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At least 541 records · Page 30

Interactive Gas Chemistry for Enhanced Science Capabilities of the Energy Exascale Earth System Model Version 3

Atmospheric chemistry plays a crucial role in Earth system models (ESMs), controlling atmospheric composition and radiative balance; it is highly interactive with the physical climate, biogeochemical cycles, and human systems. However, it often imposes computational challenges in an ESM. Here we develop a full troposphere‐stratosphere interactive chemistry module for the US Department of Energy's Energy Exascale Earth System Model (E3SM). We intentionally build a streamlined module based on E3SM version 2 that interacts with other components and maintains all of major chemical and chemistry‐climate feedbacks. The module incorporates a new, highly efficient tracer advection scheme; linearization of stratospheric chemistry; and abridged tropospheric chemical mechanism with 28 reactive tracers. This new model, E3SM‐chem, can readily perform century‐long climate simulations of ozone, methane, and nitrous oxide based on emission scenarios as well as provide hourly budgets for the gas‐phase radicals that drive aerosol chemistry. We evaluate E3SM‐chem with an atmosphere‐only simulation as in the recent climate model intercomparison project (CMIP6) finding results similar to the other CMIP6 models. For the present‐day, E3SM‐chem matches the standard measurement metrics for stratospheric and tropospheric ozone, surface air quality, other key reactive gases like carbon monoxide, and the methane lifetime. Overall, E3SM‐chem maintains the climate fidelity of the baseline model while adding at most 20% to the computational cost of the atmosphere model. Hence, interactive chemistry can be a default configuration for long climate simulations at resolutions of 1° or finer, which is crucial for producing self‐consistent chemistry‐climate feedbacks that alter the climate system.

54 ENVIRONMENTAL SCIENCES↗

The Evolution of Lidar Networks: A US Perspective

Atmospheric aerosols and clouds play an important role in climate by directly scattering and absorbing sunlight. Aerosol-cloud interactions modify the particle properties causing indirect effects, alter aerosol deposition and rainfall, and contribute substantially to the uncertainties in predicting climate effects. Aerosols also affect air quality and both constituents modulate boundary layer dynamics to a certain extent, in turn impacting aerosol transport and aerosol-cloud interactions. The spatiotemporal distribution of aerosol and cloud layers is thus important, and lidar remains the primary instrument for determining the vertical distribution of aerosols and thin clouds. Lidar still provides important information for opaque cloud layers by determining base heights. Combined lidar and radar data provide a comprehensive coverage of aerosol and cloud vertical distributions, and thus locations where and when they interact. Lidar data provide a means of constraining column aerosol loading observations (e.g. AOD) to vertical extents. In addition, lidar has proven effective at determining a proxy for boundary layer height by examining aerosol gradients and/or cloud base heights in lidar profiles. Polarized lidars provide additional information on particle shape, allowing estimates of cloud phase and separation of dust or smoke from sulfate and sea salt aerosols. Given the importance of lidar observations and a critical maturation in technology and retrieval techniques, several organizations began to build operational lidar networks around 2000. The European Aerosol Research Lidar Network (EARLINET) was started as a research focused network of advanced lidars across Europe. The Asian Dust Lidar Network (ADNET) was also developed as a regional network providing lidar profiles of dust and pollution across Eastern Asia. In the US, the NASA Micro Pulse Lidar Network (MPLNET) was created to provide global lidar profiling at key sites in the NASA Aerosol Robotic Network (AERONET). The Network for the Detection of Atmospheric Composition Change (NDACC) pre-dates these networks and many sites have lidar, but it is not strictly a lidar network and at the time focused less on the lower troposphere. Finally, there were already existing ceilometer networks operated by various meteorological agencies, but in particular here in the US the profile data has not been available. The ceilometer networks were used to provide only clouds base heights and estimates of PBL height. Thus, the distinguishing feature between lidar and ceilometer networks was historically the ability to actually provide profile information (in addition to differences in wavelength, and advanced retrievals such as the raman technique). As time progressed, each lidar network matured and developed more operational capabilities and data sets, coupled with viable data centers providing DAAC services and access to near-real-time (NRT) data. In 2008 under WMO guidance, the Global Atmospheric Watch (GAW) Aerosol Lidar Observation Network (GALION) was formed as a global network made up of the existing lidar networks. The goal was to share information, best practices, and develop frameworks and techniques for quality data. GALION grew to include several other regional lidar networks and this has led to a vast increase in quality lidar sites worldwide.

