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At least 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Simultaneous isotopic analysis of fission product Sr, Mo, and Ru in spent nuclear fuel particles by resonance ionization mass spectrometry

Abstract Fission product Sr, Mo, and Ru isotopes in six 10-μm particles of spent fuel from a pressurized water reactor were analyzed by resonance ionization mass spectrometry (RIMS) and evaluated for utility in nuclear material characterization. Previous measurements on these same samples showed widely varying U, Pu, and Am isotopic compositions owing to the samples’ differing irradiation environments within the reactor. This is also seen in Mo and Ru isotopes, which have the added complication of exsolution from the UO 2 fuel matrix. This variability is a hindrance to interpreting data from a collection of particles with incomplete provenance since it is not always possible to assign particles to the same batch of fuel based on isotopic analyses alone. In contrast, the measured 90 Sr/ 88 Sr ratios were indistinguishable across all samples. Strontium isotopic analysis can therefore be used to connect samples with otherwise disparate isotopic compositions, allowing them to be grouped appropriately for interpretation. Strontium isotopic analysis also provides a robust chronometer for determining the time since fuel irradiation. Because of the very high sensitivity of RIMS, only a small fraction of material in each of the 10 μm samples was consumed, leaving the vast majority still available for other analyses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Direct neutron-diffraction-based measurement of magnetic order in brownmillerite SrCoO 2.5 and La 0.5 Sr 0.5 CoO 2.5 thin films

Epitaxial cobaltites have emerged as exemplary materials for electrochemical gating, in large part due to their topotactic perovskite (P) ↔ brownmillerite (BM) transformations. SrCoO 3-δ , for example, can be cycled between metallic ferromagnetic P SrCoO 3 and insulating BM SrCoO 2.5 , realizing exceptional modulation of electronic, thermal, and optical properties. It is often presumed that such cycling also generates ferromagnetic–antiferromagnetic (F-AF) modulation due to the G-type AF order in bulk SrCoO 2.5 . Little is understood about magnetism in thin-film BM SrCoO 2.5 , however, meaning that the true magnetic property modulation is unclear. We address this here through a neutron diffraction study of BM La 1-x Sr x CoO 2.5 films at x = 0.5 and 1.0. Lightly compressively strained SrCoO 2.5 films are shown to retain G-type AF order, albeit with suppressed Néel temperature (~340 K). Of high interest for AF spintronics, room-temperature F–AF cycling is thus possible across the SrCoO 3-δ P ↔ BM transformation. At x = 0.5, however, BM La 0.5 Sr 0.5 CoO 2.5 films are found to exhibit no detectable G-type AF order but instead weak F order (Curie temperature ~115 K), unveiling a La 0.5 Sr 0.5 CoO 3-δ phase diagram with two distinct F phases. These results thus uncover new, unanticipated magnetic phase behavior in these materials, in addition to being directly relevant to cobaltite-based magnetoionics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Study of structural, transport and magneto-crystalline anisotropy in La 1-x Sr x MnO 3 (0.30 ≤ x ≤ 0.40) perovskite manganites

In this paper we present structural, transport, magnetic and magneto-crystalline anisotropy of La 1–x Sr x MnO 3 (х = 0.30, 0.33, 0.36, and 0.40) synthesized using the solid-state reaction method. The X-ray diffraction pattern of the samples is well indexed to the rhombohedral structure with R 3 - c space group. Lattice parameters and unit cell volume are found to decrease monotonically upon increasing Sr 2+ concentration at La 3+ site. X-ray photoelectron spectroscopy confirms the presence of Mn 4+ and Mn 3+ , the ratio of which (Mn 4+ /Mn 3+ ) increases from 0.44 to 0.64 with increasing Sr 2+ concentration. From the ρ(T) and M(T) data analysis, we find that T MI and M S are larger for x = 0.33 composition, suggesting a weakening of the double-exchange interaction due to competing super-exchange interactions in x = 0.30, 0.36 and 0.40 samples. We calculated MCA constant (K 1 ) by fitting the saturation magnetisation data at a higher magnetic field using the law of approach model, M = M S [1-a/H-b/H 2 ]-χH with K 1 2 = (105/8)bMs 2 and is in the order of 10 5 erg/cm 3 .

