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NASA NTRS2011

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.↗

NASA NTRS2003

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.↗

NASA NTRS2016

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↗

NASA NTRS1982

Clouds and wet removal as causes of variability in the trace-gas composition of the marine troposphere

A modeling study of the effects of clouds and wet removal on the chemistry of the remote marine troposphere is described. Using a time-dependent model with parameterized vertical transport to calculate trace-gas concentrations, it is found that large variations in key species (e.g., HNO3, H2CO, and H2O2) result from simulations of sporadic rainfall, changes in cloud cover, and external inputs such as surface NO sources. Depending on the frequency and intensity of an event, the effects of these perturbations may persist for several days, thereby invalidating assumptions of photochemical equilibrium in the interpretation of measurements. Long-term integrations with fixed boundary conditions and regularly occurring cloud and rain episodes demonstrate a strong sensitivity of the mean concentration of longer-lived soluble gases to precipitation frequency but also confirm the validity of using properly chosen parameterizations of wet removal in steady state calculations.

Thompson, A. M.↗

NASA NTRS2005

Atmospheric Hydroperoxides in West Antarctica: Links to Stratospheric Ozone and Atmospheric Oxidation Capacity

The troposphere above the West Antarctic Ice Sheet (WAIS) was sampled for hydroperoxides at 21 locations during 2-month-long summer traverses from 2000 to 2002, as part of US ITASE (International Transantarctic Scientific Expedition). First time quantitative measurements using an HPLC method showed that methylhydroperoxide (MHP) is the only important organic hydroperoxide occurring in the Antarctic troposphere, and that it is found at levels ten times those previously predicted by photochemical models. During three field seasons, means and standard deviations for hydrogen peroxide (H2O2) were 321+/-158 pptv, 650+/-176 pptv and 330+/-147 pptv. While MHP was detected, but not quantified in December 2000, levels in summer 2001 and 2002 were 317+128 pptv and 304+/-172.2 pptv. Results from firn air experiments and diurnal variability of the two species showed that atmospheric H2O2 is significantly impacted by a physical snow pack source between 76 and 90degS, whereas MHP is not. We show strong evidence of a positive feedback between stratospheric ozone and H2O2 at the surface. Between November-27 and December-12 in 2001, when ozone column densities dropped below 220 DU (means in 2000 and 2001 were 318 DU and 334 DU, respectively), H2O2 was 1.7 times that observed in the same period in 2000 and 2002, while MHP was only 80% of the levels encountered in 2002. Photochemical box model runs suggest that NO and OH levels on WAIS are closer to coastal values, while Antarctic Plateau levels are higher, confirming that region to be a highly oxidizing environment. The modeled sensitivity of H2O2 and particularly MHP to NO offers the potential to use atmospheric hydroperoxides to constrain the NO background and thus estimate the past oxidation capacity of the remote atmosphere. Index Terms: 0365 Atmospheric Composition and Structure: Troposphere: composition and chemistry; 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 1610 Global Change: Atmosphere (03 15,0325); 0736 Cryosphere: Snow (1827, 1863); 0724 Cryosphere: Ice Cores (4932) Keywords: hydrogen peroxide, methylhydroperoxide, Antarctica, air-snow exchange, stratospheric ozone, atmospheric oxidation capacity

Frey, Markus M.↗

NASA NTRS1994

Aerosol particles in the upper troposphere and lower stratosphere: Elemental composition and morphology of individual particles in northern midlatitudes

Atmospheric particles were collected in the midlatitude upper troposphere (UT) and lower stratosphere (LS) by inetrial impaction for subsequent electron microscopy and individual particle element analysis. More than 97% of particles analyzed on impactor substrates exposed in the LS contained only O and S in detectable quantities; these particles are believed to be acidic sulfate. Nonsulfate materials seen in the remaining particles included soot, other c-rich substances and crustal materials. Although not predominantly sulfate, usually carried a sulfer-rich coating in the LS. Samples collected very near and just below the tropopause were also dominated by sulfates. The fraction of sulfate particles analyzed on impactor substrates exposed in the UT was 91-94% of the total particle concentration. Nonsulfate substances observed in the UT samples included crustal-type material, hydrated marine salts, carbon-rich materials of several types, and metal-containing substances of uncertain origin. Most of these UT particles were not coated with detectable quantitites of sulfate.

