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Interplay of Gas-phase Reactions and Multi-phase Processes on Phase State and Growth Dynamics of Secondary Organic Aerosols

The formation, growth and evolution of secondary organic aerosols (SOA) are complex multiphase chemical processes, which represent one of the most challenging and demanding problems in research on atmospheric aerosol processes. The research goal of this project was to advance the fundamental understanding of the interplay between gas-phase chemistry and multiphase processes on phase state and growth dynamics of SOA for better predictivity of aerosol effects on climate and air quality.

54 ENVIRONMENTAL SCIENCES↗

Retrieval of Aerosol Properties from Multi-Spectral Extinction Measurements

The direct-beam spectral extinction of solar radiation contains information on atmospheric composition in a form that is essentially free from the data analysis complexities that often arise from multiple scattering. Ground based Multi-Filter Shadowband Radiometer (MFRSR) measurements provide such information for the vertical atmospheric column path, while solar occultation measurements from a satellite platform provide horizontal slices through the atmosphere. We describe application of a Multi-Spectral Atmospheric Column Extinction (MACE) analysis technique used to analyze MFRSR data also to occultation measurements made by SAGE II. For analysis, we select the 1985 Nevado del Ruiz volcanic eruption period to retrieve atmospheric profiles of ozone and NO2, and changes in the stratospheric aerosol size and optical depth. The time evolution of volcanic aerosol serves as a passive tracer to study stratospheric dynamics, and changes in particle size put constraints on the sulfur chemistry modeling of volcanic aerosols. Paper presented at The '99 Kyoto Aerosol-Cloud Workshop, held Dec 1-3, 1999, Kyoto, Japan

Lacis, Andrew A.↗

Retrieval of Aerosol Properties from Multi-Spectral Extinction Measurements

The direct-beam spectral extinction of solar radiation contains information on atmospheric composition in a form that is essentially free from the data analysis complexities that often arise from multiple scattering. Ground based Multi-Filter Shadowband Radiometer (MFRSR) measurements provide such information for the vertical atmospheric column path, while solar occultation measurements from a satellite platform provide horizontal slices through the atmosphere. We describe application of a Multi-Spectral Atmospheric Column Extinction (MACE) analysis technique used to analyze MFRSR data also to occultation measurements made by SAGE 11. For analysis, we select the 1985 Nevado del Ruiz volcanic eruption period to retrieve atmospheric profiles of ozone and NO2, and changes in the stratospheric aerosol size and optical depth. The time evolution of volcanic aerosol serves as a passive tracer to study stratospheric dynamics, and changes in particle size put constraints on the sulfur chemistry modeling of volcanic aerosols.

Lacis, Andrew A.↗

Developing a Model-based Capability to Analyze Requirements for the Climate Observing System

Models are foundational for estimating states of the earth's climate system, both as tools to extrapolate information in time and space, and as observation 'operators' used to relate what is analyzed and predicted to what is observed. Expanding the simulation approach further, observing system simulation experiments (OSSEs) are designed to mimic the complete process of analyzing the climate state by replacing real observations with entirely simulated ones determined from a model-based depiction of nature. OSSEs provide a framework to 'fly' simulated satellite instruments through a synthetic atmosphere and investigate the trade-spaces of measurements for various satellite configurations and sampling strategies, and assess their measurement impact on modeling and forecasting capabilities. Such a tool is a crucial but as yet unfulfilled need for future mission selection and design. The components of a state-of-the-art OSSE system are being assembled at the Global Modeling and Assimilation Office (GMAO, Code 610.1) at NASA/GSFC, leveraging on the GMAO's existing modeling and data assimilation infrastructure for numerical weather prediction (NWP). The OSSE framework is based on the GMAO's Goddard Earth Observing System atmospheric general circulation model, version 5 (GEOS-5) and the Gridpoint Statistical Interpolation (GSI) observational analysis scheme, combined with the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) model developed by the Atmospheric Chemistry and Dynamics Branch (Code 613.3). This system is an evolving, key component of Goddard's planned development of an Integrated Earth System Analysis (IESA) capability, which will bring together into a single, fully interactive system Goddard's modeling and assimilation efforts in atmosphere, ocean and chemistry and aerosols to provide a comprehensive analysis and prediction system for weather and climate In addition to providing a state-of-the-art capability for assimilating current observation types, GEOS-5, and the future IESA, provide the capability to identify the need for, and assess the potential impact of, future observing systems under consideration for improving weather and climate prediction.

