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Scientific Objectives, Measurement Needs, and Challenges Motivating the PARAGON Aerosol Initiative
Aerosols are involved in a complex set of processes that operate across many spatial and temporal scales. Understanding these processes, and ensuring their accurate representation in models of transport, radiation transfer, and climate, requires knowledge of aerosol physical, chemical, and optical properties and the distributions of these properties in space and time. To derive aerosol climate forcing, aerosol optical and microphysical properties and their spatial and temporal distributions, and aerosol interactions with clouds, need to be understood. Such data are also required in conjunction with size-resolved chemical composition in order to evaluate chemical transport models and to distinguish natural and anthropogenic forcing. Other basic parameters needed for modeling the radiative influences of aerosols are surface reflectivity and three-dimensional cloud fields. This large suite of parameters mandates an integrated observing and modeling system of commensurate scope. The Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) concept, designed to meet this requirement, is motivated by the need to understand climate system sensitivity to changes in atmospheric constituents, to reduce climate model uncertainties, and to analyze diverse collections of data pertaining to aerosols. This paper highlights several challenges resulting from the complexity of the problem. Approaches for dealing with them are offered in the set of companion papers.
Optical properties of Southern Hemisphere aerosols: Report of the joint CSIRO/NASA study
This study was made in support of the LAWS and GLOBE programs, which aim to design a suitable Doppler lidar system for measuring global winds from a satellite. Observations were taken from 5 deg S to 45 deg S along and off the E and SE Australian coast, thus obtaining representative samples over a large latitude range. Observations were made between 0 and 6 km altitude of aerosol physical and chemical properties in situ from the CSIRO F-27 aircraft; of lidar backscatter coefficients at 10.6 micron wavelength from the F-27 aircraft; of lidar backscatter profiles at 0.694 microns at Sale, SE Australia; and of lidar backscatter profiles at 0.532 microns at Cowley Beach, NE Australia. Both calculations and observations in the free troposphere gave a backscatter coefficient of 1-2 x 10 to the -11/m/sr at 10.6 microns, although the accuracies of the instruments were marginal at this level. Equivalent figures were 2-8 x 10 to the -9/m/sr (aerosol) and 9 x 10 to the -9 to 2 x 10 to the -8/m/sr (lidar) at 0.694 microns wavelength at Sale; and 3.7 x 10 to the -9/m/sr (aerosol) and 10 to the -8 to 10 to the -7/m/sr (lidar) at 0.532 microns wavelength at Cowley Beach. The measured backscatter coefficients at 0.694 and 0.532 microns were consistently higher than the values calculated from aerosol size distributions by factors of typically 2 to 10.
Modeling the Optical Properties of Biomass Burning Aerosols: Young Smoke Aerosols From Savanna Fires and Comparisons to Observations from SAFARI 2000
Annually, farmers in southern Africa manage their land resources and prepare their fields for cultivation by burning crop residual debris, with a peak in the burning season occurring during August and September. The emissions from these fires in southern Africa are among the greatest from fires worldwide, and the gases and aerosol particles produced adversely affect air quality large distances from their source regions, and can even be tracked in satellite imagery as they cross the Atlantic and Pacific Ocean basins. During August and September 2000 an international group of researchers participating in the Southern African Regional Science Initiate field experiment (SAFARI 2000) made extensive ground-based, airborne, and satellite measurements of these gases and aerosols in order to quantify their amounts and effects on Earth's atmosphere. In this study we interpreted the measurements of smoke aerosol particles made during SAFARI 2000 in order to better represent these particles in a numerical model simulating their transport and fate. Typically, smoke aerosols emitted from fires are concentrated by mass in particles about 0.3 micrometers in diameter (1,000,000 micrometers = 1 meter, about 3 feet); for comparison, the thickness of a human hair is about 50 micrometers, almost 200 times as great. Because of the size of these particles, at the surface they can be easily inhaled into the lungs, and in high concentrations have deleterious health effects on humans. Additionally, these particles reflect and absorb sunlight, impacting both visibility and the balance of sunlight reaching -Earth's surface, and ultimately play a role in modulating Earth's climate. Because of these important effects, it is important that numerical models used to estimate Earth's climate response to changes in atmospheric composition accurately represent the quantity and evolution of smoke particles. In our model, called the Community Aerosol and Radiation Model for Atmospheres (CARMA) we used estimates of smoke emissions based on field studies and observations made with the NASA Terra and TRMM satellites. The meteorology used to calculate the transport was based on an assimilation of observed meteorological conditions provided by the National Center for Atmospheric Research.
