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At least 235 records · Page 13

Measurement of viscosity of gaseous mixtures at atmospheric pressure

Coefficients of viscosity of various types of gas mixtures, including simulated natural-gas samples, have been measured at atmospheric pressure and room temperature using a modified capillary tube method. Pressure drops across the straight capillary tube section of a thermal mass flowmeter were measured for small, well-defined, volume flow rates for the test gases and for standard air. In this configuration, the flowmeter provides the volumetric flow rates as well as a well-characterized capillary section for differential pressure measurements across it. The coefficients of viscosity of the test gases were calculated using the reported value of 185.6 micro P for the viscosity of air. The coefficients of viscosity for the test mixtures were also calculated using Wilke's approximation of the Chapman-Enskog (C-E) theory. The experimental and calculated values for binary mixtures are in agreement within the reported accuracy of Wilke's approximation of the C-E theory. However, the agreement for multicomponent mixtures is less satisfactory, possible because of the limitations of Wilkes's approximation of the classical dilute-gas state model.

Singh, J. J.↗

Comparison of Eulerian Bin and Lagrangian Particle-Based Microphysics in Simulations of Nonprecipitating Cumulus

A single nonprecipitating cumulus congestus setup is applied to compare droplet spectra grown by the diffusion of water vapor in Eulerian bin and particle-based Lagrangian microphysics schemes. Bin microphysics represent droplet spectral evolution applying the spectral density function. In the Lagrangian microphysics, computational particles referred to as superdroplets are followed in time and space with each superdroplet representing a multiplicity of natural cloud droplets. The same cloud condensation nuclei (CCN) activation and identical representation of the droplet diffusional growth allow the comparison. The piggybacking method is used with the two schemes operating in a single simulation, one scheme driving the dynamics and the other one piggybacking the simulated flow. Piggybacking allows point-by-point comparison of droplet spectra predicted by the two schemes. Overall, the results show the impact of inherent limitations of the two microphysics simulation methods, numerical diffusion in the Eulerian scheme and a limited number of superdroplets in the Lagrangian scheme. Numerical diffusion in the Eulerian scheme results in a more dilution of the cloud upper half and thus smaller cloud droplet mean radius. The Lagrangian scheme typically has larger spatial fluctuations of droplet spectral properties. A significantly larger mean spectral width in the bin microphysics across the entire cloud depth is the largest difference between the two schemes. A fourfold increase of the number of superdroplets per grid volume and a twofold increase of the spectral resolution and thus the number of bins have small impact on the results and provide only minor changes to the comparison between simulated cloud properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

An assessment of ocean alkalinity enhancement using aqueous hydroxides: kinetics, efficiency, and precipitation thresholds

Abstract. Ocean alkalinity enhancement (OAE) is a promising approach to marine carbon dioxide removal (mCDR) that leverages the large surface area and carbon storage capacity of the oceans to sequester atmospheric CO2 as dissolved bicarbonate (HCO3-). One OAE method involves the conversion of salt in seawater into aqueous alkalinity (NaOH), which is returned to the ocean. The resulting increase in seawater pH and alkalinity causes a shift in dissolved inorganic carbon (DIC) speciation toward carbonate and a decrease in the surface ocean pCO2. The shift in the pCO2 results in enhanced uptake of atmospheric CO2 by the seawater due to gas exchange. In this study, we systematically test the efficiency of CO2 uptake in seawater treated with NaOH at aquarium (15 L) and tank (6000 L) scales to establish operational boundaries for safety and efficiency in advance of scaling up to field experiments. CO2 equilibration occurred on the order of weeks to months, depending on circulation, air forcing, and air bubbling conditions within the test tanks. An increase of ∼0.7–0.9 mol DIC per mol added alkalinity (in the form of NaOH) was observed through analysis of seawater bottle samples and pH sensor data, consistent with the value expected given the values of the carbonate system equilibrium calculations for the range of salinities and temperatures tested. Mineral precipitation occurred when the bulk seawater pH exceeded 10.0 and Ωaragonite exceeded 30.0. This precipitation was dominated by Mg(OH)2 over hours to 1 d before shifting to CaCO3,aragonite precipitation. These data, combined with models of the dilution and advection of alkaline plumes, will allow the estimation of the amount of carbon dioxide removal expected from OAE pilot studies. Future experiments should better approximate field conditions including sediment interactions, biological activity, ocean circulation, air–sea gas exchange rates, and mixing zone dynamics.

