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DOE OSTI2015

Quantifying Diurnal Cloud Radiative Effects by Cloud Type in the Tropical Western Pacific

Cloud radiative effects are examined using long-term datasets collected at the three Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facilities in the tropical western Pacific. We quantify the surface radiation budget, cloud populations, and cloud radiative effects by partitioning the data by cloud type, time of day, and as a function of large scale modes of variability such as El Niño Southern Oscillation (ENSO) phase and wet/dry seasons at Darwin. The novel facet of our analysis is that we break aggregate cloud radiative effects down by cloud type across the diurnal cycle. The Nauru cloud populations and subsequently the surface radiation budget are strongly impacted by ENSO variability whereas the cloud populations over Manus only shift slightly in response to changes in ENSO phase. The Darwin site exhibits large seasonal monsoon related variations. We show that while deeper convective clouds have a strong conditional influence on the radiation reaching the surface, their limited frequency reduces their aggregate radiative impact. The largest source of shortwave cloud radiative effects at all three sites comes from low clouds. We use the observations to demonstrate that potential model biases in the amplitude of the diurnal cycle and mean cloud frequency would lead to larger errors in the surface energy budget compared to biases in the timing of the diurnal cycle of cloud frequency. Our results provide solid benchmarks to evaluate model simulations of cloud radiative effects in the tropics.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1986

Study of the ammonia ice cloud layer in the north tropical zone of Jupiter from the infrared interferometric experiment on Voyager

An average of 51 Voyager 1 IRIS spectra of Jupiter's North Tropical Zone was analyzed to infer the abundance, vertical extent, and size distribution of the particles making up the ammonia cloud in this region. It is assumed that the cloud base coincides with the level at which 100% saturation of ammonia vapor occurs. The vertical distribution of particulates above this level is determined by assuming a constant total ammonia mixing ratio and adjusting the two phases so that the vapor is saturated throughout the cloud. A constant scaling factor then adjusts the base number density. A radiative transfer program is used that includes the effects of absorption and emission of all relevant gases as well as anisotropic scattering by cloud particles. Mie scattering from a gaussian particle size distribution is assumed. The vertical thermal structure is inferred from a temperature retrieval program that utilizes the collision induced S(0) and S(1) molecular hydrogen lines between 300 and 700.cm, and the 1304.cm methane band.

Shaffer, William A.↗

DOE OSTI2018

New particle formation leads to cloud dimming

New particle formation (NPF), nucleation of condensable vapors to the solid or liquid phase, is a significant source of atmospheric aerosol particle number concentrations. With sufficient growth, these nucleated particles may be a significant source of cloud condensation nuclei (CCN), thus altering cloud albedo, structure, and lifetimes, and insolation reaching the Earth's surface. Herein we present one of the first numerical experiments to quantify the impact of NPF on cloud radiative properties that is conducted at a convection permitting resolution and that explicitly simulates cloud droplet number concentrations. Consistent with observations, these simulations suggest that in spring over the Midwestern U.S.A., NPF occurs frequently and on regional scales. However, the simulations suggest that NPF is not associated with enhancement of regional cloud albedos as would be expected from an increase of CCN. These simulations indicate that NPF reduces ambient sulfuric acid concentrations sufficiently to inhibit growth of preexisting particles to CCN sizes. This reduction in CCN-sized particles reduces cloud albedo, resulting in a domain average positive top of atmosphere cloud radiative forcing of 10 W m-2 and up to ~ 50 W m-2 in individual grid cells relative to a simulation in which NPF is excluded.

Sullivan, Ryan C. (ORCID:0000000235001842)↗

NASA NTRS1983

Airborne measurements of Space Shuttle exhaust constituents

Airborne measurements of hydrogen chloride (HCl) and particulates made during penetrations into and flights under Space Shuttle exhaust clouds from launches STS-1, -2, and -5 are presented to permit comparison with dispersion model predictions for Space Shuttle exhaust clouds, and with previous measurements made in Titan III exhaust clouds. Analytical techniques employed for the Shuttle measurements were developed and refined during earlier Titan III exhaust cloud measurements and include the measurements of particulate concentrations, size distributions, and the partitioning of HCl between the gaseous and aerosol phases. The results are useful in understanding the dynamics of ground cloud development, atmospheric dispersion, and potential environmental effects of Shuttle effluents.

