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Ice Nucleation Measurements during TRACER (Field Campaign Report)

This campaign, Ice Nucleation Measurements during TRACER, was conducted during the TRacking Aerosol Convection Interactions ExpeRiment (TRACER) in Houston, Texas during June-September, 2022. Specifically, our ice nucleation campaign was designed to improve understanding of ice nucleating particles (INPs) and their role in deep convective clouds across the Houston region. Summertime deep convection in southeast Texas is regularly tied to the sea-breeze front (SBF) that pushes inland from the Gulf of Mexico across the region. During TRACER, three Davis Rotating Uniform size-cut Monitors (DRUM; DRUMAir 4-DRUM) were used to collect aerosols for offline ice nucleation measurements in the Brooks laboratory at Texas A&M University. The three instruments were located at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) first Mobile Facility (AMF1) in La Porte, at the ancillary site in Guy (ANC), and onboard the newly developed Texas A&M Rapid Onsite Atmospheric Measurements Van (ROAM-V). Aerosol at the main ARM TRACER site, ARM1, is expected to arise from local urban, industrial, and ship channel sources. In contrast, the ANC is isolated and rural, and can therefore provide a continental background aerosol population. On select days when convective development was forecast to be probable, ROAM-V commuted from College Station, Texas to Galveston, sampled in the morning/mid-day on the coast, and then transited to a second inland site for the afternoon/evening. Sampling from the ROAM-V allowed us to capture aerosol and meteorological differences between maritime and continental airmasses by strategically positioning the ROAM-V near the coast in the morning in the opposite airmass from the AMF1 site.

54 ENVIRONMENTAL SCIENCES↗

Dust Modeling with GEOS-Chem: Evidence for Acidic Uptake on Dust Surfaces during INTEX-B

We use measurements of aerosol ion composition and size made from the DC8 aircraft during the 2006 INTEX-B airborne campaign to identify mineral dust signatures, and look for evidence for interaction of dust with acidic components. Coating of dust with sulfate or nitrate favors the role of dust particles as cloud condensation nucleii, can promote further uptake of SO2 and N2O5, can impact NOx/HNO3 partitioning, and can shift sulfate or nitrate towards larger sizes, affecting atmospheric lifetimes for both aerosol and gas components. Mineral dust had a pervasive presence on flights made during the Northern Pacific deployment of the INTEX-B mission. We use scatter plots of ion mixing ratios with Na+ and Ca(2+) to distinguish sea salt and mineral components of the aerosol distribution, respectively. Positive correlations of non-sea-salt sulfate and nitrate with calcium indicate that the dusty air stream is associated with polluted air masses. Sulfate-ammonium scatter plots indicate sulfate to be primarily in the form of (NH4)2SO4. A positive correlation between Ca(2+) and NO-, but little evidence of NH4NO3, suggests that NO3- may be associated with mineral dust surfaces. 3-d model simulations conducted with the GEOS-Chem chemical transport model indicate that transpacific transport from East Asia was principally responsible for the dust observed from the aircraft over the Pacific. We compare the aerosol component relationships in the model with those observed. Uptake of sulfate and nitrate on the dust is not yet represented in the model.

Fairlie, T. Duncan↗

Anthropogenic pollution elevates the peak height of new particle formation from planetary boundary layer to lower free troposphere

New particle formation (NPF) and subsequent growth are primary sources of atmospheric aerosol particles and cloud condensation nuclei. Previous studies have been conducted in relatively clean environments; investigation of NPF events over highly polluted megacities is still lacking. Here in this paper we show, based on a recent yearlong aircraft campaign conducted over Beijing, China, from April 2011 to June 2012, that NPF occurrence peaks in the lower free troposphere (LT), instead of planetary boundary layer (PBL), as most previous studies have found and that the distance of NPF peak to PBL top increases with increasing aerosol loading. Further analysis reveals that increased aerosols suppress NPF in PBL, but enhance NPF in LT due to a complex chain of aerosol-radiation-photochemistry interactions that affect both NPF sources and sinks. These findings shed new light on our understanding of NPF occurrence, NPF vertical distribution, and thus their effects on atmospheric photochemistry, clouds, and climate.

