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Airborne lidar measurements of ozone and aerosols in the summertime Arctic troposphere

Ozone (O3) and aerosol distributions were remotely measured from an aircraft using a differential absorption lidar (DIAL) system as part of the 1988 NASA Global Tropospheric Experiment - Arctic Boundary Layer Experiment (ABLE-3A). The airborne DIAL system made simultaneous measurements of O3 and aerosols from the surface to above the tropopause. These measurements were made in a broad range of atmospheric conditions over the tundra, ice, and ocean regions near Barrow and Bethel, Alaska, during July and August 1988. The tropospheric composition over the Arctic was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were usually correlated with descending air from the upper troposphere or lower stratosphere. Several cases of enhanced O3 were observed during ABLE-3A in conjunction with enhanced aerosol layers in the free troposphere resulting from biomass burning. As was found in the Amazon, the products of biomass burning can significantly alter O3 concentrations in the troposphere. This paper describes the NASA airborne DIAL system and discusses the large-scale variations of O3 and aerosols observed with the airborne DIAL system during ABLE-3A.

Browell, Edward V.↗

Impact of Canadian Wildfires 2023 on North Atlantic's Region Air Quality: An Analysis Using ASDC Data

Wildfires pose a growing concern in North America due to their harmful impacts on air quality and public health, with increased wildfire activity in recent years leading to widespread smoke plumes that can transcend borders. The exposure of New York City (NYC), the most populous city in North America, to Canadian wildfire smoke highlights the substantial implications for public health and urban environments. To better understand the impact of Canadian wildfires on air quality in NYC, satellite data from the NASA Atmospheric Science Data Center (ASDC) at Langley Research Center, along with ground-based measurements and atmospheric modeling results, are analyzed. NASA's Atmospheric Science Data Center (ASDC) is in the Science Directorate located at NASA'S Langley Research Center in Hampton, Virginia. The Science Directorate's Climate Science Branch, Atmospheric Composition Branch, and Chemistry and Dynamics Branch work with ASDC to study changes in the Earth and its atmosphere. ASDC projects focus on the Earth science disciplines: Radiation Budget, Clouds, Aerosols, and Tropospheric Composition. All the products chosen for this analysis are products hosted by ASDC and available for users to obtain via our services [1].

Hazem Mahmoud↗

[Sources of Methane in the Boreal Region]

In determining the global methane budget the sources of methane must be balanced with the sinks and atmospheric inventory. The approximate contribution of the different methane sources to the budget has been establish showing the major terrestrial inputs as rice, wetlands, bogs, fens, and tundra. Measurements and modeling of production in these sources suggest that temperature, water table height and saturation along with substratum composition are important in controlling methane production and emission. The isotopic budget of 13 C and D/H in methane can be used as a tool to clarify the global budget. This approach has achieved success at constraining the inputs. Studies using the isotopic approach place constraints on global methane production from different sources. Also, the relation between the two biogenic production pathways, acetate fermentation and CO2 reduction, and the effect of substratum composition can be made using isotope measurements shows the relation between the different biogenic, thermogenic and anthropogenic sources of methane as a function of the carbon and hydrogen isotope values for each source and the atmosphere, tropospheric composition. Methane emissions from ponds and fens are a significant source in the methane budget of the boreal region. An initial study in 1993 and 1994 on the isotopic composition of this methane source and the isotopic composition in relation to oxidation of methane at the sediment surface of the ponds or fen was conducted as part of our BOREAS project. The isotopic composition of methane emitted by saturated anoxic sediment is dependent on the sediment composition and geochemistry, but will be influenced by in situ oxidation, in part, a function of rooted plant activity. The influence of oxidation mediated by rooted plant activities on the isotopic composition of methane is not well known and will depend on the plant type, sediment temperature, and numerous other variables. Information on this isotopic composition is important in both understanding the bio-geochemistry of the system and also in determining the regional and global inputs for the methane isotope budget. In determining the destruction of methane for balancing the atmospheric methane budget soil oxidation must be considered.

