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DOE OSTI2022

Bay capping via acetylene addition to polycyclic aromatic hydrocarbons: Mechanism and kinetics

The bay-capping mechanism on PAH armchair edges and the kinetics of acetylene addition to 6–6–5 and 5–6–5 bays have been explored by ab initio/RRKM-ME calculations. The bays on the edges were modeled by C 21 H 11 and C 20 H 9 radicals produced by H abstractions from 7H-benzo[c]cyclopenta[e]pyrene and dicyclopenta[cf]pyrene. The C 20 H 9 + C 2 H 2 reaction is shown to have a low entrance barrier and to rapidly form the capped product, indaceno[2,1,8,7-cdefg]pyrene, along with ethynyl substituted dicyclopenta[cf]pyrene at temperatures above 1400 K. The reactivity of C 21 H 11 is shown to be governed by the location of the unpaired electron; the π radical R1 formed by H abstraction from the CH 2 group in 7H-benzo[c]cyclopenta[e]pyrene reacts with C 2 H 2 very slowly owing to a high entrance barrier, with the bay-capping rate constant approaching 10 -16 cm 3 molecule -1 s -1 only at temperatures above 2000K. Further, this result reaffirms that the growth of π aryl radicals via acetylene addition is inefficient and reflects the generally low reactivity of such radicals where the spin density is highly delocalized over the entire polyaromatic system. Alternatively, the σ C 21 H 11 radical R2 produced by H abstraction from the five-membered ring at the bay rapidly reacts with C 2 H 2 forming the bay-capped product, with the rate constant on the order of 10 -12 cm 3 molecule -1 s -1 at T≥1500K. Rate constants for the capping reactions at the 6–6–5 and 5–6–5 bays are compared with those at the 6–0–6, 6–6–6, and 6–5–6 bays. The site-specific bay-capping rate constants have been utilized in kMC simulations of the PAH growth and the results showed measurable differences when the 6–6–5 and 5–6–5 bay-capping reactions are taken into account, including an increase of the growth rate and the formation of closed-shell PAH and a rise of the number of embedded five-membered rings accompanied with a slight decrease of their overall amount.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Structure of saguaro cactus virus 3′ translational enhancer mimics 5′ cap for eIF4E binding

The genomes of several plant viruses contain RNA structures at their 3' ends called cap-independent translation enhancers (CITEs) that bind the host protein factors such as mRNA 5' cap-binding protein eIF4E for promoting cap-independent genome translation. However, the structural basis of such 5' cap-binding protein recognition by the uncapped RNA remains largely unknown. Here, we have determined the crystal structure of a 3' CITE, panicum mosaic virus-like translation enhancer (PTE) from the saguaro cactus virus (SCV), using a Fab crystallization chaperone. The PTE RNA folds into a three-way junction architecture with a pseudoknot between the purine-rich R domain and pyrimidine-rich Y domain, which organizes the overall structure to protrude out a specific guanine nucleotide, G18, from the R domain that comprises a major interaction site for the eIF4E binding. The superimposable crystal structures of the wild-type, G18A, G18C, and G18U mutants suggest that the PTE scaffold is preorganized with the flipped-out G18 ready to dock into the eIF4E 5' cap-binding pocket. The binding studies with wheat and human eIF4Es using gel electrophoresis and isothermal titration calorimetry, and molecular docking computation for the PTE–eIF4E complex demonstrated that the PTE structure essentially mimics the mRNA 5' cap for eIF4E binding. Such 5' cap mimicry by the uncapped and structured viral RNA highlights how viruses can exploit RNA structures to mimic the host protein-binding partners and bypass the canonical mechanisms for their genome translation, providing opportunities for a better understanding of virus-host interactions and non-canonical translation mechanisms found in many pathogenic RNA viruses.