Sheridan, Patrick J.↗

NASA NTRS1980

Response of the global climate to changes in atmospheric chemical composition due to fossil fuel burning

Recent modeling of atmospheric chemical processes (Logan et al, 1978; Hameed et al, 1979) suggests that tropospheric ozone and methane might significantly increase in the future as the result of increasing anthropogenic emissions of CO, NO(x), and CH4 due to fossil fuel burning. Since O3 and CH4 are both greenhouse gases, increases in their concentrations could augment global warming due to larger future amounts of atmospheric CO2. To test the possible climatic impact of changes in tropospheric chemical composition, a zonal energy-balance climate model has been combined with a vertically averaged tropospheric chemical model. The latter model includes all relevant chemical reactions which affect species derived from H2O, O2, CH4, and NO(x). The climate model correspondingly incorporates changes in the infrared heating of the surface-troposphere system resulting from chemically induced changes in tropospheric ozone and methane. This coupled climate-chemical model indicates that global climate is sensitive to changes in emissions of CO, NO(x) and CH4, and that future increases in these emissions could augment global warming due to increasing atmospheric CO2.

Hameed, S.↗

NASA NTRS2019

Trends in Global Tropospheric Ozone Inferred from a Composite Record of TOMS/OMI/MLS/OMPS Satellite Measurements and the MERRA-2 GMI Simulation

Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show, by combining satellite measurements with a chemical transport model, that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from the Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India and East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson units (DU) (i.e., ∼15 %–20 % of average background ozone), with the largest increase (∼4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is used to aid in the interpretation of tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts the greatest increases of +6 to +7 DU over India and East Asia, very similar to the satellite measurements. In regions of significant increases in tropospheric column ozone (TCO) the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India and East Asia the trends in TCO for both GMI and satellite measurements are ∼+3 DU decade(exp −1) or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade(exp −1) for 1979–2005. The GMI simulation and satellite data also reveal a tropospheric ozone increases in ∼+4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ∼+3 DU decade−1 over the N Atlantic and NE Pacific.

Ziemke, Jerald R.↗

NASA NTRS2007

Importance of Rain Evaporation and Continental Convection in the Tropical Water Cycle

Atmospheric moisture cycling is an important aspect of the Earth's climate system, yet the processes determining atmospheric humidity are poorly understood. For example, direct evaporation of rain contributes significantly to the heat and moisture budgets of clouds, but few observations of these processes are available. Similarly, the relative contributions to atmospheric moisture over land from local evaporation and humidity from oceanic sources are uncertain. Lighter isotopes of water vapour preferentially evaporate whereas heavier isotopes preferentially condense and the isotopic composition of ocean water is known. Here we use this information combined with global measurements of the isotopic composition of tropospheric water vapour from the Tropospheric Emission Spectrometer (TES) aboard the Aura spacecraft, to investigate aspects of the atmospheric hydrological cycle that are not well constrained by observations of precipitation or atmospheric vapour content. Our measurements of the isotopic composition of water vapour near tropical clouds suggest that rainfall evaporation contributes significantly to lower troposphere humidity, with typically 20% and up to 50% of rainfall evaporating near convective clouds. Over the tropical continents the isotopic signature of tropospheric water vapour differs significantly from that of precipitation, suggesting that convection of vapour from both oceanic sources and evapotranspiration are the dominant moisture sources. Our measurements allow an assessment of the intensity of the present hydrological cycle and will help identify any future changes as they occur.

Worden, John↗

NASA NTRSDate not supplied

Long-range Transport of Siberian Biomass Burning Emissions to North America During FIREX-AQ

Biomass burning from wildfires is a significant global source of aerosol and trace gases which impact air quality, tropospheric and stratospheric composition, and climate. During the summer of 2019, wildfire activity in central and eastern Siberia occurred during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign conducted between July 24 and September 6, 2019. Ground-based lidar observations from the Autonomous Mobile Ozone Lidar for Tropospheric Experiments (AMOLITE) system in Alberta, Canada retrieved frequent anomalous ozone (O3) and aerosol lamina in the troposphere and lower stratosphere during this campaign. Data from NASA’s GEOS Composition Forecast (GEOS-CF) coupled chemistry meteorology model, TROPOspheric Monitoring Instrument (TROPOMI), Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), and ground-based insitu data were used to define the trans-Pacific and trans-Arctic transport pathway of Siberian biomass burning emissions resulting in the enhanced O3 and aerosol lamina observed by AMOLITE in western Canada. Siberian wildfires impacted North American air quality resulting in enhancements of hourly-averaged surface carbon monoxide (CO) (total CO >150 ppb) and fine particulate matter (PM2.5) (>20 μg m-3) in western Canada, however, minimal increases in surface-level O3 were measured as well as modeled by GEOS-CF. The impact in western Canada due to Siberian wildfires was much larger in the free troposphere, demonstrated by GEOS-CF and AMOLITE O3 lamina 30–40 ppb above background values and model-predicted PM2.5 lamina >30 μg m-3. In addition to tropospheric composition effects, the large wildfire activity in Siberia may have influenced the stratosphere as data from AMOLITE, CALIPSO, and GEOS-CF all suggested aerosol layers from the fires were located 13–18 km above ground level (agl). This study shows that the Siberian biomass burning emissions in the summer of 2019 impacted tropospheric/stratospheric composition in western Canada, and potentially could have influenced areas in the vicinity of FIREX-AQ airborne measurements, and future studies of FIREX-AQ chemical composition should consider how this long-range transport could have influenced the background trace gas and aerosol concentrations being investigated.

