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IceCube: Demonstration of an 883 GHz Radiometer for Ice Cloud Remote Sensing

IceCube was a technology demonstration of an 883 GHz heterodyne radiometer on a 3U CubeSat for ice cloud characterization. The project was a collaboration between Goddard Space Flight Center, Virginia Diodes Inc., and Wallops Flight Facility. IceCube was launched to the International Space Station (ISS) in April 2017, and was deployed to the orbit in May 2017. The radiometer measured ice cloud emissions from an ISS orbit for over 15 months. IceCube generated the first 883 GHz cloud map over a large operation temperature range of (5 ºC—37 ºC). Cloud ice plays a major role in the cloud precipitation process and Earth’s energy budget. Ice clouds are used in global circulation models as tuning parameters to achieve model agreement with observation at the top of the atmosphere in the radiation budget and at the bottom for precipitation, however, due to a lack of accurate ice cloud measurements large uncertainties exist in these models. Submillimeter wave remote sensing is capable of addressing this issue by measuring cloud ice mass and microphysical properties in the middle-to-upper troposphere. This fills the sensitivity gap not covered by the visible/infrared and microwave sensors [1]. The goal of IceCube was to increase the TRL of a heterodyne 883 GHz radiometer (using commercial parts) from 5 to 7 by validating the performance in a relevant spaceflight environment. The design of the radiometer was driven by frequency of operation, bandwidth, calibration, available power, and thermal environment requirements. The design included a 15 mm aperture off-axis parabolic reflector with a Potter feed horn, an 883 GHz 2nd-harmonic mixer that is fed by a local oscillator chain with a 24.3 GHz dielectric resonator (MLA), followed by a 6 GHz bandwidth centered at 9 GHz intermediate frequency assembly (IFA), receiver interface card, and power distribution unit. The IFA included an internal noise diode calibration to separate the MLA performance from the rest of the system. For this the radiometer had four operational states: antenna, antenna + noise, reference, and reference + noise; each state’s duration was 10 ms. The total power dissipation of the instrument was 5.6 W. The spacecraft had spinning capabilities to provide a cold sky view for calibration. We present the instrument design, ground test results, challenges, and highlight some of the flight measurements.

N Ehsan↗
NASA NTRS1977

The atmosphere of Saturn - An infrared perspective

A model of the radiative portion of the equatorial atmosphere of Saturn, constrained by the infrared data of various observers, has been constructed using a technique which includes the variation of thermal flux with depth. The model has a high-altitude temperature inversion due to the absorption of ultraviolet sunlight. The inversion causes the observed infrared emission peaks at 8 microns (methane) and 12 microns (ethane). Mixing ratios of these gases to hydrogen are computed from these emission features. The bottom of the modeled region occurs at the radiative convective boundary. At this level, an opaque cloud consisting of solid ammonia condensation particles is postulated. Above the cloud is a thin haze, also composed of ammonia particles. The haze is required to match infrared observations near 9.5 microns and hydrogen quadrupole equivalent widths near 0.64 micron. Predictions of the model are given for further observational tests.

Caldwell, J.↗
DOE OSTI2025

Improved Representations of Longwave Surface Emissivity to Reduce Surface and Atmospheric Heating Biases in Earth System Models

Abstract Many Earth system models (ESMs) approximate surface emissivity as a broadband constant. This approximation reduces the computational burden, yet omits the spectral structure of emissivity and atmospheric absorption. Neglecting spectral variation in surface emission introduces biases in longwave (LW) atmospheric fluxes and heating. Biases are strongest over surfaces with strongly varying emissivity and minimal atmospheric opacity. We examine these biases over water, ice, and snow surfaces. We partition spectral emissivity into the 16 spectral bands utilized by a single‐column atmospheric radiative transfer model (RRTMG_LW) commonly used in ESMs. We quantify flux and heating biases introduced by broadband assumptions relative to the spectrally resolved case for standard atmospheric profiles over each surface type. Current assumptions tend to overestimate upwelling surface fluxes; for example, the greybody assumption overestimates flux by 1.6 W/m 2 (0.52%) at the bottom of a mid‐latitude winter atmosphere over ice, and by 2.33 (1.0%) at the top of atmosphere. The blackbody assumption tends to artificially cool Earth's surface, stabilizing the lower troposphere. Interestingly, the optimal broadband emissivity can deviate from the Planck‐weighted mean by up to 3% depending on surface type and atmospheric profile. We investigate bias sensitivity to surface temperature, cloud water path, and atmospheric water vapor. Bias is most sensitive to water vapor content, and least sensitive to cloud water path. Lastly, we show that a modified greybody method with updated broadband values can reduce total surface flux bias up to 1.69 , comparable to a five‐band approach and at a fraction of the computational cost.

