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DOE OSTI2021

Dynamics of Product Branching from Radical Intermediates in Elementary Combustion Reactions (Final Technical Report)

While the total rate constant for many elementary reactions is well-characterized, understanding the product branching in complex reactions presents a formidable challenge. To gain an incisive probe of such reactions, our experiments investigate the dynamics of the product channels that arise from transient radical intermediates along the bimolecular reaction coordinates. Our recent published work uses the methodology developed in my group in the last fifteen years, using both imaging and scattering apparatuses. The experiments generate a particular isomeric form of an unstable radical intermediate along a bimolecular reaction coordinate and study the branching between the ensuing product channels of the energized radical as a function of its internal rotational and vibrational energy under collision-less conditions. The experiments use a combination of: 1) measurement of product velocity and angular distributions in a crossed laser-molecular beam apparatus, with electron bombardment detection in my lab in Chicago or 2) with tunable vacuum ultraviolet photoionization detection at Taiwan's National Synchrotron Radiation Research Center (NSRRC), and 3) velocity map imaging using state-selective REMPI and single photon VUV ionization of radical intermediates and reaction products. We also employ tunable VUV photoionization detection in our imaging apparatus, using difference frequency four-wave mixing to produce photoionization light tunable from 8 to 10.8 eV. This year of support funded our work to photolytically generate the radical intermediate important in the OH + propene reaction when OH adds to an end carbon. Our other major result this past year was on the photoionization detection of vinoxy radicals. Our experiments at the NSRRC definitively show that vinoxy dissociatively ionizes to both CH 3 + and HCO + , and establishes the absolute partial photoionization cross section of vinoxy to CH 3 + at 10.5 and 11.44 eV. This should allow experimentalists detecting vinoxy radicals produced in bimolecular reactions such as OH + propene to get good branching fractions to that product channel. Finally we initiated studies of the photodissociation of 1-bromo-2-chloroethane and 1,1-bromochloroethane at 193 nm at the NSRRC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Computational and Experimental Characterization of Intermediate Amorphous Phases in Geological Materials

In the subsurface, MgO engineered barriers are employed at the Waste Isolation Pilot Plant (WIPP), a transuranic waste repository near Carlsbad, NM. During service, the MgO will be exposed to high concentration brine environments and may form stable intermediate phases that can alter the barriers effectiveness. Here, MgO was aged in water and three different brine solutions. X-ray diffraction (XRD) and 1 H nuclear magnetic resonance (NMR) analysis were performed to identify the formation of secondary phases. After aging, ~4% of the MgO was hydrated and fine-grained powders resulted in greater loss of crystallinity than hard granular grains. 1 H magic angle spinning (MAS) NMR spectra resolved minor phases not visible in XRD, indicating that diverse 1 H environments are present along with Mg(OH) 2 . Density functional theory (DFT) simulations for several proposed Mg-O-H, Mg-CI-O-H, and Na-O-H containing phases were performed to index peaks in the experimental 1 H MAS NMR spectra. While proposed intermediate crystal structures exhibited overlapping 1 H NMR peaks, Mg-O-H intermediates were attributed to the growth of the 1.0-0.0ppm peak while the Mg-CI-O-H structures contributed to the 2.5- 5.0ppm peak in the chloride containing brines. Overall, NMR analysis of aged MgO indicates the formation of a range of possible intermediate structures that cannot be resolved with XRD analysis alone.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

IER - 551: Experiment for Unresolved Resonance of Plutonium Actinides (EUROPA): CED-1 for True Intermediate Pu Benchmark

IER-551 or the Experiment for Unresolved Resonance Of Plutonium Actinides (EUROPA), is an experiment campaign to design and execute a series of true intermediate energy plutonium critical configurations. EUROPA is a collaboration between Los Alamos National Laboratory (LANL), Oak Ridge National Laboratory (ORNL), and the French Institut de Radioprotection et de Sûreté Nucléaire (IRSN) to validate current and future evaluations of 239,240 Pu isotopes. Preliminary designs were optimized using Particle Swarm Optimization to save on computation time and the configuration with highest percentage of intermediate neutrons causing fission found was BeO-Cd. This combination has over 70% of fissions occurring from intermediate energy neutrons. Secondary considerations regarding end benchmark uncertainties and quality of nuclear data resulted in a beryllium metal only experiment proposed as the final system. This final preliminary design achieves 68% intermediate fissions, sensitivities of fission and capture cross sections of 239 Pu of 0.3021 and -0.1610 respectively.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

