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At least 559 records · Page 31

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual model, where production of new aerosol particles takes place in the continental UT from biogenic volatile organic material brought up by deep convection and converted to condensable species in the UT. Subsequently, downward mixing and transport of upper tropospheric aerosol can be a source of particles to the PBL, where they increase in size by the condensation of biogenic volatile organic compound (BVOC) oxidation products. This may be an important source of aerosol particles for the Amazonian PBL, where aerosol nucleation and new particle formation have not been observed. We propose that this may have been the dominant process supplying secondary aerosol particles in the pristine atmosphere, making clouds the dominant control of both removal and production of atmospheric particles.

54 ENVIRONMENTAL SCIENCES↗

Heterogeneous oxidation of amorphous organic aerosol surrogates by O 3 , NO 3 , and OH at typical tropospheric temperatures

Typical tropospheric temperatures render possible phase states of amorphous organic aerosol (OA) particles of solid, semisolid, and liquid. This will affect the multiphase oxidation kinetics involving the organic condensed-phase and gaseous oxidants and radicals. To quantify this effect, we determined the reactive uptake coefficients (γ) of O 3 , NO 3 , and OH by substrate films composed of single and binary OA surrogate species under dry conditions for temperatures from 213 to 313 K. A temperature-controlled coated-wall flow reactor coupled to a chemical ionization mass spectrometer was applied to determine γ with consideration of gas diffusion transport limitation and gas flow entrance effects, which can impact heterogeneous reaction kinetics. The phase state of the organic substrates was probed via the poke-flow technique, allowing the estimation of the substrates' glass transition temperatures. γ values for O 3 and OH uptake to a canola oil substrate, NO 3 uptake to a levoglucosan and a levoglucosan / xylitol substrate, and OH uptake to a glucose and glucose / 1,2,6-hexanetriol substrate have been determined as a function of temperature. We observed the greatest changes in γ with temperature for substrates that experienced the largest changes in viscosity as a result of a solid-to-liquid phase transition. Organic substrates that maintain a semisolid or solid phase state and as such a relatively higher viscosity do not display large variations in heterogeneous reactivity. From 213 to 293 K, γ values of O 3 with canola oil, of NO 3 with a levoglucosan / xylitol mixture, and of OH with a glucose / 1,2,6-hexanetriol mixture and canola oil, increase by about a factor of 34, 3, 2, and 5, respectively, due to a solid-to-liquid phase transition of the substrate. These results demonstrate that the surface and bulk lifetime of the OA surrogate species can significantly increase due to the slowed heterogeneous kinetics when OA species are solid or highly viscous in the middle and upper troposphere. This experimental study will further our understanding of the chemical evolution of OA particles with subsequent important consequences for source apportionment, air quality, and climate.

54 ENVIRONMENTAL SCIENCES↗

Tropospheric and stratospheric wildfire smoke profiling with lidar: mass, surface area, CCN, and INP retrieval

We present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area, and number concentrations in the case of wildfire smoke layers as well as estimates of smoke-related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations from backscatter lidar measurements on the ground and in space. Conversion factors used to convert the optical measurements into microphysical properties play a central role in the data analysis, in addition to estimates of the smoke extinction-to-backscatter ratios required to obtain smoke extinction coefficients. The set of needed conversion parameters for wildfire smoke is derived from AERONET observations of major smoke events, e.g., in western Canada in August 2017, California in September 2020, and southeastern Australia in January–February 2020 as well as from AERONET long-term observations of smoke in the Amazon region, southern Africa, and Southeast Asia. The new smoke analysis scheme is applied to CALIPSO observations of tropospheric smoke plumes over the United States in September 2020 and to ground-based lidar observation in Punta Arenas, in southern Chile, in aged Australian smoke layers in the stratosphere in January 2020. These case studies show the potential of spaceborne and ground-based lidars to document large-scale and long-lasting wildfire smoke events in detail and thus to provide valuable information for climate, cloud, and air chemistry modeling efforts performed to investigate the role of wildfire smoke in the atmospheric system.