Manzo, L. [Department of Earth System Science Univ↗
NASA NTRS2013

Vertical Structure of Ice Cloud Layers From CloudSat and CALIPSO Measurements and Comparison to NICAM Simulations

The shape of the vertical profile of ice cloud layers is examined using 4 months of CloudSat and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) global measurements taken on January, April, July, and October 2007. Ice clouds are selected using temperature profiles when the cloud base is located above the 253K temperature level. The obtained ice water content (IWC), effective radius, or extinction coefficient profiles are normalized by their layer mean values and are expressed in the normalized vertical coordinate, which is defined as 0 and 1 at the cloud base and top heights, respectively. Both CloudSat and CALIPSO observations show that the maximum in the IWC and extinction profiles shifts toward the cloud bottom, as the cloud depth increases. In addition, clouds with a base reaching the surface in a high-latitude region show that the maximum peak of the IWC and extinction profiles occurs near the surface, which is presumably due to snow precipitation. CloudSat measurements show that the seasonal difference in normalized cloud vertical profiles is not significant, whereas the normalized cloud vertical profile significantly varies depending on the cloud type and the presence of precipitation. It is further examined if the 7 day Nonhydrostatic Icosahedral Atmospheric Model (NICAM) simulation results from 25 December 2006 to 1 January 2007 generate similar cloud profile shapes. NICAM IWC profiles also show maximum peaks near the cloud bottom for thick cloud layers and maximum peaks at the cloud bottom for low-level clouds near the surface. It is inferred that oversized snow particles in the NICAM cloud scheme produce a more vertically inhomogeneous IWC profile than observations due to quick sedimentation.

Ham, Seung-Hee↗
NASA NTRS1981

Constraints on the composition of the Venus atmosphere from microwave measurements near 1.35 cm wavelength

The determination of the brightness temperature of Venus near 1.35 cm wavelength is reviewed. The observed brightness temperature is compared with models for the microwave emission based on the physical and chemical structure of the atmosphere as obtained from spacecraft. Upper limits are set on the concentrations of microwave-absorbing minor constituents. In particular, upper limits are determined for SO2 (180 ppm) and H2O (0.3%) for a mixing-ratio profile that is uniformly mixed up to the cloud bottom at 50 km and is rapidly depleted (scale height, approximately 1 km) at higher altitudes. The total optical depth of the cloud region at or above 50 km is less than 0.17 at 1.35 cm wavelength. The SO2 upper limit is only in marginal agreement with the spacecraft results, and it may be that the latter have been overestimated, or that the distribution of SO2 is more complex than given by the uniform mixing model.

Janssen, M. A.↗
NASA NTRS2002

Sensitivities of Modeled Tropical Cyclones to Surface Friction and the Coriolis Parameter

In this investigation the sensitivities of a 2-D tropical cyclone (TC) model to surface frictional coefficient and the Coriolis parameter are studied and their implication is discussed. The model used is an axisymmetric version of the latest version of the Goddard cloud ensemble model. The model has stretched vertical grids with 33 levels varying from 30 m near the bottom to 1140 m near the top. The vertical domain is about 21 km. The horizontal domain covers a radius of 962 km (770 grids) with a grid size of 1.25 km. The time step is 10 seconds. An open lateral boundary condition is used. The sea surface temperature is specified at 29C. Unless specified otherwise, the Coriolis parameter is set at its value at 15 deg N. The Newtonian cooling is used with a time scale of 12 hours. The reference vertical temperature profile used in the Newtonian cooling is that of Jordan. The Newtonian cooling models not only the effect of radiative processes but also the effect of processes with scale larger than that of TC. Our experiments showed that if the Newtonian cooling is replaced by a radiation package, the simulated TC is much weaker. The initial condition has a temperature uniform in the radial direction and its vertical profile is that of Jordan. The initial winds are a weak Rankin vortex in the tangential winds superimposed on a resting atmosphere. The initial sea level pressure is set at 1015 hPa everywhere. Since there is no surface pressure perturbation, the initial condition is not in gradient balance. This initial condition is enough to lead to cyclogenesis, but the initial stage (say, the first 24 hrs) is not considered to resemble anything observed. The control experiment reaches quasi-equilibration after about 10 days with an eye wall extending from 15 to 25 km radius, reasonable comparing with the observations. The maximum surface wind of more than 70 m/s is located at about 18 km radius. The minimum sea level pressure on day 10 is about 886 hPa. Thus the overall simulation is considered successful and the model is considered adequate for our investigation.