Gelaro, Ronald↗

Connecting Regional Aerosol Emissions Reductions to Local and Remote Precipitation Responses

The unintended climatic implications of aerosol and precursor emission reductions implemented to protect public health are poorly understood. We investigate the precipitation response to regional changes in aerosol emissions using three coupled chemistry-climate models: NOAA Geophysical Fluid Dynamics Laboratory Coupled Model 3 (GFDL-CM3), NCAR Community Earth System Model (CESM1), and NASA Goddard Institute for Space Studies ModelE2 (GISS-E2). Our approach contrasts a long present-day control simulation from each model (up to 400 years with perpetual year 2000 or 2005 emissions) with 14 individual aerosol emissions perturbation simulations (160-240 years each). We perturb emissions of sulfur dioxide and/or carbonaceous aerosol within six world regions and assess the significance of precipitation responses relative to internal variability determined by the control simulation and across the models. Global and regional precipitation mostly increases when we reduce regional aerosol emissions in the models, with the strongest responses occurring for sulfur dioxide emissions reductions from Europe and the United States. Precipitation responses to aerosol emissions reductions are largest in the tropics and project onto the El Nino Southern Oscillation (ENSO). Regressing precipitation onto an Indo-Pacific zonal sea level pressure gradient index (a proxy for ENSO) indicates that the ENSO component of the precipitation response to regional aerosol removal can be as large as 20% of the total simulated response. Precipitation increases in the Sahel in response to aerosol reductions in remote regions because an anomalous interhemispheric temperature gradient alters the position of the Intertropical Convergence Zone (ITCZ). This mechanism holds across multiple aerosol reduction simulations and models.

Westervelt, Daniel M.↗

Laboratory for Atmospheres 2008 Technical Highlights

The 2008 Technical Highlights describes the efforts of all members of the Laboratory for Atmospheres. Their dedication to advancing Earth Science through conducting research, developing and running models, designing instruments, managing projects, running field campaigns, and numerous other activities, is highlighted in this report. The Laboratory for Atmospheres (Code 613) is part of the Earth Sciences Division (Code 610), formerly the Earth Sun Exploration Division, under the Sciences and Exploration Directorate (Code 600) based at NASA s Goddard Space Flight Center in Greenbelt, Maryland. In line with NASA s Exploration Initiative, the Laboratory executes a comprehensive research and technology development program dedicated to advancing knowledge and understanding of the atmospheres of Earth and other planets. The research program is aimed at understanding the influence of solar variability on the Earth s climate; predicting the weather and climate of Earth; understanding the structure, dynamics, and radiative properties of precipitation, clouds, and aerosols; understanding atmospheric chemistry, especially the role of natural and anthropogenic trace species on the ozone balance in the stratosphere and the troposphere; and advancing our understanding of physical properties of Earth s atmosphere. The research program identifies problems and requirements for atmospheric observations via satellite missions. Laboratory scientists conceive, design, develop, and implement ultraviolet, infrared, optical, radar, laser, and lidar technology for remote sensing of the atmosphere. Laboratory members conduct field measurements for satellite data calibration and validation, and carry out numerous modeling activities. These modeling activities include climate model simulations, modeling the chemistry and transport of trace species on regional-to-global scales, cloud-resolving models, and development of next-generation Earth system models. Interdisciplinary research is carried out in collaboration with other laboratories and research groups within the Earth Sciences Division, across the Sciences and Exploration Directorate, and with partners in universities and other Government agencies. The Laboratory for Atmospheres is a vital participant in NASA s research agenda. Our Laboratory often has relatively large programs, sizable satellite missions, and observational campaigns that require the cooperative and collaborative efforts of many scientists. We ensure an appropriate balance between our scientists responsibility for these large collaborative projects and their need for an active individual research agenda. This balance allows members of the Laboratory to continuously improve their scientific credentials. Members of the Laboratory interact with the general public to support a wide range of interests in the atmospheric sciences. Among other activities, the Laboratory raises the public s awareness of atmospheric science by presenting public lectures and demonstrations, by making scientific data available to wide audiences, by teaching, and by mentoring students and teachers. The Laboratory makes substantial efforts to attract new scientists to the various areas of atmospheric research. We strongly encourage the establishment of partnerships with Federal and state agencies that have operational responsibilities to promote the societal application of our science products. This report describes our role in NASA s mission, gives a broad description of our research, and summarizes our scientists major accomplishments during calendar year 2008. The report also contains useful information on human resources, scientific interactions, and outreach activities.