54 ENVIRONMENTAL SCIENCES↗

Bioaerosols in the Earth system: Climate, health, and ecosystem interactions

Aerosols of biological origin play a vital role in the Earth system, particularly in the in-teractions between atmosphere, biosphere, climate, and public health. Airborne bacteria, fungal spores, pollen, and other bioparticles are essential for the reproduction and spread of organisms across various ecosystems, and they can cause or enhance human, animal, and plant diseases. Moreover, they can serve as nuclei for cloud droplets, ice crystals, and precipitation, thus influencing the hydrological cycle and climate. The actual formation, abundance, composition, and effects of biological aerosols and the atmospheric microbi-ome are, however, not yet well characterized and constitute a large gap in the scientific understanding of the interaction and co-evolution of life and climate in the Earth system. This review presents an overview of the state of bioaerosol research and highlights recent advances in terms of bioaerosol identification, characterization, transport, and transfor-mation processes, as well as their interactions with climate, health, and ecosystems, focus-ing on the role bioaerosols play in the Earth system.

Fröhlich-Nowoisky, Janine (ORCID:0000000212780054)↗

Simultaneous Retrieval of Aerosol and Surface Optical Properties from Combined Airborne- and Ground-Based Direct and Diffuse Radiometric Measurements

This paper presents a new method for simultaneously retrieving aerosol and surface reflectance properties from combined airborne and ground-based direct and diffuse radiometric measurements. The method is based on the standard Aerosol Robotic Network (AERONET) method for retrieving aerosol size distribution, complex index of refraction, and single scattering albedo, but modified to retrieve aerosol properties in two layers, below and above the aircraft, and parameters on surface optical properties from combined datasets (Cloud Absorption Radiometer (CAR) and AERONET data). A key advantage of this method is the inversion of all available spectral and angular data at the same time, while accounting for the influence of noise in the inversion procedure using statistical optimization. The wide spectral (0.34-2.30 m) and angular range (180 ) of the CAR instrument, combined with observations from an AERONET sunphotometer, provide sufficient measurement constraints for characterizing aerosol and surface properties with minimal assumptions. The robustness of the method was tested on observations made during four different field campaigns: (a) the Southern African Regional Science Initiative 2000 over Mongu, Zambia, (b) the Intercontinental Transport Experiment-Phase B over Mexico City, Mexico (c) Cloud and Land Surface Interaction Campaign over the Atmospheric Radiation Measurement (ARM) Central Facility, Oklahoma, USA, and (d) the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) over Elson Lagoon in Barrow, Alaska, USA. The four areas are dominated by different surface characteristics and aerosol types, and therefore provide good test cases for the new inversion method.

Gatebe, C. K.↗

LASE Measurements of Water Vapor, Aerosol, and Cloud Distributions in Saharan Air Layers and Tropical Disturbances

LASE (Lidar Atmospheric Sensing Experiment) on-board the NASA DC-8 measured high resolution profiles of water vapor and aerosols, and cloud distributions in 14 flights over the eastern North Atlantic during the NAMMA (NASA African Monsoon Multidisciplinary Analyses) field experiment. These measurements were used to study African easterly waves (AEWs), tropical cyclones (TCs), and the Saharan Air Layer(s) (SAL). Interactions between the SAL and tropical air were observed during the early stages of the TC development. These LASE measurements represent the first simultaneous water vapor and aerosol lidar measurements to study the SAL and its impact on AEWs and TCs. Examples of profile measurements of aerosol scattering ratios, aerosol extinction coefficients, aerosol optical thickness, water vapor mixing ratios, RH, and temperature are presented to illustrate their characteristics in SAL, convection, and clear air regions. LASE data suggest that the SAL suppresses low-altitude convection at the convection-SAL interface region. Mid-level convection associated with the AEW and transport are likely responsible for high water vapor content observed in the southern regions of the SAL on August 20, 2008. This interaction is responsible for the transfer of about 7 x 10(exp 15) J latent heat energy within a day to the SAL. Measurements of lidar extinction-to-backscatter ratios in the range 36+/-5 to 45+/-5 are within the range of measurements from other lidar measurements of dust. LASE aerosol extinction and water vapor profiles are validated by comparison with onboard in situ aerosol measurements and GPS dropsonde water vapor soundings, respectively.

