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At least 217 records · Page 12

Homogenous Surface Nucleation of Solid Polar Stratospheric Cloud Particles

A general surface nucleation rate theory is presented for the homogeneous freezing of crystalline germs on the surfaces of aqueous particles. While nucleation rates in a standard classical homogeneous freezing rate theory scale with volume, the rates in a surface-based theory scale with surface area. The theory is used to convert volume-based information on laboratory freezing rates (in units of cu cm, seconds) of nitric acid trihydrate (NAT) and nitric acid dihydrate (NAD) aerosols into surface-based values (in units of sq cm, seconds). We show that a surface-based model is capable of reproducing measured nucleation rates of NAT and NAD aerosols from concentrated aqueous HNO3 solutions in the temperature range of 165 to 205 K. Laboratory measured nucleation rates are used to derive free energies for NAT and NAD germ formation in the stratosphere. NAD germ free energies range from about 23 to 26 kcal mole, allowing for fast and efficient homogeneous NAD particle production in the stratosphere. However, NAT germ formation energies are large (greater than 26 kcal mole) enough to prevent efficient NAT particle production in the stratosphere. We show that the atmospheric NAD particle production rates based on the surface rate theory are roughly 2 orders of magnitude larger than those obtained from a standard volume-based rate theory. Atmospheric volume and surface production of NAD particles will nearly cease in the stratosphere when denitrification in the air exceeds 40 and 78%, respectively. We show that a surface-based (volume-based) homogeneous freezing rate theory gives particle production rates, which are (not) consistent with both laboratory and atmospheric data on the nucleation of solid polar stratospheric cloud particles.

Tabazadeh, A.↗

Formation of Amino Acids and Carboxylic Acids in Weakly Reducing Planetary Atmospheres by Solar Energetic Particles from the Young Sun

Life most likely started during the Hadean Eon; however, the environmental conditions which contributed to the complexity of its chemistry are poorly known. A better understanding of various environmental conditions, including global (heliospheric) and local (atmospheric, surface, and oceanic), along with the internal dynamic conditions of the early Earth, are required to understand the onset of abiogenesis. Herein, we examine the contributions of galactic cosmic rays (GCRs) and solar energetic particles (SEPs) associated with superflares from the young Sun to the formation of amino acids and carboxylic acids in weakly reduced gas mixtures representing the early Earth’s atmosphere. We also compare the products with those introduced by lightning events and solar ultraviolet light (UV). In a series of laboratory experiments, we detected and characterized the formation of amino acids and carboxylic acids via proton irradiation of a mixture of carbon dioxide, methane, nitrogen, and water in various mixing ratios. These experiments show the detection of amino acids after acid hydrolysis when 0.5% (v/v) of initial methane was introduced to the gas mixture. In the set of experiments with spark discharges (simulation of lightning flashes) performed for the same gas mixture, we found that at least 15% methane was required to detect the formation of amino acids, and no amino acids were detected in experiments via UV irradiation, even when 50% methane was used. Carboxylic acids were formed in non-reducing gas mixtures (0% methane) by proton irradiation and spark discharges. Hence, we suggest that GCRs and SEP events from the young Sun represent the most effective energy sources for the prebiotic formation of biologically important organic compounds from weakly reducing atmospheres. Since the energy flux of space weather, which generated frequent SEPs from the young Sun in the first 600 million years after the birth of the solar system, was expected to be much greater than that of GCRs, we conclude that SEP-driven energetic protons are the most promising energy sources for the prebiotic production of bioorganic compounds in the atmosphere of the Hadean Earth.