$\scriptsize\mathrm{{SQuIGG\overrightarrow{L}E}}$: Studying Quenching in Intermediate- z Galaxies—Gas, $\scriptsize\mathrm{{Angu\overrightarrow{L}ar}}$ Momentum, and Evolution

We describe the Studying Quenching in Intermediate-z Galaxies: Gas, $\scriptsize\mathrm{\rm{angu}}\overrightarrow{L}{\rm{ar}}$ momentum, and Evolution ($\scriptsize\mathrm{{SQuIGG\overrightarrow{L}E}}$) survey of intermediate-redshift post-starburst galaxies. We leverage the large sky coverage of the Sloan Digital Sky Survey to select ~1300 recently quenched galaxies at 0.5 < z ≤ 0.9 based on their unique spectral shapes. These bright, intermediate-redshift galaxies are ideal laboratories to study the physics responsible for the rapid quenching of star formation: they are distant enough to be useful analogs for high-redshift quenching galaxies, but low enough redshift that multiwavelength follow-up observations are feasible with modest telescope investments. We use the Prospector code to infer the stellar population properties and nonparametric star formation histories (SFHs) of all galaxies in the sample. We find that $\scriptsize\mathrm{{SQuIGG\overrightarrow{L}E}}$ galaxies are both very massive (M * ~ 10 11.25 M ⊙ ) and quenched, with inferred star formation rates ≲1 M ⊙ yr -1 , more than an order of magnitude below the star-forming main sequence. The best-fit SFHs confirm that these galaxies recently quenched a major burst of star formation: >75% of $\scriptsize\mathrm{{SQuIGG\overrightarrow{L}E}}$ galaxies formed at least a quarter of their total stellar mass in the recent burst, which ended just ~200 Myr before observation. We find that $\scriptsize\mathrm{{SQuIGG\overrightarrow{L}E}}$ galaxies are on average younger and more burst-dominated than most other z ≲ 1 post-starburst galaxy samples. This large sample of bright post-starburst galaxies at intermediate redshift opens a wide range of studies into the quenching process. In particular, the full $\scriptsize\mathrm{{SQuIGG\overrightarrow{L}E}}$ survey will investigate the molecular gas reservoirs, morphologies, kinematics, resolved stellar populations, active galactic nucleus incidence, and infrared properties of this unique sample of galaxies in order to place definitive constraints on the quenching process.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1990

MHD intermediate shocks in coronal mass ejections

A simplified model of coronal mass ejections is considered in which at least a portion of the interaction with the background corona involves a shock wave, and the allowable shock solutions and their compressive signatures are examined. The MHD shock-jump equations have a maximum of three possible types of solutions with an entropy rise for fixed values of the physical variables (slow, intermediate, and fast shocks). However, one of the three solution classes (the intermediate shock) is widely believed to not occur in nature and is regarded as nonevolutionary or extraneous. Without the intermediate shock, there is no multiplicity of solutions in that only one shock (or none) can occur for given physical values. All three potential shock types are considered, and it is shown solely on the basis of the shock-jump equations, that intermediate shocks must exist along some segment of the shock front for certain parametric regimes and for conditions that probably occur in some coronal mass ejections.

Steinolfson, R. S.↗

NASA NTRS1996

Gravitropism in roots of intermediate-starch mutants of Arabidopsis

Gravitropism was studied in roots of wild type (WT) Arabidopsis thaliana (L.) Heynh. (strain Wassilewskija) and three starch-deficient mutants that were generated by T-DNA insertional mutagenesis. One of these mutants was starchless while the other two were intermediate mutants, which had 51% and 60%, respectively, of the WT amount of starch as determined by light and electron microscopy. The four parameters used to assay gravitropism were: orientation during vertical growth, time course of curvature, induction, and intermittent stimulation experiments. WT roots were much more responsive to gravity than were roots of the starchless mutant, and the intermediate starch mutants exhibited an intermediate graviresponse. Our data suggest that lowered starch content in the mutants primarily affects gravitropism rather than differential growth because both phototropic curvature and growth rates were approximately equal among all four genotypes. Since responses of intermediate-starch mutants were closer to the WT response than to the starchless mutant, it appears that 51-60% of the WT level of starch is near the threshold amount needed for full gravitropic sensitivity. While other interpretations are possible, the data are consistent with the starch statolith hypothesis for gravity perception in that the degree of graviresponsiveness is proportional to the total mass of plastids per cell.