Ismail, Syed↗

Direct measurement of small particle growth and aging at SGP

Atmospheric aerosols influence climate directly by scattering and absorbing solar radiation and indirectly through their influence on the reflectivity and lifetime of clouds. But that influence is limited to only those particles large enough to efficiently interact with solar radiation (diameter, D p ≳ 100 nm) and/or to form cloud droplets at typical atmospheric supersaturations (D p ≳ 50 nm). Many cloud condensation nuclei (CCN) originate as ~1 nm nucleated particles that must grow to those threshold sizes before being lost to coagulation with larger particles. Though there is consensus that new particle formation and growth contributes significantly to total CCN concentrations, different groups using different models and assumptions have arrived at diverse estimates.

54 ENVIRONMENTAL SCIENCES↗

Comment on 'A note on the possible connection between the El Chichon eruption and ocean production in the northwest Arabian Sea during 1982' by A. E. Strong

Strong argues that the El Chichon aerosol cloud resulted in relaxed southwest monsoon circulation and the dramatically reduced seasonal phytoplankton bloom documented in the northwestern Arabian Sea during summer and fall of 1982. It is argued here that Strong's ideas suggest a clear demonstration of an atmosphere-ocean interaction with implications for the ocean's biological CO2 pump. Strong's paper highlights the fundamentally different effects of volcanic aerosols on satellite infrared and visible band observations of the ocean.

Brock, John C.↗

Updraft dynamics and microphysics: on the added value of the cumulus thermal reference frame in simulations of aerosol–deep convection interactions

One fundamental question about atmospheric moist convection processes that remains debated is whether, or under which conditions, a relevant variability in background aerosol concentrations may have a significant dynamical impact on convective clouds and their associated precipitation. Furthermore, current climate models must parameterize both the microphysical and the cumulus convection processes, but this is usually implemented separately, whereas in nature there is a strong coupling between them. As a first step to improve our understanding of these two problems, we investigate how aerosol concentrations modify key properties of updrafts in eight large-eddy-permitting regional simulations of a case study of scattered convection over Houston, Texas, in which convection is explicitly simulated and microphysical processes are parameterized. Dynamical and liquid-phase microphysical responses are investigated using the following two different reference frames: static cloudy updraft grid cells versus tracked cumulus thermals. In both frameworks, we observe the expected microphysical responses to higher aerosol concentrations, such as higher cloud number concentrations and lower rain number concentrations. In terms of the dynamical responses, both frameworks indicate weak impacts of varying aerosol concentrations relative to the noise between simulations over the observationally derived range of aerosol variability for this case study. On the other hand, results suggest that thermals are more selective than cloudy updraft grid cells in terms of sampling the most active convective air masses. For instance, vertical velocity from thermals is significantly higher at upper levels than when sampled from cloudy updraft grid points, and several microphysical variables have higher average values in the cumulus thermal framework than in the cloudy updraft framework. In addition, the thermal analysis is seen to add rich quantitative information about the rates and covariability of microphysical processes spatially and throughout tracked thermal lifecycles, which can serve as a stronger foundation for improving subgrid-scale parameterizations.

