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DOE OSTI2020

Investigating Secondary Aerosol Processes in the Amazon through Molecular-level Characterization of Semi-Volatile Organics

In areas where biogenic emissions are oxidized in the presence of anthropogenic pollutants, it has become increasingly apparent that secondary organic aerosol (SOA) formation from biogenic volatile organic compounds (BVOCs) is substantially enhanced. The Amazon forest is the dominant source of BVOCs globally, and the forest is rapidly being converted to urban and agricultural uses. We participated in a collaborative field study located in the Amazon region around Manaus, Brazil, in 2014 (Green Ocean Amazon; GoAmazon). This study was designed to comprehensively examine how BVOC emissions (specifically, the most highly emitted non-methane hydrocarbon, isoprene, and lesser studied sesquiterpenes) and their interaction with anthropogenic pollution (i.e., nitrogen oxides, sulfur dioxide, and black carbon) alter the atmosphere’s oxidative capacity, influence secondary aerosol formation, atmospheric composition and, ultimately, affect the earth’s radiation balance and climate. We provide the first hourly, in-situ measurement of 30 sesquiterpenes and 4 diterpenes, roughly estimating that sesquiterpene oxidation contributes to 10-14% of ozone reactive loss by terpenes and at least 0.4–5% (median 1 %) of total submicron OA mass. However, this is likely a low-end estimate, as evidence for additional unaccounted sesquiterpenes and their oxidation products clearly exists. We also provide new perspectives on sulfate, NO x , and particle acidity influencing isoprene-derived SOA, comparing the central Amazon environment with Southeastern U.S.A. summer, representing clean to polluted conditions, respectively. We find that summed concentrations of isoprene-derived SOA tracers correlated with particulate sulfate spanning three orders of magnitude, suggesting that 1 μg m -3 reduction in sulfate corresponds with at least ~0.5 μg m -3 reduction in isoprene-derived SOA. We also find that SOA mass derived from isoprene oxidation in the presence of NO x is primarily comprised of aerosol sulfate bound with isoprene oxidation products (i.e. organosulfates), ~97% in the Amazon and ~55% in the Southeastern U.S. We infer under natural conditions in high isoprene emission regions, preindustrial aerosol sulfate was almost exclusively isoprene-derived organosulfates, which are traditionally thought as representative of anthropogenic influence. We further report the first field observations showing that particle acidity impacts the distribution of isoprene oxidation tracers in the gas and particle phases, providing physicochemical insight into isoprene SOA formation chemistry. Coupled with other co-located measurements by the DOE Atmospheric Radiation Measurement (ARM) team and collaborating PIs at our measurement site (called T3), on the G1 aircraft, and at additional field sites (T0, T1, T2) this data set has been used to understand emission, oxidation, and particle formation pathways at the molecular level, to elucidate how these pathways change when influenced by anthropogenic sources, and to evaluate their importance for the atmospheric budget of aerosols and the earth’s radiation balance on regional scales. Recommendations: Further constraint of the role of sesquiterpenes on ozone (O 3 ) reactivity and SOA formation is limited by the availability of authentic standards and synthesized compounds of sesquiterpenes and their oxidation products. Future research efforts should focus on making such standards available via custom synthesis to allow for accurate quantification and focused oxidation experiments that will fully elucidate the chemistry of these compounds in the atmosphere. Further, reductions in aerosol sulfate (via SO 2 emissions control) continues to be one of the most effective methods to reduce SOA formation from isoprene, but the concerted role of ammonia (NH 3 ) gas emissions from (agricultural) industry and other sources requires more investigation to better understand the role of aerosol acidity in SOA formation and potential controls. As GoAmazon particles can be more acidic compared to areas with greater anthropogenic NH 3 emissions, this promotes relatively greater organosulfate (OS) formation from isoprene even in the presence of NO x . Because OS and inorganic sulfate differ in water uptake properties, this implies preindustrial aerosol sulfate (albeit less abundant) may have been less reflective than current earth system models assume. Further research should investigate the radiative impacts of organic vs inorganic sulfate in aerosols to improve model representation. Finally, future work (currently underway) should include constraint of the contributions of monoterpene (C 10 H 16 ) BVOCs and biomass burning VOCs as precursors to SOA formation in the region as well as their impacts on radiative forcing in the climate system.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2010

Reevaluating the Role of Saharan Air Layer in Atlantic Tropical Cyclogenesis and Evolution

