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DOE OSTI2023

Vertical Aerosol Profiling during SAIL (VAPS) Field Campaign Report

To more fully address the science goals of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility’s Surface Atmosphere Integrated Field Laboratory (SAIL) campaign, particularly the key science question of “How strongly do aerosols affect the surface energy and water balance by altering clouds, precipitation, and surface albedo, and how do these impacts vary seasonally?”, our campaign added instrumentation to planned tethered balloon system (TBS) flights in May and July of 2022. A key aspect of aerosol-cloud interactions is understanding cloud condensation nuclei (CCN) and ice nucleating particle (INP) populations, and how they vary seasonally and spatially. Because the interactions between aerosols and clouds is the target of this work, vertical distributions are particularly important to evaluate. Measurements of aerosol at ground level, below-cloud, and in-cloud will allow a better understanding of the airmasses that are feeding cloud-active particles into low- and mid-level clouds. Measurements of INP and aerosol populations often differ between the ground and aloft, with relationships that likely depend on regional and seasonal. Because of this, collocated measurements of aerosol, CCN, and INP, across different seasons, are crucial to reducing uncertainties in relationships between ground-level and cloud-base aerosol populations. Our campaign added online measurements of CCN using a compact CCN counter and offline filter collections for measurement of INP populations to the SAIL campaign TBS flights in May and July of 2022. The CCN instrument, the CloudPuck, flew and successfully collected data for a total of eight flights across both campaign periods. The IcePuck flew for most flights during the same period. Both instruments have continued to be used for other campaign requests in the SAIL domain. Analysis of this data was proposed through a concurrent DOE Atmospheric System Research (ASR) project submission, which was not funded in 2022. A similar proposal, which would involve analysis of the samples and data collected from this campaign, has been resubmitted in 2023 but a funding decision has not yet been made. If the proposal is again declined, we will seek other resources to ensure that this data can be analyzed.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1978

Rocket effluent: Its ice nucleation activity and related properties

To investigate the possibility of inadvertent weather modification from rocket effluent, aerosol samples were collected from an instrumented aircraft subsequent to the Voyager 1 and 2 launches. The aerosol's morphology, concentration, and size distribution were examined with an electron microscope. The elemental compositions of individual particles were analyzed with an X-ray energy spectrometer. Ice nucleus concentration was measured with a thermal diffusion chamber. The particles' physical and chemical properties were related to their ice nucleation activity. A laboratory experiment on rocket propellant exhaust was conducted under controlled conditions. Both laboratory and field experimental results indicated that rocket propellant exhaust can produce active ice nuclei and modify local weather in suitable meteorological conditions.

Parungo, F. P.↗

DOE OSTI2021

Aerosol transport pathways and source attribution in China during the COVID-19 outbreak

Abstract. Due to the coronavirus disease 2019 (COVID-19) pandemic, human activities and industrial productions were strictly restricted during January–March 2020 in China. Despite the fact that anthropogenic aerosol emissions largely decreased, haze events still occurred. Characterization of aerosol transport pathways and attribution of aerosol sources from specific regions are beneficial to air quality and pandemic control strategies. This study establishes source–receptor relationships in various regions covering all of China during the COVID-19 outbreak based on the Community Atmosphere Model version 5 with Explicit Aerosol Source Tagging (CAM5-EAST). Our analysis shows that PM2.5 burden over the North China Plain between 30 January and 19 February is mostly contributed by local emissions (40 %–66 %). For other regions in China, PM2.5 burden is largely contributed from nonlocal sources. During the most polluted days of the COVID-19 outbreak, local emissions within the North China Plain and eastern China contributed 66 % and 87 % to the increase in surface PM2.5 concentrations, respectively. This is associated with the anomalous mid-tropospheric high pressure at the location of the climatological East Asia trough and the consequently weakened winds in the lower troposphere, leading to the local aerosol accumulation. The emissions outside China, especially those from South Asia and Southeast Asia, contribute over 50 % to the increase in PM2.5 concentration in southwestern China through transboundary transport during the most polluted day. As the reduction in emissions in the near future is desirable, aerosols from long-range transport and unfavorable meteorological conditions are increasingly important to regional air quality and need to be taken into account in clean-air plans.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1978

