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At least 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
NASA NTRS2023

Heterogeneity and Chemical Reactivity of the Remote Troposphere Defined By Aircraft Measurements - Corrected

The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10 s (2 km) merged and gap-filled observations of the key reactive species driving the chemical budgets of O3 and CH4 (O3, CH4, CO, H2O, HCHO, H2O2, CH3OOH, C2H6, higher alkanes, alkenes, aromatics, NOx, HNO3, HNO4, peroxyacetyl nitrate, and other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O3 and CH4 photochemical tendencies from this modeling data stream for ATom 1. We find that 80 %–90 % of the total reactivity lies in the top 50 % of the parcels and 25 %–35 % in the top 10 %, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom 10 s data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find generally good agreement with the reactivity rates for O3 and CH4. Models distinctly underestimate O3 production below 2 km relative to the mid-troposphere, and this can be traced to lower NOx levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-to-what-matters, set of metrics for model evaluation.

Tropospheric Chemistry↗
DOE OSTI2017

Ice cloud formation potential by free tropospheric particles from long-range transport over the Northern Atlantic Ocean

Long-range transported free tropospheric particles can play a significant role on heterogeneous ice nucleation. Using optical and electron microscopy we examine the physicochemical characteristics of ice nucleating particles (INPs). Particles were collected on substrates from the free troposphere at the remote Pico Mountain Observatory in the Azores Islands, after long-range transport and aging over the Atlantic Ocean. We investigate four specific events to study the ice formation potential by the collected particles with different ages and transport patterns. We use single-particle analysis, as well as bulk analysis to characterize particle populations. Both analyses show substantial differences in particle composition between samples from the four events; in addition, single-particle microscopy analysis indicates that most particles are coated by organic material. The identified INPs contained mixtures of dust, aged sea salt and soot, and organic material acquired either at the source or during transport. The temperature and relative humidity ( RH ) at which ice formed, varied only by 5% between samples, despite differences in particle composition, sources, and transport patterns. We hypothesize that this small variation in the onset RH may be due to the coating material on the particles. Finally, this study underscores and motivates the need to further investigate how long-range transported and atmospherically aged free tropospheric particles impact ice cloud formation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Tropospheric circulation during the early twentieth century Arctic warming

The early twentieth century Arctic warming (ETCAW) between 1920 and 1940 is an exceptional feature of climate variability in the last century. Its warming rate was only recently matched by recent warming in the region. Unlike recent warming largely attributable to anthropogenic radiative forcing, atmospheric warming during the ETCAW was strongest in the mid-troposphere and is believed to be triggered by an exceptional case of natural climate variability. Nevertheless, ultimate mechanisms and causes for the ETCAW are still under discussion. Here we use state of the art multi-member global circulation models, reanalysis and reconstruction datasets to investigate the internal atmospheric dynamics of the ETCAW. We investigate the role of boreal winter mid-tropospheric heat transport and circulation in providing the energy for the large scale warming. Analyzing sensible heat flux components and regional differences, climate models are not able to reproduce the heat flux evolution found in reanalysis and reconstruction datasets. These datasets show an increase of stationary eddy heat flux and a decrease of transient eddy heat flux during the ETCAW. Moreover, tropospheric circulation analysis reveals the important role of both the Atlantic and the Pacific sectors in the convergence of southerly air masses into the Arctic during the warming event. Subsequently, it is suggested that the internal dynamics of the atmosphere played a major role in the formation in the ETCAW.

Meteorology & Atmospheric Sciences↗
DOE OSTI2018

Simulated Global Climate Response to Tropospheric Ozone-Induced Changes in Plant Transpiration

Tropospheric ozone (O 3 ) pollution is known to damage vegetation, reducing photosynthesis and stomatal conductance, resulting in modified plant transpiration to the atmosphere. We use an Earth system model to show that global transpiration response to near-present-day surface tropospheric ozone results in large-scale global perturbations to net outgoing long-wave and incoming shortwave radiation. Our results suggest that the radiative effect is dominated by a reduction in shortwave cloud forcing in polluted regions, in response to ozone-induced reduction in land-atmosphere moisture flux and atmospheric humidity. We simulate a statistically significant response of annual surface air temperature of up to ~ +1.5 K due to this ozone effect in vegetated regions subjected to ozone pollution. This mechanism is expected to further increase the net warming resulting from historic and future increases in tropospheric ozone.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Lower Tropospheric Processes: A Control on the Global Mean Precipitation Rate