The existence of the Saharan air layer (SAL), a layer of warm, dry, dusty air that frequently moves westward off of the Saharan desert of Africa and over the tropical Atlantic Ocean, has long been appreciated. As air moves over the desert, it is strongly heated from below, producing a very hot air mass at low levels. Because there is no moisture source over the Sahara, the rise in temperature causes a sharp drop in relative humidity, thus drying the air. In addition, the warm air produces a very strong jet of easterly flow in the middle troposphere called the African easterly jet that is thought to play a critical role in hurricane formation. In recent years, there has been an increased focus on the impact that the SAL has on the formation and evolution of hurricanes in the Atlantic. However, the nature of its impact remains unclear, with some researchers arguing that the SAL amplifies hurricane development and with others arguing that it inhibits it. The argument for positively influencing hurricane development is based upon the fact that the African easterly jet provides an energy source for the waves that eventually form hurricanes and that it leads to rising motion south of the jet that favors the development of deep thunderstorm clouds. The potential negative impacts of the SAL include 1) low-level vertical wind shear associated with the African easterly jet; 2) warm SAL air aloft, which increases thermodynamic stability and suppresses cloud development; and 3) dry air, which produces cold downdrafts in precipitating regions, thereby removing energy needed for storm development. As part of this recent focus on the SAL and hurricanes (which motivated a 2006 NASA field experiment), there has been little emphasis on the SAL s potential positive influences and almost complete emphasis on its possible negative influences, almost to the point of claims that the SAL is the major suppressing influence on hurricanes in the Atlantic. In this study, multiple NASA satellite data sets (TRMM, MODIS, CALIPSO, and AIRS/AMSU) and National Centers for Environmental Prediction global analyses are used to see if the proposed negative influences deserve all of the attention they have recently received. The results show that storms generally form on the southern side of the African jet, where favorable background rotation is high. The jet often helps to form the northern side of the storms and is typically stronger in storms that intensify than those that weaken, suggesting that jet-induced vertical wind shear is not a negative influence on developing storms. Warm SAL air is confined to regions north of the jet and generally does not impact the tropical cyclone precipitation south of the jet. A comparison of the environments of strongly strengthening storms and of weakening storms shows no differences in SAL structure, indicating that the SAL has little influence on whether storms weaken or intensify. The large-scale flow at upper levels above the SAL was found to be most important, with the environment of strengthening storms having very little vertical wind shear and also favoring more expansive outflow from the storm. The SAL is shown to occur in a large-scale environment that is already characteristically dry as a result of large-scale subsidence (sinking air motions). Strong surface heating and deep dry convective mixing enhance dryness at low levels, but moisten the air at midlevels. Therefore, mid-to-upper-level dryness is not a defining characteristic of the SAL, but is instead a signature of subsidence. As a result, we conclude that the SAL is not the major negative influence on hurricanes that recent studies have emphasized. It is just one of many possible influences and can be both positive and negative.

Braun, Scott A.↗

NASA NTRS2008

Science on the Moon: The Wailing Wall of Space Exploration

Science on and from the Moon has important implications for expanding human knowledge and understanding, a prospect for the 21st Century that has been under discussion for at least the past 25 years. That having been said, however, there remain many issues of international versus national priorities, strategy, economy, and politics that come into play. The result is a very complex form of human behavior where science and exploration take center stage, but many other important human options are sacrificed. To renew this dialogue about the Moon, it seems we are already rushing pell-mell into it as has been done in the past. The U.S., Japan, China, India, and Russia either have sent or plan to send satellites and robotic landers there at this time. What does a return to the Moon mean, why are we doing this now, who should pay for it, and how? The only semblance of such a human enterprise seems to be the LHC currently coming online at CERN. Can it be used as a model of international collaboration rather than a sports or military event focused on national competition? Who decides and what is the human sacrifice? There are compelling arguments for establishing science on the Moon as one of the primary goals for returning to the Moon and venturing beyond. A number of science endeavors will be summarized, beyond lunar and planetary science per se. These include fundamental physics experiments that are background-limited by the Earth's magnetic dipole moment and noise produced by its atmosphere and seismic interior. The Moon is an excellent platform for some forms of astronomy. Other candidate Moon-based experiments vary from neutrino and gravitational wave astronomy, particle astrophysics, and cosmic-ray calorimeters, to space physics and fundamental physics such as proton decay. The list goes on and includes placing humans in a hostile environment to study the long-term effects of space weather. The list is long, and even newer ideas will come from this COSPAR conference. However, whatever the list the issue of cooperation and binding collaboration remains. As observers of Moon and other space enterprises, we all know that a room full of 60 scientists will not agree on much of anything and there will probably be 60! please for more funding. People have special interests and little common sense (e.g., conflict between NSF- and NASA-funding roadmaps). Scientists are no exception. Nevertheless, CERN has done it on Earth! Can we do the same on the Moon? Some of the present generation of proposals for science from and on the Moon, plus new ones, will witness a place in space exploration's future. It is clear, however, that the world has not thought this through adequately, except for talk about an international space federation whatever that is. An outpost on the Moon with humans permanently living there much like Antarctica on Earth may be in our future. However, such planning is our collective international responsibility and not that of special-interest investigators from individual nations unless they intend to pay for it.