Rocket effluent - Its ice nucleation activity and related properties

To investigate the possibility of inadvertent weather modification from rocket effluent, aerosol samples were collected from an instrumented aircraft subsequent to the Voyager I and II launches. The aerosol's morphology, concentration and size distribution were examined with an electron microscope. The elemental compositions of individual particles were analyzed with an X-ray energy spectrometer. Ice nucleus concentration was measured with a subfreezing thermal diffusion chamber. The particles' physical and chemical properties were related to their ice nucleation activity. A laboratory experiment on rocket propellant exhaust was conducted under controlled conditions. Both laboratory and field experimental results indicated that rocket propellant exhaust can produce active ice nuclei. Their consequences for potential inadvertant weather modification demand additional study.

Parungo, F. P.↗

NASA NTRS1995

Radiative impact of aerosols generated from biomass burning

Atmospheric aerosol particles play a vital role in the Earth's radiative energy budget. They exert a net cooling influence on climate by directly reflecting the solar radiation to space and by modifying the shortwave reflective properties of clouds. Each year, increasing amounts of aerosol particles are released into the atmosphere due to biomass burning, dust storms, forest fires, and volcanic activity. These particles significantly perturb the radiative balance on local, regional, and global scales. While the detection of aerosols over water is a well established procedure, the detection of aerosols over land is often difficult due to the poor contrast between the aerosols and the underlying terrain. In this study, we use textural measures in order to detect aerosols generated from biomass burning over South America, using AVHRR data. The regional radiative effects are then examined using ERBE data. Preliminary results show that the net radiative forcing of aerosols is about -36 W/sq m.

Christopher, Sundar A.↗

NASA NTRS2001

Validation of Satellite Aerosol Retrievals from AERONET Ground-Based Measurements

Accurate and comprehensive assessment of the parameters that control key atmospheric and biospheric processes including assessment of anthropogenic effects on climate change is a fundamental measurement objective of NASA's EOS program (King and Greenstone, 1999). Satellite assessment programs and associated global climate models require validation and additional parameterization with frequent reliable ground-based observations. A critical and highly uncertain element of the measurement program is characterization of tropospheric aerosols requiring basic observations of aerosols optical and microphysical properties. Unfortunately as yet we do not know the aerosol burden man is contributing to the atmosphere and thus we will have no definitive measure of change for the future. This lack of aerosol assessment is the impetus for some of the EOS measurement activities (Kaufman et al., 1997; King et al., 1999) and the formation of the AERONET program (Holben et al., 1998). The goals of the AERONET program are to develop long term monitoring at globally distributed sites providing critical data for multiannual trend changes in aerosol loading and optical properties with the specific goal of providing a data base for validation of satellite derived aerosol optical properties. The AERONET program has evolved into an international federated network of approximately 100 ground-based remote sensing monitoring stations to characterize the optical and microphysical properties of aerosols.

Holben, Brent↗

DOE OSTI2024

Measurement report: A comparison of ground-level ice-nucleating-particle abundance and aerosol properties during autumn at contrasting marine and terrestrial locations

