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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume

Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m -3 . On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Open cells exhibit weaker entrainment of free-tropospheric biomass burning aerosol into the south-east Atlantic boundary layer

This work presents synergistic satellite, airborne and surface-based observations of a pocket of open cells (POC) in the remote south-east Atlantic. The observations were obtained over and upwind of Ascension Island during the CLouds and Aerosol Radiative Impacts and Forcing (CLARIFY) and the Layered Smoke Interacting with Clouds (LASIC) field experiments. A novel aspect of this case study is that an extensive free-tropospheric biomass burning aerosol plume that had been transported from the African continent was observed to be in contact with the boundary layer inversion over the POC and the surrounding closed cellular cloud regime. The in situ measurements show marked contrasts in the boundary layer thermodynamic structure, cloud properties, precipitation and aerosol conditions between the open cells and surrounding overcast cloud field. The data demonstrate that the overlying biomass burning aerosol was mixing down into the boundary layer in the stratocumulus cloud downwind of the POC, with elevated carbon monoxide, black carbon mass loadings and accumulation-mode aerosol concentrations measured beneath the trade-wind inversion. The stratocumulus cloud in this region was moderately polluted and exhibited very little precipitation falling below cloud base. A rapid transition to actively precipitating cumulus clouds and detrained stratiform remnants in the form of thin quiescent veil clouds was observed across the boundary into and deep within the POC. The subcloud layer in the POC was much cleaner than that in the stratocumulus region. The clouds in the POC formed within an ultra-clean layer (accumulation-mode aerosol concentrations of approximately a few cm -3 ) in the upper region of the boundary layer, which was likely to have been formed via efficient collision–coalescence and sedimentation processes. Enhanced Aitken-mode aerosol concentrations were also observed intermittently in this ultra-clean layer, suggesting that new particle formation was taking place. Across the boundary layer inversion and immediately above the ultra-clean layer, accumulation-mode aerosol concentrations were ~1000 cm -3 . Importantly, the air mass in the POC showed no evidence of elevated carbon monoxide over and above typical background conditions at this location and time of year. As carbon monoxide is a good tracer for biomass burning aerosol that is not readily removed by cloud processing and precipitation, it demonstrates that the open cellular convection in the POC is not able to entrain large quantities of the free-tropospheric aerosol that was sitting directly on top of the boundary layer inversion. This suggests that the structure of the mesoscale cellular convection may play an important role in regulating the transport of aerosol from the free troposphere down into the marine boundary layer. We then develop a climatology of open cellular cloud conditions in the south-east Atlantic from 19 years of September Moderate Resolution Imaging Spectroradiometer (MODIS) Terra imagery. This shows that the maxima in open cell frequency (> 0.25) occurs far offshore and in a region where subsiding biomass burning aerosol plumes may often come into contact with the underlying boundary layer cloud. If the results from the observational case study applied more broadly, then the apparent low susceptibility of open cells to free-tropospheric intrusions of additional cloud condensation nuclei could have some important consequences for aerosol–cloud interactions in the region.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Characterization of organic aerosol across the global remote troposphere: a comparison of ATom measurements and global chemistry models

The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 µg sm -3 ). Lower concentrations (~0.1–0.3 µg sm -3 ) are observed in the northern middle and high latitudes and very low concentrations (<0.1 µg sm -3 ) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the secondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA/OC) ratios of ~2.2–2.8, and is 30 %–60 % more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model–measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1977

Tropospheric ozone - Coupling transport and photochemistry

The budget of tropospheric ozone is re-examined in the light of lower observed nitrogen oxide densities and revised reaction rates. To estimate the relative importance of transport and photochemistry, model calculations are presented which determine one-dimensional vertical ozone profiles at midlatitudes for equinoctial conditions. These calculations imply that both photochemistry and transport are important in controlling the abundance of tropospheric ozone. It is estimated that photochemical processes produce about 0.6 times 10 to the eleventh and destroy about 1.4 times 10 to the eleventh tropospheric ozone molecules per sq cm per sec, while mixing processes transport about 1.4 times 10 to the eleventh ozone molecules per sq cm per sec from the stratosphere into the troposphere and ground level fluxes destroy about 0.6 times 10 to the eleventh ozone molecules per sq cm per sec. The sensitivity of our model calculations to transport parameters, key rate coefficients, and nitrogen oxide densities are discussed.

Chameides, W. L.↗
NASA NTRS1978

The origin of ozone in the troposphere

Examination of the distribution of tropospheric ozone indicates that surface destruction in the Northern Hemisphere (NH) should be about three times larger than in the Southern Hemisphere (SH). If, according to the traditional understanding of ozone, this species were a passive tracer in the troposphere, a threefold larger flux out of the stratosphere should exist in the NH than in the SH. However, meteorological analyses fail to support such pronounced hemispheric differences in stratosphere-troposphere exchange. Alternatively, therefore, it is hypothesized that photochemical synthesis of ozone in the troposphere may be particularly important in the NH because of asymmetries in the sources and distribution of carbon monoxide, hydrocarbons and nitric oxide.