Welton, Ellsworth J.↗

Plasma Composition Measurements in an Active Region from Solar Orbiter/SPICE and Hinode/EIS

A key goal of the Solar Orbiter mission is to connect elemental abundance measurements of the solar wind enveloping the spacecraft with extreme-UV (EUV) spectroscopic observations of their solar sources, but this is not an easy exercise. Observations from previous missions have revealed a highly complex picture of spatial and temporal variations of elemental abundances in the solar corona. We have used coordinated observations from Hinode and Solar Orbiter to attempt new abundance measurements with the Spectral Imaging of the Coronal Environment (SPICE) instrument, and benchmark them against standard analyses from the EUV Imaging Spectrometer (EIS). We use observations of several solar features in active region (AR) 12781 taken from an Earth-facing view by EIS on 2020 November 10, and SPICE data obtained one week later on 2020 November 17, when the AR had rotated into the Solar Orbiter field of view. We identify a range of spectral lines that are useful for determining the transition region and low-coronal-temperature structure with SPICE, and demonstrate that SPICE measurements are able to differentiate between photospheric and coronal magnesium/neon abundances. The combination of SPICE and EIS is able to establish the atmospheric composition structure of a fan loop/outflow area at the AR edge. We also discuss the problem of resolving the degree of elemental fractionation with SPICE, which is more challenging without further constraints on the temperature structure, and comment on what that can tell us about the sources of the solar wind and solar energetic particles.

Solar physics↗

Technology Development of a Solid State 266 nm Laser for NASA’s Dragonfly Mission

NASA’s Dragonfly mission is a rotorcraft lander which will explore several geologic locations on Saturn’s moon, Titan and investigate evidence of surface-level prebiotic chemistry as well as search for chemical signatures of water-based and/or hydrocarbon-based life. To perform molecular composition investigations in-situ, the payload includes the Dragonfly Mass Spectrometer (DraMS), being developed at NASA’s Goddard Space Flight Center (GSFC). DraMS will utilize laser desorption mass spectrometry (LDMS) to interrogate surface samples and measure the organic composition. Enabling this science capability is the Throttled Hydrocarbon Analysis by Nanosecond Optical Source (THANOS) laser being developed at NASA-GSFC. The THANOS laser is comprised of a solid state, passively Q-Switched Nd:YAG oscillator which is frequency converted to 266 nm and utilizes a RTP high voltage electro-optic for pulse energy control. The laser outputs <2.0 ns pulses with a maximum energy of approximately 200 uJ which can be emitted in 1 - 50 shot bursts at 100 Hz while performing LDMS science operations. While operating, the laser has the capability to throttle its UV pulse energy output from full attenuation to maximum energy to provide varying levels of fluence on samples in the DraMS instrument. This paper reports the technology development and space qualification effort of the THANOS laser including vibration, thermal vacuum cycling, radiation as well as Titan atmospheric composition optical damage testing performed at NASA-GSFC from 2019 through 2022.

Matthew W Mullin↗

A Ground-Based Network for Improved Validation of Satellite Carbon Dioxide and Methane Observations Over the Eastern United States

Satellite observations of greenhouse gases (GHGs), notably carbon dioxide and methane, over the Eastern United States, are currently only validated indirectly and/or sporadically. There are only four existing routine, ground-based remote sensing locations in the United States suitable for validation of satellite GHG observations: Edwards and Pasadena, CA, Lamont, OK, and Park Falls, WI as part of the Total Carbon Column Observing Network (TCCON). Among other efforts, e.g. the Network for the Detection of Atmospheric Composition Change (NDACC) and EM27/SUN deployments led by the University of Toronto, the only sites west of the Mississippi River are Park Falls, WI and Toronto, ON. The only remaining validation tools, vicarious calibration and airborne campaigns, are sporadic in space and/or time and thus coincide with only a small subsample of available soundings and conditions. As a result, satellite GHG observations over the east coast of the United States, home to more than half of its population, lack a consistent, widespread means of validation. We describe an ongoing effort to position 8 EM27/SUN spectrometers along the Eastern Seaboard over the next two years. The goals of this effort are to improve both satellite validation and our understanding of human and natural influences on the carbon cycle of the Eastern US, the former enabling the latter. This work is intended to augment past, ongoing, and future inter-agency programs, e.g., the NIST Urban Testbed, routine aircraft and aircore sampling by NOAA, and NASA’s Atmospheric Carbon and Transport (ACT)-America sub-orbital campaign, in particular by offering information on broader time and spatial scales than what is already available while maintaining the high-accuracy constraints of in situ data. We will present early analysis including siting considerations to capture local and/or background conditions and comparison to NASA’s Goddard Earth Observing System (GEOS) modeling and assimilation systems. This includes a 40-day, 3-km horizontal resolution global simulation of early 2020 and a 50-km retrospective analysis of Orbiting Carbon Observatory 2 (OCO-2) observations over 2015-present. Both are valuable tools for analyzing expected and observed signals and are useful boundary conditions for yet higher-resolution studies.

