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Climatic Effects of 1950-2050 Changes in US Anthropogenic Aerosols: Aerosol Trends and Radiative Forcing - Part 1

We calculate decadal aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950-2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980-2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970-1990, with values over the eastern US (east of 100 deg W) of −2.0Wm(exp−2 for direct forcing including contributions from sulfate (−2.0Wm−2), nitrate (−0.2Wm(exp−2), organic carbon (−0.2Wm(exp−2), and black carbon (+0.4Wm(exp−2). The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50 %. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8Wm(exp−2) direct and 1.0Wm(exp−2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3Wm(exp−2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide) suggests that a US emission control strategy focused on BC would have only limited climate benefit.

climate change

Ground-based Network and Supersite Measurements for Studying Aerosol Properties and Aerosol-Cloud Interactions

From radiometric principles, it is expected that the retrieved properties of extensive aerosols and clouds from reflected/emitted measurements by satellite (and/or aircraft) should be consistent with those retrieved from transmitted/emitted radiance observed at the surface. Although space-borne remote sensing observations contain large spatial domain, they are often plagued by contamination of surface signatures. Thus, ground-based in-situ and remote-sensing measurements, where signals come directly from atmospheric constituents, the sun, and the Earth-atmosphere interactions, provide additional information content for comparisons that confirm quantitatively the usefulness of the integrated surface, aircraft, and satellite datasets. The development and deployment of AERONET (AErosol RObotic NETwork) sunphotometer network and SMART-COMMIT (Surface-sensing Measurements for Atmospheric Radiative Transfer - Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile supersite are aimed for the optimal utilization of collocated ground-based observations as constraints to yield higher fidelity satellite retrievals and to determine any sampling bias due to target conditions. To characterize the regional natural and anthropogenic aerosols, AERONET is an internationally federated network of unique sunphotometry that contains more than 250 permanent sites worldwide. Since 1993, there are more than 480 million aerosol optical depth observations and about 15 sites have continuous records longer than 10 years for annual/seasonal trend analyses. To quantify the energetics of the surface-atmosphere system and the atmospheric processes, SMART-COMMIT instrument into three categories: flux radiometer, radiance sensor and in-situ probe. Through participation in many satellite remote-sensing/retrieval and validation projects over eight years, SMART-COMMIT have gradually refine( and been proven vital for field deployment. In this paper, we will demonstrate the capability of AERONET SMART-COMMIT in current Asian Monsoon Year-2008 campaigns that are designed and being executed to study the compelling variability in temporal scale of both anthropogenic and natural aerosols (e.g., airborne dust, smoke, mega-city pollutant). Feedback mechanisms between aerosol radiative effects and monsoon dynamics have been recently proposed, however there is a lack of consensus on whether aerosol forcing would be more likely to enhance or reduce the strength of the monsoon circulation. We envision robust approaches which well-collocated ground-based measurements and space-borne observations will greatly advance our understanding of absorbing aerosols (e.g., "Global Dimming" vs. "Elevated Heat-Pump" effects) on aerosol cloud water cycle interactions.

Tsay, Si-Chee

Cloud Cover Increase with Increasing Aerosol Absorptivity: A Counterexample to the Conventional Semidirect Aerosol Effect

We reexamine the aerosol semidirect effect using a general circulation model and four cases of the single-scattering albedo of dust aerosols. Contrary to the expected decrease in low cloud cover due to heating by tropospheric aerosols, we find a significant increase with increasing absorptivity of soil dust particles in regions with high dust load, except during Northern Hemisphere winter. The strongest sensitivity of cloud cover to dust absorption is found over land during Northern Hemisphere summer. Here even medium and high cloud cover increase where the dust load is highest. The cloud cover change is directly linked to the change in relative humidity in the troposphere as a result of contrasting changes in specific humidity and temperature. More absorption by aerosols leads to larger diabatic heating and increased warming of the column, decreasing relative humidity. However, a corresponding increase in the specific humidity exceeds the temperature effect on relative humidity. The net effect is more low cloud cover with increasing aerosol absorption. The higher specific humidity where cloud cover strongly increases is attributed to an enhanced convergence of moisture driven by dust radiative heating. Although in some areas our model exhibits a reduction of low cloud cover due to aerosol heating consistent with the conventional description of the semidirect effect, we conclude that the link between aerosols and clouds is more varied, depending also on changes in the atmospheric circulation and the specific humidity induced by the aerosols. Other absorbing aerosols such as black carbon are expected to have a similar effect.

