Showing papers by "Langley Research Center published in 2021"

NRLMSIS 2.0: A Whole-Atmosphere Empirical Model of Temperature and Neutral Species Densities

Abstract: NRLMSIS® 2.0 is an empirical atmospheric model that extends from the ground to the exobase and describes the average observed behavior of temperature, eight species densities, and mass density via a parametric analytic formulation. The model inputs are location, day of year, time of day, solar activity, and geomagnetic activity. NRLMSIS 2.0 is a major, reformulated upgrade of the previous version, NRLMSISE‐00. The model now couples thermospheric species densities to the entire column, via an effective mass profile that transitions each species from the fully mixed region below ~70 km altitude to the diffusively separated region above ~200 km. Other changes include the extension of atomic oxygen down to 50 km and the use of geopotential height as the internal vertical coordinate. We assimilated extensive new lower and middle atmosphere temperature, O, and H data, along with global average thermospheric mass density derived from satellite orbits, and we validated the model against independent samples of these data. In the mesosphere and below, residual biases and standard deviations are considerably lower than NRLMSISE‐00. The new model is warmer in the upper troposphere and cooler in the stratosphere and mesosphere. In the thermosphere, N2 and O densities are lower in NRLMSIS 2.0; otherwise, the NRLMSISE‐00 thermosphere is largely retained. Future advances in thermospheric specification will likely require new in situ mass spectrometer measurements, new techniques for species density measurement between 100 and 200 km, and the reconciliation of systematic biases among thermospheric temperature and composition data sets, including biases attributable to long‐term changes.

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Abstract: . 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. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a five-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three Intensive Observation Periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June-October), aerosol particles reaching 3–5 km in altitude are transported westward over the South-East Atlantic, where they interact with one of the largest subtropical stratocumulus subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, and due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017 and October 2018 (totaling ~350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science questions centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects; (b) effects of aerosol absorption on atmospheric circulation and clouds; (c) aerosol-cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the data set it produced.

The Korea–United States Air Quality (KORUS-AQ) field study

Abstract: The Korea-United States Air Quality (KORUS-AQ) field study was conducted during May-June 2016. The effort was jointly sponsored by the National Institute of Environmental Research of South Korea and the National Aeronautics and Space Administration of the United States. KORUS-AQ offered an unprecedented, multi-perspective view of air quality conditions in South Korea by employing observations from three aircraft, an extensive ground-based network, and three ships along with an array of air quality forecast models. Information gathered during the study is contributing to an improved understanding of the factors controlling air quality in South Korea. The study also provided a valuable test bed for future air quality-observing strategies involving geostationary satellite instruments being launched by both countries to examine air quality throughout the day over Asia and North America. This article presents details on the KORUS-AQ observational assets, study execution, data products, and air quality conditions observed during the study. High-level findings from companion papers in this special issue are also summarized and discussed in relation to the factors controlling fine particle and ozone pollution, current emissions and source apportionment, and expectations for the role of satellite observations in the future. Resulting policy recommendations and advice regarding plans going forward are summarized. These results provide an important update to early feedback previously provided in a Rapid Science Synthesis Report produced for South Korean policy makers in 2017 and form the basis for the Final Science Synthesis Report delivered in 2020.

CERES MODIS Cloud Product Retrievals for Edition 4—Part I: Algorithm Changes

Abstract: The Edition 2 (Ed2) cloud property retrieval algorithm system was upgraded and applied to the MODerate-resolution Imaging Spectroradiometer (MODIS) data for the Clouds and the Earth’s Radiant Energy System (CERES) Edition 4 (Ed4) products. New calibrations for solar channels and the use of the 1.24- $\mu \text{m}$ channel for cloud optical depth (COD) over snow improve the daytime consistency between Terra and Aqua MODIS retrievals. Use of additional spectral channels and revised logic enhanced the cloud-top phase retrieval accuracy. A new ice crystal reflectance model and a CO2-channel algorithm retrieved higher ice clouds, while a new regional lapse rate technique produced more accurate water cloud heights than in Ed2. Ice cloud base heights are more accurate due to a new cloud thickness parameterization. Overall, CODs increased, especially over the polar (PO) regions. The mean particle sizes increased slightly for water clouds, but more so for ice clouds in the PO areas. New experimental parameters introduced in Ed4 are limited in utility, but will be revised for the next CERES edition. As part of the Ed4 retrieval evaluation, the average properties are compared with those from other algorithms and the differences between individual reference data and matched Ed4 retrievals are explored. Part II of this article provides a comprehensive, objective evaluation of selected parameters. More accurate interpretation of the CERES radiation measurements has resulted from the use of the Ed4 cloud properties.

