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At least 1,531 records · Page 85
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

HETEROGENEITY IN {sup 12}CO/{sup 13}CO ABUNDANCE RATIOS TOWARD SOLAR-TYPE YOUNG STELLAR OBJECTS

This study reports an unusual heterogeneity in [{sup 12}C{sup 16}O]/[{sup 13}C{sup 16}O] abundance ratios of carbon monoxide observed in the gas phase toward seven ∼solar-mass young stellar objects (YSOs) and three dense foreground clouds in the nearby star-forming regions, Ophiuchus, Corona Australis, Orion, and Vela, and an isolated core, L43. Robust isotope ratios were derived using infrared absorption spectroscopy of the 4.7 μm fundamental and 2.3 μm overtone rovibrational bands of CO at very high spectral resolution (λ/Δλ ≈ 95,000), observed with the Cryogenic Infrared Echelle Spectrograph (CRIRES) on the Very Large Telescope. We find [{sup 12}C{sup 16}O]/[{sup 13}C{sup 16}O] values ranging from ∼85 to 165, significantly higher than those of the local interstellar medium (ISM) (∼65–69). These observations are evidence for isotopic heterogeneity in carbon reservoirs in solar-type YSO environments, and encourage the need for refined galactic chemical evolution models to explain the {sup 12}C/{sup 13}C discrepancy between the solar system and local ISM. The oxygen isotope ratios are consistent with isotopologue-specific photodissociation by CO self-shielding toward the disks, VV CrA N and HL Tau, further substantiating models predicting CO self-shielding on disk surfaces. However, we find that CO self-shielding is an unlikely general explanation for the high [{sup 12}C{sup 16}O]/[{sup 13}C{sup 16}O] ratios observed in this study. Comparison of the solid CO against gas-phase [{sup 12}C{sup 16}O]/[{sup 13}C{sup 16}O] suggests that interactions between CO ice and gas reservoirs need to be further investigated as at least a partial explanation for the unusually high [{sup 12}C{sup 16}O]/[{sup 13}C{sup 16}O] observed.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS2002

Monte Carlo Radiative Transfer Modeling of Lightning Observed in Galileo Images of Jupiter

We study lightning on Jupiter and the clouds illuminated by the lightning using images taken by the Galileo orbiter. The Galileo images have a resolution of 25 km/pixel and axe able to resolve the shape of the single lightning spots in the images, which have full widths at half the maximum intensity in the range of 90-160 km. We compare the measured lightning flash images with simulated images produced by our ED Monte Carlo light-scattering model. The model calculates Monte Carlo scattering of photons in a ED opacity distribution. During each scattering event, light is partially absorbed. The new direction of the photon after scattering is chosen according to a Henyey-Greenstein phase function. An image from each direction is produced by accumulating photons emerging from the cloud in a small range (bins) of emission angles. Lightning bolts are modeled either as points or vertical lines. Our results suggest that some of the observed scattering patterns axe produced in a 3-D cloud rather than in a plane-parallel cloud layer. Lightning is estimated to occur at least as deep as the bottom of the expected water cloud. For the six cases studied, we find that the clouds above the lightning are optically thick (tau > 5). Jovian flashes are more regular and circular than the largest terrestrial flashes observed from space. On Jupiter there is nothing equivalent to the 30-40-km horizontal flashes which axe seen on Earth.

Dyudine, U. A.↗
NASA NTRS1981

Microphysical development of a pulsating cumulus tower - A case study

In-cloud microphysical data collected within a 22-minute period during seven consecutive passes at the -13 C sampling level of a deep (base +22 C) convective cloud provide observational evidence for a secondary ice production mechanism at work in the Florida environment. The observed microphysical characteristics of the convective tower, particularly the spatial distribution and habit of the ice phase relative to the updraft, are consistent with a rime-splintering hypothesis for secondary ice production. It is shown that the cloud's updraft structure is critically important in governing the timing of the ice production by controlling the flux of graupel particles through the critical temperature zone (-3 C to -8 C). The importance of the cloud's pulsation growth dynamics on the microphysics is emphasized, particularly as it relates to rapidly glaciating cumuli.

