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At least 451 records · Page 25

Evaluation and improvement of the parameterization of aerosol hygroscopicity in global climate models using in-situ surface measurements (Final Report)

Aerosols are tiny particles suspended on the atmosphere that can interact with incoming solar radiation and affect the Earth radiative budget. They do so by scattering and absorbing solar radiation, and these properties vary depending on the aerosol size and chemical composition. Moreover, by taking up water from the surrounding air, hygroscopic aerosol particles will grow in size and change their chemical composition, thus modifying their optical properties (scattering and absorption) and their final impact on radiative forcing calculations. An accurate knowledge of aerosol hygroscopicity is crucial for estimating the net radiative impact of aerosols. We took a three-pronged approach to improve our understanding of aerosol hygroscopicity and how it is implemented in Earth system models. In the first part of our project, we developed a benchmark dataset from existing aerosol hygroscopic growth measurements made by tandem nephelometer humidogram systems. We analyzed, using a standardized methodology, observations from 26 in-situ stations around the globe. Measurement data was collected from multiple data providers, reviewed and harmonized to create a consistent dataset of the scattering enhancement factor due to aerosol water uptake. This dataset is archived in several publicly available databases for use by interested researchers. In the second part of the project, we used the benchmark hygroscopicity dataset to perform a global study on aerosol hygroscopicity and aerosol optical properties. Measurements show a global picture of scattering enhancement with larger values for Arctic and marine sites and lower for urban and desert sites. We assessed the RH dependence of aerosol radiative forcing and showed that the overall effect of aerosol hygroscopicity on DARF is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 compared to dry conditions (RH<40%). Finally, we explored using aerosol single scattering albedo (SSA) and scattering Angstrom exponent (SAE) as possible proxies for aerosol hygroscopicity. SSA showed more promise as a surrogate for the scattering enhancement factor than SAE, but neither was ideal. In the third part of the project we evaluated the output of ten Earth system models (ESMs) against the benchmark hygroscopicity dataset. ESMs utilize various schemes for aerosol hygroscopicity which had not been previously tested against observations on a global scale. We found that ESMs currently overestimate scattering enhancement due to hygroscopic growth. Model parameterizations of hygroscopicity and model chemistry are two main factors driving the observed diversity in hygroscopicity simulations among the models. In addition, our study makes several suggestions for modelers, including improving the parameterizations of organic and sea salt aerosol hygroscopicity. Future hygroscopicity model evaluation experiments should include the model data related to particles size which was not available for our study.

54 ENVIRONMENTAL SCIENCES↗

Atmospheric Aerosols

Aerosols, defined as particles and droplets suspended in air, are always present in the atmosphere. They are part of the earth-atmosphere climate system, because they interact with both incoming solar and outgoing terrestrial radiation. They do this directly through scattering and absorption, and indirectly through effects on clouds. Submicrometer aerosols usually predominate in terms of number of particles per unit volume of air. They have dimensions close to the wavelengths of visible light, and thus scatter radiation from the sun very effectively. They are produced in the atmosphere by chemical reactions of sulfur-, nitrogen- and carbon-containing gases of both natural and anthropogenic origins. Light absorption is dominated by particles containing elemental carbon (soot), produced by incomplete combustion of fossil fuels and by biomass burning. Light-scattering dominates globally, although absorption can be significant at high latitudes, particularly over highly reflective snow- or ice-covered surfaces. Other aerosol substances that may be locally important are those from volcanic eruptions, wildfires and windblown dust.

Pueschel, R. F.↗

Rayleigh, Raman and particulate scattering

Analysis of the visible and near infrared spectra of planetary atmospheres and the multiple scattering of photons within the atmosphere are discussed. Photons detected within the spectral region are solar photons which were scattered by the gas and particles in the planetary atmosphere. An example is given for the incident and emitted fluxes for a hypothetical planet with an effective temperature of 100 K. The absorption spectrum of the planetary atmosphere is discussed in terms of the various scattering processes photons undergo within the atmosphere. Three different physical processes are considered. Rayleigh scattering and Raman scattering by the gas molecules, and scattering by any cloud or dust aerosol particles in the atmosphere. The physics of each of these processes is examined.

Cochran, W. D.↗

Long-Term Land-Atmosphere Studies in Northern Alabama

A new multiyear research effort in northern Alabama will gather data on how clouds, vegetation, and tiny aerosol particles in the atmosphere interact to affect local weather and Earth’s climate.