3' cap-independent translation enhancers↗

DOE OSTI2021

Tailoring capping-layer composition for improved stability of mixed-halide perovskites

Incorporating a low dimensional (LD) perovskite capping layer on top of a perovskite absorber, improves the stability of perovskite solar cells (PSCs). However, in the case of mixed-halide perovskites, which can undergo halide segregation into single-halide perovskites, a systematic study of the capping layer's effect on mixed-halide perovskite absorber is still lacking. This study bridges this gap by investigating how the 1D perovskite capping layers on top of MAPb(I x Br 1–x ) 3 (x = 0, 0.25, 0.5, 0.75, 1) absorbers affect the films' stability. We utilize a new method, dissimilarity matrix, to investigate the image-based stability performance of capping-absorber pair compositions across time. This method overcomes the challenge of analyzing various film colors due to bandgap difference in mixed-halide perovskites. We also discover that the intrinsic absorber stability plays an important role in the overall stability outcome, despite the capping layer's support. Within the 55 unique capping-absorber pairs, we observe a notable 1D perovskite material, 1-methoxynaphthalene-2-ethylammonium chloride (2MeO–NEA–Cl or 9-Cl), that improves the stability of MAPbI 3 and MAPb(I 0.5 Br 0.5 ) 3 by at least 8 and 1.5 times, respectively, compared to bare films under elevated humidity and temperature. Surface photovoltage results also show that the accumulation of electrostatic charges on the film surface depends on the capping layer type, which could contribute to the acceleration/deceleration of degradation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Cold-cap structure in a slurry-fed electric melter

We report as glass batch is charged into an electric melter, a cold cap forms on the glass melt surface. Heat transfer to the cold cap from the molten glass below and the melter atmosphere above determines the melting rate. A mathematical model of the cold cap and the experimental kinetic data of the feed-to-glass conversion that were collected for several simulated low-activity and high-level waste melter feeds allowed us to develop relationships between the internal structure of the cold cap, its properties, its thickness, and the internal heat transfer. This contribution shows the distribution of major crystalline phases and the cumulative evolution of gases within the cold cap. It also examines the temperature, conversion degree, and heating rate the melter feed is experiencing during the passage through the cold cap and their effects on the cold-cap bottom temperature and morphology, which are important for the computational fluid dynamics simulations of melters.

36 MATERIALS SCIENCE↗

NASA NTRS1979

The influence of the Martian polar caps on the diurnal tide

The large horizontal heating gradients that exist near the edge of the Martian polar caps during spring are shown to be capable of exciting large oscillations in the diurnal tide. To a lesser extent, the daily mass cycling between cap and atmosphere can also contribute. The calculations which demonstrate this are based on classical tidal theory as applied to the cylindrical coordinate system. This is done to facilitate the representation of the heating function. Results are presented for the horizontal surface winds only. They indicate a circulation at the cap edge somewhat analogous to the smaller scale terrestrial sea breeze. The amplitude of the zonal component is largest and is increased from 1 to 10 m/sec by the modeled influence of the polar cap. When coupled with the basic flow these cap-edge tides can produce strong surface winds during spring. Such a mechanism may contribute to the ability of the south polar cap winds to generate the local dust storms observed near the cap edge at this season.

Haberle, R. M.↗

NASA NTRS1985

Comparisons of the North Polar Cap of Mars and the Earth's Northern Hemisphere snow cover

The boundaries of the polar caps of Mars have been measured on more than 3000 photographs since 1905 from the plate collection at the Lowell Observatory. For the Earth the polar caps have been accurately mapped only since the mid 1960's when satellites were first available to synoptically view the polar regions. The polar caps of both planets wax and wane in response to changes in the seasons, and interannual differences in polar cap behavior on Mars as well as Earth are intimately linked to global energy balance. In this study data on the year to year variations in the extent of the polar caps of Mars and Earth were assembled and analyzed together with data on annual variations in solar activity to determine if associations exist between these data. It was found that virtually no correlation exists between measurements of Mars north polar cap and solar variability. An inverse relationship was found between variations in the size of the north polar caps of Mars and Earth, although only 6 years of concurrent data were available for comparison.