54 ENVIRONMENTAL SCIENCES↗

Updraft Dynamics and Microphysics: On the Added Value of The Cumulus Thermal Reference Frame in Simulations of Aerosol–Deep Convection Interactions

One fundamental question about atmospheric moist convection processes that remains debated is whether, or under which conditions, a relevant variability in background aerosol concentrations may have a significant dynamical impact on convective clouds and their associated precipitation. Furthermore, current climate models must parameterize both the microphysical and the cumulus convection processes, but this is usually implemented separately, whereas in nature there is a strong coupling between them. As a first step to improve our understanding of these two problems, we investigate how aerosol concentrations modify key properties of updrafts in eight large-eddy-permitting regional simulations of a case study of scattered convection over Houston, Texas, in which convection is explicitly simulated and microphysical processes are parameterized. Dynamical and liquid-phase microphysical responses are investigated using the following two different reference frames: static cloudy updraft grid cells versus tracked cumulus thermals. In both frameworks, we observe the expected microphysical responses to higher aerosol concentrations, such as higher cloud number concentrations and lower rain number concentrations. In terms of the dynamical responses, both frameworks indicate weak impacts of varying aerosol concentrations relative to the noise between simulations over the observationally derived range of aerosol variability for this case study. On the other hand, results suggest that thermals are more selective than cloudy updraft grid cells in terms of sampling the most active convective air masses. For instance, vertical velocity from thermals is significantly higher at upper levels than when sampled from cloudy updraft grid points, and several microphysical variables have higher average values in the cumulus thermal framework than in the cloudy updraft framework. In addition, the thermal analysis is seen to add rich quantitative information about the rates and covariability of microphysical processes spatially and throughout tracked thermal lifecycles, which can serve as a stronger foundation for improving subgrid-scale parameterizations.

aerosols↗

Updraft Dynamics and Microphysics: On the Added Value of the Cumulus Thermal Reference Frame in Simulations of Aerosol–Deep Convection Interactions

One fundamental question about atmospheric moist convection processes that remains debated is whether or under what conditions a relevant variability in background aerosol concentrations may have a significant dynamical impact on convective clouds and their associated precipitation. Furthermore, current climate models must parameterize both the microphysical and the cumulus convection processes, but this is usually implemented separately, whereas in nature there is a strong coupling between them. As a first step to improve our understanding of these two problems, we investigate how aerosol concentrations modify key properties of updrafts in eight large-eddy permitting regional simulations of a case study of scattered convection over Houston, Texas, in which convection is explicitly simulated and microphysical processes are parameterized. Dynamical and liquid-phase microphysical responses are investigated using two different reference frames: static cloudy-updraft grid cells versus tracked cumulus thermals. In both frameworks we observe the expected microphysical responses to higher aerosol concentrations, such as higher cloud number concentrations and lower rain number concentrations. In terms of the dynamical responses, both frameworks indicate weak impacts of varying aerosol concentrations relative to the noise between simulations over the observationally derived range of aerosol variability for this case study. On the other hand, results suggest that thermals are more selective than cloudy-updraft grid cells in terms of sampling the most active convective air masses. For instance, vertical velocity from thermals is significantly higher at upper levels than when sampled from cloudy-updraft grid points, and several microphysical variables have higher average values in the cumulus thermal framework than in the cloudy-updraft framework. In addition, the thermal analysis is seen to add rich quantitative information about the rates and covariability of microphysical processes spatially and throughout tracked thermal lifecycles, which can serve as a stronger foundation for improving subgrid-scale parameterizations.

Daniel Hernandez-Deckers↗

Indian Summer Monsoon Drought 2009: Role of Aerosol and Cloud Microphysics

Cloud dynamics played a fundamental role in defining Indian summer monsoon (ISM) rainfall during drought in 2009. The anomalously negative precipitation was consistent with cloud properties. Although, aerosols inhibited the growth of cloud effective radius in the background of sparse water vapor, their role is secondary. The primary role, however, is played by the interactive feedback between cloud microphysics and dynamics owing to reduced efficient cloud droplet growth, lesser latent heating release and shortage of water content. Cloud microphysical processes were instrumental for the occurrence of ISM drought 2009.