54 ENVIRONMENTAL SCIENCES↗

The Co2 Profile and Analytical Model for the Pioneer Venus Large Probe Neutral Mass Spectrometer

We present a significantly updated CO2 altitude profile for Venus (64.2–0.9 km) and provide support for a potential deep lower atmospheric haze of particles (≤17 km). We extracted this information by developing a new analytical model for mass spectra obtained by the Pioneer Venus Large Probe (PVLP) Neutral Mass Spectrometer (LNMS). Our model accounts for changes in LNMS configuration and output during descent and enables the disentanglement of isobaric species via a data fitting routine that adjusts for mass-dependent changes in peak shape. The model yields CO2 in units of density (kg m−3), isotope ratios for 13C/12C and 18O/16O, and 14 measures of CO2 density across 55.4–0.9 km, which represents the most complete altitude profile for CO2 at ≤60 km to date. The CO2 density profile is also consistent with the pressure, temperature, and volumetric gas measurements from the PVLP and VeNeRa spacecraft. Nominal and low-noise operations for the LNMS mass analyzer are supported by the behaviors (e.g., ionization yields, fragmentation yields, and peak shapes) of several internal standards (e.g., CH3+, CH4+, 40Ar+, 136Xe2+, and 136Xe+), which were tracked across the descent. Lastly, our review of the CO2 profile and LNMS spectra reveals hitherto unreported partial and rapidly clearing clogs of the inlet in the lower atmosphere, along with several ensuing data spikes at multiple masses. Together, these observations suggest that atmospheric intake was impacted by particles at ≤17 km and that rapid particle degradation at the inlet yielded a temporary influx of mass signals into the LNMS.

Venus↗

Using Cosmic Ray Muons to Assess Geological Characteristics in the Subsurface

Cosmic rays are energetic nuclei and elementary particles that originate from stars and intergalactic events. The interaction of these particles with the upper atmosphere produces a wide range of secondary particles that reach the surface of the earth, of which muons are the most prominent. With enough energy, muons can travel up to a few kilometers beneath the surface of the earth before being stopped completely. The terrestrial muon flux profile and associated zenith angle can be utilized to determine geological characteristics of a location (e.g., rock overburden and density) without having to use conventional methods such as boreholes. This work uses a low-power plastic scintillator-based muon detection system as a prototype for this non-destructive geological assay methodology. Four custom designed 102 cm x 51 cm x 5 cm plastic scintillation panels are used to realize two orthogonal detection planes. Optical photons from each scintillation panel are read using OnSemi J-Series 4x4 silicon photomultiplier (SiPM) arrays in conjunction with preamplifiers. Simultaneous triggers between detectors from two planes indicate a coincidence event which is recorded using the QuarkNet data acquisition system (DAQ) from Fermi National Accelerator Laboratory. A custom detector holder was designed to securely mount the detection system and rotate the panels along the zenith to collect data at variable angles. In order to quantify the systematic uncertainties associated with the detector, such as energy depositions and angular resolution of the detector design, a Monte Carlo (MC) simulation using Geant4 is being developed. Cosmic ray flux prediction will be included in the project by adding the CORSIKA MC code to the simulation toolchain. Simulated and experimental data will drive the development and validation of a reconstruction algorithm that, upon completion, is expected to predict average overburden and rock density. Extended detector exposure to muons can be used as a means to understand changes in the surrounding environment like rock porosity. On the experimental front, muons will initially be measured at the surface, establishing the baseline flux. This is followed by recording the muon flux at variable depths and zenith angles, where the data will be used by the reconstruction algorithm to predict the overburden. The result will be benchmarked against geological surveys. The measured flux data will also be used to benchmark independent and established models. Successful proof-of-concept demonstration of this technology can open doors for long term non-invasive geological monitoring. The detector design, experimental methodology, and the benchmarking efforts are detailed in this work.