Kensei Kobayashi↗

Modeling Heatshield Erosion due to Dust Particle Impacts for Martian Entries

Heatshield design for spacecraft entering the atmosphere of Mars may be affected by the presence of atmospheric dust. Particle impacts with sufficient kinetic energy can cause spallation damage to the heatshield that must be estimated. The dust environment in terms of particle size distribution and number density can be inferred from ground-based or atmospheric observations at Mars. Using a Lagrangian approach, the particle trajectories through the shock layer can be computed using a set of coupled ordinary differential equations. The dust particles are small enough that non-continuum effects must be accounted for when computing the drag coefficient and heat transfer to the particle surface. Surface damage correlations for impact crater diameter and penetration depth are presented for fused-silica, AVCOAT, Shuttle tiles, cork, and Norcoat Liège. The cork and Norcoat Liège correlations are new and were developed in this study. The modeling equations presented in this paper are applied to compute the heatshield erosion due to dust particle impacts on the ExoMars Schiaparelli entry capsule during dust storm conditions.

Palmer, Grant↗

Modeling Heatshield Erosion Due to Dust Particle Impacts for Martian Entries

Heatshield design for spacecraft entering the atmosphere of Mars may be affected by the presence of atmospheric dust. Particle impacts with sufficient kinetic energy can cause spallation damage to the heatshield that must be estimated. The dust environment in terms of particle size distribution and number density can be inferred from ground-based or atmospheric observations at Mars. Using a Lagrangian approach, the particle trajectories through the shock layer can be computed using a set of coupled ordinary differential equations. The dust particles are small enough that non-continuum effects must be accounted for when computing the drag coefficient and heat transfer to the particle surface. Surface damage correlations for impact crater diameter and penetration depth are presented for fused-silica, AVCOAT, Shuttle tiles, cork, and Norcoat Liège. The cork and Norcoat Liège correlations are new and were developed in this study. The modeling equations presented in this paper are applied to compute the heatshield erosion due to dust particle impacts on the ExoMars Schiaparelli entry capsule during dust storm conditions.

Palmer, Grant↗

Voyager 2 plasma wave observations at Uranus

At Uranus, the Voyager 2 plasma wave investigation observed very significant phenomena related to radio emissions, dust impacts, and magnetospheric wave-particle interactions. On January 19, 1986 (R = 270 R-sub U) the plasma wave investigation detected an intense radio burst at 31 and 56 kHz, and this provided the first indication that Uranus had a magnetosphere. During the encounter, more of these sporadic bursts were observed along with relatively continuous radio emissions extending down to 10 kHz, and a sporadic narrowband radio signal with f near 5 kHz. As Voyager passed through the ring plane, the plasma wave investigation recorded a large number of dust impacts. The Voyager 2 plasma wave instrument also detected many strong electromagnetic and electrostatic plasma waves, with intensity peaks in the region within 12 Uranus radii. These waves have characteristics that can interact strongly with the local plasma and with the trapped energetic particles, leading to precipitation into the atmosphere, charged particle acceleration, and charged particle diffusion. In addition, strong wave activity was detected in the region of the bow and shock and moderate levels in the magnetic tail.

Scarf, F. L.↗

Parameterization of Cloud Optical Properties for a Mixture of Ice Particles for use in Atmospheric Models

Based on the single-scattering optical properties that are pre-computed using an improve geometric optics method, the bulk mass absorption coefficient, single-scattering albedo, and asymmetry factor of ice particles have been parameterized as a function of the mean effective particle size of a mixture of ice habits. The parameterization has been applied to compute fluxes for sample clouds with various particle size distributions and assumed mixtures of particle habits. Compared to the parameterization for a single habit of hexagonal column, the solar heating of clouds computed with the parameterization for a mixture of habits is smaller due to a smaller cosingle-scattering albedo. Whereas the net downward fluxes at the TOA and surface are larger due to a larger asymmetry factor. The maximum difference in the cloud heating rate is approx. 0.2 C per day, which occurs in clouds with an optical thickness greater than 3 and the solar zenith angle less than 45 degrees. Flux difference is less than 10 W per square meters for the optical thickness ranging from 0.6 to 10 and the entire range of the solar zenith angle. The maximum flux difference is approximately 3%, which occurs around an optical thickness of 1 and at high solar zenith angles.