Foster, J.↗

NASA NTRS1990

Year-to-year instability of the Mars south polar cap

Models of the Mars polar cap energy balance suggest that the south cap has two possible configurations at the current epoch. It can be covered all year by CO2 frost, as was observed by the Viking spacecraft, or the CO2 frost can disappear at midsummer to expose an underlying surface. The difference between the two states depends on the role of energy conducted into the subsurface. If the cap was exposed the previous year, conducted energy will cause less CO2 frost to condense in winter, and the frost will disappear completely in summer. If the cap was covered the previous year, there will be no conducted energy, and it will stay covered again. Subtle effects in the atmosphere can perturb the cap energy balance sufficiently to cause the cap to jump between states. This behavior might provide an explanation for the large southern summer water vapor abundances observed in 1969. It also explains the observed differences between the north and the south residual caps as resulting in part from a difference in the role in the annual energy balance of energy conducted into the subsurface.

Jakosky, Bruce M.↗

NASA NTRS1990

The Martian polar cap - Radiative effects of ozone, clouds, and airborne dust

The solar and thermal flux striking the polar cap of Mars is computed for various ozone, dust, and cloud abundances and for three solar zenith angles. Ozone does not significantly affect the total energy budget of the polar cap. Hence the observed hemispherical asymmetry in ozone abundance causes only an insignificant hemispherical asymmetry in the polar caps. Vertical optical depths of dust and cloud ranging from zero to 1 cause little change in the total flux absorbed by the polar cap near its edge but increase the absorbed flux significantly as one travels poleward. Hemispherical asymmetries in dust abundance, cloud cover, and surface pressure combine to cause a significant hemispherical asymmetry in the total flux absorbed by the residual polar caps, which helps to explain the dichotomy in the residual polar caps on Mars. Other processes which affect the energy budget of the polar cap are proposed and reviewed, particularly with respect to their interaction with the radiative effects of clouds and dust.

Lindner, Bernhard Lee↗

NASA NTRS1999

Driving Stresses in Mars Polar Ice Caps and Conditions for Ice Flow

Measurements of the topography of the North polar ice cap by the Mars Orbiter Laser Altimeter (MOLA) show that the ice cap is 2950 +/- 200 meters thick. The volume of the cap is about 1.2 x 10(exp 6) cu km covering an area of 1.04 x 10(exp 6) sq km, which is about 40 percent of the Greenland ice sheet in volume and 62 percent in area. The composition of the Northern cap was previously concluded to be predominately H2O, rather than CO2 ice, based on thermodynamic considerations of the insustainablity of CO2 during summer. Principal questions about the cap are: does the ice move and at what rate, is the cap currently growing or depleting in volume, and how and when was the cap formed? Recent research on terrestrial ice sheets indicates that rates of ice deformation at the low stress values characteristic of ice sheets are significantly higher than the rates given by the classic viscous-plastic flow laws commonly used.

Zwally, H. Jay↗

NASA NTRS2003

Polar Cap Disturbances: Mesosphere and Thermosphere-Ionosphere Response to Solar-Terrestrial Interactions

The Polar Cap is the Upper-Atmosphere cum Mag-netosphere region which is enclosed by the poleward boundary of the Auroral Oval and is threaded by open geomagnetic tield lines. In this region, there is normally a steady precipition (Polar "drizzle") of low energy (w 300eV) electrons that excite optical emissions from the ionosphere. At times, enhanced ionization patches are formed near the Dayside Cusp regions that drift across the Polar Cap towards the Night Sector of the Auroral Oval. Discrete auroral arcs and auroras formed during Solar Magnetic Cloud (SMC)/Coronal Mass Ejection (CME) events are also observed in the Polar Cap. Spectrophotometric observations of all these Polar Cap phenomena provide a measure of the average energy as well a energy flux of the electrons precipitating in the Polar Cap region during these disturbances. Such measurements also point to modulations of the Polar Cap Mesosphere-Lower Thermosphere (MLT) air density and temperature by zonally symmetric tides whose Hough functions peak in the Polar region. MLT cooling during Stratospheric Warming events and their relation to Polar Vortex and associated Gravity wave activities are also observed at the Polar Cap sites.