Abstract. Ice-nucleating particles (INPs) are an essential class of aerosols found worldwide that have far-reaching but poorly quantified climate feedback mechanisms through interaction with clouds and impacts on precipitation. These particles can have highly variable physicochemical properties in the atmosphere, and it is crucial to continuously monitor their long-term concentration relative to total ambient aerosol populations at a wide variety of sites to comprehensively understand aerosol–cloud interactions in the atmosphere. Hence, our study applied an in situ forced expansion cooling device to measure ambient INP concentrations and test its automated continuous measurements at atmospheric observatories, where complementary aerosol instruments are heavily equipped. Using collocated aerosol size, number, and composition measurements from these sites, we analyzed the correlation between sources and abundance of INPs in different environments. Toward this aim, we have measured ground-level INP concentrations at two contrasting sites, one in the Southern Great Plains (SGP) region of the United States with a substantial terrestrially influenced aerosol population and one in the Eastern North Atlantic Ocean (ENA) region with a primarily marine-influenced aerosol population. These measurements examined INPs mainly formed through immersion freezing and were performed at a ≤ 12 min resolution and with a wide range of heterogeneous freezing temperatures (Ts above −31 °C) for at least 45 d at each site. The associated INP data analysis was conducted in a consistent manner. We also explored the additional offline characterization of ambient aerosol particle samples from both locations in comparison to in situ data. From our ENA data, on average, INP abundance ranges from ≈ 1 to ≈ 20 L−1 (−30 °C ≤ T ≤ −20 °C) during October–November 2020. Backward air mass trajectories reveal a strong marine influence at ENA with 75.7 % of air masses originating over the Atlantic Ocean and 96.6 % of air masses traveling over open water, but analysis of particle chemistry suggests an additional INP source besides maritime aerosols (e.g., sea spray aerosols) at ENA. In contrast, 90.8 % of air masses at the SGP location originated from the North American continent, and 96.1 % of the time, these air masses traveled over land. As a result, organic-rich SGP aerosols from terrestrial sources exhibited notably high INP abundance from ≈ 1 to ≈ 100 L−1 (−30 °C ≤ T ≤ −15 °C) during October–November 2019. The probability density function of aerosol surface area-scaled immersion freezing efficiency (ice nucleation active surface site density; ns) was assessed for selected freezing temperatures. While the INP concentrations measured at SGP are higher than those of ENA, the ns(T) values of SGP (≈ 105 to ≈ 107 m−2 for −30 °C ≤ T ≤ −15 °C) are reciprocally lower than ENA for approximately 2 orders of magnitude (≈ 107 to ≈ 109 m−2 for −30 °C ≤ T ≤ −15 °C). The observed difference in ns(T) mainly stems from varied available aerosol surface areas, Saer, from two sites (Saer,SGP > Saer,ENA). INP parameterizations were developed as a function of examined freezing temperatures from SGP and ENA for our study periods.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1997

Ice Nucleation Processes in Upper Tropospheric Wave-Clouds Observed During SUCCESS

We have compared in situ measurements near the leading-edges of wave-clouds observed during the SUCCESS experiment with numerical modeling of ice nucleation. Observations of high supersaturations with respect to ice (\geq 150\%) near the leading edge of a very cold wave cloud (T < --60^\circC) are consistent with recent theoretical and laboratory studies suggesting that large supersaturations are required to homogeneously freeze sulfate aerosols. Also, the peak ice crystal number densities observed in this cloud (about 4cm -3/sup>) are consistent with the number densities calculated in our model. The consistency between model results (using homogeneous freezing and the observations indicates that the number density of effective heterogeneous ice nuclei must be no more than about 2 cm -3 . In the warmer wave-cloud (T (approx.)eq --37^\circC) relatively large ice number densities were observed (20--40 cm -3 . Our model calculations suggest that these large number densities are only possible if liquid droplets were activated at the cloud leading-edge, followed by subsequent homogeneous freezing. If sulfate aerosols had frozen before liquid droplets could be activated, then the peak ice crystal number density should have been less than 10 cm -3 .

