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NASA NTRS2000

The Abundances of Solid N2 and Gaseous CO2 in Interstellar Dense Molecular Clouds

We present 2338-2322 per centimeter (4.277-4.307 micrometer) infrared spectra of a number of N2-containing mixed molecular ices and demonstrate that the strength of the infrared "forbidden" band due to the N=N stretch near 2328 per centimeter (4.295 micrometer) is extremely sensitive to the composition of the ice. The strength of the 2328 per centimeter N2 fundamental is significantly enhanced relative to that of pure N2 ice when NH3, H2O, or CO2 are present, but is largely unaffected by the presence of CO, CH4 or O2. We use the laboratory data in coil junction with ISO data that probes several lines-of-sight through dense molecular clouds to place limits on the abundance of interstellar solid phase N2 and the composition of the ices. Deriving upper limits is complicated by the presence of overlapping absorptions due to CO2 gas in the clouds and, in some cases, to photospheric CO in the background star. These upper limits are just beginning to be low enough to constrain interstellar grain models and the composition of possible N2-bearing interstellar ices. We outline the search criteria that will need to be met if solid interstellar N2 is to be detected in the future. We also discuss some of the implications of the presence of warm CO2 gas along the lines-of-sight to embedded protostars and demonstrate that its presence may help resolve certain puzzles associated with the previously derived gas/solid CO2 ratios and the relative abundances of polar and nonpolar ices towards these objects. Finally, we briefly comment on the possible implications of these results for the interpretation of N2 detections on outer solar system bodies.

Sandford, Scott A.↗

NASA NTRS2006

From Astrochemistry to Astrobiology ...... and Back Again

Tremendous strides have been made in our understanding of interstellar material over the past twenty five years thanks to significant developments in observational infrared astronomy and laboratory astrophysics. Twenty five years ago the composition of interstellar dust was largely guessed at, the concept of ices in dense molecular clouds generally ignored, and the notion of large, abundant, gas phase, carbon-rich molecules widespread throughout the interstellar medium (ISM) considered impossible. Today the composition of interstellar dust is reasonably well understood. In molecular clouds, the birthplace of stars and planets, these cold dust particles are coated with mixed molecular ices whose composition is reasonably well constrained. Lastly, the signature of carbon-rich polycyclic aromatic hydrocarbons (PAHs), shockingly large molecules by early interstellar chemistry standards, is widespread throughout the Universe. The first part of this talk will describe how infrared spectroscopic studies of interstellar space, combined with laboratory simulations and theoretical studies of PAHs and interstellar ices, have revealed the widespread presence of interstellar PAHs and the composition of interstellar precometary ices. The remainder of the presentation will focus on the photochemical evolution of these icy materials. Within a molecular cloud, and especially the presolar nebula, materials frozen into the ices are photoprocessed by ultraviolet light and more complex molecules are produced. As these materials are the building blocks of comets and related to carbonaceous micrometeorites, they are likely to be important sources of complex materials delivered to habitable planets and their composition may be related to the origin of life.

Allamandola, L. J.↗

DOE OSTI2019

Physical and Thermodynamic Properties of Secondary Organic Materials for Modeling (Final Technical Report)

Secondary organic material constitutes more than 50% of the submicron component of atmospheric aerosol particles. This organic material is produced by oxidation of biogenic and anthropogenic volatile organic compounds. The physicochemical properties of these aerosol particles and their variability with atmospheric conditions influence many climate-relevant endpoints, such as rates of chemical reactions, production of secondary organic material, number-diameter distributions, direct radiative forcing, and cloud condensation nuclei. The results of the project research highlight a nonlabile-to-labile transition for material representative of anthropogenic secondary organic particulate matter at a threshold humidity range. This behavior differs markedly from materials representing biogenic aerosol sources, which lack such a transition. More specifically, the mass lability of atmospheric organic particulate matter, meaning its tendency to evaporate, is an important property in the mechanisms governing the climate effects. This property is affected by both the volatility and the molecular diffusivity of the constituent organic species. Via a series of laboratory experiments, the project directly determined the mass labilities of films of secondary organic material representative of anthropogenic and biogenic organic particulate matter (PM). The evaporation rates for anthropogenic organic PM increased above a threshold relative humidity (RH) between 20% and 30%, indicating rapid partitioning above a transition RH. Below the threshold, the characteristic time for equilibration was estimated at up to 1 week for a typically sized particle. In contrast, for films representing biogenic PM, no RH threshold was observed, suggesting equilibrium partitioning is rapidly obtained for all RHs. The effective molecular diffusivity for the biogenic case was at least 1000 times greater than that of the anthropogenic case. The results allow for an improved representation of anthropogenic and biogenic secondary organic aerosol formation in climate models. The results of the project also provide new measurements on how organic aerosol particles take up water and serve as cloud condensation nuclei, thus explaining the observed complex thermodynamic behaviors using a simple thermodynamic model. The project results reconciled the discrepancy between sub-saturation hygroscopicity and super-saturation cloud condensation nuclei activity for organic aerosol particles. The key to the explanation is the phase separation between hydrophobic and hydrophilic organics and the induced surface tension lowering. The results are essential for the assessment of the aerosol indirect effect on climate. In more detail, hygroscopic growth and cloud condensation nuclei activation are key processes for accurately modeling the climate impacts of organic particulate matter. Nevertheless, the microphysical mechanisms of these processes remain unresolved. The project results focus on complex thermodynamic behaviors, including humidity-dependent hygroscopicity, diameter-dependent cloud condensation nuclei activity, and liquid-liquid phase separation in the laboratory for biogenically derived secondary organic material representative of similar atmospheric organic particulate matter. These behaviors can be explained by the non-ideal mixing of water with hydrophobic and hydrophilic organic components. The non-ideality-driven liquid-liquid phase separation further enhances water uptake and induces lowered surface tension at high relative humidity, which results in a lower barrier to cloud condensation nuclei activation. By comparison, secondary organic material representing anthropogenic sources does not exhibit complex thermodynamic behavior. The combined results highlight the importance of detailed thermodynamic representations of the hygroscopicity and cloud condensation nuclei activity in models of the Earth’s climate system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1987