Sivjee, G.↗

NASA NTRS2005

Tracking Retreat of the North Seasonal Ice Cap on Mars: Results from the THEMIS Investigation

The CO2 ice caps on Mars advance and retreat with the seasons. This phenomenon was first observed by Cassini and then confirmed by numerous ground based observations in 19th and 20th centuries. With the advent of the space age observations of the seasonal ice cap were done by all orbiting spacecraft starting with Mariner 7. Viking Orbiters and more recently the Mars Global Surveyor (particularly Mars Orbiter Camera (MOC) and Thermal Emission Spectrometer (TES) instruments) have accumulated significant data on the retreat of the CO2 seasonal cap. During Mars year 2 of THEMIS operations at Mars, we planned an observational campaign in which the THEMIS instrument (onboard the Mars Odyssey spacecraft) repeatedly observed the north seasonal polar cap from midwinter to late spring. THEMIS allows simultaneous observations in both Thermal IR (12.57 m) and Visible wavelengths (0.65 m). One of the goals for this work is to initiate an interannual program for observations of the seasonal ice caps using the THEMIS instrument. The most efficient way to detect the edge between frost and bare ground is directly onboard of the spacecraft. Prior to onboard software design effort, we have developed two groundbased algorithms for automatically finding the edge of the seasonal polar cap in THEMIS IR data. The first algorithm relies on fully calibrated data and can be used for highly reliable groundbased analyses. The second method was specifically developed for processing raw, uncalibrated data in a highly efficient way. It has the potential to enable automatic, onboard detections of the seasonal cap retreat. We have experimentally confirmed that both methods produce similar results, and we have validated both methods against a model constructed from the MGS TES data from the same season.

Ivanov, A. B.↗

NASA NTRS2005

CAPS Simulation Environment Development

The final design for an effective Comet/Asteroid Protection System (CAPS) will likely come after a number of competing designs have been simulated and evaluated. Because of the large number of design parameters involved in a system capable of detecting an object, accurately determining its orbit, and diverting the impact threat, a comprehensive simulation environment will be an extremely valuable tool for the CAPS designers. A successful simulation/design tool will aid the user in identifying the critical parameters in the system and eventually allow for automatic optimization of the design once the relationships of the key parameters are understood. A CAPS configuration will consist of space-based detectors whose purpose is to scan the celestial sphere in search of objects likely to make a close approach to Earth and to determine with the greatest possible accuracy the orbits of those objects. Other components of a CAPS configuration may include systems for modifying the orbits of approaching objects, either for the purpose of preventing a collision or for positioning the object into an orbit where it can be studied or used as a mineral resource. The Synergistic Engineering Environment (SEE) is a space-systems design, evaluation, and visualization software tool being leveraged to simulate these aspects of the CAPS study. The long-term goal of the SEE is to provide capabilities to allow the user to build and compare various CAPS designs by running end-to-end simulations that encompass the scanning phase, the orbit determination phase, and the orbit modification phase of a given scenario. Herein, a brief description of the expected simulation phases is provided, the current status and available features of the SEE software system is reported, and examples are shown of how the system is used to build and evaluate a CAPS detection design. Conclusions and the roadmap for future development of the SEE are also presented.