Gadey, Harish Reddy↗

Extreme Molecular Complexity Resulting in a Continuum of Carbonaceous Species in Biomass Burning Tar Balls from Wildfire Smoke

Biomass burning emits a wide range of carbonaceous particles into the atmosphere and has negative impacts on human health and the Earth’s radiative balance. Nonvolatile spherical organic aerosol particles, commonly known as tar balls, represent one of the most abundant particles in aged biomass burning smoke. However, the detailed molecular-level composition of ambient tar balls is largely unknown but critical to access their environmental impacts. Ambient aerosol samples collected during a wildfire event, which were ~90% tar balls by number fraction, were analyzed using ultrahigh resolution Orbitrap Elite mass spectrometry with four complementary ionization modes. Our results show the molecular composition of tar balls to be complex, composed of over 10,000 molecular formulas. Model estimated saturation mass concentrations and relative humidity dependent glass transition temperatures were consistent with low volatility and solid morphology as expected for tar balls. Room-temperature evaporation kinetics showed that these particles were composed of ~90% non-volatile species. The molecular complexity detected here signifies a continuum of carbonaceous species, ranging from C3 to C45 with continuous ranges of oxygenation and hydrogen saturation for each Cn. Approximately 24% of molecular formulas were estimated the be highly aromatic, which could indicate chemical compounds with negative health effects, and which may contribute to visible light absorption. The carbon continuum observed here has significant implications for the molecular characterization of atmospheric organic matter. The level of complexity detected here should not be ignored in future studies and we demonstrate that multiple analytical methods may be required to suitably interpret this complexity on a molecular level.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Field Study of Nighttime Leakage Currents in Bifacial PV Modules: Correlation with Atmospheric Electric Field Data

Leakage currents measured on PV modules in the field originate from a potential difference between the modules' frame and the cells. They can be a relative indicator of Potential-Induced Degradation (PID) severity, especially when comparing the same module design in a different environment. As modules are not operating at night, no leakage current should be observed but our team has reported several events of nighttime leakage currents on bifacial PV modules. These events have been firstly observed during a thunderstorm that are characterized by strong atmospheric electrical field values. This lead us to believe that nighttime leakage currents could originate from the atmospheric electric charges. In this paper, we correlate nighttime leakage currents measured on bifacial PV modules with field mill data to identify the origin of nighttime leakage currents. Our results show that so far, no leakage currents at night occur when the atmospheric electric field is between 0 and 150–200 V/m (standard value for fair weather). As soon as the atmospheric electric field is out of this range, leakage currents are observed with or without rain involved. This suggests a transport of charged particles from the atmosphere to the modules' frame. A combination of heavy rain with strong atmospheric electric field results into high nighttime leakage currents with a magnitude up to 8 times higher than what observed during the day with -1500V applied. This is explained by an easier transport of the charged particles through the water droplets. Based on these results, leakage currents observed during the day might not be only due to the inherent potential difference between the frame and the cells depending on the atmospheric electric field activity. We believe that it should be taken into account in PID studies.

14 SOLAR ENERGY↗

Remote Detection of Biological Particles and Chemical Plumes Using UV Fluorescence Lidar

A lidar system based on ultraviolet (UV) laser induced fluorescence (LIF) was developed for the remote detection of atmospherically dispersed biological particles and chemical vapors. This UV fluorescence lidar has many potential applications for monitoring environmental pollution, industrial waste emission, agricultural insect control, illicit chemical processing, and military defense operations. The general goal of this work is to investigate the research issues associated with the long range detection and identification of chemicals, e.g. aromatic solvents and chemical precursors, and biological materials, e.g. bacillus thuringiensis (BT) and bacillus globiggi (BG). In the detection of biological particulates, we are particularly interested in extending the detection range of an existing solar-blind 248-nm lidar system. We are investigating the use of longer excitation laser wavelengths (i.e. lambda greater than 280-nm to have more favorable atmospheric light transmission characteristics) for improving detection range to better than 10 km. In the detection of chemical plumes, our main research objectives are to determine how accurately and sensitively a chemical plume can be located at range, and how well spectrally the chemical species can be measured to allow their identification.

J J Tiee↗

The Interaction of the Galilean Satellites with Jupiter's Magnetosphere

The Galileo orbiter has provided radio occultation measurements of the electron density profiles of the plasma surrounding lo and Europa. There have been six occultations of Io, providing twelve electron density profiles at various locations relative to the ram direction of the impinging particles of the Jupiter magnetosphere on Io, and eight profiles on Europa. The two satellites were found to have very different plasma environments, with Io having a proper ionosphere produced on top of an endogenous SO2 atmosphere by magnetospheric particle precipitation and solar EUV, while Europa has a tenuous plasma environment produced by the same mechanisms from an oxygen atmosphere itself also produced by sputtering of water ice from its surface by impinging magnetospheric particles. In both cases the observed electron density profiles are highly asymmetrical, with a compressed profile on the ram side, and an extended one on the wake side. The presence of several measurements for each satellite at different ram-to-wake directions provided data for estimating an approximate distribution of ionization from the ram direction to the wake direction.