The spread in global mean precipitation among climate models is explored in two ensembles using the complementary perspectives of surface evaporation and energy budgets. Models with higher global mean precipitation have stronger oceanic evaporation, driven by drier near-surface air. The drier surface conditions occur alongside increases in near-surface temperature and moisture at 925 hPa, which point to stronger boundary layer mixing. Correlations suggest that the degree of lower tropospheric mixing explains 18%–49% of the intermodel precipitation variance. To test this hypothesis, the degree of mixing is indirectly varied in a single-model experiment by adjusting the relative humidity threshold that controls low-cloud fraction. Indeed, increasing lower tropospheric mixing results in more global mean precipitation. Energetically, increased precipitation rates are associated with more downwelling longwave radiation to the surface and weaker sensible heat fluxes. These results highlight how lower-tropospheric processes must be better constrained to reduce the precipitation discrepancy among climate models.

58 GEOSCIENCES↗
DOE OSTI2018

Criegee intermediates and their impacts on the troposphere

We report Criegee intermediates (CIs), carbonyl oxides formed in ozonolysis of alkenes, play key roles in the troposphere. The decomposition of CIs can be a significant source of OH to the tropospheric oxidation cycle especially during nighttime and winter months. A variety of model-measurement studies have estimated surface-level stabilized Criegee intermediate (sCI) concentrations on the order of 1 × 10 4 cm -3 to 1 × 10 5 cm -3 , which makes a non-negligible contribution to the oxidising capacity in the terrestrial boundary layer. The reactions of sCI with the water monomer and the water dimer have been found to be the most important bimolecular reactions to the tropospheric sCI loss rate, at least for the smallest carbonyl oxides; the products from these reactions (e.g. hydroxymethyl hydroperoxide, HMHP) are also of importance to the atmospheric oxidation cycle. The sCI can oxidise SO 2 to form SO 3 , which can go on to form a significant amount of H 2 SO 4 which is a key atmospheric nucleation species and therefore vital to the formation of clouds. Lastly, the sCI can also react with carboxylic acids, carbonyl compounds, alcohols, peroxy radicals and hydroperoxides, and the products of these reactions are likely to be highly oxygenated species, with low vapour pressures, that can lead to nucleation and SOA formation over terrestrial regions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

The Response of the Polar Vortex to Tropospheric Temperature Eddies in an Idealized General Circulation Model

Abstract A dry-core idealized general circulation model with a stratospheric polar vortex in the Northern Hemisphere is run with a combination of simplified topography and imposed tropospheric temperature perturbations, each located in the Northern Hemisphere with a zonal wavenumber of 1. The phase difference between the imposed temperature wave and the topography is varied to understand what effect this has on the occurrence of polar vortex displacements. Geometric moments are used to identify the centroid of the polar vortex for the purposes of classifying whether or not the polar vortex is displaced. Displacements of the polar vortex are a response to increased tropospheric wave activity. Compared to a model run with only topography, the likelihood of the polar vortex being displaced increases when the warm region is located west of the topography peak, and decreases when the cold region is west of the topography peak. This response from the polar vortex is due to the modulation of vertically propagating wave activity by the temperature forcing. When the southerly winds on the western side of the topographically forced anticyclone are collocated with warm- or cold-temperature forcing, the vertical wave activity flux in the troposphere becomes more positive or negative, respectively. This is in line with recent reanalysis studies that showed that anomalous warming west of the surface pressure high, in the climatological standing wave, precedes polar vortex disturbances.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Multi-Frequency Analysis of Simulated versus Observed Variability in Tropospheric Temperature