Brad Weir↗

The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Overview and Description of Models, Simulations and Climate Diagnostics

The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting composition changes and the associated radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the associated model output. The 16 ACCMIP models have a wide range of horizontal and vertical resolutions, vertical extent, chemistry schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions are responsible for a significant range across models, mostly in the case of ozone precursors. The analysis of selected present-day climate diagnostics (precipitation, temperature, specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The model-to- model comparison of changes in temperature, specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atmospheric chemistry.

humidity↗

Characterizing Cold Giant Planets in Reflected Light: Lessons from 50 Years of Outer Solar System Exploration and Observation

A space based coronagraph, whether as part of the WFIRST/AFTA mission or on a dedicated space telescope such as Exo-C or -S, will be able to obtain photometry and spectra of multiple gas giant planets around nearby stars, including many known from radial velocity detections. Such observations will constrain the masses, atmospheric compositions, clouds, and photochemistry of these worlds. Giant planet albedo models, such as those of Cahoy et al. (2010) and Lewis et al. (this meeting), will be crucial for mission planning and interpreting the data. However it is equally important that insights gleaned from decades of solar system imaging and spectroscopy of giant planets be leveraged to optimize both instrument design and data interpretation. To illustrate these points we will draw on examples from solar system observations, by both HST and ground based telescopes, as well as by Voyager, Galileo, and Cassini, to demonstrate the importance clouds, photochemical hazes, and various molecular absorbers play in sculpting the light scattered by solar system giant planets. We will demonstrate how measurements of the relative depths of multiple methane absorption bands of varying strengths have been key to disentangling the competing effects of gas column abundances, variations in cloud height and opacity, and scattering by high altitude photochemical hazes. We will highlight both the successes, such as the accurate remote determination of the atmospheric methane abundance of Jupiter, and a few failures from these types of observations. These lessons provide insights into technical issues facing spacecraft designers, from the selection of the most valuable camera filters to carry to the required capabilities of the flight spectrometer, as well as mission design questions such as choosing the most favorable phase angles for atmospheric characterization.

atmospheric methane abundance↗

A-Train Data Depot: Integrating, Visualizing, and Extracting Cloudsat, CALIPSO, MODIS, and AIRS Atmospheric Measurements Along the A-Train Tracks

The succession of US and international Earth observing satellites that follow each other, seconds to minutes apart, across the local afternoon equator crossing is called the ATrain. The A-Train consists of the following satellites, in order of equator crossing: OCO, EOS Aqua, CloudSat, CALIPSO, PARASOL, and EOS Aura. Flying in such formation increases the number of observations, validates observations, and enables coordination between science observations, resulting in a more complete virtual science platform (Kelly, 2000). The goal of this project is to create the first ever A-Train virtual data portal/center, the A-Train Data Depot (ATDD), to process, archive, access, visualize, analyze and correlate distributed atmosphere measurements from various A-Train instruments along A-Train tracks. The ATDD will enable the free movement of remotely located A-Train data so that they are combined to create a consolidated vertical view of the Earth's Atmosphere along the A-Train tracks. Once the infrastructure of the ATDD is in place, it will be easily evolved to serve data from all A-Train data measurements: one stop shopping. The innovative approach of analyzing and visualizing atmospheric profiles along the platforms track (i.e., time) will be accommodated by reusing the GSFC Atmospheric Composition Data and Information Services Center (ACDISC) visualization and analysis tool, GIOVANNI, existing data reduction tools, on-line archiving for fast data access, access to remote data without unnecessary data transfers, and data retrieval by users finding data desirable for further study. Initial measurements utilized include CALIPSO lidar backscatter, CloudSat radar reflectivity, clear air relative humidity, water vapor and temperature from AIRS, and cloud properties and aerosols from both MODIS. This will be foilowed by associated measurements from TVILS, =MI, HIRDLS, sad TES. Given the independent nature of instrumentlplatform development, the ATDD project has been met with many interesting challenges that, once resolved, will provide a much greater understanding of the relative flight dynamics and data co-registration of the suite of A-Train instruments, thus greatly increasing the accuracy of A-Train data analysis. Some of these challenges will be illustrated and discussed. The project's early visualizations and analysis efforts illustrate the importance of managing data so that measurements from various missions can be combined to enhance the understanding of the atmosphere. A-Train data management coordination, as performed here, is extremely significant in facilitating the A-Train science of clouds, precipitation, aerosol and chemistry.