Ringham, Mallory C. (ORCID:0000000348020185)↗

Spectral Line Parameters Including Temperature Dependences of Self- and Air-Broadening in the 2 (left arrow) 0 Band of CO at 2.3 micrometers

Temperature dependences of pressure-broadened half-width and pressure-induced shift coefficients along with accurate positions and intensities have been determined for transitions in the 2<--0 band of C-12 O-16 from analyzing high-resolution and high signal-to-noise spectra recorded with two different Fourier transform spectrometers. A total of 28 spectra, 16 self-broadened and 12 air-broadened, recorded using high- purity (greater than or equal to 99.5% C-12-enriched) CO samples and CO diluted with dry air(research grade) at different temperatures and pressures, were analyzed simultaneously to maximize the accuracy of the retrieved parameters. The sample temperatures ranged from 150 to 298K and the total pressures varied between 5 and 700 Torr. A multispectrum nonlinear least squares spectrum fitting technique was used to adjust the rovibrational constants (G, B, D, etc.) and intensity parameters (including Herman-Wallis coefficients), rather than determining individual line positions and intensities. Self-and air-broadened Lorentz half-width coefficients, their temperature dependence exponents, self- and air-pressure-induced shift coefficients, their temperature dependences, self- and air-line mixing coefficients, their temperature dependences and speed dependence have been retrieved from the analysis. Speed-dependent line shapes with line mixing employing off-diagonal relaxation matrix element formalism were needed to minimize the fit residuals. This study presents a precise and complete set of spectral line parameters that consistently reproduce the spectrum of carbon monoxide over terrestrial atmospheric conditions.

Devi, V. Malathy↗

Influences of Environmental Relative Humidity and Horizontal Scale of Subcloud Ascent on Deep Convective Initiation

This study examines two factors impacting initiation of moist deep convection: free-tropospheric environmental relative humidity (φ E ) and horizontal scale of subcloud ascent (R sub ), the latter exerting a dominant control on cumulus cloud width. A simple theoretical model is used to formulate a “scale selection” hypothesis: that a minimum R sub is required for moist convection to go deep, and that this minimum scale decreases with increasing φ E . Specifically, the ratio of R 2 sub to saturation deficit (1 - φ E ) must exceed a certain threshold value that depends on cloud-layer environmental lapse rate. Idealized, large-eddy simulations of moist convection forced by horizontally varying surface fluxes show strong sensitivity of maximum cumulus height to both φ E and R sub consistent with the hypothesis. Increasing R sub by only 300–400 m can lead to a large increase (>5 km) in cloud height. A passive tracer analysis shows that the bulk fractional entrainment rate decreases rapidly with R sub but depends little on φ E . However, buoyancy dilution increases as either R sub or φ E decreases; buoyancy above the level of free convection is rapidly depleted in dry environments when R sub is small. While deep convective initiation occurs with an increase in relative humidity of the near environment from moistening by earlier convection, the importance of this moisture preconditioning is inconclusive as it is accompanied by an increase in R sub . Overall, it is concluded that small changes to R sub driven by external forcing or by convection itself could be a dominant regulator of deep convective initiation.

54 ENVIRONMENTAL SCIENCES↗

Tree foliage as a net accumulator of highly toxic methylmercury

Tree canopies are known to elevate atmospheric inputs of both mercury (Hg) and methylmercury (MeHg). While foliar uptake of gaseous Hg is well documented, little is known regarding the temporal dynamics and origins of MeHg in tree foliage, which represents typically less than 1% of total Hg in foliage. In this work, we examined the foliar total Hg and MeHg content by following the growth of five individual trees of American Beech (Fagus grandifolia) for one growing season (April–November, 2017) in North Carolina, USA. We show that similar to other studies foliar Hg content increased almost linearly over time, with daily accumulation rates ranging from 0.123 to 0.161 ng/g/day. However, not all trees showed linear increases of foliar MeHg content along the growing season; we found that 2 out of 5 trees showed elevated foliar MeHg content at the initial phase of the growing season but their MeHg content declined through early summer. However, foliar MeHg content among all 5 trees showed eventual increases through the end of the growing season, proving that foliage is a net accumulator of MeHg while foliar gain of biomass did not “dilute” MeHg content.