Biomass↗

DOE OSTI2020

Differences in fine particle chemical composition on clear and cloudy days

Clouds are prevalent and alter fine particulate matter (PM 2.5 ) mass and chemical composition. Cloud-affected satellite retrievals are subject to higher uncertainty and are often removed from data products, hindering quantitative estimates of tropospheric chemical composition during cloudy times. We examine surface PM 2.5 chemical constituent concentrations in the Interagency Monitoring of PROtected Visual Environments (IMPROVE) network in the United States during cloudy and clear-sky times defined using Moderate Resolution Imaging Spectroradiometer (MODIS) cloud flags from 2010 to 2014 with a focus on differences in particle species that affect hygroscopicity and aerosol liquid water (ALW). Cloudy and clear-sky periods exhibit significant differences in PM 2.5 mass and chemical composition that vary regionally and seasonally. In the eastern US, relative humidity alone cannot explain differences in ALW, suggesting that emissions and in situ chemistry related to anthropogenic sources exert determining impacts. An implicit clear-sky bias may hinder efforts to quantitatively understand and improve representation of aerosol–cloud interactions, which remain dominant uncertainties in models.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1999

Shipboard and Satellite Views of Elevated Tropospheric Ozone over the Tropical Atlantic in January-February 1999

During the Aerosols99 trans-Atlantic cruise from Norfolk, VA, to Cape Town, South Africa, daily ozonesondes were launched from the NOAA R/V Ronald H Brown between 17 January and 6 February l999. A composite of tropospheric ozone profiles along the latitudinal transect shows 4 zones, which are interpreted using correlative shipboard ozone, CO, water vapor, and overhead aerosol optical thickness measurements. Elevated ozone associated with biomass burning north of the ITCZ (Intertropical Convergence Zone) is prominent at 3-5 km from 10-0N, but even higher ozone (100 ppbv, 7-10 km) occurred south of the ITCZ, where it was not burning. Column-integrated tropospheric ozone was 44 Dobson Units (DU) in one sounding, 10 DU lower than the maximum in a January-February 1993 Atlantic cruise with ozonesondes [Weller et al., 1996]. TOMS tropospheric ozone shows elevated ozone extending throughout the tropical Atlantic in January 1999. Several explanations are considered. Back trajectories, satellite aerosol observations and shipboard tracers suggest a combination of convection and interhemispheric transport of ozone and/or ozone precursors, probably amplified by a lightning NO source over Africa.

Thompson, Anne M.↗

NASA NTRS2005

Chemistry, Dynamics, and Radiation of Ozone Loss: Airborne Measurements of OH, HO2, NO2, ClO, BrO, IO, ClONO2, BrONO2, ClOOCl, and H2O

This grant continued the research initially funded under NAG1-01095. This research addresses, through a combination of in situ and remote aircraft-borne instruments, the following scientific questions: Which mechanisms are responsible for the continuing erosion of ozone over midlatitudes of the Northern Hemisphere? Will the rapid loss of ozone over the Arctic in late winter continue to worsen over the next two decades? Are these large losses dynamically coupled to midlatitudes? Which mechanisms dictate the rate of exchange of material between the troposphere and stratosphere? How will these processes change in response to changes in climate? Will regional scale pollution episodes, that are emerging as predictable seasonal events, significantly affect the middle-to-upper troposphere chemical composition. If so, how will these changes alter the chemical composition of the middle world? What changes are predicted for the overworld? Why has the arctic stratosphere become colder in the late winter phase in recent years? Have increases in tropical upper troposphere temperatures increased the temperature gradient such as to change the trajectories of vertically propagating waves, thus reducing the effectiveness of the meridional circulation for transport of heat, momentum and ozone from the tropics to high latitudes?

