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At least 325 records · Page 18

Influence of peroxyacetyl nitrate (PAN) on odd nitrogen in the troposphere and lower stratosphere

Nonmethane hydrocarbon breakdown in the atmosphere produces aldehydes of which a fraction are transferred into peroxyacetyl nitrates (PAN) in the presence of NO and NO2. Since ethane is destroyed photochemically primarily above 1 km, PAN can be introduced into the upper troposphere and lower stratosphere without the need to be transported from the boundary layer where most hydrocarbons are destroyed and where PAN may be lost due to thermal decomposition and heterogeneous loss. Mixing ratios of ethane in the lower troposphere increase by a factor of 4-8 from equatorial to northern mid-latitudes. This difference is directly translatable into a PAN latitude gradient. At mid-latitudes the concentration of PAN below 20 km is 0.1 ppb comparable to and in some instances larger than predicted HO2NO2 mixing ratios. Like HO2NO2 and HNO3, PAN serves as a reservoir for odd nitrogen.

Aikin, A. C.↗

Homogenized Water Vapor Absorption Band Radiances From International Geostationary Satellites

In the past 20+ years, GEO Imagers with infrared 6.5‐μm bands have been observing the Earth's atmosphere, providing useful information of upper tropospheric moisture. Due to the instrumental differences and local viewing angles in GEO satellites, these observations are not consistent for generating climate data records (CDRs). In this study, a methodology has been developed to homogenize the 6.5‐μm radiances from the international GEO satellites, to generate a consistent CDR. Validations with Infrared Atmospheric Sounding Interferometer radiances from Metops for 2015–2017for seven GEO Imager sensors show that the GEO radiances are homogenized well with small standard deviation and biases of the differences (smaller for newer sensors), temporally stable radiometric accuracy, and weak angle dependency (even weaker for sensors with two water vapor bands). The homogenized 20+ years of consistent 6.5‐μm radiance CDR can be used to evaluate reanalysis and climate models, especially the diurnal variation of the model simulation.

Water Vapor↗

Environmental Forcing of Super Typhoon Paka's (1997) Latent Heat Structure

The distribution and intensity of total (i.e., combined stratified and convective processes) rainrate/latent heat release (LHR) were derived for tropical cyclone Paka during the period 9-21 December, 1997 from the F-10, F-11, F-13, and F-14 Defense Meteorological Satellite Special Sensor Microwave/Imager and the Tropical Rain Measurement Mission Microwave Imager observations. These observations were frequent enough to capture three episodes of inner core convective bursts that preceded periods of rapid intensification and a convective rainband (CRB) cycle. During these periods of convective bursts, satellite sensors revealed that the rainrates/LHR: 1) increased within the inner eye wall region; 2) were mainly convectively generated (nearly a 65% contribution), 3) propagated inwards; 4) extended upwards within the middle and upper-troposphere, and 5) became electrically charged. These factors may have caused the eye wall region to become more buoyant within the middle and upper-troposphere, creating greater cyclonic angular momentum, and, thereby, warming the center and intensifying the system. Radiosonde measurements from Kwajalein Atoll and Guam, sea surface temperature observations, and the European Center for Medium Range Forecast analyses were used to examine the necessary and sufficient condition for initiating and maintaining these inner core convective bursts. For example, the necessary conditions such as the atmospheric thermodynamics (i.e., cold tropopause temperatures, moist troposphere, and warm SSTs [greater than 26 deg]) suggested that the atmosphere was ideal for Paka's maximum potential intensity (MPI) to approach super-typhoon strength. Further, Paka encountered weak vertical wind shear (less than 15 m/s ) before interacting with the westerlies on 21 December. The sufficient conditions, on the other hand, appeared to have some influence on Paka's convective burst, but the horizontal moisture flux convergence values in the outer core were weaker than some of the previously examined tropical cyclones. Also, the upper tropospheric outflow generation of eddy relative angular momentum flux convergence was 4D much less than that found during moderate tropical cyclone/trough interaction. These results indicated how important the external necessary condition and the internal forcing (i.e., CRB cycle) were in generating Paka's convective bursts as compared to the external sufficient forcing mechanisms found in higher latitude tropical cyclones. Later, as Paka began to interact with the westerlies, both the necessary (i.e., strong vertical shear and colder SSTs) and sufficient (i.e., dry air intrusion) external forcing mechanisms helped to decrease Paka's rainrate.