Chao, Winston C.↗
DOE OSTI2025

Optimizing energy yield of monolithic perovskite/silicon tandem solar cells in real-world Conditions: The impact of luminescent coupling

Efficient light management is key to maximizing power conversion efficiency (PCE) in monolithic perovskite/silicon tandem solar cells. Achieving peak efficiency requires closely matched current generation in all junctions, especially in integrated configurations. However, real-world conditions vary significantly due to factors such as sunlight spectrum, diffuse-to-direct sunlight ratio, angular distribution of light, subcell temperature coefficients, and ground reflection. This study introduces a comprehensive optical and device simulation to optimize perovskite/silicon tandem cells, considering experimental luminescent coupling (LC) efficiency and its dependence on working conditions, alongside variations in radiative recombination, effect of temperature on absorptivity spectra, and cloud cover. Our results show potential energy yield improvements of up to 1.4 % with LC, based on current perovskite radiative recombination records, and up to 4 % with direct bandgap materials. Although radiative recombination's dependence on excitation intensity reduces output power and requires thicker absorbers, LC compensates for these losses. LC also lowers the optimized bandgap for the perovskite top cell from 1.72 eV to 1.64–1.68 eV, or even lower in regions with redshifted irradiance. Additionally, optimization revealed that thinner silicon bottom cells require a higher perovskite top cell bandgap, impacting the balance between fabrication cost and cell stability.

14 SOLAR ENERGY↗
NASA NTRS2007

A Numerical Study of the Urban Heat Island in the Coastal Tropical City of San Juan, Puerto Rico: Model Validation and Impacts of LCLU Changes

Urban sprawls in tropical locations are rapidly accelerating and it is more evident in islands where a large percentage of the population resides along the coasts. This paper focuses on the analysis of the impacts of land use and land cover for urbanization in the tropical coastal city of San Juan, in the tropical island of Puerto Rico. A mesoscale numerical model, the Regional Atmospheric Modeling System (RAMS), is used to study specific characteristics and patterns of the urban heat island in the San Juan Metropolitan Area (SJMA), the most noticeable urban core of the Caribbean. The research present in this paper makes use of the observations obtained during the airborne San Juan Atlas Mission in two ways. First, surface and rawinsonde data are used to validate the atmospheric model yielding satisfactory results. Second, airborne remote sensing information is used to update the model's surface characteristics to obtain a detailed configuration of the SJMA in order to perform the LCLU changes impact analysis. This analysis showed that the presence of San Juan has an impact reflected in higher air temperatures over the area occupied by the city, with positive values of up to 2.5 C, for the simulations that have specified urban LCLU indexes in the bottom boundary. One interesting result of the impact analysis was the finding of a precipitation disturbance shown as a difference in total accumulated rainfall between simulation with the city and with a potential natural vegetation induced by the presence of the urban area. Model results indicate that the urban-induced cloud formation and precipitation development occur mainly downwind of the city, including the accumulated precipitation. This spatial pattern can be explained by the presence of a-larger urbanized area in the southwest sector of the city, and of the approaching northeasterly trade winds.