Cote, Charles E.↗

An Aerosol Physical Chemistry Model for the Upper Troposphere

This report is the final report for the Cooperative Agreement NCC2-1000. The tasks outlined in the various proposals are: (1) Development of an aerosol chemistry model; (2) Utilization of satellite measurements of trace gases along with analysis of temperatures and dynamic conditions to understand ice cloud formation, dehydration and sedimentation in the winter polar regions; (3) Comparison of the HALOE and SAGE II time dependencies of the Pinatubo aerosol decay. The publications are attached.

Lin, Jin-Sheng↗

Differential Absorption Lidar (DIAL) Measurements from Air and Space

Differential absorption lidar (DIAL) systems have been used for the measurement of ozone, water vapor, and aerosols from aircraft platforms for over 18 years, yielding new insights into atmospheric chemistry, composition, and dynamics in large-scale field experiments conducted all over the world. The successful deployment of the lidar in-space technology experiment (LITE) in September 1994 demonstrated that space-based lidars can also collect valuable information on the global atmosphere. This paper reviews some of the contributions of the NASA Langley Research Center's airborne ozone and water vapor DIAL systems and space-based LITE system to the understanding of the atmosphere and discusses the feasibility and advantages of putting DIAL systems in space for routine atmospheric measurements of ozone and/or water vapor and aerosols and clouds. The technology and applications of the differential absorption lidar (DIAL) technique have progressed significantly since the first DIAL measurements of Schotland, and airborne DIAL measurements of ozone and water vapor are frequently being made in a wide range of field experiments. In addition, plans are underway to develop DIAL systems for use on satellites for continuous global measurements. This paper will highlight the history of airborne lidar and DIAL systems, summarize the major accomplishments of the NASA Langley DIAL program, and discuss specifications and goals for DIAL systems in space.

Browell, E. V.↗

Comparing the interactions between particulate matter and cloud properties over two populated cities in Texas using WRF-Chem fine-resolution modeling