Rodgers, Edward B.↗

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↗

Titan's Emergence from Winter

We summarize the changes in Titans thermal structure derived from Cassini CIRS and radio-occultation data during the transition from winter to early spring. Titan's surface, and middle atmosphere show noticeable seasonal change, whereas that in most of the troposphere is mated. This can be understood in terms of the relatively small radiative relaxation time in the middle atmosphere and much larger time scale in the troposphere. The surface exhibits seasonal change because the heat capacity in an annual skin depth is much smaller than that in the lowest scale height of the troposphere. Surface temperatures rise 1 K at raid and high latitudes in the winter northern hemisphere and cool in the southern hemisphere. Changes in in the middle atmosphere are more complicated. Temperatures in the middle stratosphere (approximately 1 mbar) increase by a few kelvin at mid northern latitudes, but those at high latitudes first increase as that region moves out of winter shadow, and then decrease. This probably results from the combined effect of increased solar heating as the suit moves higher in the sky and the decreased adiabatic warming as the sinking motions associated with the cross-equatorial meridional cell weaken. Consistent with this interpretation, the warm temperatures observed higher up at the winter polar stratopause cool significantly.

Flasar, F. Michael↗

Spaceborne lidar system for measurements of atmospheric water vapor and aerosols

The inclusion of a differential absorption lidar (DIAL) system as part of the NASA Earth Observing System (EOS) is proposed. Functioning at 720 nm, the DIAL could provide atmospheric water vapor profiles in the troposphere and stratosphere, and provide data for characterizing the physical properties of clouds. The use of frequency doubling of the laser could also open a window on the 355 nm region, and thereby molecular density and temperature profiles. The date would be of use in studies of the global hydrological cycle, the global radiation balance, climate, meteorology, and atmospheric structure and transport phenomena.

Browell, E. V.↗

How Well do State-of-the-Art Techniques Measuring the Vertical Profile of Tropospheric Aerosol Extinction Compare?

The recent Department of Energy Atmospheric Radiation Measurement (ARM) Aerosol Intensive Operations Period (AIOP, May 2003) yielded one of the best measurement sets obtained to date to assess our ability to measure the vertical profile of ambient aerosol extinction sigma(ep)(lambda) in the lower troposphere. During one month, a heavily instrumented aircraft with well-characterized aerosol sampling ability carrying well-proven and new aerosol instrumentation devoted most of the 60 available flight hours to flying vertical profiles over the heavily instrumented ARM Southern Great Plains (SGP) Climate Research Facility (CRF). This allowed us to compare vertical extinction profiles obtained from six different instruments: airborne Sun photometer (AATS-14), airborne nephelometer/absorption photometer, airborne cavity ring-down system, groundbased Raman lidar, and two ground-based elastic backscatter lidars. We find the in situ measured sigma(ep)(lambda) to be lower than the AATS-14 derived values. Bias differences are 0.002-0.004 Km!1 equivalent to 13-17% in the visible, or 45% in the near-infrared. On the other hand, we find that with respect to AATS-14, the lidar sigma(ep)(lambda) are higher: Bias differences are 0.004 Km(-1) (13%) and 0.007 Km(-1) (24%) for the two elastic backscatter lidars (MPLNET and MPLARM, lambda = 523 nm) and 0.029 Km(-1) (54%) for the Raman lidar (lambda = 355 nm). An unnoticed loss of sensitivity of the Raman lidar had occurred leading up to AIOP, and we expect better agreement from the recently restored system. Looking at the collective results from six field campaigns conducted since 1996, airborne in situ measurements of sigma(ep)(lambda) tend to be biased slightly low (17% at visible wavelengths) when compared to airborne Sun photometer sigma(ep)(lambda). On the other hand, sigma(ep)(lambda) values derived from lidars tend to have no or positive biases. From the bias differences we conclude that the typical systematic error associated with measuring the tropospheric vertical profile of the ambient aerosol extinction with current state-of-the-art instrumentation is 15-20% at visible wavelengths and potentially larger in the UV and near-infrared.