Production Mechanisms, Number Concentration, Size Distribution. Chemical Composition, and Optical Properties of Sea Spray Aerosols
Over forty scientists from six countries convened in Raleigh, NC on June 4-6 2012 to review the status and prospects of sea spray aerosol research. Participants were researchers from the oceanography and atmospheric science communities, including academia, private industry, and government agencies. The recommendations from the working groups are summarized in a science prioritization matrix that is meant to prioritize the research agenda and identify areas of investigation by the magnitude of their impact on proposed science questions. Str
Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US
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AeroCom phase III multi-model evaluation of the aerosol life cycle and optical properties using ground- and space-based remote sensing as well as surface in situ observations
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A Ten-Year Global Record of Absorbing Aerosols Above Clouds from OMI's Near-UV Observations
Aerosol-cloud interaction continues to be one of the leading uncertain components of climate models, primarily due to the lack of an adequate knowledge of the complex microphysical and radiative processes associated with the aerosol-cloud system. The situations when aerosols and clouds are found in the same atmospheric column, for instance, when light-absorbing aerosols such as biomass burning generated carbonaceous particles or wind-blown dust overlay low-level cloud decks, are commonly found over several regional of the world. Contrary to the cloud-free scenario over dark surface, for which aerosols are known to produce a net cooling effect (negative radiative forcing) on climate, the overlapping situation of absorbing aerosols over cloud can potentially exert a significant level of atmospheric absorption and produces a positive radiative forcing at top-of-atmosphere. The magnitude of direct radiative effects of aerosols above cloud depends directly on the aerosol loading, microphysical-optical properties of the aerosol layer and the underlying cloud deck, and geometric cloud fraction. We help in addressing this problem by introducing a novel product of optical depth of absorbing aerosols above clouds retrieved from near-UV observations made by the Ozone Monitoring Instrument (OMI) on board NASA's Aura platform. The presence of absorbing aerosols above cloud reduces the upwelling radiation reflected by cloud and produces a strong 'color ratio' effect in the near-UV region, which can be unambiguously detected in the OMI measurements. Physically based on this effect, the OMACA algorithm retrieves the optical depths of aerosols and clouds simultaneously under a prescribed state of atmosphere. The algorithm architecture and results from a ten-year global record including global climatology of frequency of occurrence and above-cloud aerosol optical depth, and a discussion on related future field campaigns are presented.
LASE measurements of aerosols and water vapor during TARFOX
The TARFOX (Tropospheric Aerosol Radiative Forcing Observational Experiment) intensive field campaign was designed to reduce uncertainties in estimates of the effects of anthropogenic aerosols on climate by measuring direct radiative effects and the optical, physical, and chemical properties of aerosols [1]. TARFOX was conducted off the East Coast of the United States between July 10-31, 1996. Ground, aircraft, and satellite-based sensors measured the sensitivity of radiative fields at various atmospheric levels to aerosol optical properties (i.e., optical thickness, phase function, single-scattering albedo) and to the vertical profile of aerosols. The LASE (Lidar Atmospheric Sensing Experiment) instrument, which was flown on the NASA ER-2 aircraft, measured vertical profiles of total scattering ratio and water vapor during a series of 9 flights. These profiles were used in real-time to help direct the other aircraft to the appropriate altitudes for intensive sampling of aerosol layers. We have subsequently used the LASE aerosol data to derive aerosol backscattering and extinction profiles. Using these aerosol extinction profiles, we derived estimates of aerosol optical thickness (AOT) and compared these with measurements of AOT from both ground and airborne sun photometers and derived from the ATSR-2 (Along Track and Scanning Radiometer 2) sensor on ERS-2 (European Remote Sensing Satellite-2). We also used the water vapor mixing ratio profiles measured simultaneously by LASE to derive precipitable water vapor and compare these to ground based measurements.