Cleaner burning aviation fuels can reduce contrail cloudiness

Abstract: Contrail cirrus account for the major share of aviation’s climate impact. Yet, the links between jet fuel composition, contrail microphysics and climate impact remain unresolved. Here we present unique observations from two DLR-NASA aircraft campaigns that measured exhaust and contrail characteristics of an Airbus A320 burning either standard jet fuels or low aromatic sustainable aviation fuel blends. Our results show that soot particles can regulate the number of contrail cirrus ice crystals for current emission levels. We provide experimental evidence that burning low aromatic sustainable aviation fuel can result in a 50 to 70% reduction in soot and ice number concentrations and an increase in ice crystal size. Reduced contrail ice numbers cause less energy deposition in the atmosphere and less warming. Meaningful reductions in aviation’s climate impact could therefore be obtained from the widespread adoptation of low aromatic fuels, and from regulations to lower the maximum aromatic fuel content. Burning sustainable aviation fuel blends with low levels of soot-producing aromatic components can result in a 50 to 70% reduction in soot and ice number concentrations and an increase in ice crystal size, suggest measurements of exhaust and contrail characteristics in two aircraft campaigns.

Volatile chemical product emissions enhance ozone and modulate urban chemistry.

Abstract: Decades of air quality improvements have substantially reduced the motor vehicle emissions of volatile organic compounds (VOCs). Today, volatile chemical products (VCPs) are responsible for half of the petrochemical VOCs emitted in major urban areas. We show that VCP emissions are ubiquitous in US and European cities and scale with population density. We report significant VCP emissions for New York City (NYC), including a monoterpene flux of 14.7 to 24.4 kg ⋅ d-1 ⋅ km-2 from fragranced VCPs and other anthropogenic sources, which is comparable to that of a summertime forest. Photochemical modeling of an extreme heat event, with ozone well in excess of US standards, illustrates the significant impact of VCPs on air quality. In the most populated regions of NYC, ozone was sensitive to anthropogenic VOCs (AVOCs), even in the presence of biogenic sources. Within this VOC-sensitive regime, AVOCs contributed upwards of ∼20 ppb to maximum 8-h average ozone. VCPs accounted for more than 50% of this total AVOC contribution. Emissions from fragranced VCPs, including personal care and cleaning products, account for at least 50% of the ozone attributed to VCPs. We show that model simulations of ozone depend foremost on the magnitude of VCP emissions and that the addition of oxygenated VCP chemistry impacts simulations of key atmospheric oxidation products. NYC is a case study for developed megacities, and the impacts of VCPs on local ozone are likely similar for other major urban regions across North America or Europe.

Governing AI safety through independent audits

Abstract: Highly automated systems are becoming omnipresent. They range in function from self-driving vehicles to advanced medical diagnostics and afford many benefits. However, there are assurance challenges that have become increasingly visible in high-profile crashes and incidents. Governance of such systems is critical to garner widespread public trust. Governance principles have been previously proposed offering aspirational guidance to automated system developers; however, their implementation is often impractical given the excessive costs and processes required to enact and then enforce the principles. This Perspective, authored by an international and multidisciplinary team across government organizations, industry and academia, proposes a mechanism to drive widespread assurance of highly automated systems: independent audit. As proposed, independent audit of AI systems would embody three ‘AAA’ governance principles of prospective risk Assessments, operation Audit trails and system Adherence to jurisdictional requirements. Independent audit of AI systems serves as a pragmatic approach to an otherwise burdensome and unenforceable assurance challenge. As highly automated systems become pervasive in society, enforceable governance principles are needed to ensure safe deployment. This Perspective proposes a pragmatic approach where independent audit of AI systems is central. The framework would embody three AAA governance principles: prospective risk Assessments, operation Audit trails and system Adherence to jurisdictional requirements.