Keller, V. W.↗
DOE OSTI2023

Science Plan for the Deployment of the Third ARM Mobile Facility to the Southeastern United States at the Bankhead National Forest, Alabama (AMF3 BNF)

In 2018, the U.S. Department of Energy (DOE) held a workshop for the Atmospheric Radiation Measurement (ARM) (Mather and Voyles 2013) user facility to discuss critical climate challenges and locations where key ARM Mobile Facility (AMF) observational assets could impact Earth system modeling (ESM). As an outcome, the southeast United States (SE U.S.) was identified as a high-priority region to target climate-process studies that promote a deeper understanding of the climate system and bolster ARM interactions with the community to drive ESM advancement. The DOE ARM user facility is a globally recognized leader in deploying and operating strategically located observation sites around the world for studying the properties of aerosols and clouds and their interaction with radiation, precipitation, and the Earth’s surface. In partnering with the DOE Atmospheric System Research (ASR) program, ARM solicited a multi-agency Site Science Team approach to provide input and close interaction with ARM management towards a successful SE U.S. deployment of the ARM third Mobile Facility (AMF3) (Miller et al. 2016). These efforts included identifying key locations, science drivers and instruments, and measurement strategies to address the wider climate-process needs and ESM improvement. Community input served a vital role in establishing, refining, and informing the relevant drivers and decisions regarding this AMF3 deployment. The team has identified Northern Alabama (N. AL) as regionally representative to unlock the key opportunities that will improve our understanding and model representation of aerosol, cloud, and land-surface processes and their couplings in the SE U.S. A defining aspect of the AMF3 deployment is its commitment to long-term (anticipated five-year) observations to mitigate potential seasonal-to-annual variability that often limits appropriate attribution of phenomena to local or larger-scale processes. The proposed location may leverage nearby surface networks and multi-agency and partner assets to enrich this multi-year deployment. One motivation is to understand the role of spatiotemporal variability (thermodynamic, land-surface) across aspects of the climate system, with our AMF3 team anticipating future demands on characterizing the relationships between local-to-regional cloud development and surface processes across a diverse patchwork of natural, managed, and urban landscapes as found throughout the N. AL regions. The main site targets an intact, representative, forested region – the Bankhead National Forest (BNF) – underscoring further team commitment to regionally important land-atmosphere two-way interactive studies “from the canopy to the clouds”, with enhanced tower instrumentation augmenting traditional ARM capabilities adjacent to this site. Multiple supplemental sites will also be distributed across this region, prioritizing added needs for biodiversity. Anticipated high-priority cloud science themes will target N. AL as a regional SE U.S. hotbed for high-impact weather, convective cloud onset, and shallow-to-deep cloud transitioning. Anticipated aerosol drivers will focus on chemical processes that control the evolution of organic aerosol, the seasonality and spatial distribution of water vapor and particle-phase water, and its role on aerosol optical properties. Anticipated land-atmosphere drivers consider the two-way feedbacks between surface influence on aerosols, clouds, and precipitation properties and the associated radiative impacts on plant physiology and canopy-scale fluxes. Emphasis will include the study of the impact of surface processes on aerosols via precursor emission, and on clouds via moisture flux and thermal development.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1994

H2-rich interstellar grain mantles: An equilibrium description

Experiments simulating the codeposition of molecular hydrogen and water ice on interstellar grains demonstrate that amorphous water ice at 12 K can incorporate a substantial amount of H2, up to a mole ratio of H2/H2O = 0.53. We find that the physical behavior of approximately 80% of the hydrogen can be explained satisfactorily in terms of an equilibrium population, thermodynamically governed by a wide distribution of binding site energies. Such a description predicts that gas phase accretion could lead to mole fractions of H2 in interstellar grain mantles of nearly 0.3; for the probable conditions of WL5 in the rho Ophiuchi cloud, an H2 mole fraction of between 0.05 and 0.3 is predicted, in possible agreement with the observed abundance reported by Sandford, Allamandola, & Geballe. Accretion of gas phase H2 onto grain mantles, rather than photochemical production of H2 within the ice, could be a general explanation for frozen H2 in interstellar ices. We speculate on the implications of such a composition for grain mantle chemistry and physics.