Characterization of carbonaceous aerosols during TRACER-CAT
Absorbing aerosols (AA) have an important impact on the global radiation budget and cloud properties. The composition and properties of AA can vary substantially throughout the atmosphere, depending on the particle source and the influence of chemical aging. Uncertainties associated with the radiative effects of AA remain substantial. A key contributor to this uncertainty is understanding the extent to which coatings in general, and water uptake especially, alters absorption by AA particles and how this depends on particle composition. We deployed new and existing experimental tools during the Tracking Aerosol Convection Interactions Experiment (TRACER) campaign in Houston, TX as part of the Carbonaceous Aerosols Thrust (CAT) to provide detailed characterization of aerosol optical, chemical, and physical properties. Our TRACER-CAT measurements complemented and expanded on the planned TRACER instrumentation, allowing for more detailed characterization of aerosol properties of relevance to cloud development (a core focus of TRACER), such as the composition of particles that can act as cloud condensation nuclei, than would otherwise be available. Our measurements have allowed for assessment of the relationship(s) between AA optical properties (with a focus on absorption) and the chemical and physical characteristics (including the mixing state of black carbon (BC) containing particles). These field observations occurred in collaboration with Los Alamos National Laboratory in summer 2022 during the TRACER intensive operating period. The instrumentation we co-deployed provided for measurement of (i) multi-wavelength dry aerosol absorption, scattering, and extinction, (ii) the size-dependent composition and abundance of sub-micron aerosol, differentiating between those particles that do and do not contain BC, (iii) BC-specific concentrations and size distributions, (iv) particle size, and (v) the first field measurements at an ARM site of the influence of RH on multi-wavelength absorption by ambient AA. We have leveraged the natural variability of the atmosphere and of aerosol sources in the Houston region to (i) specifically disentangle contributions to light absorption from BC, absorbing organic carbon (brown carbon), and coatings on BC, (ii) characterize the mixing state of BC and assess the factors that give rise to compositional differences between BC-containing and BC-free aerosol, and (iii) establish how water uptake influences absorption and how any such effect depends on particle composition and BC mixing state. Overall, our study contributed to the mission of the Atmospheric System Research program in multiple ways. Through the deployment of complementary, advanced instrumentation for characterization of a wide range of aerosol properties our work helped to maximize the scientific impact of the TRACER campaign. Our work also allowed for development of new insights into the relationship(s) between aerosol composition, hygroscopicity, and the mixing state of BC with aerosol optical properties. Through this, our work has provided knowledge that can improve understanding and model representation of aerosol processes as they affect the Earth’s radiation budget.
Radiative Characteristics of Aerosol During Extreme Fire Event over Siberia in Summer 2012
Microphysical and optical properties of aerosol were studied during a mega-fire event in summer 2012 over Siberia using ground-based measurements of spectral solarradiation at the AERONET site in Tomsk and satellite observations. The data were analyzed using multi-year (2003-2013) measurements of aerosol characteristics under back-ground conditions and for less intense fires, differing in burning biomass type, stage of fire, remoteness from observation site, etc. (ordinary smoke). In June-August 2012, the average aerosol optical depth (AOD, 500 nm) had been 0.95+/-0.86, about a factor of 6 larger than background values (0.16+/-0.08), and a factor of 2.5 larger than in ordinary smoke. The AOD values were extremely high on 24-28 July and reached 3-5. A comparison with satellite observations showed that ground-based measurements in the region of Tomsk not only reflect the local AOD features, but are also characteristic for the territory of Western Siberia as a whole. Single scattering albedo (SSA, 440 nm) in this period ranged from 0.91 to 0.99 with an average of approx. 0.96 in the entire wavelength range of 440-1020 nm. The increase in absorptance of aerosol particles (SSA(440 nm)=0.92) and decrease in SSA with wavelength observed in ordinary smoke agree with the data from multi-year observations in analogous situations in the boreal zone of USA and Canada. Volume aerosol size distribution in extreme and ordinary smoke had a bimodal character with significant prevalence of fine-mode particles, but in summer 2012 the mean median radius and the width of the fine-mode distribution somewhat increased. In contrast to data from multi-year observations, in summer 2012 an increase in the volume concentration and median radius of the coarse mode was observed with growing AOD.
Multiple scattering wavelength dependent backscattering of kaolin dust in the IR: Measurements and theory
Knowing the optical properties of aerosol dust is important for designing electro-optical systems and for modeling the effect on propagation of light in the atmosphere. As CO2 lidar technology becomes more advanced and is used for multiwavelength measurements, information on the wavelength dependent backscattering of aerosol dust particles is required. The volume backscattering coefficient of aerosols in the IR is relatively small. Thus, only a few field measurements of backscattering, usually at only a few wavelengths, are reported in the literature. We present spectral field measurements of backscattering of kaolin dust in the 9-11 micron wavelength range. As the quantity of dust increases, multiple scattering contributes more to the measured backscattered signal. The measurements show the effect of the dust quantity of the spectral backscatter measurements. A simple analytical two stream radiative transfer model is applied to confirm the measurements and to give insight to the multiple scattering spectra of backscattering.
