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NASA NTRS1992

Approach to derivation of SIR-C science requirements for calibration

Many of the experiments proposed for the forthcoming SIR-C mission require calibrated data, for example those which emphasize (1) deriving quantitative geophysical information (e.g., surface roughness and dielectric constant), (2) monitoring daily and seasonal changes in the Earth's surface (e.g., soil moisture), (3) extending local case studies to regional and worldwide scales, and (4) using SIR-C data with other spaceborne sensors (e.g., ERS-1, JERS-1, and Radarsat). There are three different aspects to the SIR-C calibration problem: radiometric and geometric calibration, which have been previously reported, and polarimetric calibration. The study described in this paper is an attempt at determining the science requirements for polarimetric calibration for SIR-C. A model describing the effect of miscalibration is presented first, followed by an example describing how to assess the calibration requirements specific to an experiment. The effects of miscalibration on some commonly used polarimetric parameters are also discussed. It is shown that polarimetric calibration requirements are strongly application dependent. In consequence, the SIR-C investigators are advised to assess the calibration requirements of their own experiment. A set of numbers summarizing SIR-C polarimetric calibration goals concludes this paper.

Dubois, Pascale C.↗

NASA NTRS1993

Separation of spallation and terrestrial C-14 in chondrites

Weathering products and contamination severely hamper our ability to accurately measure the C-14 spallation component in meteorites, but can give insights into a sample's terrestrial history. A procedure was developed to measure the C-14 in these components using CO and CO2 separations from temperature extractions from 200-500 mg of material. The Bruderheim (L6) chondrite was chosen as a standard following the practice of previous researchers, crosschecked against Peace River (L6), Abee (EH4), and Juvinas (EUC). Low temperature fractions (less than 900 C) give C-14 signatures consistent with a modern terrestrial C-14 source; melt fractions show elevated levels attesting to a spallogenic origin. Higher yields of CO in the melt fraction are less affected by the low levels of experimental contamination than the CO2. This fraction gave a mean CO:CO2 ratio in Bruderheim of 81.6 +/- 7.7; the ratio of the spallation component is 79.8 +/- 8.1. These values suggest equilibrium release of gases on the olivine-silica-pyroxene-iron buffer. This is corroborated by approximately equal release of the two components at 900 C. The chondrites gave an average saturation level of 54.3 +/- 2.9 dpm/kg; the achondrite gave 49.6 +/- 2.0 dpm/kg. No clear correlation with oxygen content is apparent, though shielding effects have yet to be evaluated. A further evaluation of this subject matter is given.

Cresswell, R. G.↗

NASA NTRS2014

Hi-C Observations of an Active Region Corona, and Investigation of the Underlying Magnetic Structure

The solar corona is much hotter (>=10(exp 6) K) than its surface (approx 6000 K), puzzling astrophysicists for several decades. Active region (AR) corona is again hotter than the quiet Sun (QS) corona by a factor of 4-10. The most widely accepted mechanism that could heat the active region corona is the energy release by current dissipation via reconnection of braided magnetic field structure, first proposed by E. N. Parker three decades ago. The first observational evidence for this mechanism has only recently been presented by Cirtain et al. by using High-resolution Coronal Imager (Hi-C) observations of an AR corona at a spatial resolution of 0.2 arcsec, which is required to resolve the coronal loops, and was not available before the rocket flight of Hi-C in July 2012. The Hi-C project is led by NASA/MSFC. In the case of the QS, work done by convection/granulation on the inter-granular feet of the coronal field lines translates into the heat observed in the corona. In the case of the AR, as here, there could be flux emergence, cancellation/submergence, or shear flows generating large stress and tension in coronal field loops which is released as heat in the corona. We are currently investigating the changes taking place in photospheric feet of the magnetic field involved with brightenings in the Hi-C AR corona. For this purpose, we are also using SDO/AIA data of +/- 2 hours around the 5 minutes Hi-C flight. In the present talk, I will first summarize some of the results of the Hi-C observations and then present some results from our recent analysis on what photospheric processes feed the magnetic energy that dissipates into heat in coronal loops.