Cofer, W. R., III↗

DOE OSTI2026

Investigating the Impacts of Aqueous-Phase Processing on Organic Aerosol Chemical Climatology Using ARM and ASR Observations

This project improved understanding of how atmospheric aerosol particles form and evolve, with a focus on the role of water-driven (aqueous-phase) chemical reactions in the atmosphere. These processes occur in clouds, fog, and humid air and can significantly change the composition and properties of airborne particles, known as aerosols, which influence air quality and climate. By combining field measurements, laboratory experiments, and advanced analytical techniques, the project identified key chemical signatures that allow scientists to distinguish particles formed through aqueous processes from those formed in the gas phase. Observations from multiple environments, including wildfire smoke, urban regions, and cloud-influenced areas, show that aqueous chemistry is an important pathway for particle formation and aging. The project also developed new measurement approaches using uncrewed aerial systems (UAS) to capture how aerosol composition varies with altitude, providing critical insights into how particles interact with clouds. In addition, new data analysis frameworks were created to better interpret long-term aerosol measurements and improve characterization of particle sources and transformations. These results have been integrated into a global database of aerosol measurements and used to support atmospheric modeling efforts. Overall, the project provides important tools and knowledge to improve predictions of how aerosols affect climate and air quality, particularly through their interactions with radiation and clouds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1987

The International Satellite Cloud Climatology Project - Preliminary results and its potential aspects

The ISCCP (International Satellite Cloud Climatology Project) began its operational data collection phase on July 1, 1983. Considerable research efforts ensured that the compression of basic satellite data did not reduce the information content on cloudiness. At present an operational algorithm has been developed and tested with data from several months, whereas a target for very intensive use by the research community the data from April 1985 are selected. These concur with a simultaneous data set of the ERBE. Special efforts are now underway to map also clouds over both polar regions and may lead to the development of new specific algorithms. Several preliminary results are presented in this paper.

Raschke, E.↗

DOE OSTI2015

Fast Transverse Instability and Electron Cloud Measurements in Fermilab Recycler

A new transverse instability is observed that may limit the proton intensity in the Fermilab Recycler. The instability is fast, leading to a beam-abort loss within two hundred turns. The instability primarily affects the first high-intensity batch from the Fermilab Booster in each Recycler cycle. This paper analyzes the dynamical features of the destabilized beam. The instability excites a horizontal betatron oscillation which couples into the vertical motion and also causes transverse emittance growth. This paper describes the feasibility of electron cloud as the mechanism for this instability and presents the first measurements of the electron cloud in the Fermilab Recycler. Direct measurements of the electron cloud are made using a retarding field analyzer (RFA) newly installed in the Fermilab Recycler. Indirect measurements of the electron cloud are made by propagating a microwave carrier signal through the beampipe and analyzing the phase modulation of the signal. The maximum betatron amplitude growth and the maximum electron cloud signal occur during minimums of the bunch length oscillation.

43 PARTICLE ACCELERATORS↗

DOE OSTI2023

Dark photon superradiance: Electrodynamics and multimessenger signals

We study the electrodynamics of a kinetically mixed dark photon cloud that forms through superradiance around a spinning black hole, and design strategies to search for the resulting multimessenger signals. A dark photon superradiance cloud sources a rotating dark electromagnetic field which, through kinetic mixing, induces a rotating visible electromagnetic field. Standard model charged particles entering this field initiate a transient phase of particle production that populates a plasma inside the cloud and leads to a system which shares qualitative features with a pulsar magnetosphere. We study the electrodynamics of the dark photon cloud with resistive magnetohydrodynamics methods applicable to highly magnetized plasma, adapting techniques from simulations of pulsar magnetospheres. We identify turbulent magnetic field reconnection as the main source of dissipation and electromagnetic emission, and compute the peak luminosity from clouds around solar-mass black holes to be as large as 10 43 erg/s for observationally allowed dark photon parameter space. The emission is expected to have a significant x-ray component and to potentially be periodic, with period set by the dark photon mass. The luminosity is comparable to the brightest x-ray sources in the Universe, allowing for searches at distances of up to hundreds of Mpc with existing telescopes. Finally, we discuss observational strategies, including targeted electromagnetic follow-ups of solar-mass black hole mergers and targeted continuous gravitational wave searches of anomalous pulsars.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