54 ENVIRONMENTAL SCIENCES↗

Analytical Investigation of the Role of Lateral Mixing in the Evolution of Nonprecipitating Cumulus. Part I: Developing Clouds

Evolution of nonprecipitating cumulus clouds (Cu) at the developing stage under the influence of lateral entrainment and mixing is studied analytically using a minimalistic analytical model. We present a model of an ascending cloud volume (a model of developing Cu) whose structure is determined by the processes of droplet diffusion growth/evaporation and entrainment mixing in the horizontal direction. Spatial and time changes of liquid water content, the adiabatic fraction, droplet concentration, and the mean volume droplet radius are calculated. It is shown that the existence of a nondiluted core in a growing cumulus cloud significantly depends on the cloud width and vertical velocity. While at the updraft velocity of 2 m s −1 the core of a 400-m-wide cloud becomes diluted at distances of a few hundred meters above cloud base, the core of a cloud of 1000-m width remains nondiluted at distances up to 1500 m above cloud base. The explanation of this result is simple: the increase in cloud width and the decrease in the updraft velocity increase the time during which the cloud is diluted due to mixing. Since lateral mixing synchronously decreases both the cloud water content and droplet concentration, the variation of the mean volume droplet radius is low inside the cloud. The approximate quantitative condition for cloud formation in updraft is derived. It is shown that a cloud can arise when its vertical velocity exceeds a critical value. To produce clouds, narrow turbulent plumes should ascend at higher velocity as compared to wider plumes. High humidity of the environment air is favorable for formation of clouds from plumes. The comparison of the obtained results with previously published observational data indicates a reasonable agreement. The results can be useful for parameterization purposes.

54 ENVIRONMENTAL SCIENCES↗

An Analytic Formula for Entraining CAPE in Midlatitude Storm Environments

Abstract This article introduces an analytic formula for entraining convective available potential energy (ECAPE) with an entrainment rate that is determined directly from an environmental sounding, rather than prescribed by the formula user. Entrainment is connected to the background environment using an eddy diffusivity approximation for lateral mixing, updraft geometry assumptions, and mass continuity. These approximations result in a direct correspondence between the storm-relative flow and the updraft radius and an inverse scaling between the updraft radius squared and entrainment rate. The aforementioned concepts, combined with the assumption of adiabatic conservation of moist static energy, yield an explicit analytic equation for ECAPE that depends entirely on state variables in an atmospheric profile and a few constant parameters with values that are established in past literature. Using a simplified Bernoulli-like equation, the ECAPE formula is modified to account for updraft enhancement via kinetic energy extracted from the cloud’s background environment. CAPE and ECAPE can be viewed as predictors of the maximum vertical velocity w max in an updraft. Hence, these formulas are evaluated using w max from past numerical modeling studies. Both of the new formulas improve predictions of w max substantially over commonly used diagnostic parameters, including undiluted CAPE and ECAPE with a constant prescribed entrainment rate. The formula that incorporates environmental kinetic energy contribution to the updraft correctly predicts instances of exceedance of by w max , and provides a conceptual explanation for why such exceedance is rare among past simulations. These formulas are potentially useful in nowcasting and forecasting thunderstorms and as thunderstorm proxies in climate change studies. Significance Statement Substantial mixing occurs between the upward-moving air currents in thunderstorms (updrafts) and the surrounding comparatively dry environmental air, through a process called entrainment. Entrainment controls thunderstorm intensity via its diluting effect on the buoyancy of air within updrafts. A challenge to representing entrainment in forecasting and predictions of the intensity of updrafts in future climates is to determine how much entrainment will occur in a given thunderstorm environment without a computationally expensive high-resolution simulation. To address this gap, this article derives a new formula that computes entrainment from the properties of a single environmental profile. This formula is shown to predict updraft vertical velocity more accurately than past diagnostics, and can be used in forecasting and climate prediction to improve predictions of thunderstorm behavior and impacts.