Tiwari, S. K.↗

DOE OSTI2022

Nitrogen Atom Transfer Catalysis by Metallonitrene C−H Insertion: Photocatalytic Amidation of Aldehydes

Abstract C−H amination and amidation by catalytic nitrene transfer are well‐established and typically proceed via electrophilic attack of nitrenoid intermediates. In contrast, the insertion of (formal) terminal nitride ligands into C−H bonds is much less developed and catalytic nitrogen atom transfer remains unknown. We here report the synthesis of a formal terminal nitride complex of palladium. Photocrystallographic, magnetic, and computational characterization support the assignment as an authentic metallonitrene (Pd−N) with a diradical nitrogen ligand that is singly bonded to Pd II . Despite the subvalent nitrene character, selective C−H insertion with aldehydes follows nucleophilic selectivity. Transamidation of the benzamide product is enabled by reaction with N 3 SiMe 3 . Based on these results, a photocatalytic protocol for aldehyde C−H trimethylsilylamidation was developed that exhibits inverted, nucleophilic selectivity as compared to typical nitrene transfer catalysis. This first example of catalytic C−H nitrogen atom transfer offers facile access to primary amides after deprotection.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

C−H Activation of Inert Arenes using a Photochemically Activated Guanidinato‐Magnesium(I) Compound

Abstract UV irradiation of solutions of a guanidinate coordinated dimagnesium(I) compound, [{(Priso)Mg} 2 ] 3 (Priso=[(DipN) 2 CNPr i 2 ] − , Dip=2,6‐diisopropylphenyl), in either benzene, toluene, the three isomers of xylene, or mesitylene, leads to facile activation of an aromatic C−H bond of the solvent in all cases, and formation of aryl/hydride bridged magnesium(II) products, [{(Priso)Mg} 2 (μ‐H)(μ‐Ar)] 4 – 9 . In contrast to similar reactions reported for β‐diketiminate coordinated counterparts of 3 , these C−H activations proceed with little regioselectivity, though they are considerably faster. Reaction of 3 with an excess of the pyridine, p ‐NC 5 H 4 Bu t (py Bu t ), gave [(Priso)Mg(py Bu t H)(py Bu t ) 2 ] 10 , presumably via reduction of the pyridine to yield a radical intermediate, [(Priso)Mg(py Bu t ⋅)(py Bu t ) 2 ] 11 , which then abstracts a proton from the reaction solvent or a reactant. DFT calculations suggest two possible pathways to the observed arene C−H activations. One of these involves photochemical cleavage of the Mg−Mg bond of 3 , generating magnesium(I) doublet radicals, (Priso)Mg⋅. These then doubly reduce the arene substrate to give “Birch‐like” products, which subsequently rearrange via C−H activation of the arene. Circumstantial evidence for the photochemical generation of transient magnesium radical species includes the fact that irradiation of a cyclohexane solution of 3 leads to an intramolecular aliphatic C−H activation process and formation of an alkyl‐bridged magnesium(II) species, [{Mg(μ‐Priso −H )} 2 ] 12 . Furthermore, irradiation of a 1 : 1 mixture of 3 and the β‐diketiminato dimagnesium(I) compound, [{( Dip Nacnac)Mg} 2 ] ( Dip Nacnac=[HC(MeCNDip) 2 ] − ), effects a “scrambling” reaction, and the near quantitative formation of an unsymmetrical dimagnesium(I) compound, [(Priso)Mg−Mg( Dip Nacnac)] 13 . Finally, the EPR spectrum (77 K) of a glassed solution of UV irradiated 3 is dominated by a broad featureless signal, indicating the presence of a doublet radical species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Measurement of lepton mass squared moments in B → X c ℓ ν ¯ ℓ decays with the Belle II experiment

We present measurements of the first to fourth moments of the lepton mass squared $q$ 2 of $B$ → $X_cℓ\overline{ν}_ℓ$ decays for $ℓ = e, μ$ and with $X_c$ a hadronic system containing a charm quark. These results use a sample of electron-positron collisions at the $Υ$($4S$) resonance corresponding to 62.8 fb -1 of integrated luminosity and collected by the Belle II 2 experiment in 2019 and 2020. To identify the $X_c$ system and reconstruct $q$ 2 , one of the $B$ mesons from an $Υ$($4S$) → $B\overline{B}$ decay is fully reconstructed in a hadronic decay mode using a multivariate $B$ tagging algorithm. We report raw and central moments for $q$ 2 > 1.5 $GeV$ 2 =$c$ 4 up to $q$ 2 > 8.5 $GeV$ 2 =$c$ 4 , probing up to 77% of the accessible $B$ → $X_cℓ\overline{ν}_ℓ$ phase space. This is the first measurement of moments in the experimentally challenging range of [1.5; 2.5] $GeV$ 2 =$c$ 4 . The results can be used for a new determination of |$V_{cb}$| using inclusive $B$ → $X_cℓ\overline{ν}_ℓ$ decays.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Measurement of C P asymmetries in B 0 → K S 0 K S 0 K S 0 decays at Belle II