NASA Program Space Biology↗

NASA NTRS2014

Transitional Disks Associated with Intermediate-Mass Stars: Results of the SEEDS YSO Survey

Protoplanetary disks are where planets form, grow, and migrate to produce the diversity of exoplanet systems we observe in mature systems. Disks where this process has advanced to the stage of gap opening, and in some cases central cavity formation, have been termed pre-transitional and transitional disks in the hope that they represent intermediate steps toward planetary system formation. Recent reviews have focussed on disks where the star is of solar or sub-solar mass. In contrast to the sub-millimeter where cleared central cavities predominate, at H-band some T Tauri star transitional disks resemble primordial disks in having no indication of clearing, some show a break in the radial surface brightness profile at the inner edge of the outer disk, while others have partially to fully cleared gaps or central cavities. Recently, the Meeus Group I Herbig stars, intermediate-mass PMS stars with IR spectral energy distributions often interpreted as flared disks, have been proposed to have transitional and pre-transitional disks similar to those associated with solar-mass PMS stars, based on thermal-IR imaging, and sub-millimeter interferometry. We have investigated their appearance in scattered light as part of the Strategic Exploration of Exoplanets and Disks with Subaru (SEEDS), obtaining H-band polarimetric imagery of 10 intermediate-mass stars with Meeus Group I disks. Augmented by other disks with imagery in the literature, the sample is now sufficiently large to explore how these disks are similar to and differ from T Tauri star disks. The disk morphologies seen in the Tauri disks are also found for the intermediate-mass star disks, but additional phenomena are found; a hallmark of these disks is remarkable individuality and diversity which does not simply correlate with disk mass or stellar properties, including age, including spiral arms in remnant envelopes, arms in the disk, asymmetrically and potentially variably shadowed outer disks, gaps, and one disk where only half of the disk is seen in scattered light at H. We will discuss our survey results in terms of spiral arm theory, dust trapping vortices, and systematic differences in the relative scale height of these disks compared to those around Solar-mass stars. For the disks with spiral arms we discuss the planet-hosting potential, and limits on where giant planets can be located. We also discuss the implications for imaging with extreme adaptive optics instruments. Grady is supported under NSF AST 1008440 and through the NASA Origins of Solar Systems program on NNG13PB64P. JPW is supported NSF AST 100314. 0) in marked contrast to protoplanetary disks, transitional disks exhibit wide range of structural features1) arm visibility correlated with relative scale height in disk2) asymmetric and possibly variable shadowing of outer portions some transitional disks3) confirm pre-transitional disk nature of Oph IRS 48, MWC 758, HD 169142, etc.

Protoplanetary disks↗

DOE OSTI2012

Dilute Group III-V nitride intermediate band solar cells with contact blocking layers

An intermediate band solar cell (IBSC) is provided including a p-n junction based on dilute III-V nitride materials and a pair of contact blocking layers positioned on opposite surfaces of the p-n junction for electrically isolating the intermediate band of the p-n junction by blocking the charge transport in the intermediate band without affecting the electron and hole collection efficiency of the p-n junction, thereby increasing open circuit voltage (V.sub.OC) of the IBSC and increasing the photocurrent by utilizing the intermediate band to absorb photons with energy below the band gap of the absorber layers of the IBSC. Hence, the overall power conversion efficiency of a IBSC will be much higher than an conventional single junction solar cell. The p-n junction absorber layers of the IBSC may further have compositionally graded nitrogen concentrations to provide an electric field for more efficient charge collection.

