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At least 271 records · Page 15

Non-OH Chemistry in Oxidation Flow Reactors for the Study of Atmospheric Chemistry Systematically Examined by Modeling

Oxidation flow reactors (OFRs) using low-pressure Hg lamp emission at 185 and 254 nm produce OH radicals efficiently and are widely used in atmospheric chemistry and other fields. However, knowledge of detailed OFR chemistry is limited, allowing speculation in the literature about whether some non-OH reactants, including several not relevant for tropospheric chemistry, may play an important role in these OFRs. These non-OH reactants are UV radiation, O(1D), O(3P), and O3. In this study, we investigate the relative importance of other reactants to OH for the fate of reactant species in OFR under a wide range of conditions via box modeling. The relative importance of non-OH species is less sensitive to UV light intensity than to relative humidity (RH) and external OH reactivity (OHRext), as both non-OH reactants and OH scale roughly proportional to UV intensity. We show that for field studies in forested regions and also the urban area of Los Angeles, reactants of atmospheric interest are predominantly consumed by OH. We find that O(1D), O(3P), and O3 have relative contributions to VOC consumption that are similar or lower than in the troposphere. The impact of O atoms can be neglected under most conditions in both OFR and troposphere. Under pathological OFR conditions of low RH and/or high OHRext, the importance of non-OH reactants is enhanced because OH is suppressed. Some biogenics can have substantial destructions by O3, and photolysis at non-tropospheric wavelengths (185 and 254 nm) may also play a significant role in the degradation of some aromatics under pathological conditions. Working under low O2 with the OFR185 mode allows OH to completely dominate over O3 reactions even for the biogenic species most reactive with O3. Non-tropospheric VOC photolysis may have been a problem in some laboratory and source studies, but can be avoided or lessened in future studies by diluting source emissions and working at lower precursor concentrations in lab studies, and by humidification. SOA photolysis is shown to be insignificant for most functional groups, except for nitrates and especially aromatics, which may be photolyzed at high UV flux settings. Our work further establishes the OFR's usefulness as a tool to study atmospheric chemistry and enables better experiment design and interpretation, as well as improved future reactor design.

Peng, Zhe↗

Non-OH Chemistry in Oxidation Flow Reactors for the Study of Atmospheric Chemistry Systematically Examined by Modeling

Oxidation flow reactors (OFRs) using low-pressure Hg lamp emission at 185 and 254 nm produce OH radicals efficiently and are widely used in atmospheric chemistry and other fields. However, knowledge of detailed OFR chemistry is limited, allowing speculation in the literature about whether some non-OH reactants, including several not relevant for tropospheric chemistry, may play an important role in these OFRs. These non-OH reactants are UV radiation, O(1D), O(3P), and O3. In this study, we investigate the relative importance of other reactants to OH for the fate of reactant species in OFR under a wide range of conditions via box modeling. The relative importance of non-OH species is less sensitive to UV light intensity than to relative humidity (RH) and external OH reactivity (OHRext), as both non-OH reactants and OH scale roughly proportional to UV intensity. We show that for field studies in forested regions and also the urban area of Los Angeles, reactants of atmospheric interest are predominantly consumed by OH. We find that O(1D), O(3P), and O3 have relative contributions to VOC consumption that are similar or lower than in the troposphere. The impact of O atoms can be neglected under most conditions in both OFR and troposphere. Under pathological OFR conditions of low RH and/or high OHRext, the importance of non-OH reactants is enhanced because OH is suppressed. Some biogenics can have substantial destructions by O3, and photolysis at non-tropospheric wavelengths (185 and 254 nm) may also play a significant role in the degradation of some aromatics under pathological conditions. Working under low O2 with the OFR185 mode allows OH to completely dominate over O3 reactions even for the biogenic species most reactive with O3. Non-tropospheric VOC photolysis may have been a problem in some laboratory and source studies, but can be avoided or lessened in future studies by diluting source emissions and working at lower precursor concentrations in lab studies, and by humidification. SOA photolysis is shown to be insignificant for most functional groups, except for nitrates and especially aromatics, which may be photolyzed at high UV flux settings. Our work further establishes the OFR's usefulness as a tool to study atmospheric chemistry and enables better experiment design and interpretation, as well as improved future reactor design.