36 MATERIALS SCIENCE↗
DOE OSTI2020

Momentum-resolved superconducting energy gaps of Sr 2 RuO 4 from quasiparticle interference imaging

Sr 2 RuO 4 has long been the focus of intense research interest because of conjectures that it is a correlated topological superconductor. It is the momentum space ( k -space) structure of the superconducting energy gap Δ i ( k ) on each band i that encodes its unknown superconducting order parameter. However, because the energy scales are so low, it has never been possible to directly measure the Δ i ( k ) of Sr 2 RuO 4 . In this work, we implement Bogoliubov quasiparticle interference (BQPI) imaging, a technique capable of high-precision measurement of multiband Δ i ( k ). At T = 90 mK,we visualize a set of Bogoliubov scattering interference wave-vectors q j : j = 1 – 5 consistent with eight gap nodes/minima that are all closely aligned to the (±1, ±1) crystal lattice directions on both the α and β bands. Taking these observations in combination with other very recent advances in directional thermal conductivity, temperature-dependent Knight shift, time-reversal symmetry conservation, and theory, the BQPI signature of Sr 2 RuO 4 appears most consistent with Δ i ( k ) having d x 2 – y 2 ( B 1 g ) symmetry.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Electronic nematicity in Sr 2 RuO 4

We have measured the angle-resolved transverse resistivity (ARTR), a sensitive indicator of electronic anisotropy, in high-quality thin films of the unconventional superconductor Sr 2 RuO 4 grown on various substrates. The ARTR signal, heralding the electronic nematicity or a large nematic susceptibility, is present and substantial already at room temperature and grows by an order of magnitude upon cooling down to 4 K. In Sr 2 RuO 4 films deposited on tetragonal substrates the highest-conductivity direction does not coincide with any crystallographic axis. In films deposited on orthorhombic substrates it tends to align with the shorter axis; however, the magnitude of the anisotropy stays the same despite the large lattice distortion. These are strong indications of actual or incipient electronic nematicity in Sr 2 RuO 4 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Pervasive symmetry-lowering nanoscale structural fluctuations in the cuprate La 2−𝑥 ⁢Sr 𝑥 ⁢Cu⁢O 4

The cuprate superconductors are among the most widely studied quantum materials, yet there remain fundamental open questions regarding their electronic properties and the role of structural degrees of freedom. Recent neutron and x-ray scattering measurements uncovered exponential scaling with temperature of the strength of orthorhombic fluctuations in the tetragonal phase of La 2−𝑥⁢ Sr 𝑥 ⁢Cu⁢O 4 and Tl 2 ⁢Ba 2 ⁢Cu⁢O 6+𝛿 , unusual behavior that closely resembles prior results for the emergence of superconducting fluctuations, and that points to a common origin rooted in inherent correlated structural inhomogeneity. Here, in this study, we use neutron and x-ray diffuse scattering to provide further insight into structural fluctuations in La 2−𝑥 ⁢Sr 𝑥 ⁢Cu⁢O 4 . We perform measurements up to temperatures that approach the melting point of the undoped parent compound, and we investigate the effects of in situ in-plane uniaxial elastic stress and plastic deformation. Our neutron scattering results for the parent compound La 2 ⁢Cu⁢O 4 reveal that short-range orthorhombic fluctuations persist to the maximum experimental temperature of nearly 1000 K, i.e., to a significant fraction of the crystallization temperature. At this temperature, the spatial characteristic length extracted from the momentum-space data is still about three lattice constants. The neutron scattering experiment enables quasistatic discrimination and reveals that the response is increasingly dynamic at higher temperatures. We also find that neither compressive elastic stress along the tetragonal [110] direction nor irreversible plastic deformation activating the ⟨100⟩⁢[001] slip system significantly alter the robust orthorhombic fluctuations. Overall, these results support the notion that these fluctuations couple to subtle, underlying inhomogeneity that underpins the cuprate phase diagram. Finally, in La 1.8⁢ Sr 0.2⁢ Cu⁢O 4 , we uncover low-energy structural fluctuations at a nominally forbidden reflection that are distinct from the orthorhombic distortions. While the origin of these fluctuations is not clear, they might be related to the presence of extended defects such as dislocations or stacking faults.

