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NASA NTRS1998

Analysis of Ice Nucleating Aerosol Measurements during SUCCESS: April, May 1996

This section describes our research activities during year three of this effort. In the second year, preliminary archive data sets were submitted to the SUCCESS archive. After additional analyses, final versions were prepared and submitted. These are included on the SUCCESS CD-ROM data editions that were recently released by NASA Ames. Over the range of temperature and supersaturation conditions of our measurements (15 to -40 C, and from ice saturation to approximately 15% water supersaturation), IN concentrations ranged from less than 0.1 to approximately 500 per liter, being generally greater at colder temperatures and higher supersaturations. To estimate the potential of aircraft exhaust as a source of IN, we examined data from six days of the field project when the DC-8 was following closely behind other humidity conditions of our measurements. In April 1997, a microphysical workshop was convened at NCAR to select cases for in depth analyses and to address questions about the consistency of cloud ice crystal measurements (size distributions and mass concentrations) and aerosol size distributions. We attended this meeting and contributed to the discussions. A particular concern was identified in the CN measurements. On the DC-8, CN measurements were obtained by four different investigator groups, using commercially available instrumentation. The DC-8 SUCCESS CN data showed long periods where the measurements were in substantial agreement, but there were also periods with large discrepancies. Several possible factors were identified that could help explain these discrepancies, including minimum detectable particle size, response at reduced pressures, and location of sample inlet on the aircraft.

Rogers, D. C.↗

DOE OSTI2024

Characterizing Ice Nucleating Particles Over the Southern Ocean Using Simultaneous Aircraft and Ship Observations

Abstract Supercooled liquid clouds are ubiquitous over the Southern Ocean (SO), even to temperatures below −20°C, and comprise a large fraction of the marine boundary layer (MBL) clouds. Earth system models and reanalysis products have struggled to reproduce the observed cloud phase distribution and occurrence of cloud ice in the region. Recent simulations found the microphysical representation of ice nucleation and growth has a large impact on these properties, however, measurements of SO ice nucleating particles (INPs) to validate simulations are sparse. This study presents measurements of INPs from simultaneous aircraft and ship campaigns conducted over the SO in austral summer 2018, which include the first in situ observations in and above cloud in the region. Our results confirm recent observations that INP concentrations are uniformly lower than measurements made in the late 1960s. While INP concentrations below and above cloud are similar, higher ice nucleation efficiency above cloud supports model simulations that the dominant INP composition varies with height. Model parameterizations based solely on aerosol properties capture the mean relationship between INP concentration and temperature but not the observed variability, which is likely related to the only modest correlations observed between INPs and environmental or aerosol metrics. Including wind speed in addition to activation temperature in a marine INP parameterization reduces bias but does not explain the large range of observed INP concentrations. Direct and indirect inference of marine INP size suggests MBL INPs, at least during Austral summer, are dominated by particles with diameters smaller than 500 nm.

Meteorology & Atmospheric Sciences↗

NASA NTRS1994

Heterogeneous Interactions of ClONO2 and HCl with Sulfuric Acid Tetrahydrate: Implications for the Stratosphere

The reaction probabilities for ClONO2+H2O- HOCl + HNO3 and ClONO2+ HCl Cl2 +HNO3 have been investigated on sulfuric acid tetrahydrate (SAT, H2SO4-4H2O)surfaces at temperatures between 190 and 230 K and at reactant concentrations that are typical in the lower stratosphere, using a fast-flow reactor coupled to a quadrupole mass spectrometer. The results indicate that the reaction probabilities as well as HCl uptake depend strongly on the thermodynamic state of SAT surface: they decrease significantly with decreasing H2O partial pressure at a given temperature, and decrease with increasing temperature at a given H2O partial pressure, as the SAT changes from the H2O-rich form to the H2SO4-rich form. For H2O-rich SAT at 195 K gamma(sub 1) approx. = -0.01 and gamma(sub 2) greater or equal to 0.1, whereas the values for H2SO4-rich SAT decrease by more than 2 orders of magnitude. At low concentrations of HCl, close to those found in the stratosphere, the amount of HCl taken up by H2O-rich SAT films corresponds to a coverage of the order of a tenth of a monolayer (approx. = 10(exp 14) molecules/sq cm); H2SO4-rich SAT films take up 2 orders of magnitude less HCl (les than 10(exp 12) molecules/sq cm). Substantial HCl uptake at high HCl concentrations is also observed, as a result of surface melting. The data reveal that frozen stratospheric sulfate aerosols may play an important role in chlorine activation in the winter polar stratosphere via processes similar to those occurring on the surfaces of polar stratospheric cloud particles.