54 ENVIRONMENTAL SCIENCES↗

CFD modeling of near-wall combustion and unburned methane prediction in natural gas spark ignition engines

Natural gas-powered engines play a critical role in gas drilling, compression, and transmission sectors, but methane (CH 4 ) from engine combustion slip can be significant over their lifespan, contributing to atmospheric pollution and signaling reduced engine efficiency. Here, to address this challenge, computational fluid dynamics (CFD) simulations offer valuable insights into the in-cylinder combustion process, enabling the optimization of combustion strategies and engine designs to minimize unburned CH 4 slip. This study aims to evaluate and improve combustion models for simulating the combustion process and predicting unburned CH 4 concentrations in natural gas spark-ignition (SI) engines, including engines that are part of combined reformer-engine systems. Specifically, the performance of two flamelet-based combustion models—the Extended Coherent Flame Model (ECFM) and the G-equation model—was assessed using experimental engine data collected under varying excess-air ratio (λ) conditions and fuel compositions, including natural gas and syngas blends. In addition, to enhance the predictive capabilities of the G-equation model, a flame-wall interaction (FWI) sub-model was integrated into its framework. The effects of its model parameters, such as quenching and influence distance, on combustion behavior and unburned methane predictions were analyzed in detail. The ECFM tended to predict delayed combustion phasing under diluted mixture conditions, resulting in overprediction of unburned CH 4 concentrations. In contrast, the G-equation model provided reasonable predictions of combustion pressure, while representing higher the CH 4 reduction rate across the operating condition compared to experimental data. Incorporating the FWI sub-model—with the quenching distance calculated based on a pressure-dependent relation (P -0.48 ) and a fixed influence distance of 1.5 mm—further improved the G-equation model’s accuracy in predicting CH 4 reduction rates without compromising its ability to simulate the combustion process.

Combustion model↗

A Formula for the Maximum Vertical Velocity in Supercell Updrafts

In supercell environments, previous authors have shown strong connections between the vertical wind shear magnitude, updraft width, and entrainment. Based on these results, it is hypothesized that the influences of entrainment-driven dilution on buoyancy and maximum updraft vertical velocity w in supercell environments are a predictable function of the vertical wind shear profile. It is also hypothesized that the influences of pressure perturbation forces on maximum updraft w are small because of a nearly complete offset between upward dynamic pressure forces and downward buoyant pressure forces. To address these hypotheses, we derive a formula for the maximum updraft w that incorporates the effects of entrainment-driven dilution on buoyancy but neglects pressure gradient forces. Solutions to this formula are compared with output from previous numerical simulations. This formula substantially improves predictions of maximum updraft w over past CAPE-derived formulas for maximum updraft w, which supports the first hypothesis. Furthermore, integrated vertical accelerations along trajectories show substantial offsets between dynamic and buoyant pressure forces, supporting the second hypothesis. It is argued that the new formula should be used in addition to CAPE-derived measures for w in forecast and research applications when accurate diagnosis of updraft speed is required.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US

Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.

54 ENVIRONMENTAL SCIENCES↗

Measurements of Acidic Gases and Aerosol Species Aboard the NASA DC-8 Aircraft During the Pacific Exploratory Mission in the Tropics (PEM-Tropics A)