Harvard Bounce Apparatus GoAmazon 2014/15 Field Campaign Report

The effect of relative humidity (RH) on the physical state of particulate matter during the GoAmazon 2014/15 campaign was investigated through the use of particle rebound (or lack thereof) during impaction. The physics governing particle rebound have been previously modeled and can be attributed to the surface and material properties. The physical state of secondary organic material is regulated by several factors, including the local RH, the recent RH history in the case of hysteresis, and chemical composition. Across the range of atmospheric RH, hygroscopic water uptake can occur and transitions from higher to lower viscosity phases are possible. By varying the particulate matter water content and observing particle rebound as a function of RH, the phase state of the organic material under investigation can be determined. Custom-made impactors were employed to study the effects of RH (up to 95%) on the particle physical state. Results inferred from the particle rebound measurements indicate that, under ambient conditions (RH >80%), particulate matter in Amazonia can be considered in a liquid phase state. However, during certain time periods, a fraction (10 to 30%) of particulate matter is found to rebound during the highest RH conditions, which indicates the presence of hydrophobic particles. The source of the hydrophobic particulates appears to be anthropogenic, from either biomass burning or the Manaus plume.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Cloud Coalescence: A Dynamical Instability Affecting Multiphase Environments

Mass and size distributions are the key characteristics of any astrophysical object, including the densest clumps comprising the cold phase of multiphase environments. In our recent papers, we showed how individual clouds of various sizes form and evolve in active galactic nuclei. In particular, we showed that large clouds undergo damped oscillations as a response to their formation process. Here we follow up this investigation, addressing how different size clouds interact. We find that smaller clouds become trapped in the advective flows generated by larger clouds. The explanation for this behavior leads to a rather remarkable conclusion: even in the absence of gravity, complexes of clouds are dynamically unstable. In an idealized environment (e.g., one free of turbulence and magnetic fields) a perfectly symmetric arrangement of static clouds will remain static, but any small spatial perturbation will lead to all clouds coalescing into a single, large cloud, given enough time. Here, by using numerical simulations, we investigate the main factors that determine the rate of coalescence. In addition to the cloud separation distance, we find that the transient response of clouds to a disturbance is the primary factor. Turbulent motions in the flow can easily suppress this tendency for spatially well-separated clouds to coalesce, so it is as yet unclear if this phenomenon can occur in nature. Nevertheless, this Letter casts strong doubts on a recent hypothesis that large clouds are prone to fragmentation.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

Characterization of Organosulfates and Organonitrates in Vertically Resolved Aerosols over the Southern Great Plains Field Campaign Report

Aerosol is the largest individual source of uncertainty in assessing the Earth’s radiative balance due to poorly understood aerosol processes and aerosol-cloud interactions. Thus, to constrain aerosol’s climate impacts, it is critical to understand aerosol compositions at high elevations. Organic material accounts for about 20-80% of total aerosol mass in the atmosphere and is known to play a key role in aerosol processes and cloud formation. In prior research, characterization of aerosol molecular composition has been mostly carried out at ground level. In these ground-level measurements, total speciated organosulfates and organonitrates may contribute significantly to organic aerosol mass on the order of 10-40%, most of which are from abundant biogenic volatile organic compounds such as isoprene and monoterpenes. Organosulfates and organonitrates have also been shown to be present in substantial amounts in cloud water, suggesting that they can be transported and/or directly formed at high elevations. On the other hand, the less common and more expensive aircraft studies have performed high-altitude measurements, but were often limited in the number of different altitudes sampled and in sample collection under consistent conditions. Therefore, the vertical distributions of key aerosol components such as organosulfates and organonitrates are not well understood and have not been extensively studied. Nevertheless, it is important to understand how organosulfates and organonitrates in aerosols are distributed, transformed, participate in aqueous-phase processes, and interact with high-altitude clouds.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2015

IPRT Polarized Radiative Transfer Model Intercomparison Project-Phase A

The polarization state of electromagnetic radiation scattered by atmospheric particles such as aerosols, cloud droplets, or ice crystals contains much more information about the optical and microphysical properties than the total intensity alone. For this reason an increasing number of polarimetric observations are performed from space, from the ground and from aircraft. Polarized radiative transfer models are required to interpret and analyse these measurements and to develop retrieval algorithms exploiting polarimetric observations. In the last years a large number of new codes have been developed, mostly for specific applications. Benchmark results are available for specific cases, but not for more sophisticated scenarios including polarized surface reflection and multi-layer atmospheres. The International Polarized Radiative Transfer (IPRT) working group of the International Radiation Commission (IRC) has initiated a model intercomparison project in order to fill this gap. This paper presents the results of the first phase A of the IPRT project which includes ten test cases, from simple setups with only one layer and Rayleigh scattering to rather sophisticated setups with a cloud embedded in a standard atmosphere above an ocean surface. All scenarios in the first phase A of the intercomparison project are for a one-dimensional plane-parallel model geometry. The commonly established benchmark results are available at the IPRT website

radiative transfer↗

NASA NTRS1993

Homogeneous ice nucleation and supercooled liquid water in orographic wave clouds