Dissly, Richard W.↗
NASA NTRS1977

Io's sodium emission profiles - Variations due to Io's phase and magnetic latitude

We present recent measurements of high-resolution sodium D2 emission line profiles of Io's atmosphere and cloud. The high-velocity skirts of these profiles are strongest when Io is on the magnetic equator where protons and heavy ions, which sputter atoms from Io's surface, are concentrated. The skirts are most prominent on the long-wavelength side of the line when Io is west of Jupiter, and they are most prominent on the short-wavelength side of the line when Io is east of Jupiter. Our observations also indicate that there is a shift in the emission peak with respect to Io which is correlated with Io's orbital phase angle.

Trafton, L.↗
NASA NTRS1994

Far-ultraviolet emission from the Taurus molecular cloud

Far-ultraviolet spectra of diffuse emission from a region in the Taurus molecular cloud are presented. These data were obtained with the Berkeley spectrometer on NASA's Ultraviolet Experiment (UVX) payload. The intensity of the continuum emission drops as the optical depth increases toward the denser part of the cloud, an effect which is the opposite of that observed for the diffuse flux at high galactic latitudes. At the center of the aperture, the optical depth is very large, and the continuum emission must be produced by backscattering. At the edges of the cloud, the continuum intensity rises by a factor of 2. The data are interpreted with a new radiative transfer model, which is significantly more sophisticated than its predecessors. If the grain scattering properties are constant across the cloud, a unique best-fit combination can be determined from the data. The best-fit albedo is 0.6 +/- 0.1 at 1600 A. The best-fit value for the phase factor g is 0.5 +/- 0.15. The intensity of the flourescence of H2, combined with an upper limit to the column density of atomic hydrogen associated with the cloud, sets a lower limit of about 130/cm to the density in the flourescence region. Our estimate of the flux incident on the cloud at 1000 A is a factor of 2 to 3 lower than the value required to produce the measured flourescence intensity. Most mechanisms which might reconcile the discrepancy reduce the derived albedo and phase factor.

Hurwitz, M.↗
NASA NTRS2001

The Green Ocean Over the Amazon: Implications for Cloud Electrification

A convective regime with distinct maritime characteristics (weak updraft, low CCN, prevalent coalescence and rainout, weak mixed phase reflectivity, low glaciation temperature, and little if any lightning) is documented over the Amazon basin of the South American continent, and dubbed the "green ocean". Radar, lightning, thermodynamic and AVHRR satellite observations are examined to shed light on the roles of updraft and aerosol in providing departures from the green ocean regime toward continental behavior. Extreme case studies are identified in which the updraft control is dominant and in which the aerosol control is dominant. The tentative conclusion gives importance to both updrafts and aerosol in shaping the electrification of tropical convection.

Williams, E.↗
DOE OSTI2015

MEANDERING SHALLOW ATMOSPHERIC JET AS A MODEL OF SATURN'S NORTH-POLAR HEXAGON

The Voyager flybys of Saturn in 1980–1981 revealed a circumpolar Hexagon at ∼78° north planetographic latitude that has persisted for over 30 Earth years, more than one Saturn year, and has been observed by ground-based telescopes, Hubble Space Telescope and multiple instruments on board the Cassini orbiter. Its average phase speed is very slow with respect to the System III rotation rate, defined by the primary periodicity in the Saturn Kilometric Radiation during the Voyager era. Cloud tracking wind measurements reveal the presence of a prograde jet-stream whose path traces the Hexagon’s shape. Previous numerical models have produced large-amplitude, n = 6, wavy structures with westward intrinsic phase propagation (relative to the jet). However, the observed net phase speed has proven to be more difficult to achieve. Here we present numerical simulations showing that instabilities in shallow jets can equilibrate as meanders closely resembling the observed morphology and phase speed of Saturn’s northern Hexagon. We also find that the winds at the bottom of the model are as important as the winds at the cloud level in matching the observed Hexagon’s characteristics.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRSDate not supplied