Reviews and syntheses: Arctic fire regimes and emissions in the 21st century

Abstract: . In recent years, the pan-Arctic region has experienced increasingly extreme fire seasons. Fires in the northern high latitudes are driven by current and future climate change, lightning, fuel conditions, and human activity. In this context, conceptualizing and parameterizing current and future Arctic fire regimes will be important for fire and land management as well as understanding current and predicting future fire emissions. The objectives of this review were driven by policy questions identified by the Arctic Monitoring and Assessment Programme (AMAP) Working Group and posed to its Expert Group on Short-Lived Climate Forcers. This review synthesizes current understanding of the changing Arctic and boreal fire regimes, particularly as fire activity and its response to future climate change in the pan-Arctic have consequences for Arctic Council states aiming to mitigate and adapt to climate change in the north. The conclusions from our synthesis are the following. (1) Current and future Arctic fires, and the adjacent boreal region, are driven by natural (i.e. lightning) and human-caused ignition sources, including fires caused by timber and energy extraction, prescribed burning for landscape management, and tourism activities. Little is published in the scientific literature about cultural burning by Indigenous populations across the pan-Arctic, and questions remain on the source of ignitions above 70 ∘ N in Arctic Russia. (2) Climate change is expected to make Arctic fires more likely by increasing the likelihood of extreme fire weather, increased lightning activity, and drier vegetative and ground fuel conditions. (3) To some extent, shifting agricultural land use and forest transitions from forest–steppe to steppe, tundra to taiga, and coniferous to deciduous in a warmer climate may increase and decrease open biomass burning, depending on land use in addition to climate-driven biome shifts. However, at the country and landscape scales, these relationships are not well established. (4) Current black carbon and PM 2.5 emissions from wildfires above 50 and 65 ∘ N are larger than emissions from the anthropogenic sectors of residential combustion, transportation, and flaring. Wildfire emissions have increased from 2010 to 2020, particularly above 60 ∘ N, with 56 % of black carbon emissions above 65 ∘ N in 2020 attributed to open biomass burning – indicating how extreme the 2020 wildfire season was and how severe future Arctic wildfire seasons can potentially be. (5) What works in the boreal zones to prevent and fight wildfires may not work in the Arctic. Fire management will need to adapt to a changing climate, economic development, the Indigenous and local communities, and fragile northern ecosystems, including permafrost and peatlands. (6) Factors contributing to the uncertainty of predicting and quantifying future Arctic fire regimes include underestimation of Arctic fires by satellite systems, lack of agreement between Earth observations and official statistics, and still needed refinements of location, conditions, and previous fire return intervals on peat and permafrost landscapes. This review highlights that much research is needed in order to understand the local and regional impacts of the changing Arctic fire regime on emissions and the global climate, ecosystems, and pan-Arctic communities.

Multi-model intercomparisons of air quality simulations for the KORUS-AQ campaign

Abstract: The Korea-United States Air Quality (KORUS-AQ) field study was conducted during May–June 2016 to understand the factors controlling air quality in South Korea. Extensive aircraft and ground network observations from the campaign offer an opportunity to address issues in current air quality models and reduce model-observation disagreements. This study examines these issues using model evaluation against the KORUS-AQ observations and intercomparisons between models. Six regional and two global chemistry transport models using identical anthropogenic emissions participated in the model intercomparison study and were used to conduct air quality simulations focusing on ozone (O3), aerosols, and their precursors for the campaign. Using the KORUSv5 emissions inventory, which has been updated from KORUSv1, the models successfully reproduced observed nitrogen oxides (NOx) and volatile organic compounds mixing ratios in surface air, especially in the Seoul Metropolitan Area, but showed systematic low biases for carbon monoxide (CO), implying possible missing CO sources in the inventory in East Asia. Although the DC-8 aircraft-observed O3 precursor mixing ratios were well captured by the models, simulated O3 levels were lower than the observations in the free troposphere in part due to too low stratospheric O3 influxes, especially in regional models. During the campaign, the synoptic meteorology played an important role in determining the observed variability of PM2.5 (PM diameter ≤ 2.5 μm) concentrations in South Korea. The models successfully simulated the observed PM2.5 variability with significant inorganic sulfate-nitrate-ammonium aerosols contribution, but failed to reproduce that of organic aerosols, causing a large inter-model variability. From the model evaluation, we find that an ensemble of model results, incorporating individual models with differing strengths and weaknesses, performs better than most individual models at representing observed atmospheric compositions for the campaign. Ongoing model development and evaluation, in close collaboration with emissions inventory development, are needed to improve air quality forecasting.

OMPS LP Version 2.0 multi-wavelength aerosol extinction coefficient retrieval algorithm

Abstract: . The OMPS Limb Profiler (LP) instrument is designed to provide high-vertical-resolution ozone and aerosol profiles from measurements of the scattered solar radiation in the 290–1000 nm spectral range. It collected its first Earth limb measurement on 10 January 2012 and continues to provide daily global measurements of ozone and aerosol profiles from the cloud top up to 60 and 40 km , respectively. The relatively high vertical and spatial sampling allow detection and tracking of sporadic events when aerosol particles are injected into the stratosphere, such as volcanic eruptions or pyrocumulonimbus (PyroCb) events. In this paper we discuss the newly released Version 2.0 OMPS multi-wavelength aerosol extinction coefficient retrieval algorithm. The algorithm now produces aerosol extinction profiles at 510, 600, 674, 745, 869 and 997 nm wavelengths. The OMPS LP Version 2.0 data products are compared to the SAGE III/ISS, OSIRIS and CALIPSO missions and shown to be of good quality and suitable for scientific studies. The comparison shows significant improvements in the OMPS LP retrieval performance in the Southern Hemisphere (SH) and at lower altitudes. These improvements arise from use of the longer wavelengths, in contrast with the V1.0 and V1.5 OMPS aerosol retrieval algorithms, which used radiances only at 675 nm and therefore had limited sensitivity in those regions. In particular, the extinction coefficients at 745, 869 and 997 nm are shown to be the most accurate, with relative accuracies and precisions close to 10 % and 15 %, respectively, while the 675 nm relative accuracy and precision are on the order of 20 %. The 510 nm extinction coefficient is shown to have limited accuracy in the SH and is only recommended for use between 20–24 km and only in the Northern Hemisphere. The V2.0 retrieval algorithm has been applied to the complete set of OMPS LP measurements, and the new dataset is publicly available.