Kempler, Steven↗

The miniJPAS survey: White dwarf science with 56 optical filters

We analyze the white dwarf population in miniJPAS, the first square degree observed with 56 medium-band, 145 Å in width optical filters by the Javalambre Physics of the accelerating Universe Astrophysical Survey (J-PAS), to provide a data-based forecast for the white dwarf science with low-resolution ($R$ ~ 50) photo-spectra. We define the sample of the bluest point-like sources in miniJPAS with $r$ < 21.5 mag, a point-like probability larger than 0.5, ($u$ - $r$)< 0.80 mag, and ($g$ - $i$)< 0.25 mag. This sample comprises 33 sources with spectroscopic information: 11 white dwarfs and 22 quasi-stellar objects (QSOs). We estimate the effective temperature ($T$ eff ), the surface gravity, and the composition of the white dwarf population by a Bayesian fitting to the observed photo-spectra. The miniJPAS data are sensitive to the Balmer series and the presence of polluting metals. Our results, combined with those from the Javalambre Photometric Local Universe Survey (J-PLUS) which has a lower spectral resolution but has already observed thousands of white dwarfs, suggest that J-PAS photometry would permit – down to $r$ ~ 21.5 mag and at least for sources with 7000 < $T$ eff < 22 000 K – both the classification of the observed white dwarfs into H-dominated and He-dominated with 99% confidence and the detection of calcium absorption for equivalent widths larger than 15 Å. The effective temperature is estimated with a 2% uncertainty, which is close to the 1% from spectroscopy. A precise estimation of the surface gravity depends on the available parallax information. In addition, the white dwarf population at $T$ eff > 7000 K can be segregated from the bluest extragalactic QSOs, providing a clean sample based on optical photometry alone. The J-PAS low-resolution photo-spectra would produce precise effective temperatures and atmospheric compositions for white dwarfs, complementing the data from Gaia. J-PAS will also detect and characterize new white dwarfs beyond the Gaia magnitude limit, providing faint candidates for spectroscopic follow-up.