Perlwitz, Jan

AOD Distributions and Trends of Major Aerosol Species over a Selection of the World's Most Populated Cities Based on the 1st Version of NASA's MERRA Aerosol Reanalysis

NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003-2015) and over a selection of 200 of the world's most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don't tend to fluctuate significantly on an annual basis.

Urban air pollution

Aerosol Detection from the Cloud Aerosol Transport System on the International Space Station: Algorithm Overview and Implications for Diurnal Sampling

Concentrations of particulate aerosols and their vertical placement in the atmosphere determine their interaction with the Earth system and their impact on air quality. Space-based lidar, such as the Cloud–Aerosol Transport System (CATS) technology demonstration instrument, is well-suited for determining the vertical structure of these aerosols and their diurnal cycle. Through the implementation of aerosol-typing algorithms, vertical layers of aerosols are assigned a type, such as marine, dust, and smoke, and a corresponding extinction-to-backscatter (lidar) ratio. With updates to the previous aerosol-typing algorithms, we find that CATS, even as a technology demonstration, observed the documented seasonal cycle of aerosols, comparing favorably with the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) space-based lidar and the NASA Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA-2) model reanalysis. By leveraging the unique orbit of the International Space Station, we find that CATS can additionally resolve the diurnal cycle of aerosol altitude as observed by ground-based instruments over the Maritime Continent of Southeast Asia.

Edward P Nowottnick

Applying Orbital Multi-Angle Photopolarimetric Observations to Study Properties of Aerosols in the Earth's Atmosphere: Implications of Measurements in the 1.378 µm Spectral Channel to Retrieve Microphysical Characteristics and Composition of Stratospheric Aerosols

We analyze the possibilities of orbital photopolarimetric measurements to study properties of aerosols in the Earth's atmosphere. As an example, we consider the case when such measurements are performed within a narrow spectral channel centered at 1.378 µm that allows to retrieve microphysical characteristics of stratospheric aerosols separately from those of tropospheric aerosols. We consider the case of stratospheric aerosols caused by volcanic eruption, and adopt the model of the stratosphere in the form of a homogeneous plane-parallel layer composed of polydisperse spherical particles. We use numerically exact solutions of the vector radiative transfer equation to theoretically simulate measurements carried out at various numbers of scattering angles, including: (i) radiance measurements alone; (ii) polarization measurements alone; and (iii) radiance and polarization measurements together. The results of computations show that the simultaneous use of radiance and polarization measurements at a sufficiently large number of scattering angles enables one to retrieve the optical thickness, effective radius, and refractive index of aerosols with adequate accuracy. We demonstrate how the accuracy of the derived values of the optical parameters of aerosols depends on the accuracy of measurements of the intensity and polarization of the reflected light, optical thickness of aerosol layer itself, effective radius of aerosols, width of the particle size distribution, and number of viewing angles.

Aerosols

Retrieval of Aerosol Optical Properties From GOCI-II Observations: Continuation of Long-Term Geostationary Aerosol Monitoring Over East Asia

Since the Geostationary Ocean Color Imager (GOCI) was successfully launched in 2010, the GOCI Yonsei aerosol retrieval (YAER) algorithm has been continuously updated to retrieve hourly aerosol optical properties. GOCI-II has 4 more channels including UV, finer spatial resolution (250 m), and daily full disk coverage as compared to GOCI, and was launched in February 2020, onboard the GEO-KOMPSAT-2B (GK-2B) satellite. In this study, we extended the YAER algorithm to GOCI-II data based on its improved performance in many aspects and present the first results of aerosol optical properties retrieved from GOCI-II data. Utilizing the overlapping period between the GOCI-II and GOCI in geostationary Earth orbit, we present GOCI-II aerosol retrievals for high aerosol-loading cases over East Asia and show that these have a consistent spatial distribution with those from GOCI. Furthermore, GOCI-II provides AOD at an even higher spatial resolution, revealing finer changes in aerosol concentrations. Validation results for one year data show that the GOCI-II AOD has a correlation coefficient of 0.83 and a ratio within the expected error (EE) of 59.4 % when compared with the aerosol robotic network (AERONET) data. We compared statistical metrics for the GOCI and GOCI-II AODs to assess the consistency between the two datasets. In addition, it was found that there is a strong correlation between the two datasets from the comparison of gridded GOCI and GOCI-II AOD products. It is expected that data from GOCI-II will continue long-term aerosol records with high accuracy that can be used to address air-quality issues over East Asia.