Wilson, Thomas↗

DOE OSTI2025

Activation of Semicore Electrons in Alkali Metals and Their Role in the B1–B2 Phase Transition under Pressure

Alkali fluorides are often thought of as archetypical ionic compounds whose structures can be understood in terms of the packing of rigid spheres. At ambient pressure, they assume the rocksalt (B1) structure, while under only a few GPa of pressure, the cesium chloride (B2) structure, with higher coordination numbers, is assumed for KF, RbF, and CsF. NaF requires almost 10 times more pressure to undergo this same phase transition, which has not been observed for LiF. Herein, we provide a detailed analysis, based upon quantum chemical calculations, explaining this behavior. We show that for the heavier alkali metals, the semicore p orbitals engage in metal-metal bonding in the B2 phase, facilitating the pressure-induced B1 → B2 structural transition. Furthermore, these findings suggest that the semicore orbitals of heavy alkali metals can be activated without the need of strong oxidants at very mild levels of compression, resulting in the formation of chemical bonds, challenging both traditional and modern core-valence distinctions. In addition, we argue that Cs 5p-5p bonding in CsCl occurs already at ambient pressure, stabilizing the B2 phase, and suggest experiments that may be able to detect signatures of such bonding.

Anions↗

NASA NTRS2002

Getting through to circadian oscillators: why use constant routines?

Overt 24-h rhythmicity is composed of both exogenous and endogenous components, reflecting the product of multiple (periodic) feedback loops with a core pacemaker at their center. Researchers attempting to reveal the endogenous circadian (near 24-h) component of rhythms commonly conduct their experiments under constant environmental conditions. However, even under constant environmental conditions, rhythmic changes in behavior, such as food intake or the sleep-wake cycle, can contribute to observed rhythmicity in many physiological and endocrine variables. Assessment of characteristics of the core circadian pacemaker and its direct contribution to rhythmicity in different variables, including rhythmicity in gene expression, may be more reliable when such periodic behaviors are eliminated or kept constant across all circadian phases. This is relevant for the assessment of the status of the circadian pacemaker in situations in which the sleep-wake cycle or food intake regimes are altered because of external conditions, such as in shift work or jet lag. It is also relevant for situations in which differences in overt rhythmicity could be due to changes in either sleep oscillatory processes or circadian rhythmicity, such as advanced or delayed sleep phase syndromes, in aging, or in particular clinical conditions. Researchers studying human circadian rhythms have developed constant routine protocols to assess the status of the circadian pacemaker in constant behavioral and environmental conditions, whereas this technique is often thought to be unnecessary in the study of animal rhythms. In this short review, the authors summarize constant routine methodology and what has been learned from constant routines and argue that animal and human circadian rhythm researchers should (continue to) use constant routines as a step on the road to getting through to central and peripheral circadian oscillators in the intact organism.

Non-NASA Center↗

DOE OSTI2021

Stability of Neptune’s Distant Resonances in the Presence of Planet Nine

Trans-Neptunian Objects (TNOs) in the scattered disk with 50 ≲ a ≲ 100 au are thought to cluster near Neptune’s n:1 resonances (e.g., 3:1, 4:1, and so on). While these objects spend lengthy periods of time at large heliocentric distances, if their perihelia remain less than around 40 au, their dynamical evolution is still largely coupled to Neptune’s. Conversely, around a dozen extreme TNOs with a ≳ 250 au and detached perihelia seem to exist in a regime where they are too distant to be affected by the giant planets and too close for their dynamics to be governed by external forces. Recent work suggests that the apparent alignment of these orbits in physical space is a signature of gravitational shepherding by a distant massive planet. In this paper, we investigate the evolution of TNOs in each of Neptune’s n:1 resonances between the 3:1 and 14:1. We conclude that both resonant and nonresonant objects beyond the 12:1 near ∼157 au are removed rather efficiently via perturbations from the hypothetical Planet Nine. Additionally, we uncover a population of simulated TNOs with a ≲ 100 au, 40 ≲ q ≲ 45 au, and low inclinations that experience episodes of resonant interactions with both Neptune and Planet Nine. Finally, we simulate the evolution of observed objects with a > 100 au and identify several TNOs that are potentially locked in n:1 resonances with Neptune, including the most distant known resonant candidates, 2014 JW{sub 80} and 2014 OS{sub 394},which appear to be in the 10:1 and 11:1 resonances, respectively. Our results suggest that the detection of similar remote objects might provide a useful constraint on hypotheses invoking the existence of additional distant planets.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1996