Secondary organic aerosols from anthropogenic volatile organic compounds contribute substantially to air pollution mortality

Abstract: Anthropogenic secondary organic aerosol (ASOA), formed from anthropogenic emissions of organic compounds, constitutes a substantial fraction of the mass of submicron aerosol in populated areas around the world and contributes to poor air quality and premature mortality. However, the precursor sources of ASOA are poorly understood, and there are large uncertainties in the health benefits that might accrue from reducing anthropogenic organic emissions. We show that the production of ASOA in 11 urban areas on three continents is strongly correlated with the reactivity of specific anthropogenic volatile organic compounds. The differences in ASOA production across different cities can be explained by differences in the emissions of aromatics and intermediate- and semi-volatile organic compounds, indicating the importance of controlling these ASOA precursors. With an improved model representation of ASOA driven by the observations, we attribute 340ĝ000 PM2.5-related premature deaths per year to ASOA, which is over an order of magnitude higher than prior studies. A sensitivity case with a more recently proposed model for attributing mortality to PM2.5 (the Global Exposure Mortality Model) results in up to 900ĝ000 deaths. A limitation of this study is the extrapolation from cities with detailed studies and regions where detailed emission inventories are available to other regions where uncertainties in emissions are larger. In addition to further development of institutional air quality management infrastructure, comprehensive air quality campaigns in the countries in South and Central America, Africa, South Asia, and the Middle East are needed for further progress in this area.

Evaluation and intercomparison of wildfire smoke forecasts from multiple modeling systems for the 2019 Williams Flats fire

Abstract: . Wildfire smoke is one of the most significant concerns of human and environmental health, associated with its substantial impacts on air quality, weather, and climate. However, biomass burning emissions and smoke remain among the largest sources of uncertainties in air quality forecasts. In this study, we evaluate the smoke emissions and plume forecasts from 12 state-of-the-art air quality forecasting systems during the Williams Flats fire in Washington State, US, August 2019, which was intensively observed during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign. Model forecasts with lead times within 1 d are intercompared under the same framework based on observations from multiple platforms to reveal their performance regarding fire emissions, aerosol optical depth (AOD), surface PM 2.5 , plume injection, and surface PM 2.5 to AOD ratio. The comparison of smoke organic carbon (OC) emissions suggests a large range of daily totals among the models, with a factor of 20 to 50. Limited representations of the diurnal patterns and day-to-day variations of emissions highlight the need to incorporate new methodologies to predict the temporal evolution and reduce uncertainty of smoke emission estimates. The evaluation of smoke AOD (sAOD) forecasts suggests overall underpredictions in both the magnitude and smoke plume area for nearly all models, although the high-resolution models have a better representation of the fine-scale structures of smoke plumes. The models driven by fire radiative power (FRP)-based fire emissions or assimilating satellite AOD data generally outperform the others. Additionally, limitations of the persistence assumption used when predicting smoke emissions are revealed by substantial underpredictions of sAOD on 8 August 2019, mainly over the transported smoke plumes, owing to the underestimated emissions on 7 August. In contrast, the surface smoke PM 2.5 (sPM 2.5 ) forecasts show both positive and negative overall biases for these models, with most members presenting more considerable diurnal variations of sPM 2.5 . Overpredictions of sPM 2.5 are found for the models driven by FRP-based emissions during nighttime, suggesting the necessity to improve vertical emission allocation within and above the planetary boundary layer (PBL). Smoke injection heights are further evaluated using the NASA Langley Research Center's Differential Absorption High Spectral Resolution Lidar (DIAL-HSRL) data collected during the flight observations. As the fire became stronger over 3–8 August, the plume height became deeper, with a day-to-day range of about 2–9 km a.g.l. However, narrower ranges are found for all models, with a tendency of overpredicting the plume heights for the shallower injection transects and underpredicting for the days showing deeper injections. The misrepresented plume injection heights lead to inaccurate vertical plume allocations along the transects corresponding to transported smoke that is 1 d old. Discrepancies in model performance for surface PM 2.5 and AOD are further suggested by the evaluation of their ratio, which cannot be compensated for by solely adjusting the smoke emissions but are more attributable to model representations of plume injections, besides other possible factors including the evolution of PBL depths and aerosol optical property assumptions. By consolidating multiple forecast systems, these results provide strategic insight on pathways to improve smoke forecasts.