Kliore, Arvydas J.↗

The Interaction of Io and Europa With Jupiter's Magnetosphere

The Galileo orbiter has provided radio occultation measurements of the electron density profiles of the plasma surrounding Io and Europa. There have been six occultations of Io, providing twelve electron density profiles at various locations relative to the ram direction of the impinging particles of the Jupiter magnetosphere on Io, and eight profiles on Europa. The two satellites were found to have very different plasma environments, with Io having a proper ionosphere produced on top of an endogenous SO2 atmosphere by magnetospheric particle precipitation and solar EUV, while Europa has a tenuous plasma environment produced by the same mechanisms from an oxygen atmosphere itself also produced by sputtering of water ice from its surface by impinging magnetospheric particles. In both cases the observed electron density profiles are highly asymmetrical, with a compressed profile on the ram side, and an extended one on the wake side. The presence of several measurements for each satellite at different ram-to-wake directions provided data for estimating an approximate distribution of ionization from the ram direction to the wake direction, which were compared with the results of MHD simulations.

Kliore, Arvydas J.↗

A numerical framework for simulating the atmospheric variability of supermicron marine biogenic ice nucleating particles

Abstract. We present a framework for estimating concentrations of episodically elevated high-temperature marine ice nucleating particles (INPs) in the sea surface microlayer and their subsequent emission into the atmospheric boundary layer. These episodic INPs have been observed in multiple ship-based and coastal field campaigns, but the processes controlling their ocean concentrations and transfer to the atmosphere are not yet fully understood. We use a combination of empirical constraints and simulation outputs from an Earth system model to explore different hypotheses for explaining the variability of INP concentrations, and the occurrence of episodic INPs, in the marine atmosphere. In our calculations, we examine the following two proposed oceanic sources of high-temperature INPs: heterotrophic bacteria and marine biopolymer aggregates (MBPAs). Furthermore, we assume that the emission of these INPs is determined by the production of supermicron sea spray aerosol formed from jet drops, with an entrainment probability that is described by Poisson statistics. The concentration of jet drops is derived from the number concentration of supermicron sea spray aerosol calculated from model runs. We then derive the resulting number concentrations of marine high-temperature INPs (at 253 K) in the atmospheric boundary layer and compare their variability to atmospheric observations of INP variability. Specifically, we compare against concentrations of episodically occurring high-temperature INPs observed during field campaigns in the Southern Ocean, the Equatorial Pacific, and the North Atlantic. In this case study, we evaluate our framework at 253 K because reliable observational data at this temperature are available across three different ocean regions, but suitable data are sparse at higher temperatures. We find that heterotrophic bacteria and MBPAs acting as INPs provide only a partial explanation for the observed high INP concentrations. We note, however, that there are still substantial knowledge gaps, particularly concerning the identity of the oceanic INPs contributing most frequently to episodic high-temperature INPs, their specific ice nucleation activity, and the enrichment of their concentrations during the sea–air transfer process. Therefore, targeted measurements investigating the composition of these marine INPs and drivers for their emissions are needed, ideally in combination with modeling studies focused on the potential cloud impacts of these high-temperature INPs.

54 ENVIRONMENTAL SCIENCES↗

Consolidated quarterly progress report

Planetary atmospheres, lunar structures, particle energy spectra, exobiology, space physiology, and engineering sciences - space sciences

PLANETARY ATMOSPHERE↗

Source apportionment of soot particles and aqueous-phase processing of black carbon coatings in an urban environment

Abstract. The impacts of soot particles on climate and human health depend on the concentration of black carbon (BC) as well as the thickness and composition of the coating material, i.e., organic and inorganic compounds internally mixed with BC. In this study, the size-resolved chemical composition of BC-containing aerosol was measured using a high-resolution soot particle aerosol mass spectrometer (SP-AMS) during wintertime in Fresno, California, a location influenced by abundant combustion emissions and frequent fog events. Concurrently, particle optical properties were measured to investigate the BC absorption enhancement. Positive matrix factorization (PMF) analysis was performed on the SP-AMS mass spectral measurements to explore the sources of soot particles and the atmospheric processes affecting the properties of BC coatings. The analysis revealed that residential woodburning and traffic are the dominant sources of soot particles. Alongside primary soot particles originating from biomass burning (BBOABC) and vehicles (HOABC) two distinct types of processed BC-containing aerosol were identified: fog-related oxidized organic aerosol (FOOABC) and winter-background OOABC (WOOABC). Both types of OOABC showed evidence of having undergone aqueous processing, albeit with differences. The concentration of FOOABC was substantially elevated during fog events, indicating the formation of aqueous secondary organic aerosol (aqSOA) within fog droplets. On the other hand, WOOABC was present at a relatively consistent concentration throughout the winter and was likely related to the formation of secondary organic aerosol (SOA) in both the gas phase and aerosol liquid water. By comparing the chemical properties and temporal variations in FOOABC and WOOABC, we gain insights into the key aging processes of BC aerosol. It was found that aqueous-phase reactions facilitated by fog droplets had a significant impact on the thickness and chemical composition of BC coatings, thereby affecting the light absorption and hygroscopic properties of soot particles. These findings underscore the important role of chemical reactions occurring within clouds and fogs and influencing the climate forcing of BC aerosol in the atmosphere.