Source record↗

Large-scale variability of ozone and aerosols in the summertime Arctic and sub-Arctic troposphere

The results of mesoscale and large-scale studies of the distribution of aerosols and O3 using primarily an airborne DIAL system are reported. The tropospheric composition at high latitudes is found to be strongly influenced by stratospheric intrusions. Regions of low-aerosol scattering and enhanced O3 mixing ratios are correlated with descending air from the lower stratosphere. Over 37 percent of the troposphere along the flight track at latitudes higher than 57 deg N had significantly enhanced O3 levels due to stratospheric intrusions, and in the 4-6 km latitude range the tropospheric extent of the enhanced O3 exceeded 56 percent. Ozone mixing ratios of 80 ppbv at 6 km are common, with vertical O3 gradients of over 11 ppbv/km observed across the base of strong intrusions. In the mixed layer over the tundra, O3 was in the 25-35 ppbv range with a gradient of 5.5 ppbv/km, while in the continental polar air masses, the average gradient in the lower troposphere is 7.4 ppbv/km, indicating more downward transport of O3 at higher latitudes.

Browell, E. V.↗

Ozone and aerosol distributions in the summertime troposphere over Canada

Measurements of ozone (O3) and aerosol distributions were made with an airborne lidar system in the lowland and boreal forest regions of eastern Canada during July - August 1990 as part of the NASA Global Tropospheric Experiment/Arctic Boundary Layer Expedition (ABLE) 3B. Aerosol and O3 profiles were measured simultaneously above and below the Electra aircraft from near the surface to above the tropopause on long-range flights over these important ecosystems. A broad range of atmospheric conditions were encountered during repeated flights over intensive study sites in the Hudson Bay lowlands near Moosonee, Ontario, and over the boreal forest near Schefferville, Quebec. The tropospheric composition in this high-latitude region was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were correlated with descending air from the lower stratosphere. Over 33% of the troposphere (0-12 km) along our flight track at latitudes from about 45 deg to 55 deg N had significantly enhanced O3 due to stratospheric intrusions, and in the middle to upper troposphere the extent of the enhanced O3 gnerally exceeded 40%. Ozone mixing ratios of 80 parts per billion by volume (ppbv) near 6 km were common in strong intrusions. In the boundary layer over the lowlands, O3 was in the 20-30 ppbv range with a vertical O3 gradient of 6.7 ppbv/km to about 45 ppbv at 3 km. Above 6 km the background tropospheric O3 profile was nearly constant with an average value of 53 ppbv. Due to forest fires in Canada and Alaska, plumes from biomass-burning sources were observed on many flights. Biomass-burning plumes influenced about 25% of the free troposphere below 4 km, and in some of the plumes, O3 was enhanced by 10-20 ppbv over ambient levels of 30-45 ppbv. Several air masses transported from the tropical Pacific were observed over Canada in the middle to upper troposphere with O3 levels 10-20 ppbv below background values of 50-55 ppbv.

Browell, E. V.↗

Overview of Large-Scale Transport into the Arctic in the Chemistry Climate Model Initiative (CCMI) Simulations

The transport of trace gases and aerosols is a major uncertainty in the modeling of Arctic tropospheric composition. Here we compare the large-scale midlatitude-to-Arctic transport properties among different models participating in the Chemistry Climate Modeling Initiative (CCMI). Among simulations of the recent past (1980-2010) we show that there are substantial (~30-45%) differences in transport to the Arctic free troposphere, as diagnosed through use of idealized tracers emitted over the Northern Hemisphere (NH) midlatitude surface and subject to prescribed uniform loss. In addition, we show that the spread among tracers with predominantly land-based sources is correlated with the spread in the location of the Hadley Cell edge, while the spread in tracers with zonally uniform sources is also related to differences in (parameterized) convection over oceans. Interestingly, comparisons with simulations constrained with analysis fields reveal similar, if not larger, transport differences, compared to the free-running simulations, indicating that caution should be taken when interpreting simulations constrained with analyzed winds. Finally, among simulations of the 21st century we show that models project a consistent, albeit small (~5-10%), increase in transport from the NH midlatitude surface to the Arctic upper troposphere.

Large-Scale Transpor↗

Global Impact of Lightning-Produced Oxidants

Lightning plays a major role in tropospheric oxidation, and its role on modulating tropospheric chemistry was thought to be emissions of nitrogen oxides (NOx). Recent field and laboratory measurements demonstrate that lightning generates extremely large amounts of oxidants, including hydrogen oxides (HOx) and O3. Here we implement these lightning-produced oxidants in a global chemical transport model to examine its global impact on tropospheric composition. We find that lightning-produced oxidants can increase global mass weighted OH by 0.3-10%, and affect CO, O3, and reactive nitrogen substantially, depending on the emission strength of oxidants from lightning. Our work highlights the importance and uncertainties of lightning-produced oxidants, as well as the need for rethinking the role of lightning in tropospheric oxidation chemistry.