Jensen, E. J.↗

NASA NTRSDate not supplied

The Benefit of NASA's Atmosphere Observing System (AOS) Mission Lidar and Polarimeter Observations for Health and Air Quality Applications

The Atmosphere Observing System (AOS) seeks to explore fundamental questions of how interconnections between aerosols, clouds and precipitation impact our weather and climate, addressing real-world challenges to benefit society. AOS will provide key information to enhance the communities’ ability to improve weather and air quality forecasting today, seasonal to sub-seasonal changes in the near future, and societal challenges resulting from climate change in the decades to come. A fundamental component of the AOS mission is ensuring that health and air quality applications are considered to the greatest extent possible in mission design. As a result, the Applications Impact Team (AIT) was implemented to address this objective. The overarching goal of the AIT is to help improve the capacity for transitioning science to applications to make it possible to more quickly and effectively inform decisions that will directly benefit society. We seek to maximize AOS benefit to impact decisions through early engagement in the mission development phase in order to prepare stakeholders to apply observations as soon as AOS mission data becomes available. To support these efforts, we leverage existing and near future mission applications activities and initiatives, such as the NASA CALIPSO, MAIA, TEMPO, and PACE missions to form a framework to enhance health and air quality applications for AOS. The unique synergy between lidar and polarimeter instruments onboard the AOS constellation, as well as diurnally varying observations of aerosol profiles, will provide new opportunities to engage health and air quality stakeholders for forecasting, monitoring, and warning of hazardous events (e.g., wildfire smoke, volcanic ash) that impact human health. Engaging with existing missions helps identify and understand data needs, gaps and opportunities for current and future stakeholders, determine what aerosol data products are of highest value and use, and helps connect stakeholders with current mission data that can serve as AOS proxy data, among others. In this presentation, we provide an overview of AOS aerosol observations relevant for health and air quality applications, AIT activities and initiatives and how existing aerosol satellite missions and their applications activities can play a critical role in AOS applications development during mission design.

Melanie Follette-Cook↗

NASA NTRS1998

Remote Sensing of Tropospheric Aerosols from Space: Past, Present, and Future

Aerosol particles originate from man-made sources such as urban/industrial activities,rurning associated with land use processes, wind-blown dust, and natural sources. Their interaction with sunlight and their effect on cloud microphysics forms a major uncertainty in predicting climate change. Furthermore, the lifetime of only a few days causes high spatial variability in aerosol optical and radiative properties that requires global observations from space. Remote sensing of aerosol properties from space is reviewed both for present and planned national and international satellite sensors. Techniques that are being used to enhance our ability to characterize the global distribution of aerosol properties include well-calibrated multispectral radiometers, multispectral polarimeters, and multi-angle spectroradiometers. Though most of these sensor systems rely primarily on visible to mid-infrared spectral channels, the availability of of thermal channels to aid in cloud screening is an important additional piece of information that is not always incorporated into the sensor design. In this paper we describe the various satellite sensor systems being developed by Europe, Japan, and the U.S., and highlight the advantages and disadvantages of each of these systems for aerosol applications. An important underlying theme is that the remote sensing of aerosol properties, especially aerosol size distribution and single scattering albedo, is exceedingly difficult. As a consequence, no one sensor system is capable of providing totally unambiguous information, and hence a careful intercomparison of derived products from different sensors, together with a comprehensive network of ground-based sun-photometer and sky radiometer systems, are required to advance our quantitative understanding of global aerosol characteristics.

King, Michael D.↗

DOE OSTI2020

Relationships between Immersion Freezing and Crystal Habit for Arctic Mixed-Phase Clouds—A Numerical Study