Accurate modeling of aerosol-cloud interactions is essential for reliable weather and air quality simulations, given their significant impact on precipitation patterns, cloud dynamics, and aerosol distributions. This study employed the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to examine the impact of enhanced meteorological simulations, achieved through advanced microphysics parameterization supported by data assimilation techniques, on air quality across Texas on August 19 and 20, 2022. We tested four distinct configurations: (1) the Morrison two-moment bulk microphysics scheme, (2) Morrison's with observation nudging, (3) the Spectral Bin Microphysics (SBM), and (4) SBM with observation nudging. While the SBM scheme is known for its detailed representation of aerosol-cloud interactions, our focus was on how improvements in meteorological accuracy translate to more precise air quality simulations. Our findings demonstrated a progressive improvement in simulation accuracy, starting with the Morrison's scheme and further enhanced by adopting the SBM scheme, complemented by incorporating observation nudging. Specifically, the combination of the SBM scheme and the nudging substantially enhanced the model's ability to capture convective precipitation events, as shown by better alignment with NEXRAD radar reflectivity, with R increasing from –0.21 to 0.82, IOA from 0.10 to 0.87, and NMB decreasing from 99% to 34% in Houston. The enhanced meteorology translated into more accurate PM 2.5 concentration simulations, particularly through the more accurate representation of aerosol washout during precipitation events. In Houston, the SBM scheme with nudging improved the model's PM 2.5 simulations significantly, with NMB decreasing from –20% to 5% and IOA improving from 0.43 to 0.61. In San Antonio, improvements were also notable, with NMB improved from –27% to –22%, R increased from 0.48 to 0.82, and IOA increased from 0.66 to 0.86. Furthermore, our results underscore the crucial role of accurate meteorological simulations in refining our understanding of aerosol behaviors in relation to precipitation patterns, directly enhancing the reliability and effectiveness of air quality modeling.

54 ENVIRONMENTAL SCIENCES↗

Arctic Warming in Response to Regional Aerosol Emissions Reductions

This study examines the Arctic surface air temperature response to regional aerosol emissions reductions using three fully coupled chemistry–climate models: National Center for Atmospheric Research-Community Earth System Model version 1, Geophysical Fluid Dynamics Laboratory-Coupled Climate Model version 3 (GFDL-CM3) and Goddard Institute for Space Studies-ModelE version 2. Each of these models was used to perform a series of aerosol perturbation experiments, in which emissions of different aerosol types (sulfate, black carbon (BC), and organic carbon) in different northern mid-latitude source regions, and of biomass burning aerosol over South America and Africa, were substantially reduced or eliminated. We find that the Arctic warms in nearly every experiment, the only exceptions being the U.S. and Europe BC experiments in GFDL-CM3 in which there is a weak and insignificant cooling. The Arctic warming is generally larger than the global mean warming (i.e. Arctic amplification occurs), particularly during non-summer months. The models agree that changes in the poleward atmospheric moisture transport are the most important factor explaining the spread in Arctic warming across experiments: the largest warming tends to coincide with the largest increases in moisture transport into the Arctic. In contrast, there is an inconsistent relationship (correlation) across experiments between the local radiative forcing over the Arctic and the simulated Arctic warming, with this relationship being positive in one model (GFDL-CM3) and negative in the other two. Our results thus highlight the prominent role of poleward energy transport in driving Arctic warming and amplification, and suggest that the relative importance of poleward energy transport and local forcing/feedbacks is likely to be model dependent.

Arctic↗

Comparisons of global aerosol simulations from GOCART and GMI-UMich

Global aerosol mass and optical thickness (AOT) simulated by two aerosol models (GOCART and GMI-UMich) are evaluated and the strengths and shortcomings of the model approaches are investigated. These two offline CTM models are driven by the same meteorological fields (NASA GEOS-4), use the same dynamic transport algorithm, and have the same spatial resolution. However, they differ partially in emission, dry/wet deposition, and chemistry. The simulated aerosol masses are evaluated by the surface long-term measurements and short-term field campaigns (ACE-Asia and TRACE-P). AOT are calculated using modeled aerosol mass but externally mixed for GOCART and partially internally mixed for GMI-Mich. These AOT are evaluated using satellite observations from MODIS and MISR and ground measurements from AERONET. Our work demonstrates that there are significant differences in simulated aerosol mass and AOT by the two approaches. Further investigation will be performed to evaluate each mechanism which induces the differences quantitatively by implementing GOCART-like emission, deposition, and chemistry into GMI framework.