54 ENVIRONMENTAL SCIENCES↗

High-resolution mapping of nitrogen oxide emissions in large US cities from TROPOMI retrievals of tropospheric nitrogen dioxide columns

Satellite-derived spatiotemporal patterns of nitrogen oxide (NOx) emissions can improve accuracy of emission inventories to better support air quality and climate research and policy studies. In this study, we develop a new method by coupling the chemical transport Model-Independent SATellite-derived Emission estimation Algorithm for Mixed-sources (MISATEAM) with a divergence method to map high-resolution NO x emissions across US cities using TROPOspheric Monitoring Instrument (TROPOMI) tropospheric nitrogen dioxide (NO 2 ) retrievals. The accuracy of the coupled method is validated through application to synthetic NO 2 observations from the NASA-Unified Weather Research and Forecasting (NU-WRF) model, with a horizontal spatial resolution of 4 km × 4 km for 33 large and mid-size US cities. Validation reveals excellent agreement between inferred and NU-WRF-provided emission magnitudes (R= 0.99, normalized mean bias, NMB = —0.01) and a consistent spatial pattern when comparing emissions for individual grid cells (R = 0.88 ± 0.06). We then develop a TROPOMI-based database reporting annual emissions for 39 US cities at a horizontal spatial resolution of 0.05° × 0.05° from 2018 to 2021. This database demonstrates a strong correlation (R= 0.90) with the National Emission Inventory (NEI) but reveals some bias (NMB = —0.24). There are noticeable differences in the spatial patterns of emissions in some cities. Our analysis suggests that uncertainties in TROPOMI-based emissions and potential misallocation of emissions and/or missing sources in bottom-up emission inventories both contribute to these differences.

54 ENVIRONMENTAL SCIENCES↗

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

In order to determine if a quantifiable relationship exists between the 6.7 micron radiometric patterns observed by the Nimbus-4 temperature-humidity infrared radiometer (THIR) and tropospheric dynamics, a 10-level diagnostic model is employed. The model is used to show the spatial and temporal relationships existing between radiometrically observed water vapor patterns and conventionally derived water vapor patterns, and to examine the upper and middle tropospheric water vapor budget and associated dynamics in order to assess the causes behind the spatially- and temporally-varying water vapor radiometric patterns. A particular situation involving a confluent trough located to the lee of the Rockies over the Central United States is examined.

Rodgers, E. B.↗

The tropospheric calibration model for Mariner Mars 1971

The effects of the troposphere on arrival time, range, and range rate measurement of radio signals propagating from spacecraft are examined. A tropospheric calibration model which takes into account seasonal variations, various elevations, and apparent location changes was developed. A comparison was made of the effects before and after calibration. Without calibration, a 16-m change in the distance off the spin axis, is induced for a 10-deg minimum elevation symmetrical pass. Even after calibration with the old model, the error in spin axis is still greater than 1 m. Calibration results and estimated uncertainties of the model are given in tabular form. Test results also show that the model met the required accuracy for the Mariner Mars 1971 mission.

C. C. Chao↗

A comparison of the structure and flow characteristics of the upper troposphere and stratosphere of the Northern and Southern Hemispheres

The general circulations of the Northern and Southern Hemispheres are compared with regard to the upper troposphere and stratosphere using atmospheric structure obtained from satellite, multi-channel radiance data. Specifically, the data are from the Satellite Infrared Spectrometer (SIRS) instrument aboard the Nimbus 3 spacecraft. The inter-hemispheric comparisons are based on two months of data (one summer month and one winter month) in each hemisphere. Topics studied include: mean meridional circulation in the Southern Hemisphere stratosphere; magnitude and distribution of tropospheric eddy heat flux; magnitudes of energy cycle components; and the relation of vortex structure to the breakdown climatology of the Antarctic stratospheric polar vortex.