Peng, Zhe↗

Recent spectroscopic findings concerning clay/water interactions at low humidity: Possible applications to models of Martian surface reactivity

A feasibility study assessing the utility of the adaptation of near infrared correlation spectroscopy to quantifying iron and adsorbed water in some clay-based Mars soil analog materials (MarSAM's). The work was intended to constitute Phase 1 of an approach to identifying optical analytical wavelength regions, not only for important mineral classes, but for chemically active centers within them. Many of these centers are common to unrelated mineral classes and of disproportionate influence relative to the mineral structure as a whole in determining the surface reactivity of mineral surfaces. We previously reported linearity between reflectance and total iron and total moisture over a large range of both key variables. We also discovered interesting relationships between the intensity of iron bands and the relative humidity of the systems. These relationships were confirmed. We also show that, in the low humidity range, reflectance is linearly dependent on a different kind of water from that best representing the full humidity range (the kind of water associated, in clays, with surface acidity). These relationships and the sensitivity and capability of quantitation of near infrared data indicate high promise with the production of reactive surface intermediates of products of surface reactions.

Coyne, L.↗

Satellite Infrared Radiation Measurements Prior to the Major Earthquakes

This work describes our search for a relationship between tectonic stresses and increases in mid-infrared (IR) flux as part of a possible ensemble of electromagnetic (EM) phenomena that may be related to earthquake activity. We present and &scuss observed variations in thermal transients and radiation fields prior to the earthquakes of Jan 22, 2003 Colima (M6.7) Mexico, Sept. 28 .2004 near Parkfield (M6.0) in California and Northern Sumatra (M8.5) Dec. 26,2004. Previous analysis of earthquake events has indicated the presence of an IR anomaly, where temperatures increased or did not return to its usual nighttime value. Our procedures analyze nighttime satellite data that records the general condtion of the ground after sunset. We have found from the MODIS instrument data that five days before the Colima earthquake the IR land surface nighttime temperature rose up to +4 degrees C in a 100 km radius around the epicenter. The IR transient field recorded by MODIS in the vicinity of Parkfield, also with a cloud free environment, was around +1 degree C and is significantly smaller than the IR anomaly around the Colima epicenter. Ground surface temperatures near the Parkfield epicenter four days prior to the earthquake show steady increase. However, on the night preceding the quake, a significant drop in relative humidity was indicated, process similar to those register prior to the Colima event. Recent analyses of continuous ongoing long- wavelength Earth radiation (OLR) indicate significant and anomalous variability prior to some earthquakes. The cause of these anomalies is not well understood but could be the result of a triggering by an interaction between the lithosphere-hydrosphere and atmospheric related to changes in the near surface electrical field and/or gas composition prior to the earthquake. The OLR anomaly usually covers large areas surrounding the main epicenter. We have found strong anomalies signal (two sigma) along the epicentral area signals on Dec 21, five days prior to the Northern Sumatra quake compared to the reference field for December 2001-2004 periods. Our recent results support the hypothesis of a possible relationship between a thermodynamic processes produced by increasing tectonic stress in the Earth's crust and a subsequent electro-chemical interaction between this crust and the atmosphere/ionosphere.

Ouzounov, Dimitar↗

Rolling DICE to Advance Knowledge of Land-Atmosphere Interactions

The Diurnal Land-Atmosphere Coupling Experiment (DICE) aims to explore the complex interactions between the land surface and atmospheric boundary layer, which are generally not well understood and difficult to isolate in models. The project involves over 10 different models, combining expertise from both land surface and atmospheric boundary-layer modelling groups. A simple three-stage methodology is designed to assess land-atmosphere feedbacks. Stage 1: the individual components are assessed in isolation, driven and evaluated against observational data; stage 2: the impact of coupling is investigated; stage 3: the sensitivity of the stand-alone models to variations in driving data is explored. For this initial study, a three-day clear-sky period in the mid-west USA over, an assumed simple, predominantly grass surface was simulated using data from the CASES-99 field campaign. Key conclusions from the study include: (1) the memory of vegetation state within Land Surface Models (LSMs) needs attention; (2) the height of atmospheric forcing for LSMs is important, particularly for the nocturnal boundary layer, and this has implications for both observations and vertical resolution for atmospheric models; (3) land-atmosphere feedbacks reduce errors in simulated surface fluxes at the expense of the accuracy of the variables that the models are designed to simulate (e.g., temperature, humidity and wind speed); (4) problems remain in representing the stable boundary layer in atmospheric models; (5) the mixing of temperature and humidity within the boundary layer may need to be represented separately; (6) differences in daytime profiles of heat, moisture and momentum between models are mainly due to the way the models erode the inversion at the top of the boundary layer, rather than differences in the surface fluxes. Resultant variations in modelled boundary layer heights have a substantial impact on relative humidity and could partially explain variations in coupling strength between models in the GLACE experiment.