14 SOLAR ENERGY↗

DOE OSTI2013

Intermediate connector for stacked organic light emitting devices

A device is provided, having an anode, a cathode, and an intermediate connector disposed between the anode and the cathode. A first organic layer including an emissive sublayer is disposed between the anode and the intermediate connector, and a second including an emissive sublayer is disposed between the intermediate connector and the cathode. The intermediate connector includes a first metal having a work function lower than 4.0 eV and a second metal having a work function lower than 5.0 eV. The work function of the first metal is at least 0.5 eV less than the work function of the second metal. The first metal is in contact with a sublayer of the second organic layer that includes a material well adapted to receive holes from a low work function metal.

42 ENGINEERING↗

DOE OSTI2015

Dilute group III-V nitride intermediate band solar cells with contact blocking layers

14 SOLAR ENERGY↗

DOE OSTI2017

Comparative TEA for Indirect Liquefaction Pathways to Distillate-Range Fuels via Oxygenated Intermediates

This paper presents a comparative techno-economic analysis of five conversion pathways from biomass to gasoline-, jet-, and diesel-range hydrocarbons via indirect liquefaction with specific focus on pathways utilizing oxygenated intermediates (derived either via thermochemical or biochemical conversion steps). The four emerging pathways of interest are compared with one conventional pathway (Fischer-Tropsch) for the production of the hydrocarbon blendstocks. The processing steps of the four emerging pathways include: biomass-to-syngas via indirect gasification, gas cleanup, conversion of syngas to alcohols/oxygenates, followed by conversion of alcohols/oxygenates to hydrocarbon blendstocks via dehydration, oligomerization, and hydrogenation. We show that the emerging pathways via oxygenated intermediates have the potential to be cost competitive with the conventional Fischer-Tropsch process. The evaluated pathways and the benchmark process generally exhibit similar fuel yields and carbon conversion efficiencies. The resulting minimum fuel selling prices are comparable to the benchmark at approximately $3.60 per gallon-gasoline equivalent, with potential for two new pathways to be more economically competitive. Additionally, the coproduct values can play an important role in the economics of the processes with oxygenated intermediates derived via syngas fermentation. Major cost drivers for the integrated processes are tied to achievable fuel yields and conversion efficiency of the intermediate steps, i.e., the production of oxygenates/alcohols from syngas and the conversion of oxygenates/alcohols to hydrocarbon fuels.

09 BIOMASS FUELS↗

DOE OSTI2020

Experimental and modeling study of C2–C4 alcohol autoignition at intermediate temperature conditions

C2–C4 alcohols are advantageous blendstocks identified by many research groups, including the U.S. Department of Energy Co-Optima Initiative, towards enabling efficient, boosted Spark-Ignition (SI) engines. Their use in advanced engine applications requires a comprehensive understanding of their intermediate-temperature autoignition behavior. This work reports an experimental and modeling study covering their fundamental autoignition characteristics in a twin-piston rapid compression machine at pressures of 20 and 40 bar, intermediate temperatures from 750 to 980 K, and two fuel loading conditions representative of boosted SI engines. Direct comparison between these alcohols is made, where the order of reactivity is established across different thermodynamic and fuel loading conditions. Changes in preliminary exothermicity (or intermediate-temperature heat release) displayed in single-stage autoignition across different alcohols and conditions are also quantified. This provides insight into fuel-to-fuel differences, and how these could affect advanced combustion concepts such as spark-assisted compression ignition. Kinetic models are used to simulate the experiments, and reasonable agreement is obtained. Furthermore, the sensitivity analysis results demonstrate the importance of accurately capturing the autoignition kinetics, particularly H-abstraction reactions on the parent fuels by OH and HO 2 , and the branching ratio associated with these.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Temporal variation of intermediate-depth earthquakes around the time of the M 9.0 Tohoku-oki earthquake

Here, the temporal evolution of intermediate-depth seismicity before and after the 2011 M9.0 Tohoku-oki earthquake reveals interactions between plate interface slip and deformation in the subducting slab. We investigate seismicity rate changes in the upper and lower planes of the double seismic zone beneath northeast Japan using both a β statistic approach and a temporal epidemic type aftershock sequence model. We do not observe an anomalous precursory increase in intermediate-depth earthquake activity preceding the mainshock; however, following the mainshock, we observe a rate increase for the intermediate-depth earthquakes in the upper plane. The average ratio of upper plane to lower plane activity and the mean deep aseismic slip rate both increased by factor of 2. An increase of downdip compression in the slab resulting from coseismic and postseismic deformation enhanced seismicity in the upper plane, which is dominated by events accommodating downdip shortening from plate unbending.