Jingqiu Mao↗

The Strengths and Limitations of Satellite Data for Evaluating Tropospheric Processes in Chemistry-Climate Models

There is now a wealth of satellite data products available with which to evaluate a model fs simulation of tropospheric composition and other model processes. All of these data products have their strengths and limitations that need to be considered for this purpose. For example, uncertainties are introduced into a data product when 1) converting a slant column to a vertical column and 2) estimating the amount of a total column of a trace gas (e.g., ozone, nitrogen dioxide) that resides in the troposphere. Oftentimes, these uncertainties are not well quantified and the satellite data products are not well evaluated against in situ observations. However, these limitations do not preclude us from using these data products to evaluate our model processes if we understand these strengths and limitations when developing diagnostics. I will show several examples of how satellite data products are being used to evaluate particular model processes with a focus on the strengths and limitations of these data products. In addition, I will introduce the goals of a newly formed team to address issues on the topic of "satellite data for improved model evaluation and process studies" that is established in support of the IGAC/SPARC Global Chemistry ]Climate Modeling and Evaluation Workshop.

Duncan, Bryan↗

The Equilibrium Response of Climate and Composition to Lightning

Climate change can affect atmospheric composition through perturbation of natural processes, leading to complex feedbacks. The primary atmospheric oxidants OH and ozone are very sensitive to emissions of nitrogen oxides (NO x ) from lightning, and therefore so are the subsequent chemical perturbations to long-lived greenhouse gases (e.g., methane) and aerosol chemistry and physics. Meanwhile, cloud electrification responds to both meteorology and composition (aerosol particles). Key to understanding the ultimate impact of lightning on air quality and climate is the long-term methane feedback. Here, we present simulations from the GISS ModelE2.1 chemistry-climate model in which we isolate the response of Earth’s radiative budget and composition to lightning NO x in the present day and at the end of this century by allowing the model to re-equilibrate following removal of the source. Whereas lightning initially contributes to surface ozone enhancements, longer-term responses amplified by the methane lifetime feedback reduce surface ozone on multi-decadal time scales in the northern midlatitudes. Lightning consequently contributes a strong negative radiative effect in the present day (-0.5 W m -2 ), stronger than that estimated for the anthropogenic NOx source. In addition to influencing tropospheric composition, we find significant changes in stratospheric dynamics and composition. We test the sensitivity of our results to multiple parameterizations for global lightning activity.

Lightning↗

Atmospheric Constituents in GEOS-5: Components for an Earth System Model

The GEOS-S model is being developed for weather and climate processes, including the implementation of "Earth System" components. While the stratospheric chemistry capabilities are mature, we are presently extending this to include predictions of the tropospheric composition and chemistry - this includes CO2, CH4, CO, nitrogen species, etc. (Aerosols are also implemented, but are beyond the scope of this paper.) This work will give an overview of our chemistry modules, the approaches taken to represent surface emissions and uptake of chemical species, and some studies of the sensitivity of the atmospheric circulation to changes in atmospheric composition. Results are obtained through focused experiments and multi-decadal simulations.

Pawson, Steven↗

Alabama Ground Operations during the Deep Convective Clouds and Chemistry Experiment

The Deep Convective Clouds and Chemistry (DC3) field campaign investigates the impact of deep, midlatitude convective clouds, including their dynamical, physical and lighting processes, on upper tropospheric composition and chemistry. DC3 science operations took place from 14 May to 30 June 2012. The DC3 field campaign utilized instrumented aircraft and ground ]based observations. The NCAR Gulfstream ]V (GV) observed a variety of gas ]phase species, radiation and cloud particle characteristics in the high ]altitude outflow of storms while the NASA DC ]8 characterized the convective inflow. Groundbased radar networks were used to document the kinematic and microphysical characteristics of storms. In order to study the impact of lightning on convective outflow composition, VHF ]based lightning mapping arrays (LMAs) provided detailed three ]dimensional measurements of flashes. Mobile soundings were utilized to characterize the meteorological environment of the convection. Radar, sounding and lightning observations were also used in real ]time to provide forecasting and mission guidance to the aircraft operations. Combined aircraft and ground ]based observations were conducted at three locations, 1) northeastern Colorado, 2) Oklahoma/Texas and 3) northern Alabama, to study different modes of deep convection in a variety of meteorological and chemical environments. The objective of this paper is to summarize the Alabama ground operations and provide a preliminary assessment of the ground ]based observations collected over northern Alabama during DC3. The multi ] Doppler, dual ]polarization radar network consisted of the UAHuntsville Advanced Radar for Meteorological and Operational Research (ARMOR), the UAHuntsville Mobile Alabama X ]band (MAX) radar and the Hytop (KHTX) Weather Surveillance Radar 88 Doppler (WSR ]88D). Lightning frequency and structure were observed in near real ]time by the NASA MSFC Northern Alabama LMA (NALMA). Pre ]storm and inflow proximity soundings were obtained with the UAHuntsville mobile sounding unit and the Redstone Arsenal (QAG) morning sounding.