Anderson, James G.↗

NASA NTRS2005

Chemistry, Dynamics, and Radiation of Ozone Loss: Airborne Measurements of OH, HO2, N02, Cl0, BrO, IO, ClON02, BrON02, CIOOCl, and H2O

This research addresses, through a combination of in situ and remote aircraft-borne Which mechanisms are responsible for the continuing erosion of ozone over midlatitudes of the Northern Hemisphere? Will the rapid loss of ozone over the Arctic in late winter continue to worsen over the next two decades? Are these large losses dynamically coupled to midlatitudes? Which mechanisms dictate the rate of exchange of material between the troposphere and stratosphere? How will these processes change in response to changes in climate? Will regional scale pollution episodes, that are emerging as predictable seasonal events, significantly affect the middle-to-upper troposphere chemical composition. If so, how will these changes alter the chemical composition of the middle world? What changes are predicted for the overworld? Why has the arctic stratosphere become colder in the late winter phase in recent years? Have increases in tropical upper troposphere temperatures increased the temperature gradient such as to change the trajectories of vertically propagating waves, thus reducing the effectiveness of the meridional circulation for transport of heat, momentum and ozone from the tropics to high latitudes?

Anderson, James G.↗

NASA NTRS1982

Importance of heterogeneous processes to tropospheric chemistry - Studies with a one-dimensional model

A one-dimensional, time-dependent model of tropospheric air composition is developed which incorporates several heterogeneous physical and chemical processes. The model includes the interaction of gases, aerosols, and hydrometeors through the physical mechanisms of nucleation, condensation, evaporation, coagulation, coalescence, and deliquescence. Precipitation, sedimentation, and dry deposition act to remove material from the atmosphere, while chemical transformations occur both in the vapor and the condensed phases. The model also incorporates the sources and vertical diffusion of gases and particles, as well as changes in the solar intensity caused by light-scattering from aerosols and clouds. Preliminary simulations made using this model indicate that rainout and washout processes strongly influence the distributions of tropospheric gases and aerosols under certain conditions.

Turco, R. P.↗

NASA NTRS2003

Intercomparisons of Airborne Measurements of Aerosol Ionic Chemical Composition during TRACE-P and ACE-Asia

As part of the two field studies, Transport and Chemical Evolution over the Pacific (TRACE-P), and the Asian Aerosol Characterization Experiment (ACEAsia), the inorganic chemical composition of tropospheric aerosols was measured over the western Pacific from three separate aircraft using various methods. Comparisons are made between the rapid online techniques of the Particle Into Liquid Sampler (PILS) for measurement of a suite of fine particle ionic compounds and a mist chamber (MC/IC) measurement of fine sulfate, and the longer time-integrated filter and multi-orifice impactor (MOI) measurements. Comparisons between identical PILS on two separate aircraft flying in formation showed that they were highly correlated (e.g., sulfate r(sup 2) of 0.95), but were systematically different by 10 +/- 5% (linear regression slope and 95% confidence bounds), and had generally higher concentrations on the aircraft with a low turbulence inlet and shorter inlet-to-instrument transmission tubing. Comparisons of PILS and mist chamber measurements of fine sulfate on two different aircraft during formation flying had an 3 of 0.78 and a relative difference of 39% +/- 5%. MOI ionic data integrated to the PILS upper measurement size of 1.3 pm sampling from separate inlets on the same aircraft showed that for sulfate, PILS and MOI were within 14% +/- 6% and correlated with an r(sup 2) of 0.87. Most ionic compounds were within f 30%, which is in the range of differences reported between PILS and integrated samplers from ground-based comparisons. In many cases, direct intercomparison between the various instruments is difficult due to differences in upper-size detection limits. However, for this study, the results suggest that the fine particle mass composition measured from aircraft agree to within 30-40%.

Ma, Y.↗

DOE OSTI2025

CoURAGE Urban Gas-Phase NH3

1-second Picarro gas-phase ammonia (NH3) measurements were collected as part of a 3-month intensive operation period (IOP) from mid-March through mid-June that was funded by the DOE Biological and Environment Research project in conjunction with the DOE ARM CoURAGE deployment to the greater Baltimore region. To complement the NH3 measurements at the Mt. Airy regional background S2 site, the Picarro G2103 NH3 analyzer was deployed at the urban atmospheric chemistry supersite ( 39.32057 N, 76.6246 W) to be able to compare and contrast urban vs regional NH3 and urban vs regional aerosol physicochemical properties.

Aerosol Acidity↗

NASA NTRS1973

Chemistry of the lower atmosphere

The presence of particulate matter in the lower atmosphere is considered, giving attention to the sources of particles in the troposphere, the composition of particles collected from the atmosphere, aspects of particle concentrations and size distributions, mechanisms of removal, residence times, and conditions in the lower stratosphere. The role of natural and anthropogenic pollutants in cloud and precipitation formation is discussed together with removal processes of gaseous and particulate pollutants, and the global sulfur cycle. Other topics examined include the chemical basis for climatic change and the carbon dioxide cycle. Individual items are announced in this issue.

Rasool, S. I.↗