Chou, Ming-Dah↗

Atmospheric Ionization by Solar Particles Detected by Nitrate Measurements in Antarctic Snow. FY91 AASERT

The odd nitrogen source strengths associated with Solar Proton Events (SPEs), Galactic Cosmic Rays (GCRs), and the oxidation of nitrous oxide in the Earth's middle atmosphere from 1974 through 1993 have been compared globally, at middle and lower latitudes (less than 50 deg), and polar regions (greater than 50 deg) with a two-dimensional (2-D) photochemical transport model. As discovered previously, the oxidation of nitrous oxide dominates the global odd nitrogen source while GCRs and SPEs are significant at polar latitudes. The horizontal transport of odd nitrogen, produced by the oxidation of nitrous oxide at latitudes < 50 deg, was found to be the dominant source of odd nitrogen in the polar regions with GCRs contributing substantially during the entire solar cycle. The source of odd nitrogen from SPEs was more sporadic; however, contributions during several years (mostly near solar maximum) were significant in the polar middle atmosphere.

Vitt, Francis M.↗

Atmospheric Effects of Energetic Particle Precipitation in the Arctic Winter 1978-1979 Revisited

The Limb Infrared Monitor of the Stratosphere (LIMS) measured polar stratospheric enhancements of NO2 mixing ratios due to energetic particle precipitation (EPP) in the Arctic winter of 1978-1979. Recently reprocessed LIMS data are compared to more recent measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) to place the LIMS measurements in the context of current observations. The amount of NOx (NO + NO2) entering the stratosphere that has been created by EPP in the mesosphere and lower thermosphere (EPP-NOx) has been quantified for the 1978-1979 and 2002-2003 through 2008-2009 Arctic winters. The NO2 enhancements in the LIMS data are similar to those in MIPAS and ACE-FTS data in the Arctic winters of 2002-2003, 2004-2005, 2006-2007, and 2007-2008. The largest enhancement by far is in 2003-2004 (approximately 2.2 Gmol at 1500 K), which is attributed to a combination of elevated EPP and unusual dynamics that led to strong descent in the upper stratosphere/lower mesosphere in late winter. The enhancements in 2005-2006 and 2008-2009, during which large stratospheric NOx enhancements were caused by a dynamical situation similar to that in 2003 2004, are larger than in all the other years (except 2003-2004) at 3000 K. However, by 2000 K the enhancements in 2005-2006 (2008-2009) are on the same order of magnitude as (smaller than) all other years. These results highlight the importance of the timing of the descent in determining the potential of EPP-NOx for reaching the middle stratosphere.

Holt, L. A.↗

Step Catalysis to Synthesize Fossil-Free Ammonia at Atmospheric Pressure (Final Technical Report)

Affordable fossil-free ammonia synthesis will enable high-yield sustainable crop production for a growing world population while preserving the planet and making the best use of water and land. Simple technology amenable to intermittent operation using renewable energy will be made available through step catalysis activating dinitrogen at atmospheric pressure by nitride formation. Project objectives: (1) At the single particle level, quantify and analyze N2 activation by doped or alloyed manganese macroscopic- and nano particles at atmospheric pressure, (2) Quantify and analyze ammonia synthesis from doped or alloyed metal nitride particles when contacting them with hydrogen at atmospheric pressure, and (3) Integrate experimental data and atomic-level computational models to predict the behavior of metal alloys in nitrogen activation and subsequent ammonia synthesis.

10 SYNTHETIC FUELS↗

Radiative Effects of Aerosols Generated from Biomass Burning, Dust Storms, and Forest Fires