Experimental Constraints on the Origin of Lunar High-Ti Ultramafic Glasses

Phase equilibria and dissolution rate experiments are used to develop a petrogenetic model for the high-Ti lunar ultramafic glasses. Near-liquidus phase relations of the Apollo 14 black glass, the most Ti-rich lunar ultramafic glass, are determined to 2.2-GPa. The liquidus is saturated with Cr-spinel at 1-atm, olivine between approximately 0.5- and 1.5-GPa, and low-Ca pyroxene + Cr-spinel above 1.5-GPa. Ilmenite does not crystallize near the liquidus and implies that high-Ti ultramafic glasses are not produced by melting of an ilmenite-saturated source. We infer that high-Ti ultramafic magmas are derived from low-Ti ultramafic parent magmas by assimilation of ilmenite +/- clinopyroxene +/- urKREEP +/- pigeonite in the shallow lunar interior. Heat is provided by adiabatic ascent of the low-Ti ultramafic primary magmas from the deeper lunar interior and crystallization of olivine during assimilation. The assimilation reaction is modeled by mass balance and requires that ilmenite and high-Ca pyroxene are assimilated in a approximately 3:1 ratio, a much higher ratio than the proportion in which these minerals are thought to exist in the lunar interior. In an effort to understand the kinetic controls on this reaction, the dissolution of ilmenite is examined experimentally in both low- and high-Ti lunar magmas. We find that ilmenite dissolves incongruently to Cr-spinel and a high-Ti melt. The dissolution reaction proceeds by a diffusion-controlled mechanism. An assimilation model for the origin of high-Ti melts is developed that leaves the magma ocean cumulates in their initial stratigraphic positions and obviates source hybridization models that require lunar overturn.

Wagner, T. P.↗

DOE OSTI2020

A Quantum-Based Approach to Predict Primary Radiation Damage in Polymeric Networks

Initial atomistic-level radiation damage in chemically reactive materials is thought to induce reaction cascades that can result in undesirable degradation of macroscale properties. Ensembles of quantum-based molecular dynamics (QMD) simulations can accurately predict these cascades, but extracting chemical insights from the many underlying trajectories is a labor-intensive process that can require substantial a priori intuition. We develop here a general and automated graph-based approach to extract all chemically distinct structures sampled in QMD simulations and apply our approach to predict primary radiation damage of polydimethylsiloxane (PDMS), the main constituent of silicones. A postprocessing protocol is developed to identify underlying polymer backbone structures as connected components in QMD trajectories. Furthermore, these backbones form a repository of radiation-damaged structures. A scheme for extracting and updating a library of isomorphically distinct structures is proposed to identify the spanning set and aid chemical interpretation of the repository. The analyses are applied to ensembles of cascade QMD simulations in which the four element types in PDMS are selectively excited in primary knock-on atom events. Our approach reveals a much higher degree of combinatorial complexity in this system than was inferred through radiolysis experiments. Probabilities are extracted for radiation-induced network changes including formation of branch points, carbon linkages, cycles, bond scissions, and carbon uptake into the Si–O siloxane backbone network. The general analysis framework presented here is readily extendable to modeling chemical degradation of other polymers and molecular materials and provides a basis for future quantum-informed multiscale modeling of radiation damage.

36 MATERIALS SCIENCE↗

NASA NTRS1987

An experimental low Reynolds number comparison of a Wortmann FX67-K170 airfoil, a NACA 0012 airfoil and a NACA 64-210 airfoil in simulated heavy rain