Murphy, Douglas G.↗

NASA NTRS2011

Mars Seasonal Polar Caps as a Test of the Equivalence Principle

The seasonal polar caps of Mars can be used to test the equivalence principle in general relativity. The north and south caps, which are composed of carbon dioxide, wax and wane with the seasons. If the ratio of the inertial to gravitational masses of the caps differs from the same ratio for the rest of Mars, then the equivalence principle fails, Newton's third law fails, and the caps will pull Mars one way and then the other with a force aligned with the planet's spin axis. This leads to a secular change in Mars's along-track position in its orbit about the Sun, and to a secular change in the orbit's semimajor axis. The caps are a poor E6tv6s test of the equivalence principle, being 4 orders-of-magnitude weaker than laboratory tests and 7 orders-of-magnitude weaker than that found by lunar laser ranging; the reason is the small mass of the caps compared to Mars as a whole. The principal virtue of using Mars is that the caps contain carbon, an element not normally considered in such experiments. The Earth with its seasonal snow cover can also be used for a similar test.

Rubincam, Daivd Parry↗

NASA NTRS2016

The South Residual CO2 Cap on Mars: Investigations with a Mars Global Climate Model

The CO2 cycle is one of the three controlling climate cycles on Mars. One aspect of the CO2 cycle that is not yet fully understood is the existence of a residual CO2 ice cap that is offset from the south pole. Previous investigations suggest that the atmosphere could control the placement of the south residual cap (e.g., Colaprete et al., 2005). These investigations show that topographically forced stationary eddies in the south during southern hemisphere winter produce colder atmospheric temperatures and increased CO2 snowfall over the hemisphere where the residual cap resides. Since precipitated CO2 ice produces higher surface albedos than directly deposited CO2 ice, it is plausible that CO2 snowfall resulting from the zonally asymmetric atmospheric circulation produces surface ice albedos high enough to maintain a residual cap only in one hemisphere. Our current work builds on these initial investigations with a version of the NASA Ames Mars Global Climate Model (GCM) that includes a sophisticated CO2 cloud microphysical scheme. Processes of cloud nucleation, growth, sedimentation, and radiative effects are accounted for. Simulated results thus far agree well with the Colaprete et al. study—the zonally asymmetric nature of the atmospheric circulation produces enhanced snowfall over the residual cap hemisphere throughout much of the winter season. However, the predicted snowfall patterns vary significantly with season throughout the cap growth and recession phases. We will present a detailed analysis of the seasonal evolution of the predicted atmospheric circulation and snowfall patterns to more fully evaluate the hypothesis that the atmosphere controls the placement of the south residual cap.

climate cycles on Mars↗

DOE OSTI2024

Cross-Cap Defects and Fault-Tolerant Logical Gates in the Surface Code and the Honeycomb Floquet Code

We consider the Z 2 toric code, surface code, and Floquet code defined on a nonorientable surface, which can be considered as families of codes extending Shor’s nine-qubit code. We investigate the fault-tolerant logical gates of the Z 2 toric code in this setup, which corresponds to e ↔ m exchanging symmetry of the underlying Z 2 gauge theory. We find that nonorientable geometry provides a new way for the emergent symmetry to act on the code space, and discover the new realization of the fault-tolerant Hadamard gate of the two-dimensional surface code with a single cross cap connecting the vertices nonlocally along a slit, dubbed a nonorientable surface code. This Hadamard gate can be realized by a constant-depth local unitary circuit modulo nonlocality caused by a cross cap. Via folding, the nonorientable surface code can be turned into a bilayer local quantum code, where the folded cross cap is equivalent to a bilayer twist terminated on a gapped boundary and the logical Hadamard only contains local gates with intralayer couplings when being away from the cross cap, as opposed to the interlayer couplings on each site needed in the case of the folded surface code. We further obtain the complete logical Clifford gate set for a stack of nonorientable surface codes and similarly for codes defined on Klein-bottle geometries. We then construct the honeycomb Floquet code in the presence of a single cross cap, and find that the period of the sequential Pauli measurements acts as a H Z logical gate on the single logical qubit, where the cross cap enriches the dynamics compared with the orientable case. We find that the dynamics of the honeycomb Floquet code is precisely described by a condensation operator of the Z 2 gauge theory, and illustrate the exotic dynamics of our code in terms of a condensation operator supported at a nonorientable surface. Published by the American Physical Society 2024