Martin Best↗

Low altitude temperature and humidity profile data for application to aircraft noise propagation

A data search of the weather statistics from 11 widely dispersed geographical locations within the continental United States was conducted. The sites, located long both sea-coasts and in the interior, span the northern, southern, and middle latitudes. The weather statistics, retrieved from the records of these 11 sites, consist of two daily observations taken over a 10-year period. The data were sorted with respect to precipitation and surface winds and classified into temperature intervals of 5 C and relative humidity intervals of 10 percent for the lower 1400 meters of the atmosphere. These data were assembled in a statistical format and further classified into altitude increments of 200 meters. The data are presented as sets of tables for each site by season of the year and include both daily observations.

Connor, A. B.↗

Tribological properties of polymer films and solid bodies in a vacuum environment

The tribological properties of ten different polymer based materials were evaluated in a vacuum environment to determine their suitability for possible lubrication applications in a space environment, such as might be encountered on the proposed space station. A pin-on-disk tribometer was used and the polymer materials were evaluated either as solid body disks or as films applied to 440C HT stainless steel disks. A 440C HT stainless steel hemispherically tipped pin was slid against the polymer materials. For comparison, similar tests were conducted in a controlled air atmosphere of 50 percent relative humidity air. In most instances, the polymer materials lubricated much better under vacuum conditions than in air. Thus, several of the materials show promise as lubricants for vacuum applications. Friction coefficients of 0.05 or less and polymer material wear rates of up to 2 orders of magnitude less than in air were obtained. One material showed considerable promise as a traction drive material. Relatively high friction coefficients (0.36 to 0.52) and reasonably low wear rates were obtained in vacuum.

Fusaro, Robert L.↗

Tribological properties of polymer films and solid bodies in a vacuum environment

The tribological properties of ten different polymer based materials were evaluated in a vacuum environment to determine their suitability for possible lubrication applications in a space environment, such as might be encountered on the proposed Space Station. A pin-on-disk tribometer was used and the polymer materials were evaluated either as solid body disks or as films applied to 440C HT stainless steel disks. A 440C HT stainless steel hemispherically tipped pin was slid against the polymer materials. For comparison, similar tests were conducted in a controlled air atmosphere of 50 percent relative humidity air. In most instances, the polymer materials lubricated much better under vacuum conditions than in air. Thus, several of the materials show promise as lubricants for vacuum applications. Friction coefficients of 0.05 or less and polymer material wear rates of up to 2 orders of magnitude less than in air were obtained. One material showed considerable promise as a traction drive material. Relative high friction coefficients (0.36 to 0.52) and reasonably low wear rates were obtained in vacuum.

Fusaro, Robert L.↗

Oxidation of SO2 by NO2 and O3 on carbon - Implications to tropospheric chemistry

The oxidation of SO2 to sulfate in air at 65 percent relative humidity on carbon particles was investigated gravimetrically in the presence of NO2 and O3. Approximately 1 mg samples of carbon black were exposed to continuously flowing ppbv mixtures of SO2, SO2 + NO2 and SO2 + O3 for prescribed periods of time before desorption into dry N2. Wet chemical analysis of the particles followed desorption. NO2 and O3 were found to have little, if any, effect relative to air on sulfate yields at the concentrations studied.