Wind tunnel experiments were conducted on Wortmann FX67-K170, NACA 0012, and NACA 64-210 airfoils at rain rates of 1000 mm/hr and Reynolds numbers of 310,000 to compare the aerodynamic performance degradation of the airfoils and to attempt to identify the various mechanisms which affect performance in heavy rain conditions. Lift and drag were measured in dry and wet conditions, a variety of flow visualization techniques were employed, and a computational code which predicted airfoil boundary layer behavior was used. At low angles of attack, the lift degradation in wet conditions varied significantly between the airfoils. The Wortmann section had the greatest overall lift degradation and the NACA 64-210 airfoil had the smallest. At high angles of attack, the NACA 64-210 and 0012 airfoils had improved aerodynamic performance in rain conditions due to an apparent reduction of the boundry layer separation. Performance degradation in heavy rain for all three airfoils at low angles of attack could be emulated by forced boundary layer transition near the leading edge. The secondary effect occurs at time scales consistent with top surface water runback times. The runback layer is thought to effectively alter the airfoil geometry. The severity of the performance degradation for the airfoils varied. The relative differences appeared to be related to the susceptibility of each airfoil to premature boundary layer transition.

Craig, Anthony P.↗

NASA NTRS2000

Laboratory Astrochemistry: Interstellar PAHs

Polycyclic aromatic hydrocarbons (PAHs) are now considered to be an important and ubiquitous component of the organic material in space. PAHs are found in a large variety of extraterrestrial materials such as interplanetary dust particles (IDPs) and meteoritic materials. PAHs are also good candidates to account for the infrared emission bands (UIRs) and the diffuse interstellar optical absorption bands (DIBs) detected in various regions of the interstellar medium. The recent observations made with the Infrared Space Observatory (ISO) have confirmed the ubiquitous nature of the UIR bands and their carriers. PAHs are thought to form through chemical reactions in the outflow from carbon-rich stars in a process similar to soot formation. Once injected in the interstellar medium, PAHs are further processed by the interstellar radiation field, interstellar shocks and energetic particles. A major, dedicated, laboratory effort has been undertaken to measure the physical and chemical characteristics of these complex molecules and their ions under experimental conditions that mimic the interstellar conditions. These measurements require collision-free conditions where the molecules and ions are cold and chemically isolated. The spectroscopy of PAHs under controlled conditions represents an essential diagnostic tool to study the evolution of extraterrestrial PAHs. The Astrochemistry Laboratory program will be discussed through its multiple aspects: (1) objectives, (2) approach and techniques adopted, (3) adaptability to the nature of the problem(s), and (4) results and implications for astronomy as well as for molecular spectroscopy. A review of the data generated through laboratory simulations of space environments and the role these data have played in our current understanding of the properties of interstellar PAHs will be presented. The discussion will also introduce the newest generation of laboratory experiments that are currently being developed in order to provide a closer simulation of space environments and a better support to space missions.

Salama, Farid↗

DOE OSTI2022

Iron precipitation under controlled oxygen flow: Mineralogical implications for BIF precursors in the Archean ocean

Banded iron formation (BIF) deposition in the Archean ocean is thought to have been initiated by the oxidation of dissolved iron into ferric primary precursor phases that descended through the water column and were deposited on the seafloor. Effective interpretation of the trace element and isotopic composition of BIFs in the geologic record requires an understanding of the identity and longevity of those precursor phases. Temporal and spatial variation in oxidant concentration and ocean chemistry may have driven precursor mineralogy. Furthermore, precursor phases may undergo transitions during descent and burial. This experimental study follows the evolution of iron mineralogy, speciation, and redox state during the precipitation of iron under variable oxygen fluxes and in fluids containing different iron-complexing anions (chloride, sulfate, and phosphate). Additionally, suspensions collected after incomplete oxidation were anoxically aged to simulate changes to precursor mineralogy during descent below the seawater redoxcline. Results from X-ray diffraction, sequential dissolution, colorimetric determination of Fe redox state, and Fe K-edge X-ray absorption fine structure spectroscopy showed that under all experimental conditions, intermediate precipitates collected before complete iron uptake contained mineralized ferrous iron. Purely ferric mineral assemblages were not observed until iron was removed from solution. In low-oxygen experiments, intermediate precipitates contained phases with stoichiometric Fe 2+ , including magnetite, vivianite, and green rust (GR). Chloride green rust (GR1) had more ferric iron than sulfate green rust (GR2) and more readily transitioned to magnetite via disproportionation. GR2 was stable over a broader range of iron uptake; magnetite appeared mainly as an additional oxidation product in sulfate solution. In high oxygen experiments, mineralized ferrous iron occurred in amorphous phases or as a non-stoichiometric component in ferric oxides; final ferric assemblages were less crystalline than in low-oxygen equivalents. Low concentrations of phosphate increased the total iron oxidation rate, but also increased the ferrous content of intermediate precipitates. The incorporation of phosphate stabilized GR2 and facilitated GR2 precipitation over a larger range of iron uptake. In higher concentrations of phosphate, vivianite and poorly crystalline ferric hydroxides formed in place of GR. Here, these findings suggest that over a range of possible ocean chemistries, mixed-valence phases may have been short lived but relevant precursors to BIF. Additionally, anionic chemistry and oxidant concentration are shown to influence the crystallinity and chemical resistivity of final ferric assemblages, affecting their reactivity during later anoxic burial.