79 ASTRONOMY AND ASTROPHYSICS↗

Terrestrial Planets Comparative Climatology (TPCC) mission concept

The authors and co-signers of the Terrestrial Planets Comparative Climatology (TPCC) mission concept white paper advocate that planetary science in the next decade would greatly benefit from comparatively studying the fundamental behavior of the atmospheres of Venus and Mars, contemporaneously and with the same instrumentation, to capture atmospheric response to the same solar forcing, and with a minimum of instrument-related variability. NASA’s vision is to understand the effects of the Sun on the solar system and the potential for life elsewhere (Obj,1.1 of [1]). This vision directly motivates the study of terrestrial climate histories and evolution, with the ultimate goal of understanding what factors allow the emergence and sustainability of life/biosphere. It is widely accepted that Venus, Mars, and Earth were formed at the same time and in the same neighborhood of the solar nebula [2,3], and had water—a necessary ingredient for life. In spite of strong overlap in the atmospheric composition of these planets, their current climatic states are vastly different. While Earth retains water, both Mars and Venus’ surfaces are now dry. The manner in which these terrestrial bodies evolved, and whether Mars or Venus currently hosts or previously hosted life, are fundamental mysteries in planetary science. As such, the TPCC mission concept has been developed.The TPCC guiding science goals are:(1) to understand Venus’ evolutionary history compared to Mars and Earth, and (2) to elucidate the driving forces and mechanisms of global circulation at Mars and Venus. These goals address the science question: Why have Mars’ and Venus’ climates evolved so differently from each other and from Earth’s? Furthermore, a greater depth of understanding our own solar system, enables us to understand the variability and likelihood of habitable conditions within extra-solar planetary systems.We suggest a mission architecture and payload that would determine the noble gas content and isotopic ratios, including the D/H ratio, at Venus with sufficient accuracy to identify the timeline of Venus’ climatic evolution for comparison with Mars. In addition, our concept would systematically “follow the energy” at Mars and Venus, in order to establish how solar forcing on the two atmospheric systems leads to the current balance of dynamical, chemical, and radiative processes responsible for each planet’s climatic state.This would include acquisition of the first global atmospheric wind profiles on either planet;global, continuous profiles of aerosols, gases, and water vapor at vertical resolutions higher than any previous mission;and regular UV and IR night glow observations tracking global circulation on both planets.To increase the fidelity of the planned planetary comparisons, the TPCC mission concept baseline (estimated to be New Frontiers Class)would send a single spacecraft to visit one planet and then the next, allowing measurements of each planet with the same instrumentation within similar parts of the solar cycle. The concept uses commercial solar-electric propulsion (SEP; e.g., [4])similar to the Psyche mission [5], plus a probesent deep into Venus’ atmosphere(e.g., LLISSE concept; [6]).Alternatively, “twin” spacecraft (with added probe to the Venus craft),developed at the same time,and launched close in time,would increase the overlap in operation periods and should also be studied. Either architecture is a timely alternative to independently developed and launched spacecraft payloads, which ultimately are more costly and difficult to inter-calibrate.

Leslie K. Tamppari↗

Patches for Repairing Ceramics and Ceramic-Matrix Composites

Patches consisting mostly of ceramic fabrics impregnated with partially cured polymers and ceramic particles are being developed as means of repairing ceramics and ceramic-matrix composites (CMCs) that must withstand temperatures above the melting points of refractory metal alloys. These patches were conceived for use by space-suited, space-walking astronauts in repairing damaged space-shuttle leading edges: as such, these patches could be applied in the field, in relatively simple procedures, and with minimal requirements for specialized tools. These design characteristics also make the patches useful for repairing ceramics and CMCs in terrestrial settings. In a typical patch as supplied to an astronaut or repair technician, the polymer would be in a tacky condition, denoted as an A stage, produced by partial polymerization of a monomeric liquid. The patch would be pressed against the ceramic or CMC object to be repaired, relying on the tackiness for temporary adhesion. The patch would then be bonded to the workpiece and cured by using a portable device to heat the polymer to a curing temperature above ambient temperature but well below the maximum operating temperature to which the workpiece is expected to be exposed. The patch would subsequently become pyrolized to a ceramic/glass condition upon initial exposure to the high operating temperature. In the original space-shuttle application, this exposure would be Earth-atmosphere-reentry heating to about 3,000 F (about 1,600 C). Patch formulations for space-shuttle applications include SiC and ZrO2 fabrics, a commercial SiC-based pre-ceramic polymer, and suitable proportions of both SiC and ZrO2 particles having sizes of the order of 1 m. These formulations have been tailored for the space-shuttle leading-edge material, atmospheric composition, and reentry temperature profile so as to enable repairs to survive re-entry heating with expected margin. Other formulations could be tailored for specific terrestrial applications.

Hogenson, Peter A.↗

Chemical Modeling of the Reactivity of Short-Lived Greenhouse Gases: A Model Inter-Comparison Prescribing a Well-Measured, Remote Troposphere

We develop a new protocol for merging in situ measurements with 3-D model simulations of atmospheric chemistry with the goal of integrating over the data to identify the most reactive air parcels in terms of tropospheric production and loss of the greenhouse gases ozone and methane. Presupposing that we can accurately measure atmospheric composition, we examine whether models constrained by such measurements agree on the chemical budgets for ozone and methane. In applying our technique to a synthetic data stream of 14,880 parcels along 180W, we are able to isolate the performance of the photochemical modules operating within their global chemistry-climate and chemistry-transport models, removing the effects of modules controlling tracer transport, emissions, and scavenging. Differences in reactivity across models are driven only by the chemical mechanism and the diurnal cycle of photolysis rates, which are driven in turn by temperature, water vapor, solar zenith angle, clouds, and possibly aerosols and overhead ozone, which are calculated in each model. We evaluate six global models and identify their differences and similarities in simulating the chemistry through a range of innovative diagnostics. All models agree that the more highly reactive parcels dominate the chemistry (e.g., the hottest 10% of parcels control 25-30% of the total reactivities), but do not fully agree on which parcels comprise the top 10%. Distinct differences in specific features occur, including the regions of maximum ozone production and methane loss, as well as in the relationship between photolysis and these reactivities. Unique, possibly aberrant, features are identified for each model, providing a benchmark for photochemical module development. Among the 6 models tested here, 3 are almost indistinguishable based on the inherent variability caused by clouds, and thus we identify 4, effectively distinct, chemical models. Based on this work, we suggest that water vapor differences in model simulations of past and future atmospheres may be a cause of the different evolution of tropospheric O3 and CH4, and lead to different chemistry-climate feedbacks across the models.