Measurement report: Cloud processes and the transport of biological emissions affect southern ocean particle and cloud condensation nuclei concentrations

Abstract: . Long-range transport of biogenic emissions from the coast of Antarctica, precipitation scavenging, and cloud processing are the main processes that influence the observed variability in Southern Ocean (SO) marine boundary layer (MBL) condensation nuclei (CN) and cloud condensation nuclei (CCN) concentrations during the austral summer. Airborne particle measurements on the HIAPER GV from north–south transects between Hobart, Tasmania, and 62 ∘ S during the Southern Ocean Clouds, Radiation Aerosol Transport Experimental Study (SOCRATES) were separated into four regimes comprising combinations of high and low concentrations of CCN and CN. In 5 d HYSPLIT back trajectories, air parcels with elevated CCN concentrations were almost always shown to have crossed the Antarctic coast, a location with elevated phytoplankton emissions relative to the rest of the SO in the region south of Australia. The presence of high CCN concentrations was also consistent with high cloud fractions over their trajectory, suggesting there was substantial growth of biogenically formed particles through cloud processing. Cases with low cloud fraction, due to the presence of cumulus clouds, had high CN concentrations, consistent with previously reported new particle formation in cumulus outflow regions. Measurements associated with elevated precipitation during the previous 1.5 d of their trajectory had low CCN concentrations indicating CCN were effectively scavenged by precipitation. A coarse-mode fitting algorithm was used to determine the primary marine aerosol (PMA) contribution, which accounted for % of CCN (at 0.3 % supersaturation) and cloud droplet number concentrations. Vertical profiles of CN and large particle concentrations ( Dp>0.07 µ m) indicated that particle formation occurs more frequently above the MBL; however, the growth of recently formed particles typically occurs in the MBL, consistent with cloud processing and the condensation of volatile compound oxidation products. CCN measurements on the R/V Investigator as part of the second Clouds, Aerosols, Precipitation, Radiation and atmospheric Composition Over the southeRn Ocean (CAPRICORN-2) campaign were also conducted during the same period as the SOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia, likely due to continental and coastal biogenic emissions. The Antarctic coastal source of CCN from the south, CCN sources from the midlatitudes, and enhanced precipitation sink in the cyclonic circulation between the Ferrel and polar cells (around 60 ∘ S) create opposing latitudinal gradients in the CCN concentration with an observed minimum in the SO between 55 and 60 ∘ S. The SOCRATES airborne measurements are not influenced by Australian continental emissions but still show evidence of elevated CCN concentrations to the south of 60 ∘ S, consistent with biogenic coastal emissions. In addition, a latitudinal gradient in the particle composition, south of the Australian and Tasmanian coasts, is apparent in aerosol hygroscopicity derived from CCN spectra and aerosol particle size distribution. The particles are more hygroscopic to the north, consistent with a greater fraction of sea salt from PMA, and less hygroscopic to the south as there is more sulfate and organic particles originating from biogenic sources in coastal Antarctica.

Description of the NASA Urban Air Mobility Maturity Level (UML) Scale

Abstract: As part of its assessment of the nascent passenger-carrying urban air mobility (UAM) ecosystem, NASA’s UAM Coordination and Assessment Team developed a framework known as the UAM Maturity Level (UML) scale. This framework is intended to have multiple applications including: 1) insight into the likely operational capabilities as a UAM air transportation system develops over time; 2) analysis of technology and regulatory requirements associated with the UAM maturation process; 3) assessment of the current maturity of various segments of the UAM ecosystem; 4) coordination of UAM ecosystem priorities and areas of emphasis; and 5) increasing community and public awareness of UAM and how it may affect mobility in the future. This paper describes the structure of the UML scale and its levels. The paper also describes candidate strategies for advancing between levels, along with associated regulatory gaps and considerations.

Polar Stratospheric Clouds: Satellite Observations, Processes, and Role in Ozone Depletion

Abstract: The important role of polar stratospheric clouds (PSCs) in stratospheric ozone depletion during winter and spring at high latitudes has been known since the 1980s. However, contemporary observations by the spaceborne instruments MIPAS (Michelson Interferometer for Passive Atmospheric Sounding), MLS (Microwave Limb Sounder), and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) have brought about a comprehensive and clearer understanding of PSC spatial and temporal distributions, their conditions of existence, and the processes through which they impact polar ozone. Within the SPARC (Stratosphere-troposphere Processes And their Role in Climate) PSC initiative (PSCi), those datasets have been synthesized and discussed in depth with the result of a new vortex-wide climatology of PSC occurrence and composition. We will present our results within this vPICO together with a review of the significant progress that has been made in our understanding of PSC nucleation, related dynamical processes, and heterogeneous chlorine activation. Moreover, we have compiled different techniques for parameterizing PSCs and we will show their effects in global models.