58 GEOSCIENCES↗

NASA NTRS1996

Southern Hemisphere In Situ Observations of OH, HO2, CIO and BrO from the ER-2 Aircraft for the 1994 ASHOE Mission

A summary of the first order scientific conclusions that emerged from the research done under this grant are as follows: (1) For the first time, the concentration of the key hydrogen and halogen radicals OH, H02, ClO and BrO were determined on a global scale extending from the arctic circle to the antarctic circle, over the altitude domain of the ER-2. That domain extends from 15-20 km altitude, covering a critical part of the lower stratosphere; (2) Simultaneous, in situ measurements of the concentrations of OH, H02, ClO, BrO, NO and NO2 demonstrate the predominance of odd-hydrogen and halogen free radical catalysis in determining the rate of removal of ozone in the lower stratosphere over the complete ASHOE mission. This extends to the global scale the "first look" data obtained during the NASA Stratospheric Photochemistry and Dynamics Experiment (SPADE), executed out of Ames Research Center in June 1993. This represents a major rearrangement of our understanding with respect to the hierarchy of dominant catalytic cycles controlling ozone loss in the lower stratosphere. For the past twenty years, it has been assumed that nitrogen radicals dominate the destruction rate of ozone in the lower stratosphere; (3) Throughout the altitude and latitude range covered by ASHOE, it was determined that a single catalytic cycle, HO2 + O3 yields OH + 2O2, accounted for one half of the total O3 removal in this region of the atmosphere. Halogen radical catalytic cycles were found to account for one third of the ozone loss, and nitrogen radicals were found to account for 20% of the loss; (4) Simultaneous observations of the full complement of radicals, tracers, ozone, and water vapor during ASHOE demonstrated quantitatively the coupling that exists between the rate limiting radicals and other reactive species in the photochemical reaction network. Specifically, the concentrations of ClO and HO2 are inversely correlated with the concentration of NOx. This carries the implication that the NOx effluent from the proposed High Speed Civil Transport may be less destructive to stratospheric ozone than had previously been thought. ASHOE brought this conclusion forward for the first time on a global basis; and (5) The density of BrO was measured on a global scale during ASHOE in the lower stratosphere. It was found that bromine is responsible for 55-65% of the local rate of catalytic destruction of ozone by reactions involving bromine and chlorine. Normalizing calculated loss rates to total available inorganic bromine and chlorine explicitly demonstrates that bromine is 60-80 times more efficient than chlorine in removing ozone in the lower stratosphere. An inferred value of total inorganic bromine is in excellent agreement with measurements of their source species, organic bromine compounds in the troposphere.

Anderson, James G.↗

NASA NTRS1997

Deoxypyridinoline in the Urine of Rats with Unloaded Hindlimbs

The urinary excretion of deoxypyridinoline (U-Dpd), a nonreducible collagen crosslink in bone released by osteoclastic activity, is thought to be an accurate marker of bone resorption. The role of increased resorption in the osteopenia of a space flight model which unloads the hindlimbs by suspending the tail is controversial. To assess skeletal resorption in the model we measured U-Dpd (Pyrilinks-D, Metro Biosystems, Inc.) in serial 24 hour urine specimens collected from 250 a (Y) and 450 a (M) male rats with unloaded hindlimbs for four weeks. Both groups of rats were fed AIN76 diets with calcium restricted to 0.2% in Y and to 0.1 % in M. Blood was obtained after 28 days for parathyroid hormone (PTH), 1,25-dihydroxyvitamin D (1,25-D) and alkaline phosphatase (Alkptase). Basal U-Dpd was higher and more variable in Y than M (475+/-200 vs 67+/-9, nM/mM creatinine, p<.001). Repeated measures ANOVA in Y revealed decreases in U-Dpd, 36% in control (C) and 24% in unloaded (S) rats (p<.005). There was a nadir in YS on the 14th day not observed in YC (p<.05). U-Dpd in MC showed no change, but increased in MS by the 14th day and remained elevated. At the end of the experiment, body weights in both Y and M were less in S than C (337+/-16 vs 306+/-12g and 485+/-10 vs 461+/-6g, p=.002). Bill was inversely related to U-Dpd only in M (r=0.699, p=.024). PTH, similar in C and S in Y (52+/-15 vs 42+/-7pg/ml, NS) and M (68+/-13 vs 61+/-12, NS), was unrelated to U-Dpd. 1,25-D tended toward higher values in YC than YS (197+/-103 vs 119+/-30, NS) and correlated with U-Dpd (0.773, p=.015). Alkptase, 1.3 times higher in Y than M, was similar in C and S at the end of unloading. These findings indicate that bone resorption, as reflected by U-Dpd, is suppressed in young and stimulated in mature rats exposed to a space flight model. U-Dpd reflects reduced growth from the diet change in young control and experimental rats and loss of Bill in mature animals exposed to the space flight model, 2 situations with opposite effects on bone resorption.