We received funding to provide measurements of nitric acid (HNO3), formic acid (HCOOH), acetic acid (CH3COOH), and the chemical composition of aerosols aboard the NASA Ames DC-8 research aircraft during the PEM-Tropics A mission. These measurements were successfully completed and the final data resides in the electronic archive (ftp-gte.larc.nasa.gov) at NASA Langley Research Center. For the PEM-Tropics A mission the University of New Hampshire group was first author of four different manuscripts. Three of these have now appeared in the Journal of Geophysical Research-Atmospheres, included in the two section sections on PEM-Tropics A. The fourth manuscript has just recently been submitted to this same journal as a stand alone paper. All four of these papers are included in this report. The first paper (Influence of biomass combustion emissions on the distribution of acidic trace gases over the Southern Pacific basin during austral springtime) describes the large-scale distributions of HNO3, HCOOH, and CH3COOH. Arguments were presented to show, particularly in the middle tropospheric region, that biomass burning emissions from South America and Africa were a major source of acidic gases over the South Pacific basin. The second paper (Aerosol chemical composition and distribution during the Pacific Exploratory Mission (PEM) Tropics) covers the aerosol aspects of our measurement package. Compared to acidic gases, O3, and selected hydrocarbons, the aerosol chemistry showed little influence from biomass burning emissions. The data collected in the marine boundary layer showed a possible marine source of NH3 to the troposphere in equatorial areas. This source had been speculated on previously, but our data was the first collected from an airborne platform to show its large-scale features. The third paper (Constraints on the age and dilution of Pacific Exploratory Mission-Tropics biomass burning plumes from the natural radionuclide tracer Pb-210) utilized the unexpectedly high concentrations of Pb-210 in the combustion plumes to estimate their ages and mixing along the transport route to the South Pacific basin. The final paper in the group (Tropospheric reactive-odd nitrogen over the South Pacific in austral springtime). This paper provides a summary of reactive nitrogen during PEM-Tropics A, with HNO3 and PAM showing the most impact from combustion emission.

Talbot, Robert W.↗

Diagenetic Mineralogy at Gale Crater, Mars

Three years into exploration of sediments in Gale crater on Mars, the Mars Science Laboratory rover Curiosity has provided data on several modes and episodes of diagenetic mineral formation. Curiosity determines mineralogy principally by X-ray diffraction (XRD), but with supporting data from thermal-release profiles of volatiles, bulk chemistry, passive spectroscopy, and laser-induced breakdown spectra of targeted spots. Mudstones at Yellowknife Bay, within the landing ellipse, contain approximately 20% phyllosilicate that we interpret as authigenic smectite formed by basalt weathering in relatively dilute water, with associated formation of authigenic magnetite as in experiments by Tosca and Hurowitz [Goldschmidt 2014]. Varied interlayer spacing of the smectite, collapsed at approximately 10 A or expanded at approximately 13.2 A, is evidence of localized diagenesis that may include partial intercalation of metal-hydroxyl groups in the approximately 13.2 A material. Subsequent sampling of stratigraphically higher Windjana sandstone revealed sediment with multiple sources, possible concentration of detrital magnetite, and minimal abundance of diagenetic minerals. Most recent sampling has been of lower strata at Mount Sharp, where diagenesis is widespread and varied. Here XRD shows that hematite first becomes abundant and products of diagenesis include jarosite and cristobalite. In addition, bulk chemistry identifies Mg-sulfate concretions that may be amorphous or crystalline. Throughout Curiosity's traverse, later diagenetic fractures (and rarer nodules) of mm to dm scale are common and surprisingly constant and simple in Ca-sulfate composition. Other sulfates (Mg,Fe) appear to be absent in this later diagenetic cycle, and circumneutral solutions are indicated. Equally surprising is the rarity of gypsum and common occurrence of bassanite and anhydrite. Bassanite, rare on Earth, plays a major role at this location on Mars. Dehydration of gypsum to bassanite in the dry atmosphere of Mars has been proposed but considered unlikely based on lab studies of dehydration kinetics in powdered samples. Dehydration is even less likely for bulk vein samples, as lab data show dehydration rates one to two orders of magnitude slower in bulk samples than in powders. On Mars, exposure ages of 100 Ma or more may be a significant factor in dehydration of hydrous phases.

Vaniman, David↗

Emissions Relationships in Western Forest Fire Plumes: I. Reducing the Effect of Mixing Errors on Emission Factors