Cofer, W. R., III↗

Monthly mean large-scale analyses of upper-tropospheric humidity and wind field divergence derived from three geostationary satellites

This paper describes the results from a collaborative study between the European Space Operations Center, the European Organization for the Exploitation of Meteorological Satellites, the National Oceanic and Atmospheric Administration, and the Cooperative Institute for Meteorological Satellite Studies investigating the relationship between satellite-derived monthly mean fields of wind and humidity in the upper troposphere for March 1994. Three geostationary meteorological satellites GOES-7, Meteosat-3, and Meteosat-5 are used to cover an area from roughly 160 deg W to 50 deg E. The wind fields are derived from tracking features in successive images of upper-tropospheric water vapor (WV) as depicted in the 6.5-micron absorption band. The upper-tropospheric relative humidity (UTH) is inferred from measured water vapor radiances with a physical retrieval scheme based on radiative forward calculations. Quantitative information on large-scale circulation patterns in the upper-troposphere is possible with the dense spatial coverage of the WV wind vectors. The monthly mean wind field is used to estimate the large-scale divergence; values range between about-5 x 10(exp -6) and 5 x 10(exp 6)/s when averaged over a scale length of about 1000-2000 km. The spatial patterns of the UTH field and the divergence of the wind field closely resemble one another, suggesting that UTH patterns are principally determined by the large-scale circulation. Since the upper-tropospheric humidity absorbs upwelling radiation from lower-tropospheric levels and therefore contributes significantly to the atmospheric greenhouse effect, this work implies that studies on the climate relevance of water vapor should include three-dimensional modeling of the atmospheric dynamics. The fields of UTH and WV winds are useful parameters for a climate-monitoring system based on satellite data. The results from this 1-month analysis suggest the desirability of further GOES and Meteosat studies to characterize the changes in the upper-tropospheric moisture sources and sinks over the past decade.

Schmetz, Johannes↗

The MJO Transition from Shallow to Deep Convection in CloudSat/CALIPSO Data and GISS GCM Simulations

The relationship between convective penetration depth and tropospheric humidity is central to recent theories of the Madden-Julian oscillation (MJO). It has been suggested that general circulation models (GCMs) poorly simulate the MJO because they fail to gradually moisten the troposphere by shallow convection and simulate a slow transition to deep convection. CloudSat and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) data are analyzed to document the variability of convection depth and its relation to water vapor during the MJO transition from shallow to deep convection and to constrain GCM cumulus parameterizations. Composites of cloud occurrence for 10MJO events show the following anticipatedMJO cloud structure: shallow and congestus clouds in advance of the peak, deep clouds near the peak, and upper-level anvils after the peak. Cirrus clouds are also frequent in advance of the peak. The Advanced Microwave Scanning Radiometer for EarthObserving System (EOS) (AMSR-E) columnwater vapor (CWV) increases by;5 mmduring the shallow- deep transition phase, consistent with the idea of moisture preconditioning. Echo-top height of clouds rooted in the boundary layer increases sharply with CWV, with large variability in depth when CWV is between;46 and 68 mm. International Satellite Cloud Climatology Project cloud classifications reproduce these climatological relationships but correctly identify congestus-dominated scenes only about half the time. A version of the Goddard Institute for Space Studies Model E2 (GISS-E2) GCM with strengthened entrainment and rain evaporation that produces MJO-like variability also reproduces the shallow-deep convection transition, including the large variability of cloud-top height at intermediate CWV values. The variability is due to small grid-scale relative humidity and lapse rate anomalies for similar values of CWV. 1.