2009↗

Cloud/Aerosol Parameterizations: Application and Improvement of General Circulation Models

One of the biggest uncertainties associated with climate models and climate forcing is the treatment of aerosols and their effects on clouds. The effect of aerosols on clouds can be divided into two components: The first indirect effect is the forcing associated with increases in droplet concentrations; the second indirect effect is the forcing associated with changes in liquid water path, cloud morphology, and cloud lifetime. Both are highly uncertain. This project applied a cloud-resolving model to understand the response of clouds under a variety of conditions to changes in aerosols. These responses are categorized according to the large-scale meteorological conditions that lead to the response. Meteorological conditions were sampled from various fields, which, together with a global aerosol model determination of the change in aerosols from present day to pre-industrial conditions, was used to determine a first order estimate of the response of global cloud fields to changes in aerosols. The response of the clouds in the NCAR CAM3 GCM coupled to our global aerosol model were tested by examining whether the response is similar to that of the cloud resolving model and methods for improving the representation of clouds and cloud/aerosol interactions were examined.

54 ENVIRONMENTAL SCIENCES↗

Improving the Representation of Soluble Iron in Climate Models

Mineral dust produced in the arid and semi-arid regions of the world is the dominant source of iron (Fe) in atmospheric aerosol inputs to the open ocean. The bioavailable Fe fraction of atmospheric dust is thought to regulate and occasionally limit the primary productivity in large oceanic regions, which influences the CO2 uptake from the atmosphere affecting the Earth’s climate. Because Fe bioavailability cannot be directly measured, it is assumed that the dissolved Fe or highly reactive Fe in the dust is bioavailable. The fraction of soluble Fe in dust is mainly controlled by: (1) the mineral composition of the soils and the emitted dust from the source areas; (2) the atmospheric processing that converts the Fe in Fe-bearing minerals into highly soluble forms of Fe. The project has mainly focused on constraining the mineral composition of dust aerosols (1), a previously neglected, yet a key issue to constrain the deposition of soluble iron. Deriving aerosol mineral composition requires global knowledge of the soil mineral content, which is available from poorly constrained global atlases. In addition, the mineral content of the emitted aerosol differs from that of the parent soil. Measurements of soil mineral fractions are based upon wet sedimentation (or ’wet sieving’) techniques that disturb the soil sample, breaking aggregates that are found in the original, undispersed soil that is subject to wind erosion. Wet sieving alters the soil size distribution, replacing aggregates that are potentially mobilized as aerosols with a collection of smaller particles. A major challenge is to derive the size-distributed mineral fractions of the emitted dust based upon their fractions measured from wet-sieved soils. Finally, representations of dust mineral composition need to account for mixtures of minerals. Examination of individual particles shows that iron, an element that is central to many climate processes, is often found as trace impurities of iron oxide attached to aggregates of other minerals. This is another challenge that has been tackled by the project. The project has produced a major step forward on our understanding of the key processes needed to predict the mineral composition of dust aerosols by connecting theory, modeling and observations. The project has produced novel semi-empirical and theoretical methods to estimate the emitted size distribution and mineral composition of dust aerosols. These methods account for soil aggregates that are potentially emitted from the original undisturbed soil but are destroyed during wet sieving. The methods construct the emitted size distribution of individual minerals building upon brittle fragmentation theory, reconstructions of wet-sieved soil mineral size distributions, and/or characteristic mineral size distributions estimated from observations at times of high concentration. Based on an unprecedented evaluation with a new global compilation of observations produced with the project support, we showed that the new methods remedy some key deficiencies compared to the previous state-of-the-art. This includes the correct representation of Fe-bearing phyllosilicates at silt sizes, where they are abundant according to observations. In addition, the quartz fraction of silt particles is in better agreement with measured values. In addition, we represent an additional class of iron oxide aerosol that is a small impurity embedded within other minerals, allowing it to travel farther than in its pure crystalline state. We assume that these impurities are least frequent in soils rich in iron oxides (as a result of the assumed effect of weathering that creates pure iron oxide crystals). The mineral composition of dust is also important to other interaction with climate - through shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, and the heterogeneous formation of sulfates and nitrates - and to its impacts upon human health. Despite the importance of mineral composition, models have typically assumed that soil dust aerosols have globally uniform composition. The results of this project will allow an improved estimation of the dust effects upon climate and health.