Fishman, J.↗
NASA NTRS1980

Planetary wave coupling between the troposphere and the middle atmosphere as a possible sun-weather mechanism

The possibility of planetary wave coupling between the troposphere and solar-induced alterations in the upper atmosphere providing a viable mechanism for giving rise to sun-weather relationships is investigated. Some of the observational evidence for solar-activity-induced effects on levels of the upper atmosphere ranging from the thermosphere down to the lower stratosphere are reviewed. It is concluded that there is evidence for such effects extending down to the middle stratosphere and below. Evidence is also reviewed that these effects are due to changes in solar ultraviolet emission during disturbed solar conditions. A theoretical planetary wave model is then used to see at what levels in the upper atmosphere moderate changes in the mean zonal wind state would result in tropospheric changes. It is concluded that changes in the mean zonal flow of about 20% at levels in the vicinity of 35 km or below would give rise to changes in the tropospheric planetary wave pattern that are less than but on the same order as the observed interannual variability in the tropospheric wave pattern at middle and high latitudes.

Geller, M. A.↗
NASA NTRS1981

Effects of multiple scattering and surface albedo on the photochemistry of the troposphere

The effect of treatment of incoming solar radiation on the photochemistry of the troposphere is discussed. A one dimensional photochemical model of the troposphere containing the species of the nitrogen, oxygen, carbon, hydrogen, and sulfur families was developed. The vertical flux is simulated by use of the parameterized eddy diffusion coefficients. The photochemical model is coupled to a radiative transfer model that calculates the radiation field due to the incoming solar radiation which initiates much of the photochemistry of the troposphere. Vertical profiles of tropospheric species were compared with the Leighton approximation, radiative transfer, matrix inversion model. The radiative transfer code includes the effects of multiple scattering due to molecules and aerosols, pure absorption, and surface albedo on the transfer of incoming solar radiation. It is indicated that significant differences exist for several key photolysis frequencies and species number density profiles between the Leighton approximation and the profiles generated with, radiative transfer, matrix inversion technique. Most species show enhanced vertical profiles when the more realistic treatment of the incoming solar radiation field is included

Augustsson, T. R.↗
NASA NTRS1982

Applying modeling Results in designing a global tropospheric experiment

A set of field experiments and advanced modeling studies which provide a strategy for a program of global tropospheric experiments was identified. An expanded effort to develop space applications for trospheric air quality monitoring and studies was recommended. The tropospheric ozone, carbon, nitrogen, and sulfur cycles are addressed. Stratospheric-tropospheric exchange is discussed. Fast photochemical processes in the free troposphere are considered.

Source record↗
NASA NTRS1982

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.↗
NASA NTRS1982

The possible role of heterogeneous aerosol processes in the chemistry of CH4 and CO in the troposphere

The effect of particle-gas interactions on the CH4 to CO oxidation sequence in the troposphere is investigated by developing rate expressions for the heterogeneous removal of gaseous species based on the absorption of the species by aerosol particles. The results of this analysis indicate that the homogeneous models describe the tropospheric chemistry of CO and CH4 more accurately than heterogeneous models, which suggests that heterogeneous processes may not be significant in this sequence of chemical reactions. Estimates of the CO and CH4 emission rates are not found to provide a conclusive basis on which to compare the significance of the homogeneous and heterogeneous processes. In addition, the time period during which an aerosol particle is effective in removing a trace gaseous species from the troposphere is determined to vary according to the tropospheric concentration and solubility of the particular gaseous species.

Luther, C. J.↗
NASA NTRS1983

On the maintenance of the Marine boundary layer-free tropospheric gradient of transient tracers

A simple model of the marine boundary layer is used to arrive at a steady-state budget for trace gases in this layer. Five processes maintain the tracer balance in the layer. The first is a large-scale horizontal convergence of the tracer; the second is the pumping by clouds of the tracer out of the boundary layer into the free troposphere; the third is penetration by the tracer from the free troposphere into the marine boundary from compensating subsidence in the cloud-free air surrounding cumulus clouds; the fourth is sea surface emission or deposition of the tracer; and the fifth is in situ photochemical production or loss of the tracer within the marine boundary layer. The budget equation is used in deriving an expression for the mixing ratio difference between the two regions. A scale analysis suggests that the mixing ratio difference between the marine boundary layer and the free troposphere can be an order of magnitude smaller in disturbed weather conditions than in suppressed conditions, showing that the difference in chemical concentrations between the free troposphere and the marine boundary layer cannot be rationalized solely on the basis of chemical measurements.

Gidel, L. T.↗
NASA NTRS1984

Global tropospheric chemistry: A plan for action

Prompted by an increasing awareness of the influence of human activity on the chemistry of the global troposphere, a panel was formed to (1) assess the requirement for a global study of the chemistry of the troposphere; (2) develop a scientific strategy for a comprehensive plan taking into account the existing and projected programs of the government; (3) assess the requirements of a global study in terms of theoretical knowledge, numerical modeling, instrumentation, observing platforms, ground-level observational techniques, and other related needs; and (4) outline the appropriate sequence and coordination required to achieve the most effective utilization of available resources. Part 1 presents a coordinated national blueprint for scientific investigations of biogeochemical cycles in the global troposphere. part 2 presents much of the background information of the present knowledge and gaps in the understanding of tropospheric chemical cycles and processes from which the proposed program was developed.