Studies seeking to identify a human-caused global warming signal generally rely on climate model estimates of the “noise” of intrinsic natural variability. Assessing the reliability of these noise estimates is of critical importance. We evaluate here the statistical significance of differences between climate model and observational natural variability spectra for global-mean mid- to upper-tropospheric temperature (TMT). We use TMT information from satellites and large multimodel ensembles of forced and unforced simulations. Our main goal is to explore the sensitivity of model-versus-data spectral comparisons to a wide range of subjective decisions. These include the choice of satellite and climate model TMT datasets, the method for separating signal and noise, the frequency range considered, and the statistical model used to represent observed natural variability. Of particular interest is the amplitude of the interdecadal noise against which an anthropogenic tropospheric warming signal must be detected. We find that on time scales of 5–20 years, observed TMT variability is (on average) overestimated by the last two generations of climate models participating in the Coupled Model Intercomparison Project. This result is relatively insensitive to different plausible analyst choices, enhancing confidence in previous claims of detectable anthropogenic warming of the troposphere and indicating that these claims may be conservative. A further key finding is that two commonly used statistical models of short-term and long-term memory have deficiencies in their ability to capture the complex shape of observed TMT spectra.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic

Ten-year observations of trace gases at Pico Mountain Observatory (PMO), a free troposphere site in the central North Atlantic, were classified by transport patterns using the Lagrangian particle dispersion model, FLEXPART. The classification enabled identifying trace gas mixing ratios associated with background air and long- range transport of continental emissions, which were defined as chemical signatures. Comparison between the chemical signatures revealed the impacts of natural and anthropogenic sources, as well as chemical and physical processes during long transport, on air composition in the remote North Atlantic. Transport of North American anthropogenic emissions (NA-Anthro) and summertime wildfire plumes (Fire) significantly enhanced CO and O 3 at PMO. Summertime CO enhancements caused by NA-Anthro were found to have been decreasing by a rate of 0.67 ± 0.60 ppbv/year in the ten-year period, due possibly to reduction of emissions in North America. Downward mixing from the upper troposphere and stratosphere due to the persistent Azores-Bermuda anticyclone causes enhanced O 3 and nitrogen oxides. The d [O 3 ]/d [CO] value was used to investigate O 3 sources and chemistry in different transport patterns. The transport pattern affected by Fire had the lowest d [O 3 ]/d [CO], which was likely due to intense CO production and depressed O 3 production in wildfire plumes. Slightly enhanced O 3 and d [O 3 ]/d [CO] were found in the background air, suggesting that weak downward mixing from the upper troposphere is common at PMO. Enhancements of both butane isomers were found during upslope flow periods, indicating contributions from local sources. The consistent ratio of butane isomers associated with the background air and NA-anthro implies no clear difference in the oxidation rates of the butane isomers during long transport. Based on observed relationships between non-methane hydrocarbons, the averaged photochemical age of the air masses at PMO was estimated to be 11 ± 4 days.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere

Abstract. Global observations and model studies indicate that new particle formation (NPF) in the upper troposphere (UT) and subsequent particles supply 40 %–60 % of cloud condensation nuclei (CCN) in the lower troposphere, thus affecting the Earth's radiative budget. There are several plausible nucleation mechanisms and precursor species in this atmospheric region, which, in the absence of observational constraints, lead to uncertainties in modeled aerosols. In particular, the type of nucleation mechanism and concentrations of nucleation precursors, in part, determine the spatial distribution of new particles and resulting spatial distribution of CCN from this source. Although substantial advances in understanding NPF have been made in recent years, NPF processes in the UT in pristine marine regions are still poorly understood and are inadequately represented in global models. Here, we evaluate commonly used and state-of-the-art NPF schemes in a Lagrangian box model to assess which schemes and precursor concentrations best reproduce detailed in situ observations. Using measurements of aerosol size distributions (0.003 < Dp < 4.8 µm) in the remote marine troposphere between ∼0.18 and 13 km altitude obtained during the NASA Atmospheric Tomography (ATom) mission, we show that high concentrations of newly formed particles in the tropical UT over both the Atlantic and Pacific oceans are associated with outflow regions of deep convective clouds. We focus analysis on observations over the remote Pacific Ocean, which is a region less perturbed by continental emissions than the Atlantic. Comparing aerosol size distribution measurements over the remote Pacific with box model simulations for 32 cases shows that none of the NPF schemes most commonly used in global models, including binary nucleation of sulfuric acid and water (neutral and ion-assisted) and ternary involving sulfuric acid, water, and ammonia, are consistent with observations, regardless of precursor concentrations. Through sensitivity studies, we find that the nucleation scheme among those tested that is able to explain most consistently (21 of 32 cases) the observed size distributions is that of Riccobono et al. (2014), which involves both organic species and sulfuric acid. The method of Dunne et al. (2016), involving charged sulfuric acid–water–ammonia nucleation, when coupled with organic growth of the nucleated particles, was most consistent with the observations for 5 of 32 cases. Similarly, the neutral sulfuric acid–water–ammonia method of Napari (2002), when scaled with a tuning factor and with organic growth added, was most consistent for 6 of 32 cases. We find that to best reproduce both nucleation and growth rates, the mixing ratios of gas-phase organic precursors generally need to be at least twice that of SO2, a proxy for dimethyl sulfide (DMS). Unfortunately, we have no information on the nature of oxidized organic species that participated in NPF in this region. Global models rarely include organic-driven nucleation and growth pathways in UT conditions where globally significant NPF takes place, which may result in poor estimates of NPF and CCN abundance and contribute to uncertainties in aerosol–cloud–radiation effects. Furthermore, our results indicate that the organic aerosol precursor vapors may be important in the tropical UT above marine regions, a finding that should guide future observational efforts.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Exploring the elevated water vapor signal associated with the free tropospheric biomass burning plume over the southeast Atlantic Ocean