Schmid, B.↗

The thermal structure of Triton's atmosphere - Pre-Voyager models

Spectral data from earth observations have indicated the presence of N2 and CH4 on Triton. This paper outlines the use of the 1-D radiative-convective model developed for Titan to calculate the current pressure of N2 and CH4 on Triton. The production of haze material is obtained by scaling down from the Titan value. Results and predictions for the Voyager Triton encounter are as follows: A N2-CH4 atmosphere on Triton is thermodynamically self consistent and would have a surface pressure of approximately 50 millibar; due to the chemically produced haze, Triton has a hot atmosphere with a temperature of approximately 130 K; Triton's troposphere is a region of saturation of the major constituent of the atmosphere, N2.

Mckay, Christopher P.↗

Retrieval of Aerosol Optical Depth Above Clouds from OMI Observations: Sensitivity Analysis, Case Studies

A large fraction of the atmospheric aerosol load reaching the free troposphere is frequently located above low clouds. Most commonly observed aerosols above clouds are carbonaceous particles generally associated with biomass burning and boreal forest fires, and mineral aerosols originated in arid and semi-arid regions and transported across large distances, often above clouds. Because these aerosols absorb solar radiation, their role in the radiative transfer balance of the earth atmosphere system is especially important. The generally negative (cooling) top of the atmosphere direct effect of absorbing aerosols, may turn into warming when the light-absorbing particles are located above clouds. The actual effect depends on the aerosol load and the single scattering albedo, and on the geometric cloud fraction. In spite of its potential significance, the role of aerosols above clouds is not adequately accounted for in the assessment of aerosol radiative forcing effects due to the lack of measurements. In this paper we discuss the basis of a simple technique that uses near-UV observations to simultaneously derive the optical depth of both the aerosol layer and the underlying cloud for overcast conditions. The two-parameter retrieval method described here makes use of the UV aerosol index and reflectance measurements at 388 nm. A detailed sensitivity analysis indicates that the measured radiances depend mainly on the aerosol absorption exponent and aerosol-cloud separation. The technique was applied to above-cloud aerosol events over the Southern Atlantic Ocean yielding realistic results as indicated by indirect evaluation methods. An error analysis indicates that for typical overcast cloudy conditions and aerosol loads, the aerosol optical depth can be retrieved with an accuracy of approximately 54% whereas the cloud optical depth can be derived within 17% of the true value.

Torres, O.↗

The tropospheric emission spectrometer (TES) for the Earth Observing System (EOS)

In recent years, increasing concern has been expressed about Global Change - the natural and anthropogenic alteration of the Earth's environment involving global greenhouse warming and the associated climate change, urban and regional atmospheric pollution, acid deposition, regional increases in tropospheric zone, and the decrease in stratospheric ozone. A common theme among these problems is that they all involve those tropospheric trace gases which are fundamental to the biosphere-troposphere interaction, the chemistry of the free troposphere itself, and troposphere-stratosphere exchange. The chemical species involved all have spectral signatures within the near and mid infrared that can now be measured by advanced techniques of remote-sensing infrared spectroradiometry. Such a system is the Tropospheric Emission Spectrometer (TES), now in Phase B definition for the Earth Observing System (EOS) polar platforms. TES addresses these objectives by obtaining radiometrically calibrated, linewidth-limited spectral resolution, infrared spectra of the lower atmosphere using both natural thermal emission and reflected sunlight (where appropriate) in three different, but fully programmable, modes: a gobal mode, a pointed mode, and a limb-viewing mode. The goals of TES, its instrumentation, operational modes, sensitivity and data handling are discussed.