Source record↗
NASA NTRS1985

The reservoir of ozone in the boundary layer of the eastern United States and its potential impact on the global tropospheric ozone budget

An analysis of available ozone data in the eastern two-thirds of the United States indicates that a substantial reservoir of ozone is present in the summertime. Five-year mean concentrations range from 40 to 65 ppbv. The reservoir covered an area of several million square kilometers and extends vertically from the surface to 1 to 2 km. The vertical distribution of ozone in the reservoir during midday supports a transport of additional ozone from the boundary layer to the free troposphere. Data are presented demonstrating the potential effect of transport by convective clouds and by the sea breeze circulation - mechanisms by which ozone may be transported out of the boundary layer into the free troposphere. The potential impact of this reservoir on the tropospheric ozone budget is discussed. It is shown that if less than half of the ozone mass in this reservoir is transported to the free troposphere, then the amount of ozone transported out of the boundary layer approximates the amount of ozone transported downward during a tropopause fold event.

Vukovich, F. M.↗
NASA NTRS1985

The photochemistry of methane and carbon monoxide in the troposphere in 1950 and 1985

The roughly 1 percent/year increase in tropospheric methane and roughly 2 percent/year increase in tropospheric carbon monoxide deduced from recent analyses of ground-based solar infrared spectra recorded in 1950 and 1951 have very important implications for the photochemistry and chemistry of the troposphere. Photochemical calculations indicate that as a result of the increase of methane and carbon monoxide since 1950-51, levels of the hydroxyl radical, the key species in the photochemistry of the troposphere, may have decreased by about 25 percent.

Levine, J. S.↗
NASA NTRS1986

Space opportunities for tropospheric chemistry research

The use of the Space Shuttle to measure tropospheric trace species is examined. Factors which affect the measurement of tropospheric trace species are discussed. The Academy of Sciences 1985 report categorized the trace species into levels: first-level gases include water vapor, O3, CO, and CH4, and the second-level gases are N2O, NO2, NH3, SO2, chlorofluoromethanes, and HCl. The effects of first-level gases on the earth's climate, the photochemistry/chemistry of the troposphere, and the photochemical/chemical production and destruction of the hydroxyl radical are studied; the distribution and magnitude of the hydroxyl radical in the troposphere are analyzed in terms of water vapor, O3, CO, and CH4.

Levine, Joel S.↗
NASA NTRS1986

Nonmethane hydrocarbons in the troposphere - Impact on the odd hydrogen and odd nitrogen chemistry

A one-dimensional model is utilized to study the role of nonmethane hydrocarbons (NMHCs) in tropospheric chemistry. The effects of NMHCs on tropospheric peroxyacetyl nitrate (PAN) formation are analyzed; the global distribution and seasonal variability of PAN in the troposphere of the Northern and Southern Hemispheres are examined. The NMHC-PAN measurements obtained by model simulations are compared to the photochemical theory. The seasonal cycles in NMHC abundances are predicted, and their effects on other tropospheric species are investigated.

Kasting, James F.↗
NASA NTRS1988

Chlorine-hydrocarbon photochemistry in the marine troposphere and lower stratosphere

The role of chlorine atoms in the oxidation of methane and nonmethane hydrocarbons (NMHCs) in the marine troposphere and lower stratosphere was investigated using a one-dimensional photochemical model that incorporated the chemistry of CH4, NMHCs, NO(x), O(x), and HO(x), as well as organic and inorganic halogens in the troposphere and lower stratosphere. The model predicted that chlorine atoms are present in the marine troposphere at the concentrations of about 1000/cu cm, mostly as a product of the reaction between OH and HCl released from sea spray. The results indicate that Cl atoms cause 20 to 40 percent of NMHC oxidation in the troposphere and 40 to 90 percent in the lower stratosphere. At 15 km, the NMHC-Cl reactions account for nearly 80 percent of the PAN produced. Where available, experimental data confirmed the model predictions.

Singh, H. B.↗
NASA NTRS1989

On the transfer of stratospheric ozone into the troposphere near the North Pole

A series of nearly daily ozone vertical profiles obtained at station T-3 on Fletcher's Ice Island (about 85 deg N, about 90 deg W) during the period January-March 1971 shows several significant ozone intrusions into the troposphere. These intrusions are not only associated with enhanced ozone amounts in the stratosphere but also require tropopause folding events to transport ozone into the troposphere. These folds in the arctic tropopause appear to be capable of contributing significantly to the ozone budget of the arctic troposphere during the late winter and spring seasons. The importance of tropopause folding for bringing ozone into the troposphere seen in the daily ozone profiles confirms the results found in the Arctic Gas and Aerosol Sampling Program aircraft flights.

Oltmans, Samuel J.↗