Sizing response of the Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) and Laser Aerosol Spectrometer (LAS) to changes in submicron aerosol composition and refractive index

Abstract: . We evaluate the sensitivity of the size calibrations of two commercially available, high-resolution optical particle sizers to changes in aerosol composition and complex refractive index (RI). The Droplet Measurement Technologies Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) and the TSI, Inc. Laser Aerosol Spectrometer (LAS) are two commonly used instruments for measuring the portion of the aerosol size distribution with diameters larger than nominally 60–90 nm. Both instruments illuminate particles with a laser and relate the single-particle light scattering intensity and count rate measured over a wide range of angles to the size-dependent particle concentration. While the optical block geometry and flow system are similar for each instrument, a significant difference between the two models is the laser wavelength (1054 nm for the UHSAS and 633 nm for the LAS) and intensity (about 100 times higher for the UHSAS), which may affect the way each instrument sizes non-spherical or absorbing aerosols. Here, we challenge the UHSAS and LAS with laboratory-generated, mobility-size-classified aerosols of known chemical composition to quantify changes in the optical size response relative to that of ammonium sulfate (RI of 1.52+0i at 532 nm) and NIST-traceable polystyrene latex spheres (PSLs with RI of 1.59+0i at 589 nm). Aerosol inorganic salt species are chosen to cover the real refractive index range of 1.32 to 1.78, while chosen light-absorbing carbonaceous aerosols include fullerene soot, nigrosine dye, humic acid, and fulvic acid standards. The instrument response is generally in good agreement with the electrical mobility diameter. However, large undersizing deviations are observed for the low-refractive-index fluoride salts and the strongly absorbing nigrosine dye and fullerene soot particles. Polydisperse size distributions for both fresh and aged wildfire smoke aerosols from the recent Fire Influence on Regional to Global Environments Experiment and Air Quality (FIREX-AQ) and the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP 2 Ex) airborne campaigns show good agreement between both optical sizers and contemporaneous electrical mobility sizing and particle time-of-flight mass spectrometric measurements. We assess the instrument uncertainties by interpolating the laboratory response curves using previously reported RIs and size distributions for multiple aerosol type classifications. These results suggest that, while the optical sizers may underperform for strongly absorbing laboratory compounds and fresh tailpipe emissions measurements, sampling aerosols within the atmospherically relevant range of refractive indices are likely to be sized to better than ± 10 %–20 % uncertainty over the submicron aerosol size range when using instruments calibrated with ammonium sulfate.

New particle formation in the remote marine boundary layer.

Abstract: Marine low clouds play an important role in the climate system, and their properties are sensitive to cloud condensation nuclei concentrations. While new particle formation represents a major source of cloud condensation nuclei globally, the prevailing view is that new particle formation rarely occurs in remote marine boundary layer over open oceans. Here we present evidence of the regular and frequent occurrence of new particle formation in the upper part of remote marine boundary layer following cold front passages. The new particle formation is facilitated by a combination of efficient removal of existing particles by precipitation, cold air temperatures, vertical transport of reactive gases from the ocean surface, and high actinic fluxes in a broken cloud field. The newly formed particles subsequently grow and contribute substantially to cloud condensation nuclei in the remote marine boundary layer and thereby impact marine low clouds. Globally, new particle formation represents a major source of cloud condensation nuclei. Here, the authors present evidence of frequent occurrence of new particle formation in the upper part of remote marine boundary layer following cold front passages.

Nighttime and daytime dark oxidation chemistry in wildfire plumes: an observation and model analysis of FIREX-AQ aircraft data