greenhouse gases↗

Investigating Secondary Aerosol Processes in the Amazon through Molecular-level Characterization of Semi-Volatile Organics

In areas where biogenic emissions are oxidized in the presence of anthropogenic pollutants, it has become increasingly apparent that secondary organic aerosol (SOA) formation from biogenic volatile organic compounds (BVOCs) is substantially enhanced. The Amazon forest is the dominant source of BVOCs globally, and the forest is rapidly being converted to urban and agricultural uses. We participated in a collaborative field study located in the Amazon region around Manaus, Brazil, in 2014 (Green Ocean Amazon; GoAmazon). This study was designed to comprehensively examine how BVOC emissions (specifically, the most highly emitted non-methane hydrocarbon, isoprene, and lesser studied sesquiterpenes) and their interaction with anthropogenic pollution (i.e., nitrogen oxides, sulfur dioxide, and black carbon) alter the atmosphere’s oxidative capacity, influence secondary aerosol formation, atmospheric composition and, ultimately, affect the earth’s radiation balance and climate. We provide the first hourly, in-situ measurement of 30 sesquiterpenes and 4 diterpenes, roughly estimating that sesquiterpene oxidation contributes to 10-14% of ozone reactive loss by terpenes and at least 0.4–5% (median 1 %) of total submicron OA mass. However, this is likely a low-end estimate, as evidence for additional unaccounted sesquiterpenes and their oxidation products clearly exists. We also provide new perspectives on sulfate, NO x , and particle acidity influencing isoprene-derived SOA, comparing the central Amazon environment with Southeastern U.S.A. summer, representing clean to polluted conditions, respectively. We find that summed concentrations of isoprene-derived SOA tracers correlated with particulate sulfate spanning three orders of magnitude, suggesting that 1 μg m -3 reduction in sulfate corresponds with at least ~0.5 μg m -3 reduction in isoprene-derived SOA. We also find that SOA mass derived from isoprene oxidation in the presence of NO x is primarily comprised of aerosol sulfate bound with isoprene oxidation products (i.e. organosulfates), ~97% in the Amazon and ~55% in the Southeastern U.S. We infer under natural conditions in high isoprene emission regions, preindustrial aerosol sulfate was almost exclusively isoprene-derived organosulfates, which are traditionally thought as representative of anthropogenic influence. We further report the first field observations showing that particle acidity impacts the distribution of isoprene oxidation tracers in the gas and particle phases, providing physicochemical insight into isoprene SOA formation chemistry. Coupled with other co-located measurements by the DOE Atmospheric Radiation Measurement (ARM) team and collaborating PIs at our measurement site (called T3), on the G1 aircraft, and at additional field sites (T0, T1, T2) this data set has been used to understand emission, oxidation, and particle formation pathways at the molecular level, to elucidate how these pathways change when influenced by anthropogenic sources, and to evaluate their importance for the atmospheric budget of aerosols and the earth’s radiation balance on regional scales. Recommendations: Further constraint of the role of sesquiterpenes on ozone (O 3 ) reactivity and SOA formation is limited by the availability of authentic standards and synthesized compounds of sesquiterpenes and their oxidation products. Future research efforts should focus on making such standards available via custom synthesis to allow for accurate quantification and focused oxidation experiments that will fully elucidate the chemistry of these compounds in the atmosphere. Further, reductions in aerosol sulfate (via SO 2 emissions control) continues to be one of the most effective methods to reduce SOA formation from isoprene, but the concerted role of ammonia (NH 3 ) gas emissions from (agricultural) industry and other sources requires more investigation to better understand the role of aerosol acidity in SOA formation and potential controls. As GoAmazon particles can be more acidic compared to areas with greater anthropogenic NH 3 emissions, this promotes relatively greater organosulfate (OS) formation from isoprene even in the presence of NO x . Because OS and inorganic sulfate differ in water uptake properties, this implies preindustrial aerosol sulfate (albeit less abundant) may have been less reflective than current earth system models assume. Further research should investigate the radiative impacts of organic vs inorganic sulfate in aerosols to improve model representation. Finally, future work (currently underway) should include constraint of the contributions of monoterpene (C 10 H 16 ) BVOCs and biomass burning VOCs as precursors to SOA formation in the region as well as their impacts on radiative forcing in the climate system.