DelGenio, Anthony G.↗

Remote Sensing of Crystal Shapes in Ice Clouds

Ice crystals in clouds exist in a virtually limitless variation of geometries. The most basic shapes of ice crystals are columnar or plate-like hexagonal prisms with aspect ratios determined by relative humidity and temperature. However, crystals in ice clouds generally display more complex structures owing to aggregation, riming and growth histories through varying temperature and humidity regimes. Crystal shape is relevant for cloud evolution as it affects microphysical properties such as fall speeds and aggregation efficiency. Furthermore, the scattering properties of ice crystals are affected by their general shape, as well as by microscopic features such as surface roughness, impurities and internal structure. To improve the representation of ice clouds in climate models, increased understanding of the global variation of crystal shape and how it relates to, e.g., location, cloud temperature and atmospheric state is crucial. Here, the remote sensing of ice crystal macroscale and microscale structure from airborne and space-based lidar depolarization observations and multi-directional measurements of total and polarized reflectances is reviewed. In addition, a brief overview is given of in situ and laboratory observations of ice crystal shape as well as the optical properties of ice crystals that serve as foundations for the remote sensing approaches. Lidar depolarization is generally found to increase with increasing cloud height and to vary with latitude. Although this variation is generally linked to the variation of ice crystal shape, the interpretation of the depolarization remains largely qualitative and more research is needed before quantitative conclusions about ice shape can be deduced. The angular variation of total and polarized reflectances of ice clouds has been analyzed by numerous studies in order to infer information about ice crystal shapes from them. From these studies it is apparent that pristine crystals with smooth surfaces are generally inconsistent with the data and thus crystal impurity, distortion or surface roughness is prevalent. However, conclusions about the dominating ice shapes are often inconclusive and contradictory and are highly dependent on the limited selection of shapes included in the investigations. Since ice crystal optical properties are mostly determined by the aspect ratios of the crystal components and their microscale structure, it is advised that remote sensing applications focus on the variation of these ice shape characteristics, rather than on the macroscale shape or habit. Recent studies use databases with nearly continuous ranges of crystal component aspect ratio and-or roughness levels to infer the variation of ice crystal shape from satellite and airborne remote sensing measurements. Here, the rationale and results of varying strategies for the remote sensing of ice crystal shape are reviewed. Observed systematic variations of ice crystal geometry with location, cloud height and atmospheric state suggested by the data are discussed. Finally, a prospective is given on the future of the remote sensing of ice cloud particle shapes.

clouds↗

Effects of Humidity On the Flow Characteristics of PS304 Plasma Spray Feedstock Powder Blend

The effects of environmental humidity on the flow characteristics of PS304 feedstock have been investigated. Angular and spherical BaF2-CaF2 powder was fabricated by comminution and by atomization, respectively. The fluorides were added incrementally to the nichrome, chromia, and silver powders to produce PS304 feedstock. The powders were dried in a vacuum oven and cooled to a Tom temperature under dry nitrogen. The flow of the powder was studied from 2 to 100 percent relative humidity (RH) The results suggest that the feedstock flow is slightly degraded with increasing humidity below 66 percent RH and is more affected above 66 percent RH. There was no flow above 88 percent RH. Narrower particle size distributions of the angular fluorides allowed flow up to 95 percent RH. These results offer guidance that enhances the commercial potential for this material system.

Stanford, Malcolm K.↗

Characteristics of middle and upper tropospheric clouds as deduced from rawinsonde data

The static environment of middle and upper tropospheric clouds is characterized. Computed relative humidity with respect to ice is used to diagnose the presence of cloud layer. The deduced seasonal mean cloud cover estimates based on this technique are shown to be reasonable. The cases are stratified by season and pressure thickness, and the dry static stability, vertical wind speed shear, and Richardson number are computed for three layers for each case. Mean values for each parameter are presented for each stratification and layer. The relative frequency of occurrence of various structures is presented for each stratification. The observed values of each parameter and the observed structure of each parameter are quite variable. Structures corresponding to any of a number of different conceptual models may be found. Moist adiabatic conditions are not commonly observed and the stratification based on thickness yields substantially different results for each group.

Starr, D. D. O.↗

Analysis of Saturn's Thermal Emission at 2.2-cm Wavelength: Spatial Distribution of Ammonia Vapor

This work focuses on determining the latitudinal structure of ammonia vapor in Saturn's cloud layer near 1.5 bars using the brightness temperature maps derived from the Cassini RADAR (Elachi et al., 2004) instrument, which works in a passive mode to measure thermal emission from Saturn at 2.2-cm wavelength. We perform an analysis of five brightness temperature maps that span epochs from 2005 to 2011, which are presented in a companion paper by Janssen et al. (2013a, this issue). The brightness temperature maps are representative of the spatial distribution of ammonia vapor, since ammonia gas is the only effective opacity source in Saturn's atmosphere at 2.2-cm wavelength. Relatively high brightness temperatures indicate relatively low ammonia relative humidity (RH), and vice versa. We compare the observed brightness temperatures to brightness temperatures computed using the Juno atmospheric microwave radiative transfer (JAMRT) program which includes both the means to calculate a tropospheric atmosphere model for Saturn and the means to carry out radiative transfer calculations at microwave frequencies. The reference atmosphere to which we compare has a 3x solar deep mixing ratio of ammonia (we use 1.352x10(exp -4) for the solar mixing ratio of ammonia vapor relative to H2; see Atreya, 2010) and is fully saturated above its cloud base. The maps are comprised of residual brightness temperatures-observed brightness temperature minus the model brightness temperature of the saturated atmosphere.