Bian, Huisheng↗

The Role of the SO2 Radiative Effect in Sustaining the Volcanic Winter and Soothing the Toba Impact on Climate

Volcanic eruptions are an important climate driver. The impact of Pinatubo-sized eruptions has been observed and is well constrained. The magnitude and duration of volcanic winter effects after super-eruptions such as Toba remain disputed due to disagreement between the strong cooling predicted by models, and much milder climate perturbations according to the paleo data. Here we present a re-evaluated climate impact of a Toba-sized super-eruption based on up-to-date GISS ModelE simulations. In this study, we account for all known primary mechanisms that govern the evolution of the volcanic plume and their nonlinear interactions. The SO2 radiative effects are evaluated for the first time in coupled climate simulations with the interactive atmospheric chemistry module. We found that SO2 effects on photochemistry, dynamics, and radiative forcing are especially prominent. Due to strong absorption in ultraviolet, SO2 feedback on photochemistry partially offsets the limiting effect associated with aerosol microphysical processes. SO2 greenhouse warming soothes the radiative cooling exerted by sulfate aerosols. SO2 absorption in the shortwave and longwave causes radiative heating and lofting of the volcanic plume, and boosts the efficiency of SO2 impact on photochemistry. Our analysis shows that SO2 lifetime and magnitude of effects scale up and increase with the amount of emitted material. For a Pinatubo-sized eruption, SO2 feedbacks on chemistry and dynamics are relevant only during the initial stage of the volcanic plume evolution, while local SO2 concentrations are high. For a Toba-sized eruption, SO2 effects are as important as sulfate aerosols, and produce a less extreme volcanic winter.

Sergey Osipov↗

Development and Evaluation of Chemistry‐Aerosol‐Climate Model CAM5‐Chem‐MAM7‐MOSAIC: Global Atmospheric Distribution and Radiative Effects of Nitrate Aerosol

Abstract An advanced aerosol treatment, with a focus on semivolatile nitrate formation, is introduced into the Community Atmosphere Model version 5 with interactive chemistry (CAM5‐chem) by coupling the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the 7‐mode Modal Aerosol Module (MAM7). An important feature of MOSAIC is dynamic partitioning of all condensable gases to the different fine and coarse mode aerosols, as governed by mode‐resolved thermodynamics and heterogeneous chemical reactions. Applied in the free‐running mode from 1995 to 2005 with prescribed historical climatological conditions, the model simulates global distributions of sulfate, nitrate, and ammonium in good agreement with observations and previous studies. Inclusion of nitrate resulted in ∼10% higher global average accumulation mode number concentrations, indicating enhanced growth of Aitken mode aerosols from nitrate formation. While the simulated accumulation mode nitrate burdens are high over the anthropogenic source regions, the sea‐salt and dust modes respectively constitute about 74% and 17% of the annual global average nitrate burden. Regional clear‐sky shortwave radiative cooling of up to −5 W m −2 due to nitrate is seen, with a much smaller global average cooling of −0.05 W m −2 . Significant enhancements in regional cloud condensation nuclei (at 0.1% supersaturation) and cloud droplet number concentrations are also attributed to nitrate, causing an additional global average shortwave cooling of −0.8 W m −2 . Taking into consideration of changes in both longwave and shortwave radiation under all‐sky conditions, the net change in the top of the atmosphere radiative fluxes induced by including nitrate aerosol is −0.7 W m −2 .

54 ENVIRONMENTAL SCIENCES↗

Natural and anthropogenic perturbations of the stratospheric ozone layer

The paper reviews potential causes for reduction in the ozone abundance. The response of stratospheric ozone to solar activity is discussed. Ozone changes are simulated in relation with the potential development of a fleet of high-speed stratospheric aircraft and the release in the atmosphere of chlorofluorocarbons. The calculations are performed by a two-dimensional chemical-radiative-dynamical model. The importance of heterogeneous chemistry in polar stratospheric clouds and in the Junge layer (sulfate aerosol) is emphasized. The recently reported ozone trend over the last decade is shown to have been largely caused by the simultaneous effects of increasing concentrations of chlorofluorocarbons and heterogeneous chemistry. The possibility for a reduction in stratospheric ozone following a large volcanic eruption such as that of Mount Pinatubo in 1991 is discussed.