We report a measurement of decay-time-dependent charge-parity ( C P ) asymmetries in B 0 → K S 0 K S 0 K S 0 decays. We use 387 × 10 6 B B ¯ pairs collected at the ϒ ( 4 S ) resonance with the Belle II detector at the SuperKEKB asymmetric-energy electron-positron collider. We reconstruct 220 signal events and extract the C P -violating parameters S and C from a fit to the distribution of the decay-time difference between the two B mesons. The resulting confidence region is consistent with previous measurements in B 0 → K S 0 K S 0 K S 0 and B 0 → ( c c ¯ ) K 0 decays and with predictions based on the standard model. Published by the American Physical Society 2024

Astronomy & Astrophysics↗

DOE OSTI2020

Molecular understanding of new-particle formation from α-pinene between -50 and +25 °C

Abstract. Highly oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth's climate. HOMs are formed by rapid, gas-phase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to -50°C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products, and a two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25°C to 0.7 % at -50°C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at -50°C compared with 25°C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Study of the decays χ c J → Λ Λ ¯ ω

Using ( 27.12 ± 0.14 ) × 10 8 ψ ( 3686 ) events collected with the BESIII detector, we present the first observation of the decays χ c J → Λ Λ ¯ ω , where J = 0 , 1, 2, with statistical significances of 11.7 σ , 11.2 σ , and 11.8 σ . The branching fractions of these decays are determined to be B ( χ c 0 → Λ Λ ¯ ω ) = ( 2.37 ± 0.22 ± 0.25 ) × 10 − 4 , B ( χ c 1 → Λ Λ ¯ ω ) = ( 1.01 ± 0.10 ± 0.11 ) × 10 − 4 , and B ( χ c 2 → Λ Λ ¯ ω ) = ( 1.40 ± 0.13 ± 0.17 ) × 10 − 4 , where the first uncertainties are statistical and the second are systematic. We observe no clear intermediate structures. Published by the American Physical Society 2024

Astronomy & Astrophysics↗

DOE OSTI2024

Search for X ( 3872 ) → π 0 π 0 χ c 1 , 2

Using 10.1 fb − 1 of e + e − collision data collected by the BESIII detector with center-of-mass energies between 4.15 GeV and 4.30 GeV, we search for the decays X ( 3872 ) → π 0 π 0 χ c 1 , 2 , where the X ( 3872 ) is produced in e + e − → γ X ( 3872 ) . No evidence above 3 σ is found for either decay. Upper limits at the 90% CL on the branching fractions of X ( 3872 ) → π 0 π 0 χ c 1 , 2 normalized to the branching fraction of X ( 3872 ) → π + π − J / ψ are set to be B ( X ( 3872 ) → π 0 π 0 χ c 1 ) / B ( X ( 3872 ) → π + π − J / ψ ) < 1.1 and B ( X ( 3872 ) → π 0 π 0 χ c 2 ) / B ( X ( 3872 ) → π + π − J / ψ ) < 0.5 , taking into account both statistical and systematic uncertainties. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Search for the e + e − → ϕ χ c 1 ( 3872 ) process at BESIII

Based on 368.5 p b − 1 of e + e − collision data collected at center-of-mass energies 4.914 and 4.946 GeV by the BESIII detector, the e + e − → ϕ χ c 1 ( 3872 ) process is searched for the first time. No significant signal is observed and the upper limits at the 90% confidence level on the product of the Born cross section σ ( e + e − → ϕ χ c 1 ( 3872 ) ) and the branching fraction B [ χ c 1 ( 3872 ) → π + π − J / ψ ] at 4.914 and 4.946 GeV are set to be 0.85 and 0.96 pb, respectively. These measurements provide useful information for the production of the χ c 1 ( 3872 ) at e + e − colliders and deepen our understanding about the nature of this particle. Published by the American Physical Society 2024