Atmospheres↗

Measurements of upper troposheric humidity at low temperatures during CRYSTAL-FACE

Aircraft condensation trails (contrails) and thin cirrus were studied by instruments on the NASA WB-57F high-altitude aircraft during contrails and optically thing cirrus are contrasted by different levels of supersaturation with respect to ice. During the July 13, 2002, flight of the WB-57F aircraft intercepted visible contrails produced by both the WB-57F and ER-2 aircraft. These contrails were located immediately below the local tropopause, where ambient temperatures were very low (-76 degree C). The contrails were clearly indicated by an abrupt increase in NO and a simultaneous, abrupt decrease in ice supersaturation. With in the contrail, the relative humidity was close to 130% with respect to ice, higher than expected from theory. Outside the contrails was a persistent layer of subvisible currus extending from approximately 13 to 15 km altitude. This layer was characterized y significant supersaturations because the ambient concentrations of ice particles were insufficient to significantly deplete the ice supersaturation. We will discuss in situ measurements and models simulations of humidity.

water vapor↗

Profiling of Atmospheric Water Vapor with MIR and LASE

This paper presents the first and the only simultaneous measurements of water vapor by MIR (Millimeter-wave Imaging Radiometer) and LASE (Lidar Atmospheric Sounding Experiment) on board the same ER-2 aircraft. Water vapor is one of the most important constituents in the Earth's atmosphere, as its spatial and temporal variations affect a wide spectrum of meteorological phenomena ranging from the formation of clouds to the development of severe storms. Its concentration, as measured in terms of relative humidity, determines the extinction coefficient of atmospheric aerosol particles and therefore visibility. These considerations point to the need for effective and frequent measurements of the atmospheric water vapor. The MIR and LASE instruments provide measurements of water vapor profiles with two markedly different techniques. LASE can give water vapor profiles with excellent vertical resolution under clear condition, while MIR can retrieve water vapor profiles with a crude vertical resolution even under a moderate cloud cover. Additionally, millimeter-wave measurements are relatively simple and provide better spatial coverage.

Wang, J. R.↗

On the Susceptibility of Cold Tropical Cirrus to Ice Nuclei Abundance

Numerical simulations of cirrus formation in the tropical tropopause layer (TTL) are used to evaluate the impact heterogeneous ice nuclei (IN) abundance on cold cloud microphysical properties. The model includes homogeneous and heterogeneous ice nucleation, deposition growthsublimation, and sedimentation. Reanalysis temperature and wind fields are used to force the simulations, with addition of high-frequency wave temperature variability based on in situ measurements. The model results are constrained by recent in situ observations of TTL cirrus and relative humidity, as well as satellite measurements of cirrus bulk properties and occurrence frequencies. Temperature variability driven by high-frequency waves has a dominant influence on TTL cirrus microphysical properties and occurrence frequencies, and inclusion of these waves is required to produce agreement between the simulated and observed cloud properties as well as the abundance of TTL cirrus. With a composition-independent supersaturation threshold for homogeneous freezing of aqueous aerosols, the model produces excessive ice concentrations compared with in situ observations. Inclusion of relatively numerous heterogeneous nuclei ( 100L) in the simulations improves the agreement with observed ice concentrations. However, when IN contribute significantly to TTL cirrus ice nucleation, the occurrence frequency of large supersaturations with respect to ice is less than indicated by in situ measurements. The simulated TTL cirrus extinction statistics agree with observations (within uncertainties) from both in situ and remote-sensing measurements. We find that the sensitivity of TTL cirrus extinction and ice water content statistics to heterogeneous ice nuclei abundance is relatively weak. Likewise, the simulated occurrence frequencies of TTL cirrus are insensitive to ice nuclei abundance, both in terms of cloud frequency height distribution and regional distribution throughout the tropics.

occurences↗