TPSAS-NF1676L-13393-DND

In the two plus decades since it became evident that polar stratospheric clouds (PSCs) play a major role in the springtime depletion of polar ozone, the detailed composition and morphology of PSCs has been an area of interest. Although our PSC knowledge base is substantial, there is still considerable uncertainty in specific key areas related to their composition and formation. Probably the least well understood of these is the nucleation process responsible for the formation of nitric acid trihydrate (NAT) particles and the circumstances under which NAT formation and growth leads to stratospheric denitrification. CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) is an excellent instrument for observing PSCs and has already produced an extensive set of PSC observations with unprecedented spatial and temporal resolution covering five winters. These observations are providing new insight into the key remaining questions regarding PSC composition and formation mechanisms. In this paper, we examine the CALIOP PSC observations in combination with a microphysical model in attempt to better understand the underlying physical mechanisms for NAT nucleation. Of particular interest is the early phase of the 2009-2010 Arctic winter when CALIOP frequently observed extended regions of tenuous NAT clouds, clearly before ice was present in the polar vortex. This provides unprecedented large-scale evidence that ice particles are not the only nuclei on which NAT may form. Microphysical model calculations along backward trajectories from these CALIOP NAT cloud observations are used to investigate possible ice-independent, heterogeneous NAT nucleation mechanisms. These analyses will then be expanded to other winters to assess the overall significance of an ice-independent nucleation mechanism for NAT PSCs.

M C Pitts↗
NASA NTRS2024

Mapping Cloud Microphysical Properties to Triple-Wavelength Airborne Lidar Measurements in Winter Storms: Results from the IMPACTS Field Campaign

Ice production and growth inmixed-phase cloudsgive a complicated picture of the radiative and mass characteristics due to the heterogeneity of particle shapes and sizes. Collocated airborne lidar and microphysics datasets from a recent winter storm field study are used to evaluate the effect of ice and liquid hydrometeors,observed in situ,on the multiple-wavelength backscatter coefficientvalues measured by the NASA Cloud Physics Lidarover the course of three winter deployments in the Midwestand Northeast United States.

Joseph A. Finlon↗
DOE OSTI2019

Collaborative Project: An Integrated Parameterization of Boundary Layer and Convective Mixing: The Eddy-Diffusivity/Mass-Flux (EDMF) Approach

The key goal of this project was to reduce cloud modeling deficiencies and biases by developing and implementing a new unified boundary layer and convection parameterization based on the multi-plume Eddy-Diffusivity/Mass-Flux (EDMF) approach. This is a turbulence and convection parameterization that can be considered fully unified, in the sense that it is able to represent convective processes from boundary layer convection to deep moist convection with one single parameterization. This project will ultimately lead to more accurate climate predictions, which have a significant societal impact. In general, turbulence and convection in the atmosphere are at the core of key climate prediction problems. For example: i) to reduce uncertainties in climate projections, it is essential to improve predictions of cloud feedbacks (how clouds respond to, and influence, climate change), which are controlled by the interactions between a turbulent flow with water phase transitions and radiation; (ii) to improve extreme weather prediction under climate change, it is essential to improve our understanding of how moist convection responds to a warmer world. A fully unified boundary layer and convection parameterization, such as EDMF, will help better represent and predict boundary layer, cloud and convection processes in the atmosphere during present and future climate. The following are the specific tasks that were completed and addressed the project’s objectives: i) Implementation and evaluation of the multi-plume EDMF parameterization into the Single Column Model (SCM) version of CESM; ii) Development of a fully unified multi-plume (shallow to deep convection) EDMF parameterization – that is also scale-aware; iii) Implementation and evaluation of the moist multi-plume EDMF scheme in the global version of WRF; iv) Extension and evaluation of the LES model to deep moist convection regimes; v) Implementation of EDMF in the SCM version of the LBL dynamical core.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