Beer, R.↗

On the coupled nature of atmospheric phenomena

The interactions that take place in the stratosphere and the troposphere which are important to the maintenance of the chemical, dynamic, and thermal state and of the middle atmosphere, and which may be important in the determination of the state of the lower atmosphere are reviewed. Examples of these interactions due to either natural or anthropogenic processes are discussed, and promising areas for future research are indicated. Specific topics include: (1) coupling between temperature and chemistry via temperature dependent rate constants; (2) the effect of latitudinal temperature variations on zonal winds; (3) the effect of clouds, surface albedo, and the lower atmosphere on stratospheric chemistry due to the scattering and reflection of solar radiation; (4) the effect of trace constituents on thermal structure and thermal balance; (5) the effect of the stratosphere on tropospheric climate; (6) the effect of solar UV variability on stratospheric chemistry and temperature; and (7) the effect of trace constituents on stratospheric dynamics.

Callis, L. B.↗

Effect of aerosols on the estimation of total ozone in an atmospheric column from the measurements of its ultraviolet radiance

The problem of estimating the total ozone amount of an atmospheric column in the presence of stratospheric and tropospheric aerosols is studied by means of simulated spectral measurements for the five-wavelength Nimbus 4 BUV configuration and the six-wavelength Nimbus G TOMS configuration, and by analyzing such measurements with appropriate total ozone estimation procedures. The simulated spectral measurements were generated for forty different atmospheric models arrived at by varying the total ozone content and various aerosol parameters. A total of ten different values of the solar zenith angle and eight different values of the Lambert reflectivity of the underlying surface were used. It was found that the values of total ozone in an atmospheric column estimated by the five-wavelength procedure can be in error by about + or -2% as a result of particulate contamination encountered in the terrestrial atmosphere under average conditions. Errors due to tropospheric particulate contamination can be reduced significantly by taking appropriate advantage of the additional spectral measurement offered by the Nimbus G TOMS instrument.

Dave, J. V.↗

ACE-FTS Observation of a Young Biomass Burning Plume: First Reported Measurements of C2H4, C3H6O, H2CO and PAN by Infrared Occultation from Space

In the course of our study of the upper tropospheric composition with the infrared 35 Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE FTS), we 36 found an occultation sequence that on 8 October 2005, sampled a remarkable plume near the 37 east coast of Tanzania. Model simulations of the CO distribution in the Southern hemisphere 38 are performed for this period and they demonstrate that the emissions for this event originated 39 from a nearby forest fire, after which the plume was transported from the source region to the 40 upper troposphere. Taking advantage of the very high signal-to-noise ratio of the ACE FTS 41 spectra over a wide wavenumber range (750-4400 cm(exp -1), we present in-depth analyses of the 42 chemical composition of this plume in the middle and upper troposphere, focusing on the 43 measurements of weakly absorbing pollutants. For this specific biomass burning event, we 44 report simultaneous observations of an unprecedented number of organic species. 45 Measurements of C2H4 (ethene), C3H4 (propyne), H2CO (formaldehyde), C3H6O (acetone) 46 and CH3COO2NO2 (perxoxyacetylnitrate, abbreviated as PAN) are the first reported 47 detections using infrared occultation spectroscopy from satellites. Based on the lifetime of the 48 emitted species, we discuss the photochemical age of the plume and also report, whenever 49 possible, the enhancement ratios relative to CO.

Coheur, Pierre-Francois↗

Atmospheric water vapor measurements - Comparison of microwave radiometry and lidar

The NASA/GSFC Crustal Dynamics Project microwave water vapor radiometer (J03) is evaluated in terms of measurements of the integrated precipitable water vapor content of a particular column of the troposphere. The measurements were taken during the Atmospheric Moisture Intercomparison Study (ATMIS) held at Wallops Island (Virginia) during April 1989. Water vapor sensing instruments used during ATMIS, included radiometers, radiosondes, and the NASA/GSFC Raman lidar. Comparisons between water vapor measurements by the radiometer and the lidar yielded a correlation coefficient of 0.998 and rms differences for three nights of -0.2 +/- 0.2 mm (April 11-12), -0.8 +/- 0.5 mm (April 16-17), and -0.4 +/- 0.3 mm (April 17-18). The integrated precipitable water vapor measurements for these three nights were approximately 5, 10 and 21 mm, respectively. This study shows that the radiometer provides accurate continuous measurements of the water vapor integrated through the depth of the atmosphere.