Zhang, Renyi↗

NASA NTRS2006

Processes Influencing Ozone Levels in Alaskan Forest Fires Plumes during Long-Range Transport over the North Atlantic

A case of long-range transport of a biomass burning plume from Alaska to Europe is analyzed using a Lagrangian approach. This plume was sampled several times in the free troposphere over North America, the North Atlantic and Europe by 3 different aircraft during the IGAC Lagrangian 2K4 experiment which was part of the ICARTT/ITOP measurement intensive in summer 2004. Measurements in the plume showed enhanced values of CO, VOCs and NOy, mainly in form of PAN. Observed O3 levels increased by 17 ppbv over 5 days. A photochemical trajectory model, CiTTyCAT, is used to examine processes responsible for the chemical evolution of the plume. The model was initialized with upwind data, and compared with downwind measurements. The influence of high aerosol loading on photolysis rates in the plume is investigated using in-situ aerosol measurements in the plume and lidar retrievals of optical depth as input into a photolysis code (Fast-J), run in the model. Significant impacts on photochemistry are found with a decrease of 18 percent in O3 production and 24 percent in O3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O3 increases attributed primarily to PAN decomposition during descent of the plume towards Europe. The predicted O3 changes are very dependent on temperature changes during transport, and also, on water vapor levels in the lower troposphere which can lead to O3 destruction. Simulation of mixing/dilution was necessary to reproduce observed pollutants level in the plume. Mixing was simulated using background concentrations from measurements in air masses in close proximity to the plume, and mixing timescales (averaging 6.25 days) were derived from CO changes. Observed and simulated O3/CO correlations in the plume are also compared in order to evaluate the photochemistry in the model. Observed slopes changed from negative to positive over 5 days. This change, which can be attributed largely to photochemistry, is well reproduced by multiple model runs even if slope values are slightly underestimated suggesting small underestimation of photochemical processes. The possible impact of this biomass burning plume on O3 levels in the Europe boundary layer is also examined by running the model for a further 5 days, and comparing with data collected at surface sites, such as Jungfraujoch, which showed small O3 increases and elevated CO levels. The model predicts significant changes in O3 over this 10 days due to photochemistry but the signal is largely lost due to the effects of dilution. However, measurement in several others BB plumes over Europe show that O3 impact of Alaskan fires can be punctually significant over Europe.

Real, E.↗

NASA NTRS2023

Emission Factors for Crop Residue and Prescribed Fires in the Eastern US during FIREX-AQ

Agricultural and prescribed burning activities emit large amounts of trace gases and aerosols on regional to global scales. We present a compilation of emission factors (EFs) and emission ratios (ERs) from the eastern portion of the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign in 2019 in the United States, which sampled burning of crop residues and other prescribed fire fuels. FIREX-AQ provided comprehensive chemical characterization of 53 crop residue and 22 prescribed fires. Crop residues burned at different modified combustion efficiencies (MCE), with corn residue burning at higher MCE than other fuel types. Prescribed fires burned at lower MCE (<0.90) which is typical, while grasslands burned at lower MCE (0.90) than normally observed due to moist, green, growing season fuels. Most non-methane volatile organic compounds (NMVOCs) were significantly anticorrelated with MCE except for ethanol and NMVOCs that were measured with less certainty. We identified 23 species where crop residue fires differed by more than 50% from prescribed fires at the same MCE. Crop residue EFs were greater for species related to agricultural chemical use and fuel composition as well as oxygenated NMVOCs possibly due to the presence of metals such as potassium. Prescribed EFs were greater for monoterpenes (5×). FIREX-AQ crop residue average EFs generally agreed with the previous agricultural fire study in the US but had large disagreements with global compilations. FIREX-AQ observations show the importance of regionally-specific and fuel-specific EFs as first steps to reduce uncertainty in modeling the air quality impacts of fire emissions.