Abstract The number concentration of ice particles in Arctic mixed-phase clouds is a major controlling factor of cloud lifetime. The relationships between ice nucleation mode and ice crystal habit development are not yet constrained by observations. This study uses a habit-predicting microphysical scheme within a 3D large-eddy simulation model to evaluate the relationship between immersion freezing and ice habit in a simulated Arctic mixed-phase cloud case. Three immersion freezing parameterizations are considered: a volume-dependent freezing scheme (VF), a parameterization limited to activated droplets (C-AC), and a parameterization limited to coarse aerosol particles (C-CM). Both C-AC and C-CM are based on classical nucleation theory. The freezing rate with VF is found to be greater in downdraft regions than in updraft regions due to the downdraft having a higher number concentration of large droplets. The C-AC cases show active freezing of small droplets near cloud top, whereas in the C-CM cases, mainly the 8–32- μ m-sized droplets freeze in updraft regions near the cloud base. Because the initial crystal size is assumed to affect the axis ratio of hexagonal plates, the VF cases produce crystals with larger axis ratios, resulting in smaller mode radii than the C-AC cases. In all cases, irregular polycrystals dominate near cloud top and a band-like structure develops within the cloud, which qualitatively agrees with previous observations. In the VF and C-CM cases, unactivated large droplets arising from coarse-mode aerosol particles contributed significantly to the freezing rate, producing an important influence on crystal habit.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1985

Cumulus cloud venting of mixed layer ozone

Observations are presented which substantiate the hypothesis that significant vertical exchange of ozone and aerosols occurs between the mixed layer and the free troposphere during cumulus cloud convective activity. The experiments utilized the airborne Ultra-Violet Differential Absorption Lidar (UV-DIAL) system. This system provides simultaneous range resolved ozone concentration and aerosol backscatter profiles with high spatial resolution. Evening transects were obtained in the downwind area where the air mass had been advected. Space-height analyses for the evening flight show the cloud debris as patterns of ozone typically in excess of the ambient free tropospheric background. This ozone excess was approximately the value of the concentration difference between the mixed layer and free troposphere determined from independent vertical soundings made by another aircraft in the afternoon.

Ching, J. K. S.↗

NASA NTRS1985

Cumulus cloud venting of mixed layer ozone

Ching, J. K. S.↗

DOE OSTI2022

Turbulent transport and reactions of plant-emitted hydrocarbons in an Amazonian rain forest

The processes governing the temporal and spatial patterns of isoprene and monoterpenes emitted by a rainforest in the central Amazon region of Brazil is investigated using a combination of field experiments and numerical simulations. Specifically, Large Eddy Simulations (LES) were used to resolve emissions of isoprene and monoterpenes, turbulent transport, and air chemistry. The coupled chemistry-transport LES included the effects of isoprene and monoterpenes reactivity due to reactions with hydroxyl radical and ozone. The LES results are used to compute vertically resolved budgets of isoprene and monoterpenes in the rainforest canopy in response to emissions, turbulent transport, surface deposition, and air chemistry. Our results indicated that emission and dispersion dominated the isoprene budget as the gases were transported out of the canopy space. In a region limited by nitrogen oxides (with prevailing nitric oxide levels of < 0.5 parts per billion), the in-canopy chemical destruction removed approximately 10% of locally emitted monoterpenes. Hydroxyl radical production rates from the ozonolysis of monoterpenes amounted to ≈ 2 x 10 6 radicals cm -3 s -1 and had similar magnitude to the light-dependent hydroxyl radical formation. One key conclusion was that the Amazonia rainforest abundantly emitted monoterpenes whose in-canopy ozonolysis yielded hydroxyl radicals in amounts similar to the magnitude of light-dependent formation. Reactions of monoterpenes and isoprene with hydroxyl radical and ozone were necessary for the maintenance of the Amazon rainforest canopy as a photochemically active environment suitable to generate oxidants and secondary organic aerosols.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

On the Emergence of Human Influence on Surface Air Temperature Changes Over India