Carey, Lawrence↗

Review of the Global Models Used Within Phase 1 of the Chemistry-Climate Model Initiative (CCMI)

We present an overview of state-of-the-art chemistry-climate and chemistry transport models that are used within phase 1 of the Chemistry-Climate Model Initiative (CCMI-1). The CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, tropospheric composition, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI-1 recommendations for simulations have been followed is necessary to understand model responses to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI-1 simulations with the aim of informing CCMI data users.

CCMI↗

Transient Aircraft Soot Emissions Indicate That Steady-State Measurements Likely Underestimate Real-World, Take-Off Emissions: Time-Varying Aircraft Take-Off Emissions Indices Measured at Los Angeles International Airport

Aircraft engine emissions are unique among mobile pollution sources in that their impacts affect the local air quality near airports as well as upper tropospheric composition and climate over regional-to-hemispheric scales. Furthermore, air travel and its resulting emissions are expected to rebound from the recent COVID-related lows to increase dramatically over the next several decades. Given the multi-decade service lifetime of many commercial aircraft, it is critically important to quantitatively understand the real-world emissions coming from these engines in order to inform environmental assessment and modelling activities. Here, we present a detailed analysis of aircraft emissions during take-off operations at Los Angeles International Airport. The data were collected as part of the NASA Alternative Fuel Effects on Contrails and Cruise Emissions (ACCESS) project in May 2014, and the dataset is publicly available as described by Moore et al. [1]. In particular, we focus on the time-varying nature of the plume concentrations where clear differences in particle size and non-volatile particle fraction are observed during the early portion of the take-off plume relative to the later portion of the plume. We compare the transient emissions indices measured here to engine certification values in the International Civil Aviation Organization (ICAO) Emissions Databank, which suggests that steady-state measurements may underestimate the real-world, non-volatile particle emissions. The implications of this finding for modelling aircraft particle emissions will be discussed.

Richard H. Moore↗

Joint Assimilation of CO, O3, NO2, SO2, PM, AOD, NH4, PAN, and HNO3 in Support of the Tropospheric Regional Atmospheric Composition and Emissions Reanalysis (2005 - 2024) (TRACER-I)

NASA Ames Research Center is collaborating with the NOAA Chemical Systems Laboratory (NOAA/CSL), the NASA Jet Propulsion Laboratory (JPL), the NASA Goddard Modeling and Assimilation Office, and the National Center for Atmospheric Research to prepare a 20-year Tropospheric Regional Atmospheric Composition and Emissions Reanalysis (2005 – 2024) (TRACER-I) for the continental United States during the summer ozone (O3) and wildfire seasons (April to October). TRACER-I will be a regional complement to JPL’s global Tropospheric Chemistry Reanalyses II and III. We will use WRF-Chem/DART with NOAA/CSL’s WRF-Chem setup at 12 km x 12 km horizontal resolution, 51 vertical levels, and 30 ensemble members. We will assimilate: (i) conventional meteorological observations; (ii) EPA’s Air Quality System in situ measurements of carbon monoxide (CO), O3, nitrogen dioxide (NO2), sulfur dioxide (SO2), particulate matter (PM) with diameters less than 10 µm (PM10), and PM with diameters less than 2.5 µm (PM2.5); and (iii) MOPITT, MODIS, OMI, TROPOMI, GOME-2a, MLS, TES, SCIAMACHY, CrIS, and TEMPO total/partial column and/or profile retrievals of CO, O3, NO2, SO2, aerosol optical depth (AOD), formaldehyde (HCHO), ammonia (NH4), peroxyacetyl nitrate (PAN), and/or nitric acid (HNO3) with 3-hr cycling. We will present an overview of this project, its status, and available results (likely the analysis of sensitivity experiment results from the assimilation/emissions estimation system).