air quality↗

NASA NTRSDate not supplied

The Trash Compaction Processing System (TCPS) Technology Demonstrations and Risk Reduction Activities 2023-2024

The Trash Compactor Processing System (TCPS) employs heat and pressure to safely compress spacecraft trash. The Next STEP Phase B Appendix 2 contract was awarded to Sierra Space for the development of ground and flight demonstration hardware, slated for testing on the International Space Station in 2026. Meanwhile, Ames Research Center is actively engaged in risk reduction activities related to in-house hardware, fine-tuning science objectives and test procedures.This paper will discuss the updated TCPS requirements and present the results of the risk reduction activities, which include moisture analysis, component offgas, and aerosol analysis.

Justine Tra-my Richardson↗

DOE OSTI2021

Cloud drop number concentrations over the western North Atlantic Ocean: seasonal cycle, aerosol interrelationships, and other influential factors

Cloud drop number concentrations (N d ) over the western North Atlantic Ocean (WNAO) are generally highest during the winter (DJF) and lowest in summer (JJA), in contrast to aerosol proxy variables (aerosoloptical depth, aerosol index, surface aerosol mass concentrations, surface cloud condensation nuclei (CCN) concentrations) that generally peak inspring (MAM) and JJA with minima in DJF. Using aircraft, satellite remote sensing, ground-based in situ measurement data, and reanalysis data, we characterize factors explaining the divergent seasonal cycles and furthermore probe into factors influencing N d on seasonal timescales. The results can be summarized well by features most pronounced in DJF, including features associated with cold-air outbreak (CAO) conditions such as enhanced values of CAO index, planetary boundary layer height (PBLH),low-level liquid cloud fraction, and cloud-top height, in addition to winds aligned with continental outflow. Data sorted into high- and low-N d days in each season, especially in DJF, revealed that all of these conditions were enhanced on the high-N d days, including reduced sea level pressure and stronger wind speeds. Although aerosols may be more abundant in MAM and JJA, the conditions needed to activate those particles into cloud droplets are weaker than in colder months, which is demonstrated by calculations of the strongest (weakest) aerosol indirect effects in DJF (JJA) based on comparing N d to perturbations in four different aerosol proxy variables (total and sulfate aerosol optical depth, aerosol index, surface mass concentration of sulfate). We used three machine learning models and up to 14 input variables to infer about most influential factors related to N d for DJF and JJA, with the best performance obtained with gradient-boosted regression tree (GBRT) analysis. The model results indicated that cloud fraction was the most important input variable, followed by some combination (depending on season) of CAO index and surface mass concentrations of sulfate and organic carbon. Future work is recommended to further understand aspects uncovered here such as impacts of free tropospheric aerosol entrainment on clouds, degree of boundary layer coupling, wet scavenging, and giant CCN effects on aerosol–N d relationships, updraft velocity, and vertical structure of cloud properties such as adiabaticity that impact the satellite estimation of N d .

54 ENVIRONMENTAL SCIENCES↗

NASA NTRSDate not supplied

The Representation of Aerosols in GMAO’s Newest Reanalyses

Over the past few years, NASA’s Global Modelling and Assimilation Office has been working on the configuration and production of three new reanalysis products, GEOS-IT, GiOcean, and MERRA-21C. GEOS-IT, or the Goddard Earth Observing System for Instrument Teams, is a 3D variational data assimilation system that runs in a near real time framework however retrospectively provides data back through 1998 to deliver a consistent view of the Earth-atmosphere system for the production of observational NASA products. Retrospective production for GEOS-IT is complete and the meteorology has since been used to produce the one way weakly coupled GiOcean reanalysis. Due to differences in the atmospheric model, particularly related to scavenging, aerosols are not identical in GEOS-IT and GiOcean. MERRA-21C, or the Modern Era Restrospective analysis for Research and Applications in the 21st century, is a hybrid 4D ensemble variational system at a finer horizontal resolution of 0.25 degrees. Although different in their intended use, and therefore configuration, these systems prominently feature coupling between meteorology and aerosols. The differences and similarities in the aerosol configuration between the three systems will be discussed, covering biomass burning and anthropogenic emissions as well as observations used for the assimilation of aerosol optical depth. A large emphasis will be placed on the version of the underlying aerosol module, GOCART, which underwent a complete refactoring and the addition of radiatively active brown carbon between GEOS-IT and MERRA-21C. Independent observations will be used to evaluate the performance of aerosols in both reanalyses, focusing on aerosol optical depth, surface particulate matter, and vertical profiles of aerosol backscatter.