Physics↗

DOE OSTI2021

Processing Meteorological Data for the CAP-88 PC Model at Los Alamos National Laboratory

The Environmental Protection and Compliance-Compliance Programs (EPC-CP) group at Los Alamos National Laboratory (LANL) uses the Clean Air Act Assessment Package 1988 (CAP-88, Littleton 2020) PC model (Version 4.1) to estimate radiological doses for a set of areal sectors surrounding a release location, in order to satisfy the Environmental Protection Agency (EPA) National Emission Standards for Hazardous Air Pollutants (NESHAP) dose calculation requirement in 40 CFR 61 Subpart H. Among several types of data that must be prepared for CAP-88 input is a text file of meteorological data (“WIND” file), consisting of the joint frequency of wind direction, wind speed, and atmospheric stability categories. EPC-CP produces customized WIND files by running a CAP-88 utility program on a user generated text file of wind data in a different format, known as a STability ARray (STAR) file (Turner, 1964). At LANL, EPC-CP meteorologists prepare customized STAR files with data over desired time periods at selected meteorological towers. A custom program written in Precision Visuals -Workstation Analysis and Visualization Environment (PV-WAVE), a commercial Fortran-like language, is used to read LANL meteorological data and write a STAR file; the executable filename is “Star.out”. However, the outdated PV-WAVE utility program is being phased out by EPC-CP, due to the inefficient process to run it and an inability to modify the code. To preserve the ability to create customized meteorological data for CAP-88 in a way that will be easy to use and maintain, a new replacement utility program, written in the Python programming language, has been developed. The new, improved program reads a data file from any LANL meteorological tower, and at each desired observation time, determines the wind direction, wind speed, and stability categories defined in the CAP-88 documentation. The frequencies of all combinations of the three sets of categories are calculated and written to a file in the STAR format, which can later be converted to a WIND file for input into CAP-88.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Thermal Spray toolpath development for a capped cylinder (“cake pan”) substrate

A near net shape coating is desired to be applied to the outer surface of a capped cylinder (“cake pan”) type substrate using thermal spray technology. A capped cylinder geometry is more complex than simple coupon-level substrate substrates (e.g., flat panels, cylinders) and thus requires a more complex toolpath to deposit a uniform coating. This report documents a practical theoretical approach to calculating relative torch-to-substrate speeds for coating the cylindrical, corner, and cap region of a rotating capped cylinder based on fundamental thermal spray toolpath principles. A preliminary experimental test deposited a thermal spray coating onto a mock substrate using toolpath speeds calculated by the theoretical approach proposed. The mock substrate was metallographically inspected to assess coating uniformity across the cylindrical, corner, and cap region. Inspection of the mock substrate revealed qualitatively uniform coating microstructure and thickness where theoretically predicted, demonstrating the viability of the proposed toolpath method and associated calculations. Pathways forward to optimizing coating uniformity at the cap center are proposed as near term suggested future work.

42 ENGINEERING↗

NASA NTRS1974

Climatic variations on Mars. II - Evolution of carbon dioxide atmosphere and polar caps

The long-term variations in the atmospheric pressure and the polar cap temperature of Mars resulting from the obliquity oscillations are discussed. In performing these calculations, the assumption is made that the atmosphere is in equilibrium with perennial CO2 ice deposits at the north pole, as is proposed by Leighton and Murray (1966). If heat transport by the atmosphere is neglected, the temperature of CO2 ice at the poles ranges from about 130 K to about 160 K, the corresponding atmospheric pressure rising from a few tenths of a millibar to about 30 mbar, respectively. The neglect of atmospheric heat transport probably underestimates the peak pressure. Because the altitude of the south cap is about 2 km higher than that of the north cap, CO2 ice is unstable there and will migrate to the north cap at a rate of about 10 g/sq cm yr, the implication being that the south residual cap is water ice. A simplified model of the annual polar caps and pressure fluctuations is also presented.

Ward, W. R.↗