Atmospheric aerosol particles, both natural and anthropogenic, are important to the earth's radiative balance. They scatter the incoming solar radiation and modify the shortwave reflective properties of clouds by acting as Cloud Condensation Nuclei (CCN). Although it has been recognized that aerosols exert a net cooling influence on climate (Twomey et al. 1984), this effect has received much less attention than the radiative forcings due to clouds and greenhouse gases. The radiative forcing due to aerosols is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign (Houghton et al. 1990). Atmospheric aerosol particles generated from biomass burning, dust storms and forest fires are important regional climatic variables. A recent study by Penner et al. (1992) proposed that smoke particles from biomass burning may have a significant impact on the global radiation balance. They estimate that about 114 Tg of smoke is produced per year in the tropics through biomass burning. The direct and indirect effects of smoke aerosol due to biomass burning could add up globally to a cooling effect as large as 2 W/sq m. Ackerman and Chung (1992) used model calculations and the Earth Radiation Budget Experiment (ERBE) data to show that in comparison to clear days, the heavy dust loading over the Saudi Arabian peninsula can change the Top of the Atmosphere (TOA) clear sky shortwave and longwave radiant exitance by 40-90 W/sq m and 5-20 W/sq m, respectively. Large particle concentrations produced from these types of events often are found with optical thicknesses greater than one. These aerosol particles are transported across considerable distances from the source (Fraser et al. 1984). and they could perturb the radiative balance significantly. In this study, the regional radiative effects of aerosols produced from biomass burning, dust storms and forest fires are examined using the Advanced Very High Resolution Radiometer (AVHRR) Local Area Coverage (LAC) data and the instantaneous scanner ERBE data from the NOAA-9 and NOAA-10 satellites.

Christopher Sundar A.↗

Application of advanced causal analyses to identify processes governing secondary organic aerosols

Abstract Understanding how different physical and chemical atmospheric processes affect the formation of fine particles has been a persistent challenge. Inferring causal relations between the various measured features affecting the formation of secondary organic aerosol (SOA) particles is complicated since correlations between variables do not necessarily imply causality. Here, we apply a state-of-the-art information transfer measure coupled with the Koopman operator framework to infer causal relations between isoprene epoxydiol SOA (IEPOX-SOA) and different chemistry and meteorological variables derived from detailed regional model predictions over the Amazon rainforest. IEPOX-SOA represents one of the most complex SOA formation pathways and is formed by the interactions between natural biogenic isoprene emissions and anthropogenic emissions affecting sulfate, acidity and particle water. Since the regional model captures the known relations of IEPOX-SOA with different chemistry and meteorological features, their simulated time series implicitly include their causal relations. We show that our causal model successfully infers the known major causal relations between total particle phase 2-methyl tetrols (the dominant component of IEPOX-SOA over the Amazon) and input features. We provide the first proof of concept that the application of our causal model better identifies causal relations compared to correlation and random forest analyses performed over the same dataset. Our work has tremendous implications, as our methodology of causal discovery could be used to identify unknown processes and features affecting fine particles and atmospheric chemistry in the Earth’s atmosphere.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Particle-Charge Spectrometer

An instrument for rapidly measuring the electric charges and sizes (from approximately 1 to approximately 100 micrometers) of airborne particles is undergoing development. Conceived for monitoring atmospheric dust particles on Mars, instruments like this one could also be used on Earth to monitor natural and artificial aerosols in diverse indoor and outdoor settings for example, volcanic regions, clean rooms, powder-processing machinery, and spray-coating facilities. The instrument incorporates a commercially available, low-noise, ultrasensitive charge-sensing preamplifier circuit. The input terminal of this circuit--the gate of a field-effect transistor--is connected to a Faraday-cage cylindrical electrode. The charged particles of interest are suspended in air or other suitable gas that is made to flow along the axis of the cylindrical electrode without touching the electrode. The flow can be channeled and generated by any of several alternative means; in the prototype of this instrument, the gas is drawn along a glass capillary tube (see upper part of figure) coaxial with the electrode. The size of a particle affects its rate of acceleration in the flow and thus affects the timing and shape of the corresponding signal peak generated by the charge-sensing amplifier. The charge affects the magnitude (and thus also the shape) of the signal peak. Thus, the signal peak (see figure) conveys information on both the size and electric charge of a sensed particle. In experiments thus far, the instrument has been found to be capable of measuring individual aerosol particle charges of magnitude greater than 350 e (where e is the fundamental unit of electric charge) with a precision of +/- 150 e. The instrument can sample particles at a rate as high as several thousand per second.

Fuerstenau, Stephen↗

Global Atmospheric Aerosol Modeling

Global aerosol models are used to study the distribution and properties of atmospheric aerosol particles as well as their effects on clouds, atmospheric chemistry, radiation, and climate. The present article provides an overview of the basic concepts of global atmospheric aerosol modeling and shows some examples from a global aerosol simulation. Particular emphasis is placed on the simulation of aerosol particles and their effects within global climate models.