Allison Collow↗

NASA NTRS2008

CALIPSO Observations of Volcanic Aerosol in the Stratosphere

In the stratosphere, the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) has observed the presence of aerosol plumes associated with the eruptions several volcanoes including Montserrat (May 2006), Chaiten (May 2008), and Kasatochi (August 2008). While the dense ash plumes from these eruptions dissipate relatively quickly, CALIPSO continued to detect an enhanced aerosol layer from the Montserrat eruption from the initial observations in June 2006 well into 2008. Solar occultation missions were uniquely capable of monitoring stratospheric aerosol. However, since the end of long-lived instruments like the Stratospheric Aerosol and Gas Experiment (SAGE II), there has been no clear space-based successor instrument. A number of active instruments, some employing new techniques, are being evaluated as candidate sources of stratospheric aerosol data. Herein, we examine suitability of the CALIPSO 532-nm aerosol backscatter coefficient measurements.

Thomason, Larry W.↗

NASA NTRS2022

Chapter 10 - Remote Sensing Measurements of Aerosol Properties

Satellite instruments have proven especially capable at monitoring the quantity of airborne particles in columns of atmosphere, globally. This chapter describes the principles of satellite measurements and retrieval algorithms, and surveys current instruments and their capabilities. We outline the issues associated with retrieval algorithms, such as surface characterization and aerosol proximity to clouds, and the challenges with interpretation of the results. The relationship between measured aerosol properties and climate-relevant aerosol properties simulated in models is outlined, as well as how measurements are used to evaluate models. Most space-based aerosol instruments are passive sensors that measure reflected sunlight at multiple wavelengths, some at multiple viewing angles. A few are active sensors that send out their own laser light and measure the returned signal. Except when clouds are present, the excess amount of light scattered back to space, beyond that expected from the surface and atmospheric gas, is attributed to aerosol. Satellite measurements are used in many ways in aerosol research. They often provide the only method for monitoring hazardous phenomena such as major wildfire and volcanic eruption plumes, especially in remote areas. Stable, long-term, near-global-scale satellite data records make it possible to identify regional and global aerosol trends. Aerosol radiative effects on climate can be quantified on a near-global scale and used to estimate the strength of aerosol–radiation and aerosol–cloud interactions as well as to evaluate climate model simulations of these interactions. Aerosol-type mapping from satellite imagery is helpful for source attribution, model validation, and to constrain particle light-absorption properties that are essential for radiative forcing calculations. The range of aerosol properties retrieved from satellite observations has grown considerably since the first global estimates of aerosol optical depth (τ a) over ocean were made in the late 1970s. Methods for retrieving particle size and light-absorption properties were explored in the 1990s using multispectral, multi-angle observations, and polarization in visible and near-infrared wavelengths. Sensitivity to particle light absorption, primarily from black or brown carbon content, improved with the inclusion of UV channels, and sensitivity to very thin aerosol layers in the upper troposphere and lower stratosphere was advanced with the use of limb-sounding instruments and active sensors. There are limitations to every measurement technique, including satellite aerosol remote sensing. For wide-swath, passive instruments, aerosol retrievals near clouds can present substantial challenges as far as 15 km away due to cloud-scattered light contaminating the signal. In nearly all cases, retrievals over bright snow and ice surfaces are precluded because surface reflectance uncertainties can overwhelm the aerosol signal. Similarly, meteorological cloud is identified and masked out where possible. Data from passive sensors also lack vertical resolution except those that view toward the limb or where multi-angle imagery is acquired over plumes from wildfires, erupting volcanoes, and wind-blown dust. Yet, passive sensors provide vastly more coverage than the active instruments that mitigate these issues. Particle microphysical information is qualitative from all remote sensing techniques, relying on proxies to infer particle composition, hygroscopicity, and the amount of light-absorbing material. Further, particles smaller than about 200 nm diameter cannot be distinguished from atmospheric gas molecules with remote sensing, which hinders studies of cloud condensation nuclei and their effects on clouds. Most satellite instruments dedicated to aerosol observations are in low-Earth, near-polar, sun-synchronous orbits, which means they cross the equator at the same local time each day. Most are set on cycles that repeat approximately every 16 days, which makes it difficult to monitor aerosol evolution locally. Geostationary satellites make it possible to observe changes occurring from minutes to hours over regions up to 8000 km in size, but lack coverage of high latitudes, and often provide more limited constraints on aerosol properties. Ground-truth data are vital for satellite aerosol-retrieval validation. The AErosol RObotic NETwork (AERONET) of sun photometers was created in 1993 and has become an established global network of over 350 instruments for validating satellite measurements. The network, as well as global networks of ground-based lidars, solar flux radiometers and other sun photometers, are widely used for evaluating global satellite retrievals and model simulations. NASA's Earth Observing System (EOS) program beginning in 1999 led to improvements in reliability, spatial resolution, and spectral resolution (and hence, to improved particle size discrimination and light absorption properties). Satellite payloads include advanced broad-swath and multi-angle imagers, along with the first space-based active sensor focused largely on long-term aerosol monitoring. Since about 2002, Europe's SENTINEL and operational meteorological satellite fleets are also providing sustained aerosol observations, with planned continuation until at least 2030. Satellite remote sensing instruments offer valuable data for evaluating aerosol representations in global climate models. They have been used to assess aerosol optical and physical properties, trends and distributions, and are applied increasingly as direct model constraints in data assimilation to create global aerosol reanalysis products. Aerosol optical depth is the most common quantity adopted for routine model evaluation, including multiwavelength data to loosely constrain particle-size distributions. These evaluations of multiple models have revealed general biases in their regional aerosol amounts and seasonal patterns of transport and removal. Although satellite measurements have near-global coverage, substantial errors can be introduced into the model observation comparison unless attention is paid to spatial and temporal collocation, cloud screening, subgrid-scale variability, and measurement uncertainties that vary with retrieval conditions.