AOD

Evaluation of UKESM aerosol size and composition using ATom measurements indicates missing marine aerosol formation mechanisms

Atmospheric aerosols influence climate through their interactions with radiation and clouds, yet large uncertainties remain in their simulation by global models. This study evaluates the United Kingdom Earth System Model version 1.1 (UKESM1.1) using global-scale aircraft observations from the Atmospheric Tomography (ATom) mission, focusing on aerosol lifecycle processes in the remote marine atmosphere. We assess model performance in simulating aerosol precursor vapours, number size distributions, chemical composition, and environmental conditions. Several process improvements are tested, including sulfuric acid-ammonia nucleation, ammonium nitrate scheme, methanesulfonic acid condensation, and low-temperature isoprene-derived secondary organic aerosol formation. Model biases differ significantly between the upper troposphere (UT) and the marine boundary layer (MBL). In the UT, UKESM1.1 overestimates nucleation and Aitken mode particles while underestimating accumulation mode, indicating insufficient growth. In the MBL, the model overestimates primary aerosols (e.g. seasalt) and precursor gases but underestimates nucleation and Aitken mode particles, even after incorporating updated nucleation and ammonium nitrate scheme. The persistence of low aerosol number concentrations, despite overestimated precursors, suggests missing formation pathways likely involving other species such as iodine, amines, and organic vapours. These limitations result in an unbalanced cloud condensation nuclei budget that over-relies on primary emissions. Sensitivity tests reveal that model outputs are strongly influenced by dimethyl sulfide emissions and vapour condensation schemes. Our results highlight the need for future model development to prioritise mechanistic representation of currently missing aerosol sources, rather than relying on empirical tuning, to improve aerosol-climate interaction estimates.

He, Xu-Cheng [Univ. of Cambridge (United Kingdom);

Aerosol effect on Umkehr ozone profiles using Stratospheric Aerosol and Gas Experiment II measurements

This study examines 1211 cases of coincident ozone profiles derived from 1164 Umkehrs and 928 Stratospheric Aerosol and Gas Experiment II (SAGE II) profiles within 1000 km and 12 hours between October 1984 and April 1989 to study the stratospheric-aerosol effect on Umkehr ozone profiles. Because of the close correspondence of stratospheric aerosol optical depth at the SAGE II-measured 0.525-micrometer wavelength and the extrapolated 0.32 Umkehr wavelength determined in this study we use the 0.525-micrometer data to determine the aerosol effect on Umkehr profiles. At the 95% confidence level, we find the following errors to the Umkehr ozone amounts: in Umkehr layer 9 (-2.9 +/- 2.1), layer 8 (-2.3 +/- 1.1), layer 7 (0.1 +/- 1.1), layer 6 (2.2 +/- 1.0), layer 5 (-1.5 +/- 0.8), and layer 4 (-2.4 +/- 1.7) in percent ozone amount per 0.01 stratospheric aerosol optical depth. These results agree with previous theoretical and empirical studies within their respective error bounds in layers 9, 8, and 7. The results in layers 6, 5, and 4 differ significantly from those in previous works. Using only those eight stations with more than 47 coincidences results in mean aerosol effects that are not significantly different from the 14-station results. Because SAGE II and Umkehr produce different ozone retrievals in layer 9 and because the intralayer correlation of SAGE II ozone and aerosol in layer 9 is nonzero, one must exercise some caution in attributing the entire SAGE II-Umkehr difference in this layer to an aerosol effect.

Newchurch, M. J.