THE INFLOW SIGNATURE TOWARD DIFFERENT EVOLUTIONARY PHASES OF MASSIVE STAR FORMATION

We analyze both HCN J = 1–0 and HNC J = 1–0 line profiles to study the inflow motions in different evolutionary stages of massive star formation: 54 infrared dark clouds (IRDCs), 69 high-mass protostellar objects (HMPOs), and 54 ultra-compact H ii regions (UCHIIs). Inflow asymmetry in the HCN spectra seems to be prevalent throughout all the three evolutionary phases, with IRDCs showing the largest excess in the blue profile. In the case of the HNC spectra, the prevalence of blue sources does not appear, apart from for IRDCs. We suggest that this line is not appropriate to trace the inflow motion in the evolved stages of massive star formation, because the abundance of HNC decreases at high temperatures. This result highlights the importance of considering chemistry in dynamics studies of massive star-forming regions. The fact that the IRDCs show the highest blue excess in both transitions indicates that the most active inflow occurs in the early phase of star formation, i.e., in the IRDC phase rather than in the later phases. However, mass is still inflowing onto some UCHIIs. We also find that the absorption dips of the HNC spectra in six out of seven blue sources are redshifted relative to their systemic velocities. These redshifted absorption dips may indicate global collapse candidates, although mapping observations with better resolution are needed to examine this feature in more detail.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1982

The relationship between carbon monoxide abundance and visual extinction in interstellar clouds

Carbon monoxide column densities are compared to visual extinctions toward field stars in the rho Oph and Taurus molecular cloud complexes. The relationship of C(0-18) column density to extinction is established, and new determinations for (C-13)O column densities are given for a range of visual extinctions extended to beyond 20 mag. A prescription for determining hydrogen column densities and masses of molecular clouds from observations of CO isotopes is presented and discussed critically. These measurements agree well with the predictions of gas phase chemistry models which include chemical fractionation and selective isotopic photodestruction. The functional dependence of the C(O-18) column density on extinction is characterized by two different regimes separated by a distinct transition observed to occur at 4 mag in both molecular cloud complexes, whereas the functional dependence of (C-13)O is quite different in the two regions. Some saturation is found to occur for C(O-18) emission at high visual extinction and use the rarer isotopic species C(O-17) and (C-13)(O-18) to correct for it.

Frerking, M. A.↗
NASA NTRS1991

The chemistry of dense interstellar clouds

The basic theme of this program is the study of molecular complexity and evolution in interstellar and circumstellar clouds incorporating the biogenic elements. Recent results include the identification of a new astronomical carbon-chain molecule, C4Si. This species was detected in the envelope expelled from the evolved star IRC+10216 in observations at the Nobeyama Radio Observatory in Japan. C4Si is the carrier of six unidentified lines which had previously been observed. This detection reveals the existence of a new series of carbon-chain molecules, C sub n Si (n equals 1, 2, 4). Such molecules may well be formed from the reaction of Si(+) with acetylene and acetylene derivatives. Other recent research has concentrated on the chemical composition of the cold, dark interstellar clouds, the nearest dense molecular clouds to the solar system. Such regions have very low kinetic temperatures, on the order of 10 K, and are known to be formation sites for solar-type stars. We have recently identified for the first time in such regions the species of H2S, NO, HCOOH (formic acid). The H2S abundance appears to exceed that predicted by gas-phase models of ion-molecule chemistry, perhaps suggesting the importance of synthesis on grain surfaces. Additional observations in dark clouds have studied the ratio of ortho- to para-thioformaldehyde. Since this ratio is expected to be unaffected by both radiative and ordinary collisional processes in the cloud, it may well reflect the formation conditions for this molecule. The ratio is observed to depart from that expected under conditions of chemical equilibrium at formation, perhaps reflecting efficient interchange between cold dust grains in the gas phase.