This study investigates ice nucleation mechanisms in cold lenticular wave clouds, a cloud type characterized by quasi-steady-state air motions and microphysical properties. It is concluded that homogeneous ice nucleation is responsible for the ice production in these clouds at temperatures below about -33 C. The lack of ice nucleation observed above -33 C indicates a dearth of ice-forming nuclei, and hence heterogeneous ice nucleation, in these clouds. Aircraft measurements in the temperature range -31 to -41 C show the following complement of simultaneous and abrupt changes in cloud properties that indicate a transition from the liquid phase to ice: disappearance of liquid water; decrease in relative humidity from near water saturation to ice saturation; increase in mean particle size; change in particle concentration; and change in temperature due to the release of latent heat. A numerical model of cloud particle growth and homogeneous ice nucleation is used to aid in interpretation of our in situ measurements. The abrupt changes in observed cloud properties compare favorably, both qualitatively and quantitatively, with results from the homogeneous ice nucleation model. It is shown that the homogeneous ice nucleation rates from the measurements are consistent with the temperature-dependent rates employed by the model (within a factor of 100, corresponding to about 1 C in temperature) in the temperature range -35 deg to -38 C. Given the theoretical basis of the modeled rates, it may be reasonable to apply them throughout the -30 to -50 C temperature range considered by the theory.

Heymsfield, Andrew J.↗

DOE OSTI2016

A MULTIPLE SCATTERING POLARIZED RADIATIVE TRANSFER MODEL: APPLICATION TO HD 189733b

We present a multiple scattering vector radiative transfer model that produces disk integrated, full phase polarized light curves for reflected light from an exoplanetary atmosphere. We validate our model against results from published analytical and computational models and discuss a small number of cases relevant to the existing and possible near-future observations of the exoplanet HD 189733b. HD 189733b is arguably the most well observed exoplanet to date and the only exoplanet to be observed in polarized light, yet it is debated if the planet’s atmosphere is cloudy or clear. We model reflected light from clear atmospheres with Rayleigh scattering, and cloudy or hazy atmospheres with Mie and fractal aggregate particles. We show that clear and cloudy atmospheres have large differences in polarized light as compared to simple flux measurements, though existing observations are insufficient to make this distinction. Futhermore, we show that atmospheres that are spatially inhomogeneous, such as being partially covered by clouds or hazes, exhibit larger contrasts in polarized light when compared to clear atmospheres. This effect can potentially be used to identify patchy clouds in exoplanets. Given a set of full phase polarimetric measurements, this model can constrain the geometric albedo, properties of scattering particles in the atmosphere, and the longitude of the ascending node of the orbit. The model is used to interpret new polarimetric observations of HD 189733b in a companion paper.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1995

Improvements of an ice-phase microphysics parameterization for use in numerical simulations of tropical convection

It is important to properly simulate the extent and ice water content of tropical anvil clouds in numerical models that explicitly include cloud formation because of the significant effects that these clouds have on the radiation budget. For this reason, a commonly used bulk ice-phase microphysics parameterization was modified to more realistically simulate some of the microphysical processes that occur in tropical anvil clouds. Cloud ice growth by the Bergeron process and the associated formation of snow were revised. The characteristics of graupel were also modified in accord with a previous study. Numerical simulations of a tropical squall line demonstrate that the amount of cloud ice and the extent of anvil clouds are increased to more realistic values by the first two changes.

Krueger, Steven K.↗

NASA NTRS2008

Cloud-Resolved Simulations of Lightning NOx in an Observed Hector Thunderstorm

Cloud chemistry simulations are being performed for a "Hector" storm observed on 16 November 2005 during the SCOUT-03lACTIVE campaigns based in Darwin, Australia. The primary objective of these simulations is to estimate the average production of NO per lightning flash during the storm. The 3-D WRF-AqChem model is being used for these calculations. This modeling package contains the WRF nonhydrostatic cloud-resolving model, online gas- and aqueous-phase chemistry, and a lightning algorithm (Barth et al., 2007). Early morning soundings of temperature, water vapor and winds are used to initialize the model. Surface heating of the Tiwi Islands is simulated in the model to induce convection. Observations from the Egrett, Falcon, Geophysica, and Dornier aircraft in air undisturbed by the storm are used to construct composite initial condition chemical profiles. Convective transport in the model is tested using tracer species such as CO and O3. Lightning flashes observed by the LINET network are input to the model and a lightning placement scheme is used to inject the resulting NO into the simulated cloud. Various scenarios of NO production per flash are used for cloud-to-ground and intracloud flashes in a series of simulations for the storm. Resulting NO, mixing ratios from each simulation are compared with upper tropospheric anvil observations (from the Geophysica and Egrett aircraft) to determine the best fit with the mean NOx at anvil altitudes, the profile shape, and the frequency distribution of NOx values. We will compare the results for lightning NO production from this tropical thunderstorm with similar analyses conducted for several midlatitude and subtropical convective events.