aerosol properties↗

NASA NTRS2023

The Extreme Forest Fires in California/Oregon in 2020: Aerosol Optical and Physical Properties and Comparisons of Aged Versus Fresh Smoke

Wildfire activity in the western United States during August to October 2020 was exceptional in terms of the fire severity and area burned. Extremely dry biomass fuels from near historic multi-year drought conditions were further exacerbated with very hot and dry conditions in 2020. These conditions when coupled with strong offshore flow allowed many ignitions to grow into extremely large and severe wildfires. Long-term monitoring at a few AERONET sites in California showed that the number of days with high Aerosol Optical Depth at 440 nm (AOD 440 >1) in 2020 was greater than any other year going back to the beginning of the data records in 2002. A wide range of fine mode particle volume median radii were retrieved from AERONET data over the course of these fires suggesting significant variability in combustion conditions and aging processes. Additionally, the fine mode radii in some of these smoke plumes in 2020 were very large especially at high AOD (∼0.22–0.32 μm volume median radius), likely due to both coagulation and condensation occurring during aging at very high particulate concentrations. The largest fine mode particle radii combined with narrow distributions resulted in some very rare AOD spectra showing peak AOD at 500 nm and decreasing to lower AOD at both shorter and longer wavelengths. The most extreme retrieved size distributions and associated measured AOD spectra were principally observed in long-distance transported smoke plumes from these western United States fires at sites in Colorado, Maryland and Virginia, possibly due to further aging during transport. Additionally, strong absorption was sometimes observed at short wavelengths with much lower single scattering albedo at 440 nm compared to 675 nm in some plumes consistent with significant brown carbon (BrC) and/or coated black carbon (BC) absorption in biomass burning particles. This strong spectral absorption signature observed at some California sites and dates remained similarly strong in some smoke plumes observed at some east coast sites in Maryland and Virginia, thereby suggesting that the lifetime of these particular BrC and/or coated BC absorbing species was greater than 5 days.