Summer Aerosol and Trace Gas Observations in Houston, Texas Using an Adaptable Mobile Facility
An aerosol container featuring a shared inlet system was deployed to Houston, Texas in July 2022, enabling direct, high-time-resolution in situ measurements of aerosols and trace gases. The internal rack system and floorplan was designed for adaptable modularity to elucidate aerosol physicochemical processes at fine scales. The design allowed for the deployment of a core instrument suite and additional customized research grade instruments. A heterogeneous mixture of aerosols was observed during three regimes: (1) intermittent black carbon (BC) and diurnal variations in aerosol chemical composition, (2) observed particle growth associated with SO 2 , (3) transported supermicron dust. The high variability of observed particles and gases in high time resolution indicated a complex urban area with multiple local and regional sources and processes. Particle growth rates of 7–16 nm/hr were observed for submicron particles during periods when SO 2 was >0.5 ppbv. Two periods of multi-day long-range transport events of dust from the African Sahara were observed in the supermicron and submicron particle modes with total mass concentrations up to 30 μg m −3 . Aerosol scattering angstrom exponents and extinction coefficients (B ext ) increased with humidity as a function of particle composition. The measurements demonstrate collaborative capabilities that can be used to increase observations of aerosol processing, microphysical and optical properties, internal mixing state, and supermicron aerosol that are not parameterized or missing in global Earth energy system models.
Radiative Importance of Aerosol-Cloud Interaction
Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have even greater consequences. Presently we know that through the use of fossil fuel and land-use changes we have increased the concentration of greenhouse gases in the atmosphere. In parallel, we have seen a modest increase of global temperature in the last century. These two observations have been linked as cause and effect by climate models, but this connection is still experimentally not verified. The spatial and seasonal distribution of aerosol forcing is different from that of greenhouse gases, thus generating a different spatial fingerprint of climate change. This fingerprint was suggested as a method to identify the response of the climate system to anthropogenic forcing of greenhouse gases and aerosol. The aerosol fingerprint may be the only way to firmly establish the presence (or absence) of human impact on climate. Aerosol-cloud interaction through the indirect effect will be an important component of establishing this fingerprint.
EPCAPE-PT-LANL Measurements: Condensation Particle Counter
Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Condensational particle counter 3070 (TSI) Calibration: No calibration during the campaign. Files: data_10sec_CPC.csv, data_10min_CPC.csv Header: - NumberConcentration[/cm3]: Number concentration of aerosol particles measured by the CPC, expressed in particles per cubic centimeter. - NumberConcentration[/cm3]_QC: Number concentration of aerosol particles after quality control adjustments or filtering, expressed in particles per cubic centimeter. - QualityControl_Flag[bool]: A boolean flag indicating whether the measurement is flagged for quality control checks, (0=pass) - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active (true) or inactive (false) during the measurement
Turbulent properties from Doppler lidar
Permanent and mobile facilities deployed by the ARM program cover a wide range of climatic regions, with a suite of active remote-sensing of cloud and aerosol profiles complemented by comprehensive in-situ measurements of the chemical, physical and optical properties of aerosol measured at the surface. To be able to fully exploit these datasets requires an understanding of the transport from the surface and within the atmosphere, especially within the planetary boundary layer. This requires a method of identifying when the surface and atmosphere are dynamically-linked. Determining the state of the boundary layer, and defining a well-mixed boundary-layer, is therefore suitably described in terms of mixing; here, we will assume that mixing essentially means turbulent mixing. This necessitates accurate measurements of the winds and turbulent mixing in the atmosphere. Doppler lidar is an excellent tool for observing turbulent properties, and ARM has deployed commercially available Doppler lidars at many of the fixed and mobile facilities. Doppler lidars have been shown to provide accurate retrievals of wind and turbulent properties within the boundary layer , however, robust characterization and calculation of the Doppler lidar measurement uncertainties is required before deriving higher level data products.
EPCAPE-PT-LANL Measurements: Photoacoustic Extinctometer
Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Photoacoustic Extinctiometer at 870 nm (Droplet Measurement Technology) Header: - AbsorptionNoise_870nm[1/Mm]: Noise level associated with the absorption measurement at 870 nm, expressed in inverse megameters (Mm⁻¹). - Absorption_870nm[1/Mm]: Absorption coefficient of aerosols measured at 870 nm, expressed in inverse megameters (Mm⁻¹). - Extinction_870nm[1/Mm]: Extinction coefficient of aerosols measured at 870 nm, expressing the sum of scattering and absorption by aerosols, in inverse megameters (Mm⁻¹). - Scattering_870nm[1/Mm]: Scattering coefficient of aerosols measured at 870 nm, expressed in inverse megameters (Mm⁻¹). - BackgroundAbsorption_870nm[1/Mm]: Background absorption measurement at 870 nm, used to correct the primary absorption data, expressed in inverse megameters (Mm⁻¹). - BackgroundScattering_870nm[1/Mm]: Background scattering measurement at 870 nm, used to correct the primary scattering data, expressed in inverse megameters (Mm⁻¹). - Temperature[C]: The ambient temperature at the time of the measurement, expressed in degrees Celsius. - RelativeHumidity[%]: The relative humidity at the time of the measurement, expressed as a percentage. - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active (true) or inactive (false) during the measurement