Arnaud, Sara B.↗

NASA NTRS2011

Thoughts Without Content are Empty, Intuitions Without Concepts are Blind - Determinism and Contingency Revisited

Was the emergence of life a predictable outcome of chemical evolution on earth? Could evolution produce life very different from ours? These are one of the oldest questions in the field of the origin of life that not only have broad philosophical implications but also impact how we approach the problem from the methodological standpoint. Framing the issue in terms of the dichotomy between contingency and determinism is not a fortunate because these two terms in their conventional meaning are neither mutually exclusive nor jointly exhaustive. Determinism, represented in natural sciences by Newtonian physics, relies on the assumption that every event is causally determined by a chain of previous events. In the context of the origin of life it means that once the initial conditions on the early earth have been specified further evolution follows inevitably. Considering uncertainties about conditions on the prebiotic earth, many plausible sets of initial conditions can be defined, each followed by a separate deterministic trajectory. This conventional understanding of determinism does not admit contingency. Further, it has no implications for evaluating how many sets of initial conditions lead to the emergence of life. It appears that a better framing of the problem is as follows: given plausible sets of initial conditions on the early earth how probable and broadly spread are evolutionary trajectories that lead to life? Instead of undertaking an impossible task of specifying microscopic initial conditions for all components of the system one uses a reduced representation of this system and specify only a small set of essential macroscopic parameters, values (or ranges of values) of which can be identified, inferred or estimated from experiment, theory or historical record. The following evolutionary trajectories are still governed by laws of physics and chemistry but become probabilistic and "contingency" is admitted as variations in other variables in the system. A similar reasoning is common in other fields of science, for example in statistical mechanics. Some trajectories lead to life, perhaps in different forms, whereas others do not. Of our true interest is the ratio of these two outcomes. The issue of determinism does not directly enter the picture. The debate about the likelihood of the emergence of life is quite old. One view holds that the origin of life is an event governed by chance, and the result of so many random events (contingencies) is unpredictable. This view was eloquently expressed by Monod. In his book "Chance or Necessity" he argued that life was a product of "nature's roulette." In an alternative view, expressed in particular by deDuve and Morowitz, the origin of life is considered a highly probable or even inevitable event (although its details need not be determined in every respect). Only in this sense the origin of life can be considered a "deterministic event".

Pohorille, Andrew↗

DOE OSTI2024

Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism

Abstract. The oxidation of dimethyl sulfide (DMS) in the marine atmosphere represents an important natural source of non-sea-salt sulfate aerosol, but the chemical mechanisms underlying this process remain uncertain. While recent studies have focused on the role of the peroxy radical isomerization channel in DMS oxidation, this work revisits the impact of the other channels (OH addition and OH abstraction followed by bimolecular RO2 reaction) on aerosol formation from DMS. Due to the presence of common intermediate species, the oxidation of dimethyl sulfoxide (DMSO) and dimethyl disulfide (DMDS) can shed light on these two DMS reaction channels; they are also both atmospherically relevant species in their own right. This work examines the OH oxidation of DMSO and DMDS, using chamber experiments monitored by chemical ionization mass spectrometry and aerosol mass spectrometry to study the full range of sulfur-containing products across a range of NO concentrations. The oxidation of both compounds is found to lead to rapid aerosol formation (which does not involve the intermediate formation of SO2), with a substantial fraction (14 %–47 % S yield for DMSO and 5 %–21 % for DMDS) of reacted sulfur ending up in the particle phase and the highest yields observed under elevated NO conditions. Aerosol is observed to consist mainly of sulfate, methanesulfonic acid, and methanesulfinic acid. In the gas phase, the NOx dependence of several products, including SO2 and S2-containing organosulfur species, suggest reaction pathways not included in current mechanisms. Based on the commonalities with the DMS oxidation mechanism, DMSO and DMDS results are used to reconstruct DMS aerosol yields; these reconstructions roughly match DMS aerosol yield measurements from the literature but differ in composition, underscoring remaining uncertainties in sulfur chemistry. This work indicates that both the abstraction and addition channels contribute to rapid aerosol formation from DMS and highlights the need for more study into the fate of small sulfur radical intermediates (e.g., CH3S, CH3SO2, and CH3SO3) that are thought to play central roles in the DMS oxidation mechanism.