In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the southeast Atlantic (SEA) Ocean, resulting in aerosol effects which vary with time and location. Much work has focused on the effects of these aerosol plumes, but previous studies have also described an elevated free tropospheric water vapor signal over the SEA. Water vapor influences climate in its own right, and it is especially important to consider atmospheric water vapor when quantifying aerosol-cloud interactions and aerosol radiative effects. Here we present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA Ocean. In observations collected from multiple independent instruments on the NASA P-3 aircraft (from near-surface to 6-7 km), we observe a strongly linear correlation between pollution indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. The focus of the current study is on the especially strong correlation observed during the ORACLES-2016 deployment (out of Walvis Bay, Namibia), but a similar relationship is also observed in the August 2017 and October 2018 ORACLES deployments. Using reanalyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and specialized WRF-Chem simulations, we trace the plume-vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper tropospheric air and then is subjected to conditions of strong westward advection, namely the southern African easterly jet (AEJ-S). Our analysis indicates that air masses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ~5-6 km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. Due to a combination of conditions and mixing between the smoky, moist continental boundary layer and the dry and fairly clean upper-troposphere air above (~6 km), the smoky, humid air is transported by strong zonal winds and then advected over the SEA (to the ORACLES flight region) following largely isentropic trajectories. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories support this interpretation. This work thus gives insights into the conditions and processes which cause water vapor to covary with plume strength. Better understanding of this relationship, including how it varies spatially and temporally, is important to accurately quantify direct, semi-direct, and indirect aerosol effects over this region.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1975

Stratospheric ozone - The possible effects of tropospheric-stratospheric feedback

The existence of tropospheric-stratospheric feedback mechanisms affecting variations in stratospheric ozone indicates the need to model the complete tropospheric-stratospheric system. For instance, a decrease in stratospheric ozone results in increased photolytic destruction of nitrous oxide in the troposphere and thereby reduced production of nitric oxide in the stratosphere. Estimates indicate that this mechanism will result in a recovery in atmospheric ozone of about 6 to 13 percent of the initial perturbation.

Chameides, W. L.↗
NASA NTRS1977

Effects of tropospheric and ionospheric refraction errors in the utilization of GEOS-C altimeter data

The effects of tropospheric and ionospheric refraction errors are analyzed for the GEOS-C altimeter project in terms of their resultant effects on C-band orbits and the altimeter measurement itself. Operational procedures using surface meteorological measurements at ground stations and monthly means for ocean surface conditions are assumed, with no corrections made for ionospheric effects. Effects on the orbit height due to tropospheric errors are approximately 15 cm for single pass short arcs (such as for calibration) and 10 cm for global orbits of one revolution. Orbit height errors due to neglect of the ionosphere have an amplitude of approximately 40 cm when the orbits are determined from C-band range data with predominantly daylight tracking. Altimeter measurement errors are approximately 10 cm due to residual tropospheric refraction correction errors. Ionospheric effects on the altimeter range measurement are also on the order of 10 cm during the GEOS-C launch and early operation period.