Spieker, R. J. [Univ. of Minnesota, Minneapolis, M↗
DOE OSTI2022

Strong increase in ultrasound attenuation below T c in Sr 2 RuO 4 : Possible evidence for domains

Recent experiments suggest that Sr 2 RuO 4 has a two-component superconducting order parameter (OP). A two-component OP has multiple degrees of freedom in the superconducting state that can result in low-energy collective modes or the formation of domain walls—a possibility that would explain a number of experimental observations including the smallness of the signature of time reversal symmetry breaking at T c and telegraph noise in critical current experiments. We use resonant ultrasound spectroscopy to perform ultrasound attenuation measurements across the superconducting T c of Sr 2 RuO 4 . We find that compressional sound attenuation increases by a factor of 7 immediately below T c , in sharp contrast with what is found in both conventional (s-wave) and high-T c (d-wave) superconductors. Our observations are most consistent with the presence of domain walls that separate different configurations of the superconducting OP. Here, the fact that we only observe an increase in sound attenuation for compressional strains, and not for shear strains, suggests an inhomogeneous superconducting state formed of two distinct, accidentally degenerate superconducting OPs that are not related to each other by symmetry. Whatever the mechanism, a factor of 7 increase in sound attenuation is a singular characteristic that must be reconciled with any potential theory of superconductivity in Sr 2 RuO 4 .

36 MATERIALS SCIENCE↗
DOE OSTI2022

Absence of precursor incommensurate charge order in electronic nematic Ba 0.35 Sr 0.65 Ni 2 As 2

Recent discoveries of charge order and electronic nematic order in the iron-based superconductors and cuprates have pointed towards the possibility of nematic and charge fluctuations playing a role in the enhancement of superconductivity. The Ba 1–x Sr x Ni 2 As 2 system, closely related in structure to the BaFe 2 As 2 system, has recently been shown to exhibit both types of ordering without the presence of any magnetic order. We report single-crystal x-ray diffraction experiments on Ba 0.35 Sr 0.65 Ni 2 As 2 , providing evidence that the previously reported incommensurate charge order with wave-vector (0, 0.28, 0) tet in the tetragonal state of BaNi 2 As 2 vanishes by 65% Sr substitution together with nematic order. Furthermore, our measurements suggest that the nematic and incommensurate charge orders are closely tied in the tetragonal state and show that the (0, 0.33, 0) tri charge ordering in the triclinic phase of BaNi 2 As 2 evolves to become (0, 0.5, 0) tri charge ordering at x = 0.65 before vanishing at x = 0.71.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Exploring magnetic anisotropy and robustness of the J eff = 1/2 state under substantial orthorhombic distortion in Sr 2 IrO 4 thin films

Here, we present a comprehensive study revealing the intricate interplay of the magnetic anisotropy and orthorhombic distortion in thin films of Sr 2 IrO 4 through a Ca 3 Ru 2 O 7 substrate. By inducing a pronounced orthorhombic distortion along the direction of oxygen octahedral edges, we effectively modulated the uniaxial magnetic anisotropy in the system. Remarkably divergent responses along the easy and hard magnetic axes were unveiled through x-ray magnetic circular dichroism (XMCD) measurements under magnetic fields. Specifically, the spin flop transition observed when the magnetic field aligns with the hard axis allows us to estimate the magnetic anisotropy energy, which is around 14.2 µeV, close to that estimated from the single magnon peak measured via Raman spectroscopy. The observed anisotropy energy remains notably lower than the linear estimates derived from the strain-anisotropy energy relationship outlined in H.-H. Kim et al., Nat. Commun. 13, 6674 (2022). This underscores the enduring preservation of the isotropic character of the J eff = 1/2 states. This is also supported by the negligible XMCD intensity ratio at the L 2 edge compared to that of the L 3 edge. Furthermore, the branching ratio determined from x-ray absorption spectroscopy shows that the expectation value of the spin-orbit coupling is similar to that of bulk Sr 2 IrO 4 single crystals. Our findings indicate that even under a substantial anisotropic biaxial distortion, Sr 2 IrO 4 remains remarkably proximate to the J eff = 1/2 state. This study not only provides valuable information in understanding the interplay between magnetic anisotropy and strain but also the robustness of the J eff = 1/2 state under octahedral distortion within materials exhibiting emergent quantum phenomena.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Cross sections of the 83 Rb⁢(p,γ)⁢ 84 Sr and 84 Kr⁢(p,γ)⁢ 85 Rb reactions at energies characteristic of the astrophysical γ process