Comarazamy, Daniel E.↗
NASA NTRS2007

Impacts of Urbanization in the Coastal Tropical City of San Juan, Puerto Rico

Urban sprawl in tropical locations is rapidly accelerating and it is more evident in islands where a large percentage of the population resides along the coasts. This paper focuses on the analysis of the impacts of land use and land cover for urbanization in the tropical coastal city of San Juan, in the Caribbean island of Puerto Rico. A mesoscale numerical model, the Regional Atmospheric Modeling System (RAMS), is used to study the impacts of land use for urbanization in the environment including specific characteristics of the urban heat island in the San Juan Metropolitan Area (SJMA), one of the most noticeable urban cores of the Caribbean. The research also makes use of the observations obtained during the airborne San Juan Atlas Mission. Surface and rawinsonde data from the mission are used to validate the atmospheric model yielding satisfactory results. Airborne high resolution remote sensing data are used to update the model's surface characteristics in order to obtain a more accurate and detailed configuration of the SJMA and perform a climate impact analysis based on land cover/land use (LCLU) changes. The impact analysis showed that the presence of the urban landscape of San Juan has an impact reflected in higher air temperatures over the area occupied by the city, with positive values of up to 2.5 C, for the simulations that have specified urban LCLU indexes in the model's bottom boundary. One interesting result of the impact analysis was the finding of a precipitation disturbance shown as a difference in total accumulated rainfall between the present urban landscape and with a potential natural vegetation, apparently induced by the presence of the urban area. Results indicate that the urban enhanced cloud formation and precipitation development occur mainly downwind of the city, including the accumulated precipitation. This spatial pattern can be explained by the presence of a larger urbanized area in the southwest sector of the city, and of the approaching northeasterly trade winds. No significant impacts were found in the sea breeze patterns of the city.

Comarazamy, Daniel E.↗
NASA NTRS2007

Impacts of Urbanization in the Coastal Tropical City of San Juan, Puerto Rico

Urban sprawl in tropical locations is rapidly accelerating and it is more evident in islands where a large percentage of the population resides along the coasts. This paper focuses on the analysis of the impacts of land use and land cover for urbanization in the tropical coastal city of San Juan, in the Caribbean island of Puerto Rico. A mesoscale numerical model, the Regional Atmospheric Modeling System (RAMS), is used to study the impacts of land use for urbanization in the environment including specific characteristics of the urban heat island in the San Juan Metropolitan Area (SJMA), one of the most noticeable urban cores of the Caribbean. The research also makes use of the observations obtained during the airborne San Juan Atlas Mission. Surface and raw insonde data from the mission are used to validate the atmospheric model yielding satisfactory results. Airborne high resolution remote sensing data are used to update the model's surface characteristics in order to obtain a more accurate and detailed configuration of the SJMA and perform a climate impact analysis based on land cover/land use (LCLU) changes. The impact analysis showed that the presence of the urban landscape of San Juan has an impact reflected in higher air temperatures over the area occupied by the city, with positive values of up to 2.5 degrees C, for the simulations that have specified urban LCLU indexes in the model's bottom boundary. One interesting result of the impact analysis was the finding of a precipitation disturbance shown as a difference in total accumulated rainfall between the present urban landscape and with a potential natural vegetation, apparently induced by the presence of the urban area. Results indicate that the urban-enhanced cloud formation and precipitation development occur mainly downwind of the city, including the accumulated precipitation. This spatial pattern can be explained by the presence of a larger urbanized area in the southwest sector of the city, and of the approaching northeasterly trade winds.

Comarazamy, Daniel E.↗
NASA NTRS2006

Spitzer Spectroscopy of Low-Mass Dwarfs - Clouds and Chemistry at the Bottom of the IMF

Brown dwarfs and low-mass stars show evidence of complicated atmospheres, including a variety of molecular species and clouds. Infrared observations are one of the best probes of the physics of these objects, but up until recently these observations have been limited in studies from ground-based telescopes by atmospheric absorption and insufficient sensitivity. With the launch of the Spitzer Space Telescope with its Infrared Spectrograph (IRS) instrument we now have the capability to undertake a systematic study of the atmospheric structure and chemistry in these cool objects. The IRS Dim Suns team has compiled spectra from objects ranging from M1 dwarfs with effective temperatures 3,800K of down to T8 dwarfs with effective temperatures of 700. This talk will present these results and discuss their implications for our understanding of cool dwarf atmospheric physics and structure.