Astronomy & Astrophysics↗

DOE OSTI2024

Measurement of C P Violation in B 0 → ψ ( → ℓ + ℓ − ) K S 0 ( → π + π − ) Decays

A measurement of time-dependent C P violation in the decays of B 0 and B ¯ 0 mesons to the final states J / ψ ( → μ + μ − ) K S 0 , ψ ( 2 S ) ( → μ + μ − ) K S 0 and J / ψ ( → e + e − ) K S 0 with K S 0 → π + π − is presented. The data correspond to an integrated luminosity of 6 fb − 1 collected at a center-of-mass energy of s = 13 TeV with the LHCb detector. The C P -violation parameters are measured to be S ψ K S 0 = 0.717 ± 0.013 ( stat ) ± 0.008 ( syst ) and C ψ K S 0 = 0.008 ± 0.012 ( stat ) ± 0.003 ( syst ) . This measurement of S ψ K S 0 represents the most precise single measurement of the CKM angle β to date and is more precise than the current world average. In addition, measurements of the C P -violation parameters of the individual channels are reported and a combination with the LHCb Run 1 measurements is performed. © 2024 CERN, for the LHCb Collaboration 2024 CERN

Aaij, R. (ORCID:0000000305331952)↗

DOE OSTI2020

Electrical and Elastic Properties of Individual Single-Layer Nb 4 C 3 T x MXene Flakes

2D carbides and nitrides (MXenes) are widely recognized for their exceptional promise for numerous applications. However, physical property measurements of their individual monolayers remain very limited despite their importance for revealing the intrinsic physical properties of MXenes. The first mechanical and electrical measurements of individual single-layer flakes of Nb 4 C 3 T x MXene, which are prepared via an improved synthetic method are reported. Characterization of field-effect transistor devices based on individual single-layer Nb 4 C 3 T x flakes shows an electrical conductivity of 1024 ± 165 S cm -1 , which is two orders of magnitude higher than the previously reported values for bulk Nb 4 C 3 T x assemblies, and an electron mobility of 0.41 ± 0.27 cm 2 V -1 s -1 . Atomic force microscopy nanoindentation measurements of monolayer Nb 4 C 3 T x membranes yield an effective Young's modulus of 386 ± 13 GPa, assuming a membrane thickness of 1.26 nm. This is the highest value reported for nanoindentation measurements of solution-processable 2D materials, revealing the potential of Nb 4 C 3 T x as a primary component for various mechanical applications. In conclusion, the agreement between the mechanical properties of 2D Nb 4 C 3 T x MXene and cubic NbC suggests that the extensive experimental data on bulk carbides could be useful for identifying new MXenes with improved functional characteristics.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Enhanced Rate Capability of Ion‐Accessible Ti 3 C 2 T x ‐NbN Hybrid Electrodes

Abstract Although 2D Ti 3 C 2 T x is a good candidate for supercapacitors, the restacking of nanosheets hinders the ion transport significantly at high scan rates, especially under practical mass loading (>10 mg cm −2 ) and thickness (tens of microns). Here, Ti 3 C 2 T x ‐NbN hybrid film is designed by self‐assembling Ti 3 C 2 T x with 2D arrays of NbN nanocrystals. Working as an interlayer spacer of Ti 3 C 2 T x , NbN facilitates the ion penetration through its 2D porous structure; even at extremely high scan rates. The hybrid film shows a thickness‐independent rate performance (almost the same rate capabilities from 2 to 20 000 mV s −1 ) for 3 and 50 µm thick electrodes. Even a 109 µm thick Ti 3 C 2 T x ‐NbN electrode shows a better rate performance than 25 µm thick pure Ti 3 C 2 T x electrodes. This method may pave a way to controlling ion transport in electrodes composed of 2D conductive materials, which have potential applications in high‐rate energy storage and beyond.

Wang, Hao↗

DOE OSTI2020

The Critical Role of Reductive Steps in the Nickel-Catalyzed Hydrogenolysis and Hydrolysis of Aryl Ether C-O Bonds

Hydrogenolysis of the aromatic C-O bond in aryl ethers is catalyzed by Ni in decalin or water at 150 °C. Observations of a significant kinetic isotope effect (kH/kD = 5.7) for the reactions of diphenyl ether under H2 and D2 and a positive dependence of the rate on H2 chemical potential in decalin indicate that addition of H to the aromatic ring is the rate-limiting step rather than C-O scission. Hydrogen addition occurs on the metal before C-O bond scission. DFT calculations indicate that hydrogen atom addition to the ortho position followed by C-O scission is energetically more feasible than C-O scission followed by H addition to either phenoxyl or phenyl moieties. Hydrogenolysis initiated via H addition in water is more selective (~75 %) compared to reactions in decalin (~30 %). The high selectivity for hydrogenolysis is attributed to stabilization of polar transition state by water as a polar solvent.