Global Aerosol Radiative Forcing Derived from Sea WiFS-Inferred Aerosol Optical Properties

Aerosol optical properties inferred from the Sea-viewing Wide Field-of-view Sensor (SeaWiFS) radiance measurements are used to compute the aerosol shortwave radiative forcing using a radiative transfer model. The aerosol optical thickness at the wavelength of 865-nm is taken from the SeaWIFS archive. It is found that the nominal optical thickness over oceans ranges from 0.1 to 0.2. Using a maritime aerosol model and the radiances measured at the various SeaWiFS channels, the Angstrom exponent is determined to be 0.2174, the single-scattering albedo to be 0.995, and the asymmetry factor to be 0.786. The radiative transfer model has eight bands in the visible and ultraviolet spectral regions and three bands in the near infrared. It includes the absorption due to aerosols, water vapor, carbon dioxide, and oxygen, and the scattering due to aerosols and gases (Rayleigh scattering). The radiative forcing is computed over global oceans for four months (January, April, July, and October, 1998) to represent four seasons. It is found that the aerosol radiative forcing is large and changes significantly with seasons near the continents with large-scale forest fires and desert dust. Averaged over oceans and the four months, the aerosol radiative forcing is approximately 7 W/sq m at the top of the atmosphere. This large radiative forcing is expected to have a significant cooling effect on the Earth's climate as implied from simulations of a number of general circulation models.

Chou, Ming-Dah

North Atlantic Aerosol Radiative Impacts Based on Satellite Measurements and Aerosol Intensive Properties from TARFOX and ACE-2

We estimate the impact of North Atlantic aerosols on the net short-wave flux at the tropopause by combining satellite-derived aerosol optical depth (AOD) maps with model aerosol properties determined via closure analyses in TARFOX and ACE 2. We exclude African dust, primarily by restricting latitudes to 25-60 N. The analyses use in situ aerosol composition measurements and air- and ship-borne sun-photometer measurements of AOD spectra. The aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. Its midvisible single-scattering albedo is 0.9. which is in the range obtained from in situ measurements of scattering and absorption in both TARFOX and ACE 2. Combining satellite-derived AOD maps with the aerosol model yields maps of 24-hour average net radiative flux changes. For simultaneous AVHRR, radiance measurements exceeded the sunphotometer AODs by about 0.04. However. shipboard sunphotometer and AVHRR AODs agreed Within 0.02 for data acquired during satellite overflights on two other days. We discuss attempts to demonstrate column closure within the MBL by comparing shipboard sunphotometer AODs and values calculated from simultaneous shipboard in-situ aerosol size distribution measurements. These comparisons were mostly unsuccessful, but they illustrate the difficulties inherent in this type of closure analysis. Specifically, AODs derived from near-surface in-situ size distribution measurements are extremely sensitive to the assumed hygroscopic growth model that itself requires an assumption of particle composition as a function of height and size, to the radiosonde-measured relative humidity, and to the vertical profile of particle number. We investigate further the effects of hygroscopic particle growth within the MBL by using shipboard lidar aerosol backscatter profiles together with the sunphotometer AOD.

Russell, P. B.

On the Feasibility of Studying Shortwave Aerosol Radiative Forcing of Climate Using Dual-Wavelength Aerosol Backscatter Lidar

The current low confidence in the estimates of aerosol-induced perturbations of Earth's radiation balance is caused by the highly non-uniform compositional, spatial and temporal distributions of tropospheric aerosols on a global scale owing to their heterogeneous sources and short lifetimes. Nevertheless, recent studies have shown that the inclusion of aerosol effects in climate model calculations can improve agreement with observed spatial and temporal temperature distributions. In light of the short lifetimes of aerosols, determination of their global distribution with space-borne sensors seems to be a necessary approach. Until recently, satellite measurements of tropospheric aerosols have been approximate and did not provide the full set of information required to determine their radiative effects. With the advent of active aerosol remote sensing from space (e.g., PICASSO-CENA), the applicability fo lidar-derived aerosol 180 deg -backscatter data to radiative flux calculations and hence studies of aerosol effects on climate needs to be investigated.