Goss, Matthew B. (ORCID:0000000226885463)↗

NASA NTRSDate not supplied

Wind Tunnel Testing of AFC over a Deflected Aileron on the High-Lift Common Research Model

Active flow control (AFC) using discrete fluidic actuators distributed along the span, just upstream of the deflected aileron of the 10% scale high-lift version of the Common Research Model (CRM-HL), was evaluated during a wind tunnel test in the NASA Langley 14- by 22-Foot Subsonic Tunnel. For this set of experiments, a new outboard section was fabricated incorporating a deflectable aileron. Aileron deflection angles of 0, 7.5, 16, and 25 were investigated. This experimental investigation is in response to a recent study by Boeing potential to use AFC with a drooped aileron during takeoff to improve lift-to-drag ratio (L/D) by as much as 5%, depending on AFC mass flow rate. AFC is used at deflection angles above the nominal deflection of 7.5 to control the resulting flow separation that occurs and potentially improve L/D. Improvements in aircraft low-speed L/D can affect vehicle range and/or payload. Tuft flow visualization data, steady and unsteady surface pressure data, and force and moment data are used to compare the flowfields with and without AFC. Parameters varied include actuator momentum coefficient and aileron deflection angle. The surface pressure and tuft flow visualization results indicate that without AFC, the flow over a majority of the aileron upper surface is separated for aileron deflection angles larger than 7.5. When AFC is applied, the flow is reattached to the aileron. Force and moment results show that a local increase in lift leads to an increase in L/D of at least 3.5% using mass flow rates thought to be available from air sources onboard a commercial transport.

AFC↗

NASA NTRSDate not supplied

Wind Tunnel Testing of AFC over a Deflected Aileron on the High-Lift Common Research Model

AFC↗

NASA NTRS2000

Recent Results From The Nasa Earth Science Terra Mission and Future Possibilities

The NASA Earth Sciences Enterprise has made some remarkable strides in recent times in using developing, implementing, and utilizing spaceborne observations to better understand how the Earth works as a coupled, interactive system of the land, ocean, and atmosphere. Notable examples include the Upper Atmosphere Research (UARS) Satellite, the Topology Ocean Experiment (TOPEX) mission, Landsat-7, SeaWiFS, the Tropical Rainfall Monitoring Mission (TRMM), Quickscatt, the Shuttle Radar Topography Mission (SRTM), and, quite recently, the Terra'/Earth Observing System-1 mission. The Terra mission, for example, represents a major step forward in providing sensors that offer considerable advantages and progress over heritage instruments. The Moderate Resolution Imaging Spectrometer (MODIS), the Multi-angle Imaging SpectroRadiometer (MISR), the Measurements of Pollution in the Troposphere (MOPITT), the Advanced Spaceborne Thermal Emissions and Reflections (ASTER) radiometer, and the Clouds and Earth's Radiant Energy System (CERES) radiometer are the instruments involved. Early indications in March indicate that each of these instruments are working well and will be augmenting data bases from heritage instruments as well as producing new, unprecedented observations of land, ocean, and atmosphere features. Several missions will follow the Terra mission as the Earth Observing mission systems complete development and go into operation. These missions include EOS PM-1/'Aqua', Icesat, Vegetation Canopy Lidar (VCL), Jason/TOPEX Follow-on, the Chemistry mission, etc. As the Earth Observing systems completes its first phase in about 2004 a wealth of data enabling better understanding of the Earth and the management of its resources will have been provided. Considerable thought is beginning to be placed on what advances in technology can be implemented that will enable further advances in the early part of the 21st century; e.g., in the time from of 2020. Concepts such as 'constellation' missions or 'formation flying' with 'sensorcraft', 'sensor webs', autonomous operation of satellites, more on-board processing and delivery to individual users, data synthesis and analysis in real-time, etc. are being considered. With the data now having been and soon to be received plus the very real possibilities of further advances in use and applicability of data the potential for very significant gains in knowledge for Earth studies and applications looks quite high in the next decade or two.

Salomonson, Vincent V.↗