Pickering, Kenneth↗

NASA NTRS1994

Interstellar Ice and Dust: The Feedstock of the Solar System

Studying the chemical and isotopic composition of interstellar ice and dust provides insight into the composition and chemical history of the solid bodies in the solar nebula and the nature of the material subsequently brought into the inner part of the solar system by comets and meteorites. It is now possible to probe the composition of these microscopic interstellar particles (some hundreds of light years away), thanks to substantial progress in two areas: astronomical spectroscopic techniques in the middle-infrared, the spectral region most diagnostic of composition; and laboratory simulations which realistically reproduce the critical conditions in various interstellar environments. High quality infrared spectra of many different astronomical sources, some associated with dark molecular clouds, and others in the diffuse interstellar medium (DISM) are now available. What comparisons of these spectra with laboratory spectra tell us about the complex organic components of these materials is the subject of this talk. Most interstellar material is concentrated in large molecular clouds where simple molecules are formed by gas phase and dust grain surface reactions. Gaseous species (except H2) striking the cold (10K) dust will stick, forming an icy grain mantle. This accretion, coupled with energetic particle bombardment and UV photolysis, will produce a complex chemical mixture containing volatile, non-volatile, and isotopically fractionated species. One can compare spectra of the diffuse and dense interstellar medium with the spectra of analogs produced in the laboratory under conditions which mimic those in these different environments. In this way one can determine the composition and abundances of the major constituents present and place general constraints on the types and relative abundances of organics coating the grains. Ices in dense clouds contain H2O, CH3OH, CO, perhaps some NH3 and H2CO, as well as nitriles and ketones or esters. There is some evidence that the later, more complex species, are also present on the grains in the DISM. The evidence for these materials, in addition to carbon rich materials such as amorphous carbon, microdiamonds, and polycyclic aromatic hydrocarbons will be reviewed and the possible connection with meteoritic organics will be discussed.

Allamandola, L. J.↗

NASA NTRS1995

Astronomical Problems and Laboratory Solutions

Studying the chemical and isotopic composition of interstellar ice and dust provides insight into the composition and chemical history of the solid bodies in the solar nebula and the nature of the material subsequently brought into the inner part of the solar system by comets and meteorites. It is now possible to probe the composition of these microscopic interstellar particles (some hundreds of light years away), thanks to substantial progress in two areas: astronomical spectroscopic techniques in the middle-infrared, the spectral region most diagnostic of composition; and laboratory simulations which realistically reproduce the critical conditions in various interstellar environments. High quality infrared spectra of many different astronomical sources, some associated with dark molecular clouds, and others in the diffuse interstellar medium (DISM) are now available. What comparisons of these spectra with laboratory spectra tell us about the complex organic components of these materials is the subject of this talk. Most interstellar material is concentrated in large molecular clouds where simple molecules are formed by gas phase and dust grain surface reactions. Gaseous species (except H2) striking the cold (10K) dust will stick, forming an icy grain mantle. This accretion, coupled with energetic particle bombardment and UV photolysis, will produce a complex chemical mixture containing volatile, non-volatile, and isotopically fractionated species. One can compare spectra of the diffuse and dense interstellar medium with the spectra of analogs produced in the laboratory under conditions which mimic those in these different environments. In this way one can determine the composition and abundances of the major constituents present and place general constraints on the types and relative abundances of organics coating the grains. Ices in dense clouds contain H2O, CH3OH, CO, perhaps some NH3 and H2CO, as well as nitriles and ketones or esters. there is some evidence that the later, more complex species, are also present on the grains in the DISM. The evidence for these materials, in addition to carbon rich materials such as amorphous carbon, microdiamonds, and polycyclic aromatic hydrocarbons will be reviewed and the possible connection with meteoritic organics will be discussed.

Allamandola, L. J.↗