54 ENVIRONMENTAL SCIENCES↗

Tethered Balloon System Ozone Profiles during CoURAGE Summer Intensive Operational Period Field Campaign Report

During the summer IOP, the small ARM field campaign CRGTBSO3 collected measurements to gain an improved understanding of differences between the atmospheric composition in and just above the marine layer at the CoURAGE TBS site near the eastern shore of Chesapeake Bay. CRGTBSO3 included guest instrumentation with ozone (O 3 ) profile measurements on the TBS and surface O3 and meteorological measurements at the TBS site. An En-Sci 2Z electrochemical cell (ECC) ozonesonde (Komhyr 1969, 1986, Witte et al. 2018) was included on the TBS. The ozonesonde was connected to an InterMet iMet-4RSB radiosonde, and the overall data collected included vertical profiles of ozone, relative humidity, temperature, pressure, and altitude. The CRGTBSO3 iMet-4 radiosonde data is identical to that of the iMet in the Tethered Balloon System Merged Data Product (TBSMERGED; Gaustad and Dexheimer 2025). The TBSMERGED data product also includes meteorological data from a different sensor, the iMet XQ2. In some cases, the iMet XQ2 relative humidity (RH) data may be more accurate than the iMet-4, such as for some instances when the iMet-4 RH data stays at 100% for an extended period throughout a profile.

54 ENVIRONMENTAL SCIENCES↗

Reconciling Assumptions in Bottom-up and Top-down Approaches for Estimating Aerosol Emission Rates from Wildland Fires using Observations from FIREX-AQ

Accurate fire emissions inventories are crucial to predict the impacts of wildland fires on air quality and atmospheric composition. Two traditional approaches are widely used to calculate fire emissions: a satellite-based top-down approach and a fuels-based bottom-up approach. However, these methods often considerably disagree on the amount of particulate mass emitted from fires. Previously available observational datasets tended to be sparse, and lacked the statistics needed to resolve these methodological discrepancies. Here, we leverage the extensive and comprehensive airborne in situ and remote sensing measurements of smoke plumes from the recent Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign to statistically assess the skill of the two traditional approaches. We use detailed campaign observations to calculate and compare emission rates at an exceptionally high-resolution using three separate approaches: top-down, bottom-up, and a novel approach based entirely on integrated airborne in situ measurements. We then compute the daily average of these high-resolution estimates and compare with estimates from lower resolution, global top-down and bottom-up inventories. We uncover strong, linear relationships between all of the high-resolution emission rate estimates in aggregate, however no single approach is capable of capturing the emission characteristics of every fire. Global inventory emission rate estimates exhibited weaker correlations with the high-resolution approaches and displayed evidence of systematic bias. The disparity between the low resolution global inventories and the high-resolution approaches is likely caused by high levels of uncertainty in essential variables used in bottom-up inventories and imperfect assumptions in top-down inventories. Plain Language Summary Smoke emitted by wildland fires is dangerous to human health and contributes to climate change.To predict and evaluate the impacts of fires, we need to know how much smoke is emitted into the atmosphere. There are two state-of-the-art methods used to estimate the mass of smoke emitted by fires, but they often disagree. In this study, we use unusually detailed measurements collected using an aircraft that flew within wildland fire smoke plumes to calculate the amount ofsmoke emitted from fires in the Western United States. We compare emission rates derived from the exceptionally high spatial and temporal resolution approach to the two traditional, lower resolution approaches to understand why they sometimes diverge

E B Wiggins↗

Quantifying Sources and Sinks of Reactive Gases in the Lower Atmosphere Using Airborne Flux Observations