58 GEOSCIENCES↗

DOE OSTI2023

An innovative approach for atrazine electrochemical oxidation modelling: Process parameter effect, intermediate formation and kinetic constant assessment

Water reuse for irrigation activities is becoming a crucial worldwide challenge due to the depletion of water sources. Anyway, agricultural drainage can potentially contain dangerous contaminants such as metals, pesticides, and herbicides, including atrazine. To address the need for agriculture wastewater purification, we investigated atrazine removal from simulated wastewater by electro-oxidation using platinum-coated titanium electrodes on a lab-scale experimental apparatus. The effects of electrolyte composition and concentration, i.e. ionic strength and applied current density on atrazine removal, were investigated. The results demonstrated that the electrochemical oxidation of the herbicide occurred through two routes, depending on the presence or absence of oxidizing chlorine species. The generation of intermediates during the treatment was monitored and quantified by evaluating the effect of an inert electrolyte (NaClO 4 ) versus an oxidizable chlorine species (NaCl). In both experimental conditions, five intermediates were identified, including desethyl-atrazine (DEA), hydroxyatrazine (ATZ-OH), desisopropyl-atrazine (DIA) and desethyl-desisopropyl-atrazine (DEDIA). A degradation mechanism and a model for describing hydroxyl radicals and active chlorine species contributions at ATZ oxidation were also proposed. Intermediate evolution profiles suggest that ATZ degradation can be considered as a series–parallel reaction system. Finally, the energy requirement assessment for ATZ removal was carried out. The highest ATZ removal (≅98%) was achieved with NaCl = 0.08 M, J = 60 A/m −2 , and E C = 5.83 kWh m −3 . Results highlight that atrazine removal was improved when an active chlorine species (NaCl) was present in the water solution. Moreover, the addition of chlorine species during electro-oxidation is an energy-saving strategy. Collectively, electro-oxidation technique can be efficiently applied to treat polluted water in order to meet the needs of recycling water quality and reduce resource consumption.

Electro-chemical oxidation↗

DOE OSTI2020

Formation and transformation of manganese(III) intermediates in the photochemical generation of manganese(IV) oxide minerals

As important natural oxidants and adsorbents, manganese (Mn) oxide minerals affect the speciation, bioavailability and fate of pollutants and nutrient elements. It was found that birnessite-type Mn(IV) oxide minerals can be formed in the presence of NO 3 – and solar irradiation. However, the photochemical formation and transformation processes from Mn 2+ to Mn(IV) oxide minerals remain unclear. In this work, the Mn(IV) oxide minerals were confirmed to be photochemically formed mainly due to the disproportionation of Mn(III) intermediates generated from the oxidation of Mn 2+ in the presence of NO 3 – under UV light irradiation. The oxidation rate of Mn 2+ to Mn(IV) oxide minerals decreased with increasing initial Mn 2+ concentration due to the lower disproportionation rate. The increase in NO 3 – concentration, pH and temperature promoted Mn 2+ photochemical oxidation. The photochemical formation rate of Mn(IV) oxide minerals increased with increasing ligand concentrations at low ligand concentrations. Ligands affected the formation of Mn(IV) oxide minerals by promoting the formation and reducing the reactivity of Mn(III) intermediates. Altogether, this work reveals the important role of Mn(III) intermediates in the formation of natural Mn oxide minerals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

In-operando surface-sensitive probing of electrochemical reactions on nanoparticle electrocatalysts: Spectroscopic characterization of reaction intermediates and elementary steps of oxygen reduction reaction on Pt