Redemann, Jens

Remote Sensing of Aerosol and Non-Aerosol Absorption

Remote sensing of aerosol from the new satellite instruments (e.g. MODIS from Terra) and ground based radiometers (e.g. the AERONET) provides the opportunity to measure the absorption characteristics of the ambient undisturbed aerosol in the entire atmospheric column. For example Landsat and AERONET data are used to measure spectral absorption of sunlight by dust from West Africa. Both Application of the Landsat and AERONET data demonstrate that Saharan dust absorption of solar radiation is several times smaller than the current international standards. This is due to difficulties of measuring dust absorption in situ, and due to the often contamination of dust properties by the presence of air pollution or smoke. We use the remotely sensed aerosol absorption properties described by the spectral sin le scattering albedo, together with statistics of the monthly optical thickness for the fine and coarse aerosol derived from the MODIS data. The result is an estimate of the flux of solar radiation absorbed by the aerosol layer in different regions around the globe where aerosol is prevalent. If this aerosol forcing through absorption is not included in global circulation models, it may be interpreted as anomalous absorption in these regions. In a preliminary exercise we also use the absorption measurements by AERONET, to derive the non-aerosol absorption of the atmosphere in cloud free conditions. The results are obtained for the atmospheric windows: 0.44 microns, 0.66 microns, 0.86 microns and 1.05 microns. In all the locations over the land and ocean that were tested no anomalous absorption in these wavelengths, was found within absorption optical thickness of +/- 0.005.

Kaufman, Y. J.

Evaluation of SAGE II and Balloon-Borne Stratospheric Aerosol Measurements: Evaluation of Aerosol Measurements from SAGE II, HALOE, and Balloonborne Optical Particle Counters

Stratospheric aerosol measurements from the University of Wyoming balloonborne optical particle counters (OPCs), the Stratospheric Aerosol and Gas Experiment (SAGE) II, and the Halogen Occultation Experiment (HALOE) were compared in the period 1982-2000, when measurements were available. The OPCs measure aerosol size distributions, and HALOE multiwavelength (2.45-5.26 micrometers) extinction measurements can be used to retrieve aerosol size distributions. Aerosol extinctions at the SAGE II wavelengths (0.386-1.02 micrometers) were computed from these size distributions and compared to SAGE II measurements. In addition, surface areas derived from all three experiments were compared. While the overall impression from these results is encouraging, the agreement can change with latitude, altitude, time, and parameter. In the broadest sense, these comparisons fall into two categories: high aerosol loading (volcanic periods) and low aerosol loading (background periods and altitudes above 25 km). When the aerosol amount was low, SAGE II and HALOE extinctions were higher than the OPC estimates, while the SAGE II surface areas were lower than HALOE and the OPCS. Under high loading conditions all three instruments mutually agree to within 50%.

Hervig, Mark

Dependence of Aerosol Light Absorption and Single-Scattering Albedo On Ambient Relative Humidity for Sulfate Aerosols with Black Carbon Cores

Atmospheric aerosols frequently contain hygroscopic sulfate species and black carbon (soot) inclusions. In this paper we report results of a modeling study to determine the change in aerosol absorption due to increases in ambient relative humidity (RH), for three common sulfate species, assuming that the soot mass fraction is present as a single concentric core within each particle. Because of the lack of detailed knowledge about various input parameters to models describing internally mixed aerosol particle optics, we focus on results that were aimed at determining the maximum effect that particle humidification may have on aerosol light absorption. In the wavelength range from 450 to 750 nm, maximum absorption humidification factors (ratio of wet to 'dry=30% RH' absorption) for single aerosol particles are found to be as large as 1.75 when the RH changes from 30 to 99.5%. Upon lesser humidification from 30 to 80% RH, absorption humidification for single particles is only as much as 1.2, even for the most favorable combination of initial ('dry') soot mass fraction and particle size. Integrated over monomodal lognormal particle size distributions, maximum absorption humidification factors range between 1.07 and 1.15 for humidification from 30 to 80% and between 1.1 and 1.35 for humidification from 30 to 95% RH for all species considered. The largest humidification factors at a wavelength of 450 nm are obtained for 'dry' particle size distributions that peak at a radius of 0.05 microns, while the absorption humidification factors at 700 nm are largest for 'dry' size distributions that are dominated by particles in the radius range of 0.06 to 0.08 microns. Single-scattering albedo estimates at ambient conditions are often based on absorption measurements at low RH (approx. 30%) and the assumption that aerosol absorption does not change upon humidification (i.e., absorption humidification equal to unity). Our modeling study suggests that this assumption alone can introduce absolute errors in estimates of the midvisible single-scattering albedo of up to 0.05 for realistic dry particle size distributions. Our study also indicates that this error increases with increasing wavelength. The potential errors in aerosol single-scattering albedo derived here are comparable in magnitude and in addition to uncertainties in single-scattering albedo estimates that are based on measurements of aerosol light absorption and scattering.