Atmospheric composition is governed by the interplay of emissions, chemistry, deposition, and transport. Substantial questions surround each of these processes, especially in forested environments with strong biogenic emissions. Utilizing aircraft observations acquired over a forest in the southeast U.S., we calculate eddy covariance fluxes for a suite of reactive gases and apply the synergistic information derived from this analysis to quantify emission and deposition fluxes, oxidant concentrations, aerosol uptake coefficients, and other key parameters. Evaluation of results against state-of-the-science models and parameterizations provides insight into our current understanding of this system and frames future observational priorities. As a near-direct measurement of fundamental process rates, airborne fluxes offer a new tool to improve biogenic and anthropogenic emissions inventories, photochemical mechanisms, and deposition parameterizations.

emission↗

Evaluation of Near-Tropopause Ozone Distributions in the Global Modeling Initiative Combined Stratosphere/Troposphere Model with Ozonesonde Data

The NASA Global Modeling Initiative has developed a combined stratosphere/troposphere chemistry and transport model which fully represents the processes governing atmospheric composition near the tropopause. We evaluate model ozone distributions near the tropopause, using two high vertical resolution monthly mean ozone profile climatologies constructed with ozonesonde data, one by averaging on pressure levels and the other relative to the thermal tropopause. Model ozone is high biased at the SH tropical and NH midlatitude tropopause by approx. 45% in a 4 deg. latitude x 5 deg. longitude model simulation. Increasing the resolution to 2 deg. x 2.5 deg. increases the NH tropopause high bias to approx. 60%, but decreases the tropical tropopause bias to approx. 30%, an effect of a better-resolved residual circulation. The tropopause ozone biases appear not to be due to an overly vigorous residual circulation or excessive stratosphere/troposphere exchange, but are more likely due to insufficient vertical resolution or excessive vertical diffusion near the tropopause. In the upper troposphere and lower stratosphere, model/measurement intercomparisons are strongly affected by the averaging technique. NH and tropical mean model lower stratospheric biases are less than 20%. In the upper troposphere, the 2 deg. x 2.5 deg. simulation exhibits mean high biases of approx. 20% and approx. 35% during April in the tropics and NH midlatitudes, respectively, compared to the pressure averaged climatology. However, relative-to-tropopause averaging produces upper troposphere high biases of approx. 30% and 70% in the tropics and NH midlatitudes. This is because relative-to-tropopause averaging better preserves large cross-tropopause O3 gradients, which are seen in the daily sonde data, but not in daily model profiles. The relative annual cycle of ozone near the tropopause is reproduced very well in the model Northern Hemisphere midlatitudes. In the tropics, the model amplitude of the near tropopause annual cycle is weak. This is likely due to the annual amplitude of mean vertical upwelling near the tropopause, which analysis suggests is approx. 30% weaker than in the real atmosphere.

Considine, David B.↗

Southern Ocean Cloud Properties Derived From CAPRICORN and MARCUS Data

The properties of Southern Ocean (SO) liquid phase non precipitating clouds (hereafter clouds) are examined using shipborne data collected during the Measurements of Aerosols, Radiation and Clouds over the Southern Ocean and the Clouds Aerosols Precipitation Radiation and atmospheric Composition Over the SoutheRN ocean I and II campaigns that took place south of Australia during Autumn 2016 and Summer 2017–2018. Cloud properties are derived using data from W-band radars, lidars, and microwave radiometers using an optimal estimation algorithm. The SO clouds tended to have larger liquid water paths (LWP, 115 ± 117 g m -2 ), smaller effective radii (re, 8.7 ± 3 μm), and higher number concentrations (N d , 90 ± 107 cm-3) than typical values of eastern ocean basin stratocumulus. The clouds demonstrated a tendency for the LWP to increase with Nd presumably due to precipitation suppression up to Nd of approximately 100 cm -3 when mean LWP decreased with increasing Nd. Due to higher optical depth, cloud albedos were less susceptible to changes in Nd compared to subtropical stratocumulus. The highest latitude clouds of the datasets, observed along and near the Antarctic coast, presented a distinctly bimodal character. One mode had the properties of marine clouds further north. Additionally, the other mode occurred in an aerosol environment characterized by high cloud condensation nuclei concentrations and elevated sulfate aerosol without obvious continental aerosol markers. These regions of higher cloud condensation nuclei tended to have higher Nd, smaller re and higher LWP suggesting sensitivity of cloud properties to seasonal biogenic aerosol production in the high latitude SO.

54 ENVIRONMENTAL SCIENCES↗