We have measured the cross section of the Rb 83 ( p , γ ) Sr 84 radiative capture reaction in inverse kinematics using a radioactive beam of Rb 83 at incident energies of 2.4 and 2.7 A MeV. Prior to the radioactive beam measurement, the Kr 84 ( p , γ ) Rb 85 radiative capture reaction was measured in inverse kinematics using a stable beam of Kr 84 at an incident energy of 2.7 A MeV. The effective relative kinetic energies of these measurements lie within the relevant energy window for the γ process in supernovae. The central values of the measured partial cross sections of both reactions were found to be 0.17 – 0.42 times the predictions of statistical model calculations. Assuming the predicted cross section at other energies is reduced by the same factor leads to a slightly higher calculated abundance of the p nucleus Sr 84 , caused by the reduced rate of the Sr 84 ( γ , p ) Rb 83 reaction derived from the present measurement.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Spin-orbit coupling controlled ground states in the double perovskite iridates $\textit{A}_2\textit{B}$IrO$_6$ ($\textit{A}$ = Ba, Sr; $\textit{B}$ = Lu, Sc)

Iridates with the 5$d^4$ electronic configuration have attracted recent interest due to reports of magnetically ordered ground states despite longstanding expectations that their strong spin-orbit coupling would generate a $\textit{J}$ = 0 electronic ground state for each Ir 5+ ion. The major focus of prior research has been on the double perovskite iridates Ba 2 YIrO 6 and Sr 2 YIrO 6 , where the nature of the ground states (i.e., ordered vs nonmagnetic) is still controversial. Here, in this work, we present neutron powder diffraction, high-energy-resolution fluorescence-detected x-ray absorption spectroscopy (HERFD-XAS), resonant inelastic x-ray scattering (RIXS), magnetic susceptibility, and muon spin relaxation data on the related double perovskite iridates Ba 2 LuIrO 6 , Sr 2 LuIrO 6 , Ba 2 ScIrO 6 , and Sr 2 ScIrO 6 that enable us to gain a general understanding of the electronic and magnetic properties for this family of materials. Our HERFD-XAS and RIXS measurements establish $\textit{J}$ = 0 electronic ground states for the Ir 5+ ions in all cases, with similar values for Hund's coupling $J_H$ and the spin-orbit coupling constant $λ_{\text{SOC}}$. Our bulk susceptibility and muon spin relaxation data find no evidence for long-range magnetic order or spin freezing, but they do exhibit weak magnetic signals that are consistent with extrinsic local moments. Our results indicate that the large $λ_{\text{SOC}}$ is the key driving force behind the electronic and magnetic ground states realized in the $5d^4$ double perovskite iridates, which agrees well with conventional wisdom.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Magnetosynthesis effect on magnetic order, phonons, and magnons in single-crystal Sr 2 ⁢ IrO 4

It was shown earlier that applying a magnetic field during the growth of Sr 2 IrO 4 , also known as “field-alteration”, induces significant changes to its structural, magnetic, and transport properties. However, the microscopic nature of these changes is enigmatic. Here, in this study, we employed resonant elastic and inelastic x-ray scattering, as well as Raman scattering, to investigate samples from two batches of Sr 2 IrO 4 grown in magnetic fields of different strengths. Our findings reveal that samples grown in a weaker magnetic field have similar magnetic order to non-altered samples, whereas those grown in a stronger field show a different stacking of weak in-plane ferromagnetic moments. Additionally, we observed significant softening and broadening of select Raman-active phonons in the field altered samples, with a stronger effect in the samples grown in the stronger field. We discuss insights that our results provide into the microscopic nature of field-alteration in Sr 2 IrO 4 .

36 MATERIALS SCIENCE↗
DOE OSTI2024

Advances in heavy alkaline earth chemistry provide insight into complexation of weakly polarizing Ra 2+ , Ba 2+ , and Sr 2+ cations

Numerous technologies—with catalytic, therapeutic, and diagnostic applications—would benefit from improved chelation strategies for heavy alkaline earth elements: Ra 2+ , Ba 2+ , and Sr 2+ . Unfortunately, chelating these metals is challenging because of their large size and weak polarizing power. We found 18-crown-6-tetracarboxylic acid (H 4 COCO) bound Ra 2+ , Ba 2+ , and Sr 2+ to form M(H x COCO) x–2 . Upon isolating radioactive 223 Ra from its parent radionuclides ( 227 Ac and 227 Th), 223 Ra 2+ reacted with the fully deprotonated COCO 4- chelator to generate Ra(COCO) 2- (aq) (log K Ra(COCO)2- = 5.97 ± 0.01), a rare example of a molecular radium complex. Comparative analyses with Sr 2+ and Ba 2+ congeners informed on what attributes engendered success in heavy alkaline earth complexation. Chelators with high negative charge [-4 for Ra(COCO) 2- (aq) ] and many donor atoms [≥11 in Ra(COCO) 2- (aq) ] provided a framework for stable complex formation. These conditions achieved steric saturation and overcame the weak polarization powers associated with these large dicationic metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Structural and phonon anomalies in the superconducting Bi 2 Sr 2 CaCu 2 O 8+σ with varying doping level at high pressures