Wang, Meng↗

DOE OSTI2021

Impurity Control in Catalyst Design: The Role of Sodium in Promoting and Stabilizing Co and Co 2 C for Syngas Conversion

The design of supported heterogeneous catalysts requires a detailed understanding of the structure and chemistry of the active surface. Although the chemical components of the active phase, support material, and process feed are typically considered to be the most important factors governing catalyst structure and performance, many common commercial supports contain trace impurities, which can have profound effects on catalyst properties. In this work, we study silica–supported cobalt–based catalysts, which are widely used in syngas conversion to value–added products. Supported metallic Co is a commercial Fischer–Tropsch catalyst, whereas Co 2 C has shown promise for the direct conversion of syngas to higher oxygenates. This study examines the effects of Na, a commonly detected support impurity and a frequently used promoter, on the structure and reactivity of Co and Co 2 C. We show that trace Na impurities significantly decrease catalyst activity of supported metallic Co, and that high Na concentrations result in Co 2 C formation and a loss in Fischer–Tropsch activity. However, in Co 2 C catalysts, Na plays an important role in stabilizing the Co 2 C phase, but excess Na decreases catalyst activity. We use insitu X–ray absorption spectroscopy to study Co 2 C formation and decomposition in the Na–free catalyst under carburization and reaction conditions. Lastly, the work reveals the importance of carefully controlling alkali metal content, particularly at trace levels, in catalyst design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Gas–Phase Preparation of the 14π Hückel Polycyclic Aromatic Anthracene and Phenanthrene Isomers (C 14 H 10 ) via the Propargyl Addition–BenzAnnulation (PABA) Mechanism

Polycyclic aromatic hydrocarbons (PAHs) imply the missing link between resonantly stabilized free radicals and carbonaceous nanoparticles, commonly referred to as soot particles in combustion systems and interstellar grains in deep space. Whereas gas phase formation pathways to the simplest PAH – naphthalene (C 10 H 8 ) – are beginning to emerge, reaction pathways leading to the synthesis of the 14π Hückel aromatic PAHs anthracene and phenanthrene (C 14 H 10 ) are still incomplete. Here, by utilizing a chemical microreactor in conjunction with vacuum ultraviolet (VUV) photoionization (PI) of the products followed by detection of the ions in a reflectron time-of-flight mass spectrometer (ReTOF-MS), the reaction between the 1'- and 2'-methylnaphthyl radicals (C 11 H 9 •) with the propargyl radical (C 3 H 3 •) accesses anthracene (C 14 H 10 ) and phenanthrene (C 14 H 10 ) via the Propargyl Addition–BenzAnnulation (PABA) mechanism in conjunction with a hydrogen assisted isomerization. Furthermore, the preferential formation of the thermodynamically less stable anthracene isomer compared to phenanthrene suggests a kinetic, rather than a thermodynamics control of the reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Diversifying and perennializing plants in agroecosystems alters retention of new C and N from crop residues

Abstract Managing soils to retain new plant inputs is key to moving toward a sustainable and regenerative agriculture. Management practices, like diversifying and perennializing agroecosystems, may affect the decomposer organisms that regulate how new residue is converted to persistent soil organic matter. Here we tested whether 12 years of diversifying/perennializing plants in agroecosystems through extended rotations or grassland restoration would decrease losses of new plant residue inputs and, thus, increase retention of carbon (C) and nitrogen (N) in soil. We tracked dual‐labeled ( 13 C and 15 N), isotopically enriched wheat ( Triticum aestivum ) residue in situ for 2 years as it decomposed in three agroecosystems: maize–soybean (CS) rotation, maize–soybean–wheat plus red clover and cereal rye cover crops (CSW2), and spring fallow management with regeneration of natural grassland species (seven to 10 species; SF). We measured losses of wheat residue (C wheat and N wheat ) in leached soil solution and greenhouse gas fluxes, as well as how much was recovered in microbial biomass and bulk soil at 5‐cm increments down to 20 cm. CSW2 and SF both had unique, significant effects on residue decomposition and retention dynamics that were clear only when using nuanced metrics that able to tease apart subtle differences. For example, SF retained a greater portion of C wheat in 0–5 cm surface soils (155%, p = 0.035) and narrowed the C wheat to N wheat ratio ( p < 0.030) compared to CS. CSW2 increased an index of carbon‐retention efficiency, C wheat retained in the mesocosm divided by total measured, from 0.18 to 0.27 (49%, p = 0.001), compared to CS. Overall, we found that diversifying and extending the duration of living plants in agroecosystems can lead to greater retention of new residue inputs in subtle ways that require further investigation to fully understand.

McDaniel, Marshall D.↗