Aerosol↗

DOE OSTI2022

Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic

Abstract. Formation of atmospheric ice plays a crucial role in the microphysical evolution of mixed-phase and cirrus clouds and thus climate. How aerosol particles impact ice crystal formation by acting as ice-nucleating particles (INPs) is a subject of intense research activities. To improve understanding of atmospheric INPs, we examined daytime and nighttime particles collected during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign conducted in summer 2017. Collected particles, representative of a remote marine environment, were investigated for their propensity to serve as INPs in the immersion freezing (IMF) and deposition ice nucleation (DIN) modes. The particle population was characterized by chemical imaging techniques such as computer-controlled scanning electron microscopy with energy-dispersive X-ray analysis (CCSEM/EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine-structure spectroscopy (STXM/NEXAFS). Four major particle-type classes were identified where internally mixed inorganic–organic particles make up the majority of the analyzed particles. Following ice nucleation experiments, individual INPs were identified and characterized by SEM/EDX. The identified INP types belong to the major particle-type classes consisting of fresh sea salt with organics or processed sea salt containing dust and sulfur with organics. Ice nucleation experiments show IMF events at temperatures as low as 231 K, including the subsaturated regime. DIN events were observed at lower temperatures of 210 to 231 K. IMF and DIN observations were analyzed with regard to activated INP fraction, ice-nucleation active site (INAS) densities, and a water activity-based immersion freezing model (ABIFM) yielding heterogeneous ice nucleation rate coefficients. Observed IMF and DIN events of ice formation and corresponding derived freezing rates demonstrate that the marine boundary layer aerosol particles can serve as INPs under typical mixed-phase and cirrus cloud conditions. The derived IMF and DIN parameterizations allow for implementation in cloud and climate models to evaluate predictive effects of atmospheric ice crystal formation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Bayesian Cloud Property Retrievals from ARM Active and Passive Measurements

The optimum use of the continuous measurements of thermodynamics, radiation, aerosols, clouds and precipitation from the DOE Atmospheric Radiation Measurement (ARM) program is key to achieve the DOE Atmospheric System Research (ASR)’s objectives. One of the key mission requirements is to retrieve cloud and precipitation properties, as well as vertical motion parameters, along the vertical cross- section defined by the profiling active sensors. Such retrievals are challenging to perform continuously in the entire spectrum of cloud and precipitation conditions due to the large natural microphysical and dynamical variability, the often-limited information content in the measurements, and the lack of proper characterization of measurement quality and uncertainty. Today, the acquisition of new remote and in-situ sensors by the ARM program creates opportunities to address the microphysical retrieval problem by exploiting new, more robust retrieval techniques and integrating various scattered advancements in both sensor techniques and retrieval algorithms. During this project, we constructed a robust Bayesian Markov chain Monte Carlo (MCMC) cloud property retrieval algorithm that includes a state of the art radar forward model. Our MCMC-based retrieval produces both the best estimate of height-resolved cloud and precipitation properties in the radar profile, as well as an estimate of the in-cloud vertical motion and turbulence. In addition, the MCMC algorithm automatically produces robust and flexible estimates of retrieval uncertainty. We tested the algorithm on several synthetic cloud profiles obtained from large eddy simulation (LES) models with bin-resolved microphysics.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2005

NASA's East and Southeast Asia Initiatives: BASE-ASIA and EAST-AIRE

Airborne dust from northern China influences air quality and regional climate in Asia during springtime. However, with the economic growth in China, increased emission of particulate air pollutants from industrial and vehicular sources will not only impact the earth's radiation balance, but also adversely affect human health year round. In addition, both of dust and aerosol pollutants can be transported swiftly across the Pacific affecting North America within a few days. Asian dust and pollutant aerosols can be detected by their colored appearance using current Earth observing satellites (e.g., MODIS, SeaWiFS, TOMS, etc.) and by sunphotometers deployed on the surface of the earth. Biomass burning has been a regular practice for land clearing and conversion in many countries, especially those in Africa, South America, and Southeast Asia. However, the climatology of Southeast Asia is very different than that of Africa and South America, such that large-scale biomass burning causes smoke to interact extensively with clouds during the peak-burning season of March to April. Globally significant sources of greenhouse gases (eg., CO2, CH4), chemically active gases (e.g., NO, CO, HC, CH3Br), and atmospheric aerosols are produced by biomass burning. These gases influence the Earth-atmosphere system, impacting both global climate and tropospheric chemistry. Some aerosols can serve as cloud condensation nuclei, which play a role in determining cloud lifetime and precipitation, altering the earth's radiation and water budgets. Biomass burning also affects the biogeochemical cycling of nitrogen and carbon compounds; the hydrological cycle; land surface reflectivity and emissivity; and ecosystem biodiversity and stability. Two NASA initiatives, EAST-AIRE (East Asian Study of Tropospheric Aerosols: an International Regional Experiment) and BASE-ASIA (Biomass-burning Aerosols in South East-Asia: Smoke Impact Assessment) will be presented. The objectives of these initiatives is to develop a better understanding of the impacts of aerosols on regional-to-global climate, hydrological and carbon cycles, and tropospheric chemistry.