Studies of emission factors from biomass burning using aircraft data complement the results of lab studies and extend them to conditions of immense hot conflagrations. We illustrate and discuss emission relationships for 422 individual samples from many forest-fire plumes in the Western US. The samples are from two NASA investigations: ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) and SEAC4RS (Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys). This work provides sample-by-sample enhancement ratios (EnRs) for 23 gases and particulate properties. Many EnRs provide candidates for emission ratios (ERs, corresponding to the EnR at the source) when the origin and degree of transformation is understood and appropriate. From these, emission factors (EFs) can be estimated when the fuel dry mass consumed is known or can be estimated using the carbon mass budget approach. This analysis requires understanding the interplay of mixing of the plume with surrounding air. Some initial examples emphasize that measured C(tot) = CO2 + CO in a fire plume does not necessarily describe the emissions of the total carbon liberated in the flames, C(burn). Rather, it represents C(tot) = C(burn) + C(bkgd), which includes possibly varying background concentrations for entrained air. Consequently, we present a simple theoretical description for plume entrainment for multiple tracers from flame to hundreds of kilometers downwind and illustrate some intrinsic linear behaviors. The analysis suggests a Mixed Effects Regression Emission Technique (MERET), which can eliminate occasional strong biases associated with the commonly used normalized excess mixing ratio (NEMR) method. MERET splits C(tot) to reveal C(burn) by exploiting the fact that C(burn) and all tracers respond linearly to dilution, while each tracer has consistent EnR behavior (slope of tracer concentration with respect to C(burn)). The two effects are separable. Two or three or preferably more emission indicators are required as a minimum; here we used ten. Limited variations in the EnRs for each tracer can be incorporated and the variations and co-variations analyzed. The percentage CO yield (or the modified combustion efficiency) plays some role. Other co-relationships involving nitrogen and organic classes are more prominent; these have strong relationships to the C(burn) to O3 emission relationship. In summary, MERET allows fine spatial resolution (EnRs for individual observations) and comparison of similar plumes distant in time and space. Alkene ratios provide us with an approximate photochemical timescale. This allows discrimination and definition, by fire situation, of ERs, allowing us to estimate emission factors.

Chatfield, Robert B.↗

From the Primitive Atmosphere to the Prebiotic Soup to the Pre-RNA World

Organic compounds would have been produced in an earth's atmosphere that was reducing. The soup would contain amino and hydroxy acids, together with smaller amounts of purines and pyrimidines. The presence' of sugars is less likely, although they can be produced by the formose reaction from formaldehyde. However, the prebiotic synthesis of RNA has not been demonstrated. One problem is that ribose is not produced selectively over other pentoses and hexoses, except under special conditions. The second problem is that ribose is unstable, with a half-life at pH7 and 100 C of 73 minutes (44 years at 0 C). Other sugars are similarly unstable. Another problem is that there is no efficient prebiotic synthesis of polyphosphates, nor the glycosidic bond of nucleosides. This suggests that there may have been an informational macromolecule that preceded RNA. The RNA world refers to the time when RNA carried both the genetic information and the catalytic activity, and was subsequently converted to the DNA/protein world when protein synthesis began. Preceeding the RNA world was the Pre-RNA world, where a backbone different from ribose phosphate was used, and the bases may have been different from adenine, uracil, guanine and cytosine. We have shown recently that cytosine and uracil can be synthesized efficiently under prebiotic conditions using a dried lagoon model instead of the usual dilute ocean hypothesis. In addition, we have shown that uracil adds formaldehyde efficiently to give 5- hydroxymethyl uracil, which in turn adds various nucleophiles to give uracil analogs of most of the amino acids that occur in proteins. For example, the ammonia, guanidine and imidazole adducts from the analogs of lysine, arginine and histidine. This suggests that the catalytic potential of RNA may have been much more extensive than previously assumed. The major problem is finding out what was the precursor to the ribose phosphate backbone. This will be the key to developing prebiotic self-replicating systems.

Miller, Stanley L.↗

Cloud microphysical structure analysis based on high-resolution insitu measurements