The effects of stimulated star formation on the evolution of the galaxy. III - The chemical evolution of nonlinear systems

The evolution of models for star formation in galaxies with disk and halo components is discussed. Two phases for the halo (gas and stars) and three for the disk (including clouds) are used in these calculations. The star-formation history is followed using nonlinear phase-coupling models which completely determine the populations of the phases as a function of time. It is shown that for a wide range of parameters, including the effects of both spontaneous and stimulated star formation and mass exchange between the spatial components of the system, the observed chemical history of the galaxy can easily be obtained. The most sensitive parameter in the detailed metallicity and star-formation history for the system is the rate of return of gas to the diffuse phase upon stellar death.

Shore, Steven N.↗

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 OSTI2013

IONIZATION IN ATMOSPHERES OF BROWN DWARFS AND EXTRASOLAR PLANETS. III. BREAKDOWN CONDITIONS FOR MINERAL CLOUDS

Electric discharges were detected directly in the cloudy atmospheres of Earth, Jupiter, and Saturn, are debatable for Venus, and indirectly inferred for Neptune and Uranus in our solar system. Sprites (and other types of transient luminous events) have been detected only on Earth, and are theoretically predicted for Jupiter, Saturn, and Venus. Cloud formation is a common phenomenon in ultra-cool atmospheres such as in brown dwarf and extrasolar planetary atmospheres. Cloud particles can be expected to carry considerable charges which may trigger discharge events via small-scale processes between individual cloud particles (intra-cloud discharges) or large-scale processes between clouds (inter-cloud discharges). We investigate electrostatic breakdown characteristics, like critical field strengths and critical charge densities per surface, to demonstrate under which conditions mineral clouds undergo electric discharge events which may trigger or be responsible for sporadic X-ray emission. We apply results from our kinetic dust cloud formation model that is part of the DRIFT-PHOENIX model atmosphere simulations. We present a first investigation of the dependence of the breakdown conditions in brown dwarf and giant gas exoplanets on the local gas-phase chemistry, the effective temperature, and primordial gas-phase metallicity. Our results suggest that different intra-cloud discharge processes dominate at different heights inside mineral clouds: local coronal (point discharges) and small-scale sparks at the bottom region of the cloud where the gas density is high, and flow discharges and large-scale sparks near, and maybe above, the cloud top. The comparison of the thermal degree of ionization and the number density of cloud particles allows us to suggest the efficiency with which discharges will occur in planetary atmospheres.

79 ASTRONOMY AND ASTROPHYSICS↗

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 OSTI2013

Use of ARM observations and numerical models to determine radiative and latent heating profiles of mesoscale convective systems for general circulation models

We examined cloud radar data in monsoon climates, using cloud radars at Darwin in the Australian monsoon, on a ship in the Bay of Bengal in the South Asian monsoon, and at Niamey in the West African monsoon. We followed on with a more in-depth study of the continental MCSs over West Africa. We investigated whether the West African anvil clouds connected with squall line MCSs passing over the Niamey ARM site could be simulated in a numerical model by comparing the observed anvil clouds to anvil structures generated by the Weather Research and Forecasting (WRF) mesoscale model at high resolution using six different ice-phase microphysical schemes. We carried out further simulations with a cloud-resolving model forced by sounding network budgets over the Niamey region and over the northern Australian region. We have devoted some of the effort of this project to examining how well satellite data can determine the global breadth of the anvil cloud measurements obtained at the ARM ground sites. We next considered whether satellite data could be objectively analyzed to so that their large global measurement sets can be systematically related to the ARM measurements. Further differences were detailed between the land and ocean MCS anvil clouds by examining the interior structure of the anvils with the satellite-detected the CloudSat Cloud Profiling Radar (CPR). The satellite survey of anvil clouds in the Indo-Pacific region was continued to determine the role of MCSs in producing the cloud pattern associated with the MJO.

54 ENVIRONMENTAL SCIENCES↗

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↗