Irvine, W. M.↗
DOE OSTI2024

RCEMIP-II: mock-Walker simulations as phase II of the radiative–convective equilibrium model intercomparison project

Abstract. The radiative–convective equilibrium (RCE) model intercomparison project (RCEMIP) leveraged the simplicity of RCE to focus attention on moist convective processes and their interactions with radiation and circulation across a wide range of model types including cloud-resolving models (CRMs), general circulation models (GCMs), single-column models, global cloud-resolving models, and large-eddy simulations. While several robust results emerged across the spectrum of models that participated in the first phase of RCEMIP (RCEMIP-I), two points that stand out are (1) the strikingly large diversity in simulated climate states and (2) the strong imprint of convective self-aggregation on the climate state. However, the lack of consensus in the structure of self-aggregation and its response to warming is a barrier to understanding. Gaining a deeper understanding of convective aggregation and tropical climate will require reducing the degrees of freedom with which convection can vary. Therefore, we propose phase II of RCEMIP (RCEMIP-II) that utilizes a prescribed sinusoidal sea surface temperature (SST) pattern to provide a constraint on the structure of convection and move one critical step up the model hierarchy. This so-called “mock-Walker” configuration generates features that resemble observed tropical circulations. The specification of the mock-Walker protocol for RCEMIP-II is described, along with example results from one CRM and one GCM. RCEMIP-II will consist of five required simulations: three simulations with the same three mean SSTs as in RCEMIP-I but with an SST gradient and two additional simulations at one of the mean SSTs with different values of the SST gradients. We also test the sensitivity to the imposed SST gradient and the domain size. Under weak SST gradients, unforced self-aggregation emerges across the entire domain, similar to what was found in RCEMIP. As the SST gradient increases, the convective region narrows and is more confined to the warmest SSTs. At warmer mean SSTs and stronger SST gradients, low-frequency variability in the convective aggregation emerges, suggesting that simulations of at least 200 d may be needed to achieve robust equilibrium statistics in this configuration. Simulations with different domain sizes generally have similar mean statistics and convective structures, depending on the value of the SST gradient. The prescribed SST boundary condition is the only difference in the set-up between RCEMIP-II and RCEMIP-I, which enables comparison between the two; however, we also welcome participation in RCEMIP-II from models that did not participate in RCEMIP-I.

Geology↗
NASA NTRS1999

A Study of Direct and Cloud-Mediated Radiative Forcing of Climate Due to Aerosols