Redemann, Jens

Aerosol-Cloud Interactions during Tropical Deep Convection: Evidence for the Importance of Free Tropospheric Aerosols

NASA's 2002 CRYSTAL-FACE field experiment focused on the formation and evolution of tropical cirrus cloud systems in southern Florida. Multiple aircraft extensively sampled cumulonimbus dynamical and microphysical properties, as well as characterizing ambient aerosol populations both inside and outside the full depth of the convective column. On July 18, unique measurements were taken when a powerful updraft was traversed directly by aircraft, providing a window into the primary source region of cumulonimbus anvil crystals. Observations of the updraft, entered at approximately l0 km altitude and -34 C, indicated more than 200 cloud particles per mL at vertical velocities exceeding 20 m/s and the presence of significant condensation nuclei and liquid water within the core. In this work, aerosol and cloud phase observations are integrated by simulating the updraft conditions using a large-eddy resolving model with 3 explicit multiphase microphysics, including treatment of size-resolved aerosol fields, aerosol activation and freezing, and evaporation of cloud particles back to the aerosol phase. Simulations were initialized with observed thermodynamic and aerosol size distributions profiles and convection was driven by surface fluxes assimilated from the ARPS forecast model. Model results are consistent with the conclusions that most crystals are homogeneously frozen droplets and that entrained free tropospheric aerosols may contribute a significant fraction of the crystals. Thus most anvil crystals appear to be formed aloft in updraft cores, well above cloud base. These conclusions are supported by observations of hydrometeor size distribution made while traversing the dore, as well as aerosol and cloud particle size distributions generally observed by aircraft below 4km and crystal properties generally observed by aircraft above 12km.

Ackerman, A.

Temporal Variation of Aerosol Properties at a Rural Continental Site and Study of Aerosol Evolution through Growth Law Analysis

Aerosol size distributions were measured by a Scanning Mobility Particle Sizer (SMPS) onboard the CIRPAS Twin Otter aircraft during 16 flights at the Southern Great Plains (SGP) site in northern central Oklahoma as part of the Aerosol Intensive Operation period in May, 2003. During the same period a second SMPS was deployed at a surface station and provided continuous measurements. Combined with trace gas measurements at the SGP site and back-trajectory analysis, the aerosol size distributions provided insights into the sources of aerosols observed at the SGP site. High particle concentrations, observed mostly during daytime, were well correlated with the sulfur dioxide (SO2) mixing ratios, suggesting nucleation involving sulfuric acid is likely the main source of newly formed particles at the SGP. Aerosols within plumes originating from wildfires in Central America were measured at the surface site. Vertically compact aerosol layers, which can be traced back to forest fires in East Asia, were intercepted at altitudes over 3000 meters. Analyses of size dependent particle growth rates for four periods during which high cloud coverage was observed indicate growth dominated by volume controlled reactions. Sulfate accounts for 50% to 72% of the increase in aerosol volume concentration; the rest of the volume concentration increase was likely due to secondary organic species. The growth law analyses and meteorological conditions indicate that the sulfate was produced mainly through aqueous oxidation of SO2 in clouds droplets and hydrated aerosol particles.

Wang, Jian

HSRL-2 Observations of Aerosol Variability During an Aerosol Build-up Event in Houston and Comparisons With WRF-Chem

The NASA Langley airborne multi-wavelength High Spectral Resolution Lidar (HSRL-2) provides vertical distribution of aerosol optical properties as curtains of aerosol extinction, backscatter and depolarization along the flight track, plus intensive properties that are used to infer aerosol type and external mixing of types. Deployed aboard the NASA Langley King Air on the DISCOVER-AQ field mission in Houston in September 2013, HSRL-2 flew a pattern that included 18 ground sites, repeated four times a day, coordinated with a suite of airborne in situ measurements. The horizontally and vertically resolved curtains of HSRL-2 measurements give an unparalleled view of the spatial and temporal variability of aerosol, which provide broad context for interpreting other measurements and models. Detailed comparisons of aerosol extinction are made with the WRF-Chem chemical transport model along the HSRL-2 flight path. The period from Sept. 11-14 is notable for a large aerosol build-up and persistent smoke layers. We investigate the aerosol properties using the vertically resolved HSRL-2 measurements and aerosol typing analysis plus WRFChem model tracers and back trajectories, and modeling of humidification effects.

Burton, Sharon P.