxes yielded best-fit values of omega(sub midvis) 0.90 +/- 0.04 for the polluted boundary layer. Although these results have the virtue of describing the column aerosol unperturbed by sampling, they are subject to questions about representativeness and other uncertainties (e.g., thermal offsets, unknown gas absorption) The other techniques gave larger values for omega(sub midvis) for the polluted boundary layer, with a typical result of omega(sub midvis) = 0.95 +/- 0.04. Current uncertainties in omega are large in terms of climate effects More tests are needed of the consistency among different methods and of humidification effects on omega.

Russell, P. B.↗

Widespread Biomass Burning Smoke Throughout the Remote Troposphere

Biomass burning emits ~34–41 Tg yr−1 of smoke aerosol to the atmosphere. Biomass burning aerosol directly influences the Earth’s climate by attenuation of solar and terrestrial radiation; however, its abundance and distribution on a global scale are poorly constrained, particularly after plumes dilute into the background remote troposphere and are subject to removal by clouds and precipitation. Here we report global-scale, airborne measurements of biomass burning aerosol in the remote tropo-sphere. Measurements were taken during four series of seasonal flights over the Pacific and Atlantic Ocean basins, each with near pole-to-pole latitude coverage. We find that biomass burning particles in the remote troposphere are dilute but ubiquitous, accounting for one-quarter of the accumulation-mode aerosol number and one-fifth of the aerosol mass. Comparing our obser-vations with a high-resolution global aerosol model, we find that the model overestimates biomass burning aerosol mass in the remote troposphere with a mean bias of >400%, largely due to insufficient wet removal by in-cloud precipitation. After updat-ing the model’s aerosol removal scheme we find that, on a global scale, dilute smoke contributes as much as denser plumes to biomass burning’s scattering and absorption effects on the Earth’s radiation field.

Biomass burning↗

The Relationship Of Size Distributions To Spectral (300 - 700 Nm) Extinction Parameterization Of Ambient In Situ Aerosols Measured During FIREX-AQ And The Influence Of Aerosol Composition

Hyperspectral (300 - 700 nm, 0.7 nm resolution) aerosol extinction spectra were measured at seven fires in six states in the western United States during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign in July and August 2019. Obtained using an in situ aerosol sampling method, these spectra are directly comparable to other in situ aerosol measurements such as size distribution and composition. A previous deployment of the in situ Spectral Aerosol Extinction (SpEx) instrument that measured fine mode aerosols (50% size cut of 1.3 µm particle diameter) around the Korean peninsula showed that over this spectral range 2nd order polynomials provided a better fit to the logarithmically transformed spectra than linear fits (representative of Ångström exponents). The two fit parameters (a1, a2) of the polynomials are related to the classic Ångström exponent but provide additional information via their two-dimensional parameter space. The previous work was limited by the lack of commensurate size distribution information. Here, using the FIREX-AQ spectra set it is possible to expand on the previous analysis in three specific ways: 1) size distribution information is available to further elucidate how size distribution maps into (a1, a2) space, 2) the sampled size distributions include larger particles than the Korean study, and 3) the FIREX-AQ data set exhibits smoke-related spectral features in the UV part of the spectrum that are not present in background air nor were they observed previously in the Korean study. The UV spectral features are particularly intriguing as they likely arise from the absorption component of the extinction measurement and therefore may be related to composition. The relationships between the ambient in situ aerosol size distributions, the extinction spectra, and composition will be presented.

Carolyn Jordan↗

NOAA backscatter studies

In the past year, NOAA has measured and analyzed another year's worth of backscatter over Boulder, CO. The average profile was computed from 80 satellite observations of backscatter spread throughout the year, using NOAA's CO2 coherent lidar operating at a wavelength of 10.59 microns. The seasonal averages show a familiar trend (highest backscattering in spring, perhaps due to Asian dust or biomass burning, and lowest backscattering in fall). The 1990 average profile was not significantly different from the 1988 or 1989 profiles, except that it displays a slight increase in the upper troposphere, perhaps due to the Redoubt Volcano. The NOAA's backscatter processing program (BETA) was refined to enable the calculation of gaseous absorption effects based on rawinsonde measurements, as well as using atmospheric models. NOAA participated in two intercomparisons of aerosol measuring instruments near Boulder, called FRLAB (Front Range Lidar, Aircraft, and Balloon Experiment). Considerable effort was also put into developing a multiagency science proposal to NASA headquarters to work with both JPL and NASA-Marshall to produce an airborne Doppler lidar facility for the DC-8.

Post, Madison J.↗

A pulsed CO2 Doppler lidar for boundary layer monitoring

A monostatic, master oscillator power amplifier (MOPA), CO2 pulsed Doppler lidar was constructed and tested. The system is compact (120 x 60 cm), operates at high pulse repetition rates (greater than 1 kHz) and is intended for simultaneous Doppler/Differential Absorption Lidar (DIAL) monitoring of the planetary boundary layer. Details of the system design, hard target calibrations, and aerosol returns are presented.

Pearson, Guy N.↗