The Intergovernmental Panel on Climate Change (IPCC) has reported that in the southeastern US and eastern China, the general greenhouse warming due to anthropogenic gaseous emissions is dominated by the cooling effect of anthropogenic aerosols. To verify this model prediction in eastern China and southeastern US, we analyzed regional patterns of climate changes at 72 stations in eastern China during 1951- 94 (44 years), and at 52 stations in the southeastern US during 1949-94 (46 years) to detect the fingerprint of aerosol radiative forcing. It was found that the mean rates of change of annual mean daily, maximum, minimum temperatures and diurnal temperature range (DTR) in eastern China were 0.8, -0.2, 1.8, and -2.0 C/100 years respectively, while the mean rates of change of annual mean daily, maximum, minimum temperatures and DTR in the southeastern US were -0.2, -0.6, 0.2, and -0.8 C/100 years, respectively. This indicates that the high rate of increase in annual mean minimum temperature in eastern China results in a slightly warming trend of daily temperature, while the high rate of decrease in annual mean maximum temperature and low rate of increase in annual mean minimum temperature lead to the cooling trend of daily temperature in the southeastern US. We found that the warming from the longwave forcing due to both greenhouse gases and aerosols was completely counteracted by the shortwave aerosol forcing in the southeastern US in the past 46 years. A slightly overall warming trend in eastern China is evident; winters have become milder. This finding is explained by hypothesizing that increasing energy usage during the past 44 years has resulted in more coal and biomass burning, thus increasing the emission of absorbing soot and organic aerosols in eastern China. Such emissions, in addition to well-known Asia dust and greenhouse gases, may be responsible for the winter warming trend in eastern China that we have reported here. The sensitivity of aerosol radiative properties to aerosol composition, size distribution, relative humidity (RH) is examined for the following aerosol systems: inorganic and organic ions (Cl-, Br-, NO3 -, SO4 2-, Na+, NH4 +, K+, Ca2+, Mg2+, HCOO-, CH3COO-, CH3CH2COO-, CH3COCOO-, OOCCOO2-, MSA-1); water-insoluble inorganic and organic compounds (elemental carbon, n-alkanes, SiO2, Al2O3, Fe2O3 and other organic compounds). The partial molar refraction method was used to calculate the real part of the refractive index. It was found that the asymmetry factor increased by approximately 48% with the real part varying from 1.40 to 1.65, and the single scattering albedo decreased by 24% with the imaginary part varying from -0.005 to -0.1. The asymmetry factor increased by 5.4 times with the geometric standard deviation varying from 1.2 to 3.0. The radiation transmission is very sensitive to the change in size distribution; other factors are not as significant. To determine the aerosol direct radiative forcing (ADRF), the aerosol optical depth (AOD) values at the three operational wavelengths (415, 500 and 673 nm) were determined at a regionally representative site, namely, Mt. Gibbs (35.78 deg N, 82.29 deg W, elevation 2006 m) in Mt. Mitchell State Park, NC, and a site located in an adjacent valley (Black Mountain, 35.66 deg N, 82.38 deg W, elevation 951 m) in the southeastern US. The two sites are separated horizontally by 10 km and vertically by 1 km. It was found that the representative total AOD values at 500 nm at the valley site for highly polluted (HP), marine (M) and continental (C) air masses were 0.68 +/- 0.33, 0.29 +/- 0.19 and 0.10 +/- 0.04, respectively. A search-graph method was used to retrieve the columnar size distribution (number concentration N, effective radius reff and geometric standard deviation=?g) from the optical depth observations at three operational wavelengths. The ground albedo, single scattering albedo and imaginary part of the refractive index were calculated using a mathematically unique procedure involving a Mie code and a radiative transfer code in conjunction with the retrieved aerosol size distribution, AOD, and diffuse-direct irradiance ratio. It was found that N, r(eff) and sigma(g) were in the ranges of 10 to 1.7 x 10(exp 4)/cubic cm, 0.09 to 0.68 micrometers and 1.12 to 2.95, respectively. The asymmetry factor and single scattering albedo were in the ranges of 0.63 to 0.75 and 0.74 to 0.97 respectively. The ground albedo for the forested terrain and imaginary part of refractive index were found to be in the ranges of 0.06 to 0.29 and 0.005 to 0.051 respectively. On the basis of these aerosol radiative properties obtained at the research sites and computations using the Column Radiation Model (CRM) of National Center of Atmospheric Research (NCAR) Community Climate Model (CCM3), it was found that the average cloud-free 24-hour ADRF values were -13 +/- 8, -8 +/- 3, -33 +/- 16 W/square m for marine, continental, and polluted air masses, respectively. On the assumption that the fractional coverage of clouds is 0.61, it was estimated that the annual mean ADRF was 7 +/- 2 W/square m in the southeastern US. The review with respect to the current knowledge of organic acids shows that aerosol formate and acetate concentrations range from 0.02 to 5.3 nmol/cubic m and from 0.03 to 12.4 nmol/cubic m respectively, and that between 34% to 77% of formate and between 21% to 66% of acetate are present in the fine fraction of aerosols. It was found that although most (98-99%) of these volatile organic acids were present in the gas phase, their concentrations in the aerosol particles were sufficient to make them a good candidate for cloud condensation nuclei (CCN). It is hypothesized that organic acids are at least one of the primary sources of CCN in the atmosphere due to their ubiquitous presence in the troposphere, especially over the continental forested areas. The results of our measurements at Palmer Station, Antarctica show that the daily average CCN concentrations at 0.3% and 1% supersaturations ranged from 0.3 to 160/cubic cm and from 4 to 168/cubic cm, respectively, during the period from 17 January to 26 February, 1994. New evidence for substantial and definitive CCN enhancement near and within cloud has been observed at Mt. Mitchell, North Carolina. The results show that the average monthly CCN concentrations were 460 +/- 217, 386 +/- 286, 429 +/- 228 and 238 +/- 134/cubic cm for in-cloud, overcast, clear and rainy conditions, respectively. The typical CCN spectra show that there were a lot of small CCN produced and the ion concentrations (especially H+ and SO4 2-) were very high during the CCN enhancement period. The significantly positive correlation between black carbon (BC) and CCN at 1% supersaturation indicates that a percentage of the BC measured at the site may be in the form of an internal mixture and participated in the formation of CCN.