Tsay, S.↗

NASA NTRS2004

Dust, Pollution, and Biomass Burning Aerosols in Asian Pacific: A Column Satellite-Surface Perspective

Airborne dusts from northern China contribute a significant part of the air quality problem and, to some extent, regional climatic impact in Asia during spring-time. However, with the economical growth in China, increases in the emission of air pollutants generated from industrial and vehicular sources will not only impact the radiation balance, but adverse health effects to humans all year round. In addition, both of these dust and air pollution clouds can transport swiftly across the Pacific reaching North America within a few days, possessing an even larger scale effect. The Asian dust and air pollution aerosols can be detected by its colored appearance on current Earth observing satellites (e.g., MODIS, SeaWiFS, TOMS, etc.) and its evolution monitored by satellites and surface network. Biomass burning has been a regular practice for land clearing and land conversion in many countries, especially those in Africa, South America, and Southeast Asia. However, the unique climatology of Southeast Asia is very different than that of Africa and South America, such that large-scale biomass burning causes smoke to interact extensively with clouds during the peak-burning season of March to April. Significant global sources of greenhouse gases (e.g., CO2, CH4), chemically active gases (e.g., NO, CO, HC, CH3Br), and atmospheric aerosols are produced by biomass burning processes. These gases influence the Earth-atmosphere system, impacting both global climate and tropospheric chemistry. Some aerosols can serve as cloud condensation nuclei, which play an important role in determining cloud lifetime and precipitation, hence, altering the earth's radiation and water budget. Biomass burning also affects the biogeochemical cycling of nitrogen and carbon compounds from the soil to the atmosphere; the hydrological cycle (i.e., run off and evaporation); land surface reflectivity and emissivity; as well as ecosystem biodiversity and stability. Two new initiatives, EAST-AIRE (East Asian Study of Tropospheric Aerosols: an International Regional Experiment) and BASE-ASIA (Biomass-burning Aerosols in South East-Asia: Smoke Impact Assessment) will be presented and discussed their contribution to better understand the impacts of aerosols on regional-to-global climate, hydrological and carbon cycles, and tropospheric chemistry.

Tsay, Si-Chee↗

DOE OSTI2024

Baselining the Indirect Effect by Improving Quantification of Sea Spray and Marine Sources at Ascension Island (Final Report)