Human activities in terms of greenhouse gas (GHG) emissions and aerosols resulting from the combustion of fossil fuels have been shown to have affected the temperature of the Earth on global and continental scales. The surface air temperature (TAS) over India has also been observed to be increasing over the last 100 years. Understanding the underlying causes of regional climate change over India can help in developing appropriate mitigation and adaptation strategies. Differentiating signals of externally forced climate changes from the noise of natural internal variability generally becomes more difficult as spatial scale reduces. Therefore detecting and attributing the influence of external forcings such as GHGs and aerosols is harder at local and regional scales. In this study, we applied a detection and attribution (D&A) method to study annual and seasonal mean TAS over the Indian region. We found that the observed warming over India from 1906 to 2005 cannot be explained by natural climate variability alone. We found that the warming is largely driven by the increase in GHGs, and partially offset by regional anthropogenic emissions of aerosols. These results were confirmed for the shorter 1956–2005 period, but results were sensitive to the choice of observational data set. Furthermore, the changes cannot be explained by internal climate variability or natural external forcings alone, but are compatible with the responses to combined anthropogenic GHG and aerosol forcings.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Impact of Meteorological Factors on the Mesoscale Morphology of Cloud Streets during a Cold-Air Outbreak over the Western North Atlantic

We report postfrontal clouds (PFC) are ubiquitous in the marine boundary layer, and their morphology is essential to estimating the radiation budget in weather and climate models. Here we examine the roles of sea surface temperature (SST) and meteorological factors in controlling the mesoscale morphology and evolution of shallow clouds associated with a cold-air outbreak that occurred on 1 March 2020 during phase I of the Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE). Our results show that the simulated PFC structure and ambient conditions by the Weather Research and Forecasting (WRF) Model are generally consistent with observations from GOES-16 and dropsonde measurements. We also examine the thermodynamical and dynamical influences in the cloud mesoscale morphology using WRF sensitivity experiments driven by two meteorological forcing datasets with different domain-mean SST and spatial gradients, which lead to dissimilar values of hydrometeor water path and cloud core fraction. The SST from ERA5 leads to weaker stability and higher inversion height than the SST from FNL does. In addition, the use of large-scale meteorological forcings from ERA5 yields a distinctive time evolution of wind direction shear in the inner domain, which favors the formation and persistence of longer cloud rolls. Both factors contribute to a change in the time evolution of domain-mean water path and cloud core fraction of cloud streets. Our study takes advantage of the simulation driven by the differences between two large-scale forcing datasets to illustrate the importance of SST and wind direction shear in the cloud street morphology in a realistic scenario.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1974

A remote sensing study of Pacific hurricane Ava

Aircraft, Skylab, NOAA-2, ATS-3, and NIMBUS-5 recently obtained a variety of measurements of Pacific hurricane Ava. These measurements are unusually broad in scope and include satellite observed passive microwave emissivities at 13.9 and 19.5 GHz, active microwave scattering cross-sections at 13.9 GHz, and near infrared and visible images. Essentially simultaneous aircraft measurements of wind speed, waves, whitecaps, 1.4 and 13-15 GHz passive microwave emissivities, 1.4 GHz active microwave images, sea surface temperatures, pressure fields, and aerosol size distributions were also obtained. A brief description of sensors and platforms is presented along with some in-depth details of results obtained.

Ross, D.↗

NASA NTRS2019

Connecting Crop Productivity, Residue Fires, and Air Quality over Northern India

Northwestern India is known as the “breadbasket” of the country producing two-thirds of food grains, with wheat and rice as the principal crops grown under the crop rotation system. Agricultural data from India indicates a 25% increase in the post-monsoon rice crop production in Punjab during 2002–2016. NASA’s A-train satellite sensors detect a consistent increase in the vegetation index (net 21%) and post-harvest agricultural fire activity (net ~60%) leading to nearly 43% increase in aerosol loading over the populous Indo-Gangetic Plain in northern India. The ground-level particulate matter (PM2.5) downwind over New Delhi shows a concurrent uptrend of net 60%. The effectiveness of a robust satellite-based relationship between vegetation index—a proxy for crop amounts, and post-harvest fires—a precursor of extreme air pollution events, has been further demonstrated in predicting the seasonal agricultural burning. An efficient crop residue management system is critically needed towards eliminating open field burning to mitigate episodic hazardous air quality over northern India.

Hiren Jethva↗