Here we examined the effect of the lattice compression on the crystal structure of the Bi 2 Sr 2 CaCu 2 O 8+σ superconductor with nearly optimally doped and overdoped composition using X-ray diffraction technique. Our studies show that at high pressures (up to 30 GPa ) the doping level does not affect the crystal structure of this superconductor. Along with this, structural anomalies in ratio appear at a pressure that corresponds to that at which T c begins to decrease. This fact indicates a close connection between the observed anomalies and superconductivity. We also studied the effect of doping and pressure on the T c (P) and on the Raman active lattice modes of the Bi 2 Sr 2 CaCu 2 O 8+σ superconductors. We find universal suppression of the T c by the pressure starting from the critical pressure P c in the range from 9 to 16 GPa, depending on the doping level of the Bi 2 Sr 2 CaCu 2 O 8+σ samples. Concomitantly, we observe phonon anomalies around 10 to 20 GPa, which indicate possible pressure-induced charge redistribution in BiO layers. These newly detected anomalies may be related to the changes in the electronic structure which compete with the superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Theoretical study of CO2 capture mechanisms of SrO and Sr(OH)2.nH2O (n=0,1,8)

This presentation encapsulated the use of density functional theory (DFT) to investigate the mechanism of CO2 conversion on various crystal surfaces, including SrO, Sr(OH)2, Sr(OH)2·H2O, and Sr(OH)2·8H2O. The study provides unique insights into the fundamental mechanism for CO2 capture using SrO and its hydrated forms.

catalyst performance↗
DOE OSTI2020

Flexible Magnetic Polymer Composite Substrate with Ba 1.5 Sr 1.5 Z Hexaferrite Particles of VHF/Low UHF Patch Antennas for UAVs and Medical Implant Devices

Our goal is to fabricate flexible magnetic polymer composites as antenna substrates for very high frequency (VHF)/low ultra high frequency (UHF) antennas for unmanned aerial vehicles (UAVs) and medical devices. Magnetodielectric materials, which have permeability (μ) similar to permittivity (ε), have attracted great attention, because they facilitate miniaturization of microwave devices while keeping or enhancing electromagnetic characteristics. Mechanically millled Ba 1.5 Sr 1.5 Co 2 Fe 24 O 41 (Ba 1.5 Sr 1.5 Z) hexaferrite particles were used to increase permeability in the interesting frequency band. The microwave properties of Ba 1.5 Sr 1.5 Z composites were predicted and measured. Hansen’s zero-order analysis of antenna bandwidth and electromagnetic field simulation showed that the hexaferrite-based flexible composite could enhance a bandwidth and achieve the miniaturization of antennas as well. The magnetic antenna substrates can be a good solution to integrate antennas into the UAVs whose dimensions are comparable to or larger than communication wavelength.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Early High-contrast Imaging Results with Keck/NIRC2-PWFS: The SR 21 Disk

High-contrast imaging of exoplanets and protoplanetary disks depends on wave front sensing and correction made by adaptive optics instruments. Classically, wave front sensing has been conducted at optical wavelengths, which made high-contrast imaging of red targets such as M-type stars or extincted T Tauri stars challenging. Keck/NIRC2 has combined near-infrared (NIR) detector technology with the pyramid wave front sensor (PWFS). With this new module we observed SR 21, a young star that is brighter at NIR wavelengths than at optical wavelengths. Compared with the archival data of SR 21 taken with the optical wave front sensing we achieved ~20% better Strehl ratio in similar natural seeing conditions. Further post-processing utilizing angular differential imaging and reference-star differential imaging confirmed the spiral feature reported by the Very Large Telescope/Spectro-Polarimetric High-contrast Exoplanet REsearch instrument polarimetric observation, which is the first detection of the SR 21 spiral in total intensity at L' band. We also compared the contrast limit of our result (10 -4 at 0.'4 and 2 × 10 -5 at 1.'0) with the archival data that were taken with optical wave front sensing and confirmed the improvement, particularly at ≤0.'5. Our observation demonstrates that the NIR PWFS improves AO performance and will provide more opportunities for red targets in the future.

79 ASTRONOMY AND ASTROPHYSICS↗