Hendricks, Johannes↗

Properties and effects of dust particles suspended in the Martian atmosphere

Direct measurements of the optical depth above the two Viking landers are presented for a period covering the summer, fall, and winter seasons in the Northern Hemisphere, a time period during which two global dust storms occurred. The data are used to define the properties of suspended dust particles in the Martian atmosphere and to assess their role in a number of meteorological and geological processes. Major conclusions are that (1) both the radiative effects of dust particles and the thermodynamical effects of large-scale atmospheric motions have a significant impact on the vertical temperature structure; (2) Pertinent feedback effects play an important part in the generation of some local dust storms, in the expansion of local dust storms to global proportions, and in the subsequent decay of global dust storms; (3) An important mechanism for the removal of dust particles from the atmosphere is the CO2 condensation-sedimentation process; and (4) that the polar laminae are constructed from atmospheric dust and water ice is hypothesized.

Pollack, J. B.↗

High resolution variability in wet deposition in the southeastern United States

Rainwater chemistry is determined by atmospheric pollutants and particles which vary spatially and temporally. Industrial and agricultural activities and meteorological events (e.g. sea breezes, severe weather, blowing dust) alter atmospheric particle and trace gas compositions. These gases and particles are scavenged by cloud and rain droplets that drive wet deposition. During an Intensive Operation Period (IOP) from April to October 2021, rainwater was collected at higher frequency intervals, usually daily, after precipitation events at three locations on the Savannah River Site (SRS). The farthest locations were separated by approximately 20 km. The mean concentration (μeq/L) of seven ions followed the Cl⁻ > SO 4 2− > Na⁺ > NO 3 ⁻ > K⁺ > Mg 2+ > Ca 2+ downward trend. Ion concentrations were compared to background ion concentrations from the National Atmospheric Deposition Program (NADP). The high frequency monthly averaged SRS data compared well with the monthly averaged NADP background but demonstrated extensive variability. In some months in 2021, the high frequency data compared better to the NADP site near the coast while in other months inland sites compared better. Strong spatial variability for ion concentrations was observed across SRS which was attributed to localized impacts in rainfall spatial variability. High frequency measurements allowed for comparison to regional weather patterns indicating influences from the Atlantic Ocean, Gulf of Mexico, and cities. This can account for spatial variability in the wet deposition flux. Sea breezes, Saharan dust, and anthropogenic sources were shown to impact wet deposition flux variability. Higher frequency precipitation chemistry sampling at numerous locations better captures ion concentration variability and improves measurement representativeness.

54 ENVIRONMENTAL SCIENCES↗

Chapter 11 - Aerosol–Radiation Interactions

This chapter describes the aerosol–radiation interactions of absorption, scattering, and emission of electromagnetic radiation by atmospheric aerosol particles, which alter the fluxes of radiative energy in the atmosphere. The chapter begins by defining some fundamental processes, including the particle physical and optical properties that determine the amount of light scattered and absorbed. It then outlines the factors that determine the radiative effect of aerosol–radiation interactions in the atmosphere, including the solar zenith angle, the properties of underlying surfaces, the influence of clouds, and atmospheric temperature, and humidity profiles. It defines the magnitude of the aerosol radiative effect on the climate system as well as the radiative forcing over the industrial period determined from satellite measurements and models for clear-sky and all-sky conditions.

scattering absorption↗

Evaluation of energetic particle effects on BUV data and atmospheric ozone

To aid investigations of energetic particle effects on the backscattered ultraviolet (BUV) instrumentation aboard Nimbus 4, solar proton events characterized as polar cap absorption events occurring in the period April 1970 to April 1976 were summarized. Energetic particle effects on total ozone above the 4 mb pressure level measured by Nimbus 4 were analyzed. Proceedings of a workshop meeting of operation aurorozone are included as background material for possible effects of bremsstrahlung on atmospheric ozone.

Herman, J. R.↗