54 ENVIRONMENTAL SCIENCES↗

Modeling the Entry of Micrometeoroids into the Atmospheres of Earth-like Planets

The temperature profiles of micrometeors entering the atmospheres of Earth-like planets are calculated to determine the altitude at which exogenous organic compounds may be released. Previous experiments have shown that flash-heated micrometeorite analogs release organic compounds at temperatures from roughly 500 to 1000 K [1]. The altitude of release is of great importance because it determines the fate of the compound. Organic compounds that are released deeper in the atmosphere are more likely to rapidly mix to lower altitudes where they can accumulate to higher abundances or form more complex molecules and/or aerosols. Variables that are explored here are particle size, entry angle, atmospheric density profiles, spectral type of the parent star, and planet mass. The problem reduces to these questions: (1) How much atmosphere does the particle pass through by the time it is heated to 500 K? (2) Is the atmosphere above sufficient to attenuate stellar UV such that the mixing timescale is shorter than the photochemical timescale for a particular compound? We present preliminary results that the effect of the planetary and particle parameters have on the altitude of organic release.

Pevyhouse, A. R.↗

Photochemical Haze Formation in the Atmospheres of Super-Earths and Mini-Neptunes

UV (ultraviolet) radiation can induce photochemical processes in the atmospheres of exoplanet and produce haze particles. Recent transmission spectra of super-Earths and mini-Neptunes have demonstrated the possibility that exoplanets have haze/cloud layers at high altitudes in their atmospheres. Haze particles play an important role in planetary atmospheres because they affect the chemistry, dynamics, and radiation flux in planetary atmospheres, and may provide a source of organic material to the surface which may impact the origin or evolution of life. However, very little information is known about photochemical processes in cool, high-metallicity exoplanetary atmospheres. We present here photochemical haze formation in laboratory simulation experiments with UV radiation; we explored temperatures ranging from 300 to 600 degrees Kelvin and a range of atmospheric metallicities (100 times, 1000 times, and 10000 times solar metallicity). We find that photochemical hazes are generated in all simulated atmospheres, but the haze production rates appear to be temperature dependent: the particles produced in each metallicity group decrease as the temperature increases. The images taken with an atomic force microscope (AFM) show that the particle size (15 nanometers to 190 nanometers) varies with temperature and metallicity. Our results provide useful laboratory data on the photochemical haze formation and particle properties, which can serve as critical inputs for exoplanet atmosphere modeling, and guide future observations of exoplanets with the Transiting Exoplanet Survey Satellite (TESS), the James Webb Space Telescope (JWST), and the Wide-Field Infrared Survey Telescope (WFIRST).

He, Chao↗

Chemical transport models often underestimate inorganic aerosol acidity in remote regions of the atmosphere

The inorganic fraction of fine particles affects numerous physicochemical processes in the atmosphere. However, there is large uncertainty in its burden and composition due to limited global measurements. Here, we present observations from eleven different aircraft campaigns from around the globe and investigate how aerosol pH and ammonium balance change from polluted to remote regions, such as over the oceans. Both parameters show increasing acidity with remoteness, at all altitudes, with pH decreasing from about 3 to about -1 and ammonium balance decreasing from almost 1 to nearly 0. We compare these observations against nine widely used chemical transport models and find that the simulations show more scatter (generally R 2 < 0.50) and typically predict less acidic aerosol in the most remote regions. These differences in observations and predictions are likely to result in underestimating the model-predicted direct radiative cooling effect for sulfate, nitrate, and ammonium aerosol by 15–39%.

54 ENVIRONMENTAL SCIENCES↗