In this paper we present an in-operando spectroscopic study of the reaction intermediates involved in ORR on electrified Pt nanoparticle electrocatalysts. To accomplish this, we have synthesized Ag-Pt core–shell nanoparticles, that contain a thin shell of Pt (~1 nm) uniformly deposited on a larger Ag core (~60 nm). We show that these nanostructures are ideal platforms for in-operando Plasmon Enhanced Raman Spectroscopy (PERS) of ORR on Pt. We combined these PERS studies with DFT calculations to assign the measured vibrational spectra to relevant surface intermediates as a function of electrocatalyst potential. Overall, these vibrational assignments were further verified and validated by performing PERS measurements using de-oxygenated and heavy oxygen (O 2 -18) saturated electrolyte. These studies allowed us to identity the presence of critical reaction intermediates (OH, O 2 , OOH, and H 2 O) as the function of operating voltage on the Pt surface and derive voltage-dependent elementary step mechanisms of the reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Large structural modulations in the relaxor ferroelectric and intermediate state of strontium rich members (x>0.6) of the Sr{sub x}Ba{sub 1−x}Nb{sub 2}O{sub 6} (sbn) solid solution series

The amplitudes of the positional, occupational and adp modulations of sbn mixed crystals are strongly enhanced for high strontium contents. The increase of structural modulations is accompanied by reduced spontaneous electric polarization largely due to smaller off-center shifts of the niobium atoms. Beyond the room temperature ferroelectric – intermediate transition near x=0.77, anomal large U{sub 33} atomic displacement parameters of the niobium atoms indicate static disorder caused by loss of orientational coupling between residual shifts of Nb atoms in neighboring NbO{sub 6} octahedra. Change of satellite intensities show a reduction from two-dimensional to one-dimensional modulation which is not consistent with tetragonal symmetry. The pseudo-tetragonally twinned crystal structure of sbn82 was refined in the orthorhombic super-space group A2mm(½0γ)000. The apparent tetragonal symmetry of the other investigated sbn samples also seems to be due to pseudo tetragonal twinning with equal twin volumes. The modulations mainly consist of cooperatively tilted NbO{sub 6} octahedra and wave-like ordered incomplete occupation of the largest cation sites (Me2a and b) by Ba{sup 2+} and Sr{sup 2+}. Furthermore, the atomic displacement parameters of the Me2 sites are strongly modulated. - Graphical abstract: Satellite reflections and modulation coefficients in the solid solution series Sr{sub x}Ba{sub 1−x}Nb{sub 2}O{sub 6}. - Highlights: • The modulationed structures are refined for the whole composition range of sbn32–sbn82 in tetragonal and orthorhombic setting. • The amplitudes of positional, occupational and adp modulations increase strongly with the strontium content. • Evidence is presented that the sbn crystals are pseudo tetragonally twinned. • The ferroelectric–intermediate paraelectric transition is not accompanied by a change of symmetry. • Anomal adp of intermediate (non-ferroelectric) sbn82 indicate loss of coupling between off-center shifts of neighboring niobium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Reactive Intermediates or Inert Graphene? Temperature- and Pressure-Determined Evolution of Carbon in the CH 4 –Ni(111) System

Atomic-level identification of carbon intermediates under reaction conditions is essential for carbon-related heterogeneous catalysis. Using the in operando technique of near-ambient-pressure X-ray photoelectron spectroscopy, we have identified in this paper various carbon intermediates during the thermal decomposition of CH 4 on Ni(111), including *CH, *C 1 /Ni 3 C, *C n (n ≥ 2), and clock-reconstructed Ni 2 C at different temperature regions (300–900 K). These “reactive” carbon precursors can either react with probing molecules such as O 2 at room temperature or be etched away by CH 4 . They can also develop into graphene flakes under controlled conditions: a temperature between 800 and 900 K and a suitable CH 4 pressure (10 –3 –10 –1 mbar, depending on temperature). The growth rate of graphene is significantly restrained at higher CH 4 pressures, due to the accelerated etching of its carbon precursors. The identification of in operando carbon intermediates and the control of their evolution have great potential in designing heterogeneous catalysts for the direct conversion of methane. Finally, the observed carbon aggregation/etching equilibrium reveals an underlying mechanism in coking prevention and in the fabrication of large-area single-crystal graphene, where the suppression of seeding density and etching up of small grains are required.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