Abstract: . Wildfires are increasing in size across the western US, leading to increases in human smoke exposure and associated negative health impacts. The impact of biomass burning (BB) smoke, including wildfires, on regional air quality depends on emissions, transport, and chemistry, including oxidation of emitted BB volatile organic compounds (BBVOCs) by the hydroxyl radical (OH), nitrate radical ( NO3 ), and ozone ( O3 ). During the daytime, when light penetrates the plumes, BBVOCs are oxidized mainly by O3 and OH. In contrast, at night or in optically dense plumes, BBVOCs are oxidized mainly by O3 and NO3 . This work focuses on the transition between daytime and nighttime oxidation, which has significant implications for the formation of secondary pollutants and loss of nitrogen oxides ( NO x = NO + NO 2 ) and has been understudied. We present wildfire plume observations made during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality), a field campaign involving multiple aircraft, ground, satellite, and mobile platforms that took place in the United States in the summer of 2019 to study both wildfire and agricultural burning emissions and atmospheric chemistry. We use observations from two research aircraft, the NASA DC-8 and the NOAA Twin Otter, with a detailed chemical box model, including updated phenolic mechanisms, to analyze smoke sampled during midday, sunset, and nighttime. Aircraft observations suggest a range of NO3 production rates (0.1–1.5 ppbv h−1 ) in plumes transported during both midday and after dark. Modeled initial instantaneous reactivity toward BBVOCs for NO3 , OH, and O3 is 80.1 %, 87.7 %, and 99.6 %, respectively. Initial NO3 reactivity is 10– 104 times greater than typical values in forested or urban environments, and reactions with BBVOCs account for >97 % of NO3 loss in sunlit plumes ( jNO2 up to 4 × 10 - 3 s - 1 ), while conventional photochemical NO3 loss through reaction with NO and photolysis are minor pathways. Alkenes and furans are mostly oxidized by OH and O3 (11 %–43 %, 54 %–88 % for alkenes; 18 %–55 %, 39 %–76 %, for furans, respectively), but phenolic oxidation is split between NO3 , O3 , and OH (26 %–52 %, 22 %–43 %, 16 %–33 %, respectively). Nitrate radical oxidation accounts for 26 %–52 % of phenolic chemical loss in sunset plumes and in an optically thick plume. Nitrocatechol yields varied between 33 % and 45 %, and NO3 chemistry in BB plumes emitted late in the day is responsible for 72 %–92 % (84 % in an optically thick midday plume) of nitrocatechol formation and controls nitrophenolic formation overall. As a result, overnight nitrophenolic formation pathways account for 56 %±2 % of NOx loss by sunrise the following day. In all but one overnight plume we modeled, there was remaining NOx (13 %–57 %) and BBVOCs (8 %–72 %) at sunrise.

Measurement report: Long-range transport patterns into the tropical northwest Pacific during the CAMP2Ex aircraft campaign: Chemical composition, size distributions, and the impact of convection

Abstract: . The tropical Northwest Pacific (TNWP) is a receptor for pollution sources throughout Asia and is highly susceptible to climate change, making it imperative to understand long-range transport in this complex aerosol-meteorological environment. Measurements from the NASA Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP 2 Ex; 24 August to 5 October 2019) and back trajectories from the National Oceanic and Atmospheric Administration Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT) were used to examine transport into the TNWP from the Maritime Continent (MC), peninsular Southeast Asia (PSEA), East Asia (EA), and the West Pacific (WP). A mid-campaign monsoon shift on 20 September 2019 led to distinct transport patterns between the southwest monsoon (SWM; before 20 September) and monsoon transition (MT; after 20 September). During the SWM, long-range transport was a function of southwesterly winds and cyclones over the South China Sea. Low- (high-) altitude air generally came from MC (PSEA), implying distinct aerosol processing related to convection and perhaps wind shear. The MT saw transport from EA and WP, driven by Pacific northeasterly winds, continental anticyclones, and cyclones over the East China Sea. Composition of transported air differed by emission source and accumulated precipitation along trajectories (APT). MC air was characterized by biomass burning tracers while major components of EA air pointed to Asian outflow and secondary formation. Convective scavenging of PSEA air was evidenced by considerable vertical differences between aerosol species but not trace gases, as well as notably higher APT and smaller particles than other regions. Finally, we observed a possible wet scavenging mechanism acting on MC air aloft that was not strictly linked to precipitation. These results are important for understanding the transport and processing of air masses with further implications for modeling aerosol lifecycles and guiding international policymaking to public health and climate, particularly during the SWM and MT.

Chemical transport models often underestimate inorganic aerosol acidity in remote regions of the atmosphere

Abstract: The inorganic fraction of fine particles affects numerous physicochemical processes in the atmosphere. However, there is large uncertainty in its burden and composition due to limited global measurements. Here, we present observations from eleven different aircraft campaigns from around the globe and investigate how aerosol pH and ammonium balance change from polluted to remote regions, such as over the oceans. Both parameters show increasing acidity with remoteness, at all altitudes, with pH decreasing from about 3 to about −1 and ammonium balance decreasing from almost 1 to nearly 0. We compare these observations against nine widely used chemical transport models and find that the simulations show more scatter (generally R2 < 0.50) and typically predict less acidic aerosol in the most remote regions. These differences in observations and predictions are likely to result in underestimating the model-predicted direct radiative cooling effect for sulfate, nitrate, and ammonium aerosol by 15–39%. The acidity of inorganic aerosols in remote areas is often higher than predicted by chemical transport models, which may lead to an underestimation of direct radiative cooling, according to global aircraft observations of pH and ammonium balance in aerosols

CERES MODIS Cloud Product Retrievals for Edition 4—Part II: Comparisons to CloudSat and CALIPSO