Roellig, Thomas L.↗
NASA NTRS1993

The correlation of alkalis and aluminum during high-temperature volatilization of albite and nepheline

Our previous study of high-temperature evaporation of mafic targets has shown a systematic enrichment of newly-formed condensates in silicon and alkalis and depletion in refractory elements (Al, Ca, Ti). This effect, which is consistent with the volatility of the elements, was also tested for several experiments with acidic targets. In one case it was the impact evaporation of granite targets using a light-gas gun facility. Analyses of the condensate which was collected during the impact show that it was enriched in Al and Na so that the composition of the condensate became close to nepheline. In the work of Nagahara, an incongruent evaporation of alkali feldspars under stationary conditions has been also proposed. These discoveries required a more detailed study of high-temperaure evaporation of monomineralic Al-silicate targets. In these experiments, we have used samples of oligoclase and of nepheline. Vaporization of samples was performed in a hermetic cell filled with helium at normal temperature and pressure using a powerful Nd-laser focused on the sample. Laser pulses had the following parameters: luminous energy approximately 600 J, duration approximately 10(exp -3) s, density of luminosity was approximately 5 x 10(exp 6) W/sq cm, the temperature of vaporization is about 3000-4000 K. About 4 cm from the sample, a nickel foil was placed on which the condensate was collected. Films of condensate were analyzed using X-Ray Photo-Electron spectrometer ES-2401. The measurement of internal chemical composition and of the charging state of elements through the whole depth of the condensed films was made layer by layer with argon-ion etching of 200 A of the film per step. Results of this study are given. The bottom layers of condensed film correspond to the front parts of the evaporated cloud or to condensation at the beginning of the evaporative process and surface layers to condensation at the end of the process.

Dikov, Yu. P.↗
NASA NTRS2010

Improved Cloud Condensation Nucleus Spectrometer

An improved thermal-gradient cloud condensation nucleus spectrometer (CCNS) has been designed to provide several enhancements over prior thermal- gradient counters, including fast response and high-sensitivity detection covering a wide range of supersaturations. CCNSs are used in laboratory research on the relationships among aerosols, supersaturation of air, and the formation of clouds. The operational characteristics of prior counters are such that it takes long times to determine aerosol critical supersaturations. Hence, there is a need for a CCNS capable of rapid scanning through a wide range of supersaturations. The present improved CCNS satisfies this need. The improved thermal-gradient CCNS (see Figure 1) incorporates the following notable features: a) The main chamber is bounded on the top and bottom by parallel thick copper plates, which are joined by a thermally conductive vertical wall on one side and a thermally nonconductive wall on the opposite side. b) To establish a temperature gradient needed to establish a supersaturation gradient, water at two different regulated temperatures is pumped through tubes along the edges of the copper plates at the thermally-nonconductive-wall side. Figure 2 presents an example of temperature and supersaturation gradients for one combination of regulated temperatures at the thermally-nonconductive-wall edges of the copper plates. c) To enable measurement of the temperature gradient, ten thermocouples are cemented to the external surfaces of the copper plates (five on the top plate and five on the bottom plate), spaced at equal intervals along the width axis of the main chamber near the outlet end. d) Pieces of filter paper or cotton felt are cemented onto the interior surfaces of the copper plates and, prior to each experimental run, are saturated with water to establish a supersaturation field inside the main chamber. e) A flow of monodisperse aerosol and a dilution flow of humid air are introduced into the main chamber at the inlet end. The inlet assembly is designed to offer improved (relative to prior such assemblies) laminar-flow performance within the main chamber. Dry aerosols are subjected to activation and growth in the supersaturation field. f) After aerosol activation, at the outlet end of the main chamber, a polished stainless-steel probe is used to sample droplets into a laser particle counter. The probe features an improved design for efficient sampling. The counter has six channels with size bins in the range of 0.5- to 5.0-micron diameter. g) To enable efficient sampling, the probe is scanned along the width axis of the main chamber (thereby effecting scanning along the temperature gradient and thereby, further, effecting scanning along the supersaturation gradient) by means of a computer-controlled translation stage.