Brasseur, Guy P.↗

Preliminary XANES Analysis of Laboratory Analogs of Titan Tholins

Titan, the largest moon of Saturn, is a fascinating object. It is the only other object in the Solar System, besides Earth, with a dense (1.5 bar at the surface) atmosphere whose composition is dominated by N2, with CH4 as the second most abundant gas. A complex organic chemistry between N2 and CH4, induced by solar UV photons and energetic particles, results in the formation of a large variety of organic compounds, including hydrocarbons (e.g., C2H2, C2H4, C2H6, C3H4, C6H6), nitriles (e.g., HCN, HNC, HC3N, CH3CN, C2N2), as well as larger molecules that include aromatic and heteroaromatic compounds [1]. This complex organic chemistry also leads to the formation of aerosols that play an important role in Titan’s atmospheric dynamics, climate, as well as surface composition and processes. Because of its N2-based dense atmosphere, and its CH4 cycle that resembles the hydrological cycle on Earth, Titan is often considered to be an analog of early Earth. In recent years, Titan’s atmosphere and surface were monitored in detail by the NASA Cassini mission, which orbited the Saturnian system from 2004 to 2017, as well as the ESA Huygens probe, which plunged into Titan’s atmosphere and landed on its surface in 2005.

Titan↗

Update on the NASA GEOS-5 Aerosol Forecasting and Data Assimilation System

GEOS-5 is the Goddard Earth Observing System model. GEOS-5 is maintained by the NASA Global Modeling and Assimilation Office. Core development is within GMAO,Goddard Atmospheric Chemistry and Dynamics Laboratory, and with external partners. Primary GEOS-5 functions: Earth system model for studying climate variability and change, provide research quality reanalyses for supporting NASA instrument teams and scientific community, provide near-real time forecasts of meteorology,aerosols, and other atmospheric constituents to support NASA airborne campaigns.

GEOS-5↗

Integrated Modeling of Aerosol, Cloud, Precipitation and Land Processes at Satellite-Resolved Scales

With support from NASA's Modeling and Analysis Program, we have recently developed the NASA Unified-Weather Research and Forecasting model (NU-WRF). NU-WRF is an observation-driven integrated modeling system that represents aerosol, cloud, precipitation and land processes at satelliteresolved scales. "Satellite-resolved" scales (roughly 1e25 km), bridge the continuum between local (microscale), regional (mesoscale) and global (synoptic) processes. NU-WRF is a superset of the National Center for Atmospheric Research (NCAR) Advanced Research WRF (ARW) dynamical core model, achieved by fully integrating the GSFC Land Information System (LIS, already coupled to WRF), the WRF/ Chem enabled version of the Goddard Chemistry Aerosols Radiation Transport (GOCART) model, the Goddard Satellite Data Simulation Unit (G-SDSU), and custom boundary/initial condition preprocessors into a single software release, with source code available by agreement with NASA/GSFC. Full coupling between aerosol, cloud, precipitation and land processes is critical for predicting local and regional water and energy cycles.

Satellite-resolved↗

Airborne DIAL System for Remote Tropospheric Sensing

Spatial distribution of gases and of aerosols measured. Airborne DIAL system uses two frequency-doubled Nd:YAG lasers and mounted in NASA Wallops Electra aircraft. Multipurpose airborne differential absorption lidar (DIAL) system, developed at Langley Research Center, remotely measures profiles of various gases and aerosols in diverse atmospheric investigations. Capability to rapidly determine spatial distribution of gases such as ozone, water vapor, sulfur dioxide, and nitrogen dioxide and to measure simultaneously distribution of aerosols at several laser wavelengths provides opportunity for developing extensive data base for examining complex interaction of atmospheric dynamics and chemistry.

Browell, E. V.↗