54 ENVIRONMENTAL SCIENCES↗

Biogenic Aerosols—Effects on Clouds and Climate (BAECC) Final Campaign Summary

Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the Northern latitudes throughout the United States, Canada, Russia, and Scandinavia, are, of all biomes, among the most active areas of atmospheric aerosol formation. The formation of aerosol particles and their growth to cloud condensation nuclei sizes in these areas are associated with biogenic volatile organic emissions (BVOC) from vegetation and soil.

54 ENVIRONMENTAL SCIENCES↗

Science Plan Biogenic Aerosols – Effects on Clouds and Climate (BAECC)

Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the northern latitudes throughout the United States, Canada, Russia and Scandinavia, are among the most active areas of atmospheric aerosol formation among all biomes. The formation of aerosol particles and their growth to the sizes of cloud condensation nuclei in these areas are associated with biogenic volatile organic emissions from vegetation and soil.

Petäjä, T↗

Urbanization-induced land and aerosol impacts on storm propagation and hail characteristics

Changes in land surface and aerosol characteristics from urbanization can affect dynamic and microphysical properties of severe storms, thus affecting hazardous weather events resulting from such storms such as hail and tornado. We examine the joint and individual effects of urban land and anthropogenic aerosols of Kansas City on a severe convective storm observed during the 2015 Plains Elevated Convection At Night (PECAN) field campaign, focusing on storm evolution, convective intensity, and hail characteristics. The simulations are carried out at the cloud-resolving scale (1 km) using a version of WRF-Chem in which the spectral-bin microphysics (SBM) is coupled with the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC). It is found that the urban land effect of Kansas City initiated a much stronger convective cell and the storm got further intensified when interacting with stronger turbulence induced by the urban land. The urban land effect also changed the storm path by diverting the storm toward the city mainly resulting from enhanced urban land-induced convergence in the urban area and around the urban-rural boundaries. The joint effect of urban land and anthropogenic aerosols enhances occurrences of both severe hail and significant severe hail by ~ 20% by enhancing hail formation and growth from riming. Overall the urban land effect on convective intensity and hail is relatively larger than the anthropogenic aerosol effect, but the joint effect is much notable than either of the individual effects, emphasizing the importance to consider both effects in evaluating urbanization effects.

Lin, Yun↗

Climatic impact of volcanic eruptions

Studies have attempted to 'isolate' the volcanic signal in noisy temperature data. This assumes that it is possible to isolate a distinct volcanic signal in a record that may have a combination of forcings (ENSO, solar variability, random fluctuations, volcanism) that all interact. The key to discovering the greatest effects of volcanoes on short-term climate may be to concentrate on temperatures in regions where the effects of aerosol clouds may be amplified by perturbed atmospheric circulation patterns. This is especially true in subpolar and midlatitude areas affected by changes in the position of the polar front. Such climatic perturbation can be detected in proxy evidence such as decrease in tree-ring widths and frost rings, changes in the treeline, weather anomalies, severity of sea-ice in polar and subpolar regions, and poor grain yields and crop failures. In low latitudes, sudden temperature drops were correlated with the passage overhead of the volcanic dust cloud (Stothers, 1984). For some eruptions, such as Tambora, 1815, these kinds of proxy and anectdotal information were summarized in great detail in a number of papers and books (e.g., Post, 1978; Stothers, 1984; Stommel and Stommel, 1986; C. R. Harrington, in press). These studies lead to the general conclusion that regional effects on climate, sometimes quite severe, may be the major impact of large historical volcanic aerosol clouds.

Rampino, Michael R.↗