Yu, Shao-Cai↗
DOE OSTI2015

Saturated Monoglyceride Polymorphism and Gel Formation of Biodiesel Blends

Crystallization or gel formation of normal paraffins in diesel fuel under cold weather conditions leading to fuel filter clogging is a common problem. Cold weather operability of biodiesel (B100) and blends with diesel fuel presents additional complexity because of the presence of saturated monoglycerides (SMGs) and other relatively polar species. Currently, the cloud point measurement (a measure of when the first component crystallizes out of solution) is used to define the lowest temperature at which the fuel can be used without causing cold weather issues. While filter plugging issues have declined, there still remain intermittent unexpected problems above the cloud point for biodiesel blends. Development of a fundamental understanding of how minor components in biodiesel crystallize, gel, and transform is needed in order to prevent these unexpected issues. We have found that SMGs, a low level impurity present in B100 from the production process, can crystallize out of solution and undergo a solvent-mediated polymorphic phase transformation to a more stable, less soluble form. This causes them to persist at temperatures above the cloud point once they have some out of solution. Additionally, we have found that SMGs can cause other more soluble, lower melting point minor components in the B100 to co-crystallize and come out of solution. Monoolein, another minor component from the production process is an unsaturated monoglyceride with a much lower melting point and higher solubility than SMGs. It is able to form a co-crystal with the SMGs and is found together with the SMGs on plugged filters we have analyzed in our laboratory. An observation of isolated crystals in the lab led us to believe that the SMGs may also be forming a gel-like network with components of the B100 and diesel fuel. During filtration experiments, we have noted that in some cases a solid layer of crystals forms and blocks the filter completely, while in other cases this does not occur. Because SMGs are polar and can form layered networks once a sufficient amount of crystals have come out of solution, we recently began investigating the ability of SMGs to form a gel network with fuel components as well as with other minor polar components in the fuel in order to obtain a fundamental understanding of the mechanism of formation. It has been well established that this type of phenomena occurs in sub-sea pipelines where a chief crystallizing component begins to crystallize out of solution. Once a sufficient amount of crystals exists, a volume spanning network of solid crystals can trap liquid crude oil and form a solid-like gel network. We are investigating whether this type of phenomena can occur with SMGs and both fatty acid methyl esters from the B100 and normal paraffins from diesel fuel. Additionally, SMGs are well known to incorporate water into their layered crystal structure. Water is often used to stabilize less stable polymorphic forms of SMGs, therefore water was another minor component of interest. Also of interest is glycerin which has been found on clogged filters in our laboratory.

30 DIRECT ENERGY CONVERSION↗