Oceans cover two-thirds of the Earth and understanding the interactions of aerosols with clouds in these large marine regions requires quantifying the man-made contributions to the budget of cloud-drop forming particles (known as cloud condensation nuclei, or CCN) relative to the non-manmade “baseline” conditions and understanding the meteorology of boundary layer clouds. Modeling studies have shown substantial uncertainties and sensitivities to natural marine CCN sources, meaning that to reduce uncertainties in indirect effects we must be able to better quantify the CCN budget in ocean regions. While models provide important constraints on these uncertainties, actually reducing uncertainties requires substantial observations in open-ocean and coastal regions in order to establish the baseline on which manmade emissions are added. The tropical South Atlantic Ocean is one of the least-sampled regions of the planet, making the comprehensive measurements of the Department of Energy Atmospheric Radiation Measurement Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign provides the longest record of aerosol size distribution measurements from a differential mobility analyzer in a cloud-influenced marine location in the ARM database, with 17 months of ground-based aerosol size distribution measurements. This project addressed the research topic of Aerosol-Cloud Interactions (ACI) by supporting three publications from the LASIC measurements: 1. The ARM measurements were combined with a new value-added technique that was pioneered by the Russell group for quantifying sea salt. This quantification of sea salt uses supermicron scattering measurements for retrieving reasonable sea spray mass concentrations, providing the best-available, observationally-constrained estimate of the sea spray mode properties when supermicron size distribution measurements are not available. 2. The fitted modes of the distribution were used to investigate the signatures of cloud processing for very clean to very smoky aerosol conditions, revealing not only differences in the particles that activate in clouds but also in the mechanisms that control that droplet formation process. In clean air, the size required to form a cloud droplet is influenced by the number of particles, as well as how quickly particles take up water during growth in cloud. 3. Building on this aerosol characterization, cloud and meteorological conditions were used to evaluate aerosol-related changes in cloud albedo and optical depth. We introduced a new method of decomposing the impact of aerosols on clouds known as the Twomey effect by incorporating retrieved supersaturation from two independent sets of observations to constrain the feedback of aerosol particles on cloud properties. The method quantifies the reduction of the Twomey effect at high aerosol concentrations, which has never been explained quantitatively by observations. In addition, the results provide the first direct validation for the conditions observed in the tropical South Atlantic of a parcel-based approach that is embedded in many climate models. Together these findings illustrate how ARM extended field campaigns in stratocumulus-covered regions can be used to constrain ACI processes with direct observations, providing specific radiative effects without models. By making such process-specific constraints available to improve ACI in global climate models, ARM observations play a key role in supporting model development.

58 GEOSCIENCES↗

NASA NTRS1996

High Resolution Doppler Lidar

This Grant supported the development of an incoherent lidar system to measure winds and aerosols in the lower atmosphere. During this period the following activities occurred: (1) an active feedback system was developed to improve the laser frequency stability; (2) a detailed forward model of the instrument was developed to take into account many subtle effects, such as detector non-linearity; (3) a non-linear least squares inversion method was developed to recover the Doppler shift and aerosol backscatter without requiring assumptions about the molecular component of the signal; (4) a study was done of the effects of systematic errors due to multiple etalon misalignment. It was discovered that even for small offsets and high aerosol loadings, the wind determination can be biased by as much as 1 m/s. The forward model and inversion process were modified to account for this effect; and (5) the lidar measurements were validated using rawinsonde balloon measurements. The measurements were found to be in agreement within 1-2 m/s.

Source record↗

NASA NTRS2015

Aerosol-Cloud Interactions in the South-East Atlantic: Knowledge Gaps, Planned Observations to Address Them, and Implications for Global Climate Change Modeling

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical Stratocumulus (Sc) cloud decks in the world. The stratocumulus "climate radiators" are critical to the regional and global climate system. They interact with dense layers of BB aerosols that initially overlay the cloud deck, but later subside and are mixed into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects. As emphasized in the latest IPCC report, the global representation of these aerosol-cloud interaction processes in climate models is one of the largest uncertainty in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for global climate change scenarios. We discuss the current knowledge of aerosol and cloud property distributions based on satellite observations and sparse suborbital sampling, and describe planned field campaigns in the region. Specifically, we describe the scientific objectives and implementation of the following four synergistic, international research activities aimed at providing a process-level understanding of aerosol-cloud interactions over the SE Atlantic: 1) ORACLES (Observations of Aerosols above Clouds and their interactions), a five-year investigation between 2015 and 2019 with three Intensive Observation Periods (IOP), recently funded by the NASA Earth-Venture Suborbital Program, 2) CLARIFY-2016 (Cloud-Aerosol-Radiation Interactions and Forcing: Year 2016), a comprehensive observational and modeling programme funded by the UK's Natural Environment Research Council (NERC), and supported by the UK Met Office. 3) LASIC (Layered Atlantic Smoke Interactions with Clouds), a funded deployment of the DOE (Department of Energy) ARM Mobile Facility (AMF1) to Ascension Island, nominally for April 1 2016 - March 31 2017, and 4) ONFIRE (Observations of Fire's Impact on the southeast Atlantic Region), a proposed deployment of the NCAR C-130 aircraft to Sao Tome Island in 2017.

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