This study investigates the microphysical parameters and shapes of droplet size distributions (DSDs) along three aircraft traverses of developing convective clouds during Cloud Aerosol Interactions and Precipitation Enhancement Experiment (CAIPEEX) Phase III 2015 at a sampling frequency of 25 Hz. The droplet number concentration (Nc, cm -3 ), and liquid water content (LWC, g m -3 ) present steep gradients within zones of a few tens of meters near the cloud edges and relatively gentle gradients in the strong updraft zones. Sometimes, the horizontal LWC distribution resembles a trapezoidal shape with steep LWC and Nc gradients near the cloud edges. The LWC maximums (LWC max ) are lower than the adiabatic LWCs, but the high adiabatic fractions in the cloud core indicate low dilution. High LWC/LWC max , largest droplets, and narrow and similarly shaped DSDs are found in the regions of high updrafts. Zones of low LWC/LWC max are found close to the cloud edges, where DSDs are highly diverse, containing both large and small droplets. Finally, we analyze the mixing diagrams. Significant in-phase turbulent fluctuations in LWC and N c were found. The effective radii change slightly across cloud updraft zones but decrease at the zone of low LWC/LWC max ratio close to cloud edges. The spectra of LWC and N c obey Kolmogorov -5/3 turbulence law. The radii of the correlation of LWC and N c in updraft zones are of several tens of meters. Filaments up to 120–175 m in size are also noticed.

54 ENVIRONMENTAL SCIENCES↗

Stratospheric Aerosol Measurements

Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses implicating manmade fluorocarbons as cause of the --'ozone hole'; (5) The current soot loading is too small to be of environmental (radiative and chemical) consequence. However, the fractal nature of soot distinguishes it aerodynamically and radiatively from sulfuric acid droplets such that its stratospheric residence time is longer, mainly because of vertical transport against gravity due to gravito-photophoretic forces. Thus it may accumulate and become of environmental concern in the future.

Pueschel, Rudolf, F.↗

Planar Strain-Rate-Free Diffusion Flames: Initiation, Properties, and Extinction

An effectively strain-rate-free diffusion flame constitutes the most vigorous laminar combustion of initially unmixed reactive gases. Such a diffusion flame is characterized by a relatively long residence time and by a relatively large characteristic length scale. If such a flame were also planar, providing high symmetry, it would be particularly suitable for experimental and theoretical investigations of key combustion phenomena, such as multicomponent diffusion, chemical kinetics, and soot inception, growth, and oxidation. Unfortunately, a planar strain-rate-free diffusion flame is highly disrupted in earth-gravity (e.g., in a counterflow-diffusion-flame apparatus) because of the very rapid onset (approx. 100 ms) of gravity-induced instability. Accordingly, a specially dedicated apparatus was designed, fabricated, and initially checked out for the examination of a planar strain-rate-free diffusion flame in microgravity. Such a diffusion flame may be formed within a hollowed-out squat container (initially configured as 25 cm x 25 cm x 9 cm), with isothermal, noncatalytic, impervious walls. At test initiation, a thin metallic sheet (approx. 1 mm in thickness) that separates the internal volume into two equal portions, each of dimensions 25 cm x 25 cm x 4.5 cm, is withdrawn, by uniform translation (approx. 50 cm/s) in its own plane, through a tightly fitting slit in one side wall. Thereupon, diluted fuel vapor (initially confined to one half-volume of the container) gains access to diluted oxygen (initially with the same pressure, density, and temperature as the fuel, but initially confined to the other half-volume). After a brief delay (approx. 10 ms), to permit limited but sufficient-for-flammability diffusional interpenetration of fuel vapor and oxidizer, burning is initiated by discharge of a line igniter, located along that side wall from which the trailing edge of the separator withdraws. The ignition spawns a triple-flame propagation across the 25 cm x 25 cm centerplane. When a diffusion flame is emplaced in the centerplane, any subsequent travel, and change in temperature, of that planar diffusion flame may be tracked, along with the effectively spatially uniform but temporally evolving pressure within the container. Eventually, nearly complete depletion of the stoichiometrically deficient reactant, along with heat loss to the container surfaces, effects extinction. These data afford an opportunity to check theoretical models of diffusion and chemical kinetics under conditions ranging from intense burning to flame out, or, alternatively, to evolve simple empirical representations of these phenomena. Thus, the project sought to utilize microgravity testing to elucidate commonly encountered phenomenology, arising in the commonly-encountered mode of combustion (whether related to heating, manufacturing, boiling, and propulsion, or to uncontrolled, free-burning fire in structures and wildland vegetation), of those commonly utilized fuels usually categorized as gaseous fuels (such as hydrogen, natural gas, and propane, which are gaseous under atmospheric conditions).

Fendell, Francis↗