Leu, Ming-Taun↗
NASA NTRS1990

An extremely carbon-poor planetary nebula in the Small Magellanic Cloud

An optical and ultraviolet study is presented of object 28 of Sanduleak et al. (1978) in the SMC. This object is an extreme type of I PN which apparently has undergone all three stages of nuclear dredge-up together with an appreciable amount of convective envelope burning. Optical and UV data are well-represented by a model in which the central star has a temperature of 180,000 K and a radius of 0.09 solar radius. A nebular mass of 0.71 solar mass and a central star mass of 0.65-0.71 solar mass are inferred. The object apparently evolved from a massive progenitor with main-sequence mass greater than five solar masses, which underwent both second and third nuclear dredge-up and very efficient hot bottom burning.

Meatheringham, Stephen J.↗
NASA NTRS2001

Venus Multiprobe Mission

A summary of the proposal for the Discovery Program Venus Multiprobe Mission (VMPM) which was submitted in 1994 will be presented. The major goal of the mission was to provide sufficient observations of winds and thermal structure in the Venus atmosphere that the mechanism producing the atmospheric superrotation could be identified. The superrotation has been a major unsolved problem of planetary science for over 30 years. In spite of many theoretical efforts and many spacecraft missions to Venus, the principal driving mechanism(s) remain undetermined. Sixteen small probes, modeled after the Pioneer Venus small probes, would enter the Venus atmosphere, and measure winds, temperatures, and pressures from 60 km to the surface. Towards the bottom of the atmosphere, measurements would be made at 10 meter intervals. Temperature and pressure measurements are similar to those used on Pioneer Venus, but are four times more sensitive. Winds would be obtained by dual-frequency, differential. long-baseline interferometry, using S- and X-band transmitters on the probes, and four receiving telescopes round the Pacific rim. The precision of wind measurements is 0.05 ms- 1 or better, at least twenty times more precise than for Pioneer Venus. Ground based observations occurring in conjunction with the multiprobe entries would provide a temporal context for the upper boundary to the probe observations. UV and near IR features would be tracked for periods of hours to weeks to obtain cloud level zonal mean and transient eddy circulations with accuracies of 10 /ms or better. The data would be processed into wind and opacity maps. A hierarchy of atmospheric numerical models would be used to distinguish different dynamical elements existing in the data. Primary among the models was the development of a Venus general circulation model containing all known physical processes.

Young, Richard E.↗
DOE OSTI2025

Exploring the impact of surface topography on Rayleigh-Bénard dry convection in the Pi cloud chamber using OpenFOAM: In cylindrical and rectangular geometries

The Pi convection-cloud chamber can generate steady-state turbulence in both rectangular and cylindrical shapes via Rayleigh-Bénard convection (RBC) by maintaining warm bottom and cold top surfaces. Although most experiments in the Pi chamber were conducted in cylindrical shapes, all previous Pi chamber simulations were conducted in a rectangular shape due to the limitations of those models to discretize a cylindrical domain when using the finite difference method therein. Here, we use OpenFOAM, an open-source finite-volume-based Computational Fluid Dynamics (CFD) software package, to conduct Large-Eddy Simulation (LES) of dry RBC in the Pi chamber at high Rayleigh numbers (10 8 to 10 9 ). Results show that large-scale circulation (LSC) direction varies in the chamber with a constant side wall temperature. Imposing a slight temperature imbalance at the side wall ranging from 0.1 to 0.7 degrees can lock the LSC, aligning better with Pi chamber observations, particularly at higher Rayleigh numbers. In addition, we examine the impact of surface topography on LSC and heat transfer in RBC systems within cylindrical and rectangular shapes under varying conditions. Results show that roughing top/bottom surfaces by adding bars of a few tens millimeters height can strengthen thermal plumes and enhance temperature fluctuations in the chamber. Furthermore, we observe that different bar height configurations lead to notable changes in LSC orientation and thermal stratification, highlighting the complex interactions between surface features and convection patterns. This finding highlights how surface topography and chamber geometry affect Rayleigh-Bénard convection, improving understanding of turbulent heat transfer and atmospheric boundary-layer processes. Direct Numerical Simulations (DNS) are also conducted to validate LES results. In conclusion, while LES effectively captures qualitative behaviors seen in DNS, it tends to underestimate velocity variances near walls, illustrating a trade-off between computational efficiency and accuracy.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Directed Gas-Phase Formation of Azulene (C 10 H 8 ): Unraveling the Bottom-Up Chemistry of Saddle-Shaped Aromatics