data assimilation↗

The global troposphere - Biogeochemical cycles, chemistry, and remote sensing

The chemical composition of the troposphere is controlled by various biogeochemical cycles that couple the atmosphere with the oceans, the solid earth and the biosphere, and by atmospheric photochemical/chemical reactions. These cycles and reactions are discussed and a number of key questions concerning tropospheric composition and chemistry for the carbon, nitrogen, oxygen and sulfur species are identified. Next, various remote sensing techniques and instruments capable of measuring and monitoring tropospheric species from the ground, aircraft and space to address some of these key questions are reviewed. Future thrusts in remote sensing of the troposphere are also considered.

Levine, J. S.↗

Reactive Nitrogen, Ozone and Ozone Production in the Arctic Troposphere and the Impact of Stratosphere-Troposphere Exchange

We analyze the aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellite (ARCTAS) mission together with the GEOS-5 CO simulation to examine O3 and NOy in the Arctic and sub-Arctic region and their source attribution. Using a number of marker tracers and their probability density distributions, we distinguish various air masses from the background troposphere and examine their contribution to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has mean O3 of approximately 60 ppbv and NOx of approximately 25 pptv throughout spring and summer with CO decreases from approximately 145 ppbv in spring to approximately 100 ppbv in summer. These observed CO, NOx and O3 mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in the past two decades in processes that could have changed the Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses with mean O3 concentration of 140-160 ppbv are the most important direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin is the only notable driver of net O3 formation in the Arctic due to its sustainable high NOx (75 pptv in spring and 110 pptv in summer) and NOy (approximately 800 pptv in spring and approximately 1100 pptv in summer) levels. The ARCTAS measurements present observational evidence suggesting significant conversion of nitrogen from HNO3 to NOx and then to PAN (a net formation of approximately 120 pptv PAN) in summer when air of stratospheric origin is mixed with tropospheric background during stratosphere-to-troposphere transport. These findings imply that an adequate representation of stratospheric O3 and NOy input are essential in accurately simulating O3 and NOx photochemistry as well as the atmospheric budget of PAN in tropospheric chemistry transport models of the Arctic. Anthropogenic and biomass burning pollution plumes observed during ARCTAS show highly elevated hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contribute significantly to O3 in the Arctic troposphere except in some of the aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

Liang, Q.↗

Water Vapor and its Isotopic Composition in the Upper Troposphere and Stratosphere

Any theory of water vapor in the tropical tropopause layer (TTL) must explain both the abundance and isotopic composition of water there. We have previously presented a model of the TTL that simulated the abundance of water vapor as well as the details of the vertical profile. That model included the effects of 'overshooting convection', which injects dry air directly into the TTL. Here, we present results for the model after modifying it to include water's stable isotope HDO. The model is capable of accurately simulating the recently observed, nearly uniform HDO depletion (delta D) in the TTL. We find that lofted ice is necessary to accurately simulate the profile of delta D in the TTL, as has been suggested previously. We also find that vertical mixing due to overshooting convection plays an important role in maintaining the observed profile. Finally, any theory of lofted ice requires a complementary source of dry air in the TTL; without that, the TTL will rapidly saturate and the lofted ice will not evaporate.

Dessler, A. E.↗

The Impact of ENSO on Trace Gas Composition in the Upper Troposphere to Lower Stratosphere

The El Nino-Southern Oscillation (ENSO) is the dominant mode of interannual variability in the tropical troposphere and its effects extend well into the stratosphere. Its impact on atmospheric dynamics and chemistry cause important changes to trace gas constituent distributions. A comprehensive suite of satellite observations, reanalyses, and chemistry climate model simulations are illuminating our understanding of processes like ENSO. Analyses of more than a decade of observations from NASAs Aura and Aqua satellites, combined with simulations from the Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM) and other Chemistry Climate Modeling Initiative (CCMI) models, and the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) reanalysis have provided key insights into the response of atmospheric composition to ENSO. While we will primarily focus on ozone and water vapor responses in the upper troposphere to lower stratosphere, the effects of ENSO ripple through many important trace gas species throughout the atmosphere. The very large 2015-2016 El Nino event provides an opportunity to closely examine these impacts with unprecedented observational breadth. An improved quantification of natural climate variations, like those from ENSO, is needed to detect and quantify anthropogenic climate changes.

ENSO↗