Adler, R. F.↗

Interhemispheric comparison of atmospheric circulation features as evaluated from Nimbus satellite data. A comparison of the structure and flow characteristics of the upper troposphere and stratosphere of the Northern and Southern Hemispheres

The general circulations of the Northern and Southern Hemispheres are compared with regard to the upper troposphere and stratosphere, using atmospheric structure obtained from multi-channel radiance data from the satellite infrared spectrometer instrument aboard the Nimbus 3 spacecraft. The inter-hemispheric comparisons are based on two months of data (one summer month and one winter month) in each hemisphere. Topics studied include: (1) mean meridional circulation in the Southern Hemisphere stratosphere; (2) magnitude and distribution of tropospheric eddy heat flux; (3) relative importance of standing and transient eddies in the two hemispheres; (4) magnitudes of energy cycle components; and (5) the relation of vortex structure to the breakdown climatology of the Antarctic stratospheric polar vortex.

Reiter, E. R.↗

The production of nitric oxide in the troposphere as a result of solid-rocket-motor afterburning

As part of an ongoing assessment of the environmental effects of solid-rocket-motor operations in the troposphere, estimates were made of the nitric oxide produced in the troposphere by the space shuttle and Titan 3-C boosters. Calculations were made with the low-altitude plume computer program and included the effects of coupled finite-rate chemistry and turbulent mixing. A recent measurement of nitric oxide taken in the effluent cloud of a Titan 3-C booster is compared with calculations made with this computer code. The various chemical reactions of the exhaust gases are listed in tabular form.

Stewart, R. B.↗

The influence of the diabatic heating in the troposphere on the stratosphere

In order to simulate the seasonal variation of the stratospheric circulation in a zonal mean circulation model, a Newtonian heating function and a detailed heating function were applied to the troposphere and stratosphere, respectively. The purpose of this study was to investigate the response of stratospheric circulation to alterations of the radiative equilibrium temperature of the troposphere.

Turner, R. E.↗

Photochemistry of tropospheric ozone

A photochemical equilibrium model of minor constituent chemistry in the troposphere was constructed to investigate the photochemistry of tropospheric ozone. We find that photochemical production must be supplemented by additional sources to account for observed ozone levels in clean air, while photochemical loss is more important than surface destruction as an ozone loss mechanism. Photochemically produced ozone is sensitive to the NO(x) background in the model, exhibiting a maximum of about 0.5 ppb of NO(x).

Stewart, R. W.↗

Measurement of tropospheric 300 nm solar ultraviolet flux for determination of O/1D/ photoproduction rate

The tropospheric importance of the OH radical, and the reaction scheme that leads to its formation, are now being widely investigated. Ozone photolysis at wavelengths no greater than 318 nm produces O(1D), a small fraction of which then reacts with water vapor to yield OH. Although experimental data are available for the O(1D) quantum yield, as well as the O3 absorption cross section, all previous tropospheric photochemical models have had to use theoretical calculations to determine the UV flux. Discussed in this paper are aircraft spectral measurements of the solar UV flux at two altitudes - 2 and 6 km. These results have been compared with three theoretical approaches. The measured experimental fluxes have been combined here with recent quantum yield data to calculate the O(1D) photoproduction rate for various albedo values. This rate is larger than that used in models by about a factor of 2 for reasonable values of assumed albedo.

Sellers, B.↗

Tropospheric ozone distributions measured with an airborne laser absorption spectrometer

Measurements of tropospheric ozone have been made in the southern and middle California regions and over the Pacific Ocean during two series of flights in February and May 1977. The data were obtained by using a laser absorption spectrometer, a nadir-viewing instrument which remotely measures the ozone column abundance between ground level and aircraft altitude by interacting with ozone at specific wavelengths near 9.5 microns. The measurements indicate significantly lower ozone abundances above the Mojave Desert region as compared with farm, forest, and urban areas. The average tropospheric column density was found to be 0.0027 atm cm/km over the California region and 0.0035 atm cm/km over the Pacific Ocean region 1000-2000 km west of the coast of Mexico.