England, Martin N.↗

Climatic consequences of observed ozone loss in the 1980s: Relevance to the greenhouse problem

Recently published findings using satellite and ground-based observations indicate a large winter and summertime decrease in the column abundance of ozone at high and middle latitudes during the last decade. Using a simple ozone depletion profile reflecting the observed decrease in ozone column abundance, Ramaswamy et al. (1992) showed that the negative radiative forcing that results from the ozone decrease between 1979 and 1990 approximately balanced the greenhouse climate forcing due to the chlorofluorocarbons emitted during the same period. Here, we extend the forcing analyses by calculating the equilibrium surface temperature response explicitly, using an updated version of the Atmospheric and Environmental Research two-dimensional radiative-dynamical seasonal model. The calculated steady state responses suggest that the surface cooling due to the ozone depletion in the lower stratosphere offsets about 30% of the surface warming due to greenhouse gases emitted during the same decade. The temperature offset is roughly a factor of 2 larger than the corresponding offset obtained from forcing intercomparisons. This result appears to be related to the climate feedback mechanisms operating in the model troposphere, most notably that associated with atmospheric meridional heat transport. Thus a comprehensive assessment of ozone change effects on the predicted greenhouse warming cannot be accomplished based on forcing evaluations alone. Our results also show that calculations adopting a seasonally and latitudinally dependent ozone depletion profile produce a negative forcing about 50% smaller than that calculated for the depletion profile used by Ramaswamy et al. (1992).

Molnar, G. I.↗

On possible interactions between upper and lower atmosphere

Comparison of geomagnetic data with data on tropospheric and stratospheric circulation characteristics shows a statistically highly significant shrinking in areal extent of the stratospheric vortex from the third to the eight day following a geomagnetic storm. During the contraction of the polar vortex edge, the mean height of the vortex central contour decreases only slightly. This indicates that a stratospheric warming event is associated with a steepening of the contour gradient rather than a warming over the entire area of the stratospheric polar vortex. The troposphere reacts to these weak, but nevertheless significant stratospheric warming events by a shrinkage of the area of the 500-mb cold air pool. It is shown that the observed warming of the stratosphere that follows a geomagnetically disturbed key day cannot be explained by simple radiation absorption.

Macdonald, B. C.↗

On possible interactions between upper and lower atmosphere

Geomagnetic data was compared with data on tropospheric and stratospheric circulation characteristics; a statistically significant shrinking was found in areal extent of the stratospheric vortex from the third to the eighth day following a 'geomagnetic storm' The meridionality of the 30 640-m contour line at 10 millibars increases markedly from 5 to 8 days after the storm. During the contraction of the polar vortex edge, the mean height of the vortex central contour decreases only slightly. This indicates that a stratospheric warming event is associated with a steepening of the contour gradient rather than a warming over the entire area of the stratospheric polar vortex. The troposphere reacts to these weak, but significant, stratospheric warming events by a shrinkage of the area of the 500-millibar cold air pool. This shrinkage commences about 3 days after the stratospheric warming. The investigation indicates that the energy input into the stratosphere that is received in conjunction with the geomagnetic disturbance has to come at a propitious time, when the stratospheric-tropospheric circulation system is not already undergoing a major readjustment because of an inherent dynamic instability.

Macdonald, B. C.↗

Tropospheric trace gases

Trace gas concentrations in the atmosphere reflect in part the overall metabolism of the biosphere, and in part the broad range of human activities such as agriculture, production of industrial chemicals, and combustion of fossil fuels and biomass. There is compelling evidence that the composition of the atmosphere is now changing. Observed trends in trace gas levels are reviewed and implications for the chemistry of the atmosphere are discussed. Throughout the discussion, particular emphasis is given to those species which are now increasing in the atmosphere.

Gammon, R.↗