Goad, C. C.↗
NASA NTRS1976

Upper tropospheric dynamics as reflected in Nimbus 4 THIR 6.7-micron data

An investigation was conducted of the spatial and temporal relationships existing between the radiometrically observed water vapor patterns in cloud free areas and the conventionally derived water vapor patterns. The upper and middle tropospheric water vapor budget and the associated dynamics were examined to obtain a basis for a more definite evaluation of the significance of the Nimbus 4 radiometric 6.7-micrometer observations for the study of tropospheric dynamics in cloud free areas. A large-amplitude trough situated to the lee of the Rocky Mountains over the central U.S. between April 30 and May 1, 1970, was selected for the investigation because it best illustrated large upper tropospheric dynamic variations.

Rodgers, E. B.↗
NASA NTRS1979

Tropospheric effects on the middle atmosphere and vice-versa

The mechanisms by which phenomena occurring in the troposphere can affect that atmospheric region lying above the tropopause and below the mesopause are discussed as well as mechanisms by which middle atmospheric phenomena affect the tropospheric circulation, and how the middle atmosphere may act as a medium by which extraterrestrial effects may give rise to changes in tropospheric circulation. Energetics and external energy sources are considered. Aspects of vertical coupling examined include upward, downward, radiational, chemical, and electrical modes.

Geller, M. A.↗
NASA NTRS1979

Tropospheric limitations on the accuracy of phase measurement of coordinates in astronomy

The effect of tropospheric fluctuation on the accuracy of phase measurements of coordinates is discussed. The nature of the averaging of the tropospheric effects, if N coordinate measurements of duration T with period mu are made, is investigated. Various averaging modes depending on the relation of the various time parameters are investigated. Equations taking into account the correlations between individual observations are presented. It is shown that the correlation interval between the individual observations is always greater than the fluctuation period of tropospheric inhomogeneities typical for a given baseline.

Dravskikh, A. F.↗
NASA NTRS1978

Global atmospheric sampling program - Prospects for establishing a tropospheric ozone budget from commercial aircraft data

A preliminary analysis of zonally averaged, ozone concentration data obtained from commercial (GASP) aircraft between the equator and 60 deg North indicates that ozone in the upper troposphere exhibits a primary maximum during the spring, and, in middle latitudes, a secondary maximum in the summer of both 1975 and 1976. A late-fall/early-winter minimum also appears and seems consistent with previous upper air measurements. The April ozone maximum has been well documented and appears at the time when the stratospheric ozone content is greatest and cyclogenetic activity is most vigorous. However, the secondary maximum in June has not been widely observed or quoted as a unique feature. It is hypothesized that the rapid ascent of the tropopause between midspring and summer could account for the incorporation of ozone-rich, stratospheric air into the upper troposphere with a subsequent dilution during the following months. This may explain certain aspects of the annual ozone cycle in the lower troposphere which occasionally exhibit a bimodal distribution during the warm season.

Falconer, P. D.↗
NASA NTRS1979

Application of a microprocessor controlled lidar to tropospheric ozone measurements

A microprocessor controlled lidar system under construction at the NASA Goddard Space Flight Center is described and the problems in making space-based measurements of tropospheric ozone are considered. The differential absorption lidar using a dual wavelength, pulsed CO2 laser and direct detection receiver can significantly improve the existing global data base on tropospheric ozone burden. Sensitivity to tropospheric ozone can be obtained in the spaceborne version of lidar by selecting laser lines located in the wings of the target zone lines. Simulation studies using various laser line pairs in the P-branch of the CO2 9.4 micron band show that the ozone burden retrieval may be weighted to particular altitude regions. These simulation studies are based on numerical integration of differences in absorption coefficient at the two selected laser wavelengths using the AFGL absorption line parameter compilations, U.S. Standard Atmosphere ozone profile, and laser software. Simulation, data collection and reduction are performed by a microprocessor subsystem of the CO2 lidar.

Stewart, R. W.↗