Abstract: Assessments of the Clouds and the Earth’s Radiant Energy System Edition 4 (Ed4) cloud retrievals are critical for climate studies. Ed4 cloud parameters are evaluated using instruments in the A-Train Constellation. Cloud-Aerosol LiDAR with Orthogonal Polarization (CALIOP) and Cloud Profiling Radar (CPR) retrievals are compared with Ed4 retrievals from the Aqua Moderate-Resolution Imaging Spectroradiometer (MODIS) as a function of the CALIOP horizontal averaging (HA) scale. Regardless of the HA scale, MODIS daytime (nighttime) water cloud fraction (CF) is greater (less) than that from CALIOP. MODIS ice CF is less than CALIOP overall, with the largest differences in polar regions. Ed4 and CALIOP retrieve the same cloud phase in 70%–98% of simultaneous observations depending on the time of day, surface conditions, HA scales, and type of cloud vertical structure. Mean cloud top height (CTH) differences for single-layer water clouds over snow-/ice-free surfaces are less than 100 m. Base altitude positive biases of 170–460 m may be impacted by CPR detection limitations. Average MODIS ice CTHs are underestimated by 70 m for some deep convective clouds and up to ~2.2 km for thin cirrus. Ice cloud base altitudes are typically underestimated (overestimated) during daytime (nighttime). MODIS and CALIOP cirrus optical depths over oceans are within 46% and 5% for daytime and nighttime observations, respectively. Ice water path differences depend on the CALIOP retrieval version and warrant further investigation. Except for daytime cirrus optical depth, Ed4 cloud property retrievals are at least as accurate as other long-term operational cloud property retrieval systems.

The Global Budget of Atmospheric Methanol: New Constraints on Secondary, Oceanic, and Terrestrial Sources

Abstract: 29 Methanol is the second-most abundant organic gas in the remote atmosphere af30 ter methane, but its sources are poorly understood. Here, we report a global budget of 31 methanol constrained by observations from the ATom aircraft campaign as implemented 32 in the GEOS-Chem global atmospheric chemistry model. ATom observations under back33 ground marine conditions can be fit in the model with a surface ocean methanol con34 centration of 61 nM and a methanol yield of 13% from the newly implemented CH3O2+OH 35 reaction. While terrestrial biogenic emissions dominate the global atmospheric methanol 36 budget, secondary production from CH3O2 + OH and CH3O2 + CH3O2 accounts for 37 29% of the total methanol source, and makes up the majority of methanol in the back38 ground marine atmosphere sampled by ATom. Net emission from the ocean is compar39 atively minor, particularly because of rapid deposition from the marine boundary layer. 40 Aged anthropogenic and pyrogenic plumes sampled in ATom featured large methanol 41 enhancements to constrain the corresponding sources. Methanol enhancements in py42 rogenic plumes did not decay with age, implying in-plume secondary production. The 43 atmospheric lifetime of methanol is only 5.3 days, reflecting losses of comparable mag44 nitude from photooxidation and deposition. GEOS-Chem model results indicate that methanol 45 photochemistry contributes 5%, 4%, and 1.5% of the tropospheric burdens of formalde46 hyde, CO, and ozone respectively, with particularly pronounced effects in the tropical 47 upper troposphere. The CH3O2 + OH reaction has substantial impacts on radical bud48 gets throughout the troposphere and should be included in global atmospheric chemistry 49 models. 50 Plain Language Summary 51 Methanol is the most abundant non-methane organic gas in the lower atmosphere, 52 but the magnitudes of its sources and sinks remain uncertain. Here, we evaluate a global 53 atmospheric chemistry model against recent observations of methanol in the remote at54 mosphere to better constrain the methanol budget. We show that, relative to past stud55 ies, the new data suggest a smaller atmospheric methanol source from the ocean and a 56 larger source from gas-phase chemistry. Methanol emitted from the oceans plays a par57 ticularly small role in the atmosphere because it is quickly deposited back to the ocean 58 surface. We incorporate these updates into the global model and evaluate their impor59 tance for atmospheric chemistry more broadly, showing that methanol directly and in60 directly influences the abundances of many other tropospheric trace gases. 61

Nearfield Summary and Analysis of the Third AIAA Sonic Boom Prediction Workshop C608 Low Boom Demonstrator

Abstract: A summary and statistical analysis of the nearfield Computational Fluid Dynamics (CFD) submissions for the Third AIAA Sonic Boom Prediction Workshop is provided with a focus on the C608 Low Boom Flight Test Demonstrator. The C608 is more complex in terms of geometry and propulsion boundary conditions than previous workshops cases and is more representative of vehicles with lower ground loudness and the potential for lower annoyance. The nearfield signatures submitted by the participants are propagated to the ground to compute statistics of loudness measures over the vehicle sonic boom carpet. Principle component analysis is used to extract the primary variation modes. Context from previous sonic boom workshops indicates that this workshop has the lowest variation even though the case is more challenging because it is quieter and more complex. The international state-of-the-art results documented in this summary indicates that nearfield CFD variation is low enough for meaningful low-boom design and can contribute toward the discussion of replacing the prohibition of overland supersonic flight with a certification standard.