Menzies, R. T.↗

The effect of anthropogenic carbon monoxide on the methane budget of the troposphere

Photochemical model calculations indicate that significant perturbations in tropospheric OH, CH4, and related compounds may occur in the coming decades due to increased anthropogenic emissions of CO and NO(x). The magnitude and direction of the perturbation depends on future emission rates of CO and NO(x) and also on the efficiency with which urban NO(x) is transported to the ambient atmosphere. If CO and NO(x) emissions increase at comparable rates, the CO effect on OH will dominate and OH will decrease while CH4 increases. The effects of a variation in tropospheric OH, halocarbons, and other compounds include a perturbation to stratospheric ozone and the atmosphere's thermal equilibrium.

Chameides, W. L.↗

Tropospheric ozone

Photochemical equilibrium models have been used to study the effect of recent revisions in important chemical reaction rates on the calculated tropospheric ozone concentration. Reasonable agreement with observed values is obtained if the NO(x) background is approximately 0.02 to 0.03 ppb, about an order of magnitude less than used in many previous model studies, but consistent with present nitrogen budget considerations and with observations of NO2. Chemical production and loss of ozone may dominate transport terms depending on values of key chemical rate constants and of the NO(x) background. This is consistent with the structure observed in the mean annual latitudinal distribution of ozone since ozone is its own chemical precursor and regions of enhanced stratosphere-troposphere exchange are also regions of enhanced photochemical activity.

Stewart, R. W.↗

Effect of tropospheric aerosols upon atmospheric infrared cooling rates

The effect of tropospheric aerosols on atmospheric infrared cooling rates is investigated by the use of recent models of infrared gaseous absorption. A radiative model of the atmosphere that incorporates dust as an absorber and scatterer of infrared radiation is constructed by employing the exponential kernel approximation to the radiative transfer equation. Scattering effects are represented in terms of a single scattering albedo and an asymmetry factor. The model is applied to estimate the effect of an aerosol layer made of spherical quartz particles on the infrared cooling rate. Calculations performed for a reference wavelength of 0.55 microns show an increased greenhouse effect, where the net upward flux at the surface is reduced by 10% owing to the strongly enhanced downward emission. There is a substantial increase in the cooling rate near the surface, but the mean cooling rate throughout the lower troposphere was only 10%.

Harshvardhan, MR.↗

Optimum frequencies of passive microwave radiometer for tropospheric path-length correction

Radio-astronomical observations require accurate calibration of tropospheric path length. Such calibration can be achieved by microwave radiometers operating near the 22-GHz water vapor line. However, the performances of current passive microwave radiometers are meteorology-profile dependent. This is due mainly to incorrect frequency combinations and to saturation of brightness temperatures. By properly selecting an optimum frequency pair and removing the saturation effect, the dependency is alleviated and can be further adjusted by surface measurements alone. Hence, a universal calibration equation is applicable to all environmental conditions. Optimum frequency pairs are systematically searched. Simulation analysis indicates that calibration for the tropospheric water-vapor path-length error is better than 0.3 cm at zenith and better than 2 cm for an elevation angle as low as 10 deg.

Wu, S.-C.↗

Coupling of ionosphere and troposphere during the occurrence of isolated tornadoes on November 20, 1973

The paper examines the coupling between the ionosphere and the troposphere during time periods with isolated tornadoes on the stormy day of November 20, 1973. Observations are made with a high-frequency CW Doppler array system, in which radio receivers located at a central site monitored signals transmitted from three independent remote sites on three sets of frequencies (4.0125, 4.759, 5.734 MHz) and reflected off the ionosphere approximately halfway between the transmitter and receiver sites. It is shown that the sources of the gravity waves associated with tornadoes are always on the squall lines and near the tornado touchdown locations, and that analyses of ionospheric Doppler sounder observations of medium-scale gravity waves can contribute to the understanding of the coupling between the ionosphere and the troposphere during periods of severe storm activity.

Hung, R. J.↗