The azulene (C 10 H 8 ) molecule, the simplest polycyclic aromatic hydrocarbon (PAH) carrying a fused seven- and five-membered ring, is regarded as a fundamental molecular building block of saddle-shaped carbonaceous nanostructures such as curved nanographenes in the interstellar medium. However, an understanding of the underlying gas-phase formation mechanisms of this nonbenzenoid 10π-Hückel aromatic molecule under low-temperature conditions is in its infancy. Here, by merging crossed molecular beam experiments with electronic structure calculations and molecular dynamics simulations, our investigations unravel an unconventional low-temperature, barrierless route to azulene via the reaction of the simplest organic radical, methylidyne (CH), with indene (C 9 H 8 ) through ring expansion. This reaction might represent the initial step toward to the formation of saddle-shaped PAHs with seven-membered ring moieties in hydrocarbon-rich cold molecular clouds such as the Taurus Molecular Cloud-1 (TMC-1). These findings challenge conventional wisdom that molecular mass growth processes to nonplanar PAHs, especially those containing seven-membered rings, operate only at elevated pressure and high-temperature conditions, thus affording a versatile low-temperature route to contorted aromatics in our galaxy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1994

Clouds, hazes, and the stratospheric methane abundance in Neptune

Analysis of high-spatial-resolution (approximately 0.8 arcsec) methane band and continuum imagery of Neptune's relatively homogeneous Equatorial Region yields significant constraints on (1) the stratospheric gaseous methane mixing ratio (f(sub CH4, S)), (2) the column abundances and optical properties of stratospheric and tropospheric hydrocarbon hazes, and (3) the wavelength-dependent single-scattering albedo of the 3-bar opaque cloud. From the center-to-limb behavior of the 7270-A and 8900-A CH4 bands, the stratospheric methane mixing ratios is limited to f(sub CH4, S) less than 1.7 x 10(exp -3), with a nominal value of f(sub CH4, S) = 3.5 x 10(exp -4), one to two orders of magnitude less than pre-Voyager estimates, but in agreement with a number of recent ultraviolet and thermal infrared measurements, and largely in agreement with the tropopause mixing ratio implied by Voyager temperature measurements. Upper limits to the stratospheric haze mass column abundance and 6190-A and 8900-A haze opacities are 0.61 micrograms/sq cm and 0.075 and 0.042, respectively, with nominal values of 0.20 micrograms/sq cm and 0.025 and 0.014 for the 0.2 micrometers radius particles preferred by the recent Voyager PPS analysis of Pryor et al. (1992). The tropospheric CH4 haze opacities are comparable to that found in the stratosphere, i.e., upper limits of 0.104 and 0.065 at 6190 A and 8900 A, respectively, with nominal values of 0.085 and 0.058. This indicates a column abundance less than 11.0 micrograms/sq cm, corresponding to the methane gas content within a well-mixed 3% methane tropospheric layer only 0.1 cm thick near the 1.5-bar CH4 condensation level. Conservative scattering is ruled out for the opaque cloud near 3 bars marking the bottom of the visible atmosphere. Specifically, we find cloud single-scattering albedos of 0.915 +/- 0.006 at 6340 A, 0.775 +/- 0.012 at 7490 A, and 0.803 +/- 0.010 at 8260 A. Global models utilizing a complete global spectrum confirm the red-absorbing character of the 3-bar cloud. The global-mean model has approximately 7.7 times greater stratospheric aerosol content than the Equatorial Region. An analysis of stratospheric haze precipitation rates indicates a steady-state haze production rate of 0.185-1.5 x 10(exp -14) g/sq cm/s, in agreement with recent theoretical photochemical estimates. Finally, reanalysis of the Voyager PPS 7500-A phase angle data utilizing the f(sub CH4, S) value derived here confirms the Pryor et al. result of a tropospheric CH4 haze opacity of a few tenths in the 22-30 degs S latitude region, several times that of the Equatorial Region or of the globe. The factor-of-10 reduction in f(sub CH4, S) below that assumed by Pryor et al. implies decreased gas absorption and consequently a decrease in the forward-scattering component of tropospheric aerosols.

Baines, Kevin H.↗