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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Preparation of ternary hydrophobic magnetic deep eutectic solvents and an investigation into their physicochemical properties

Hydrophobic magnetic deep eutectic solvents (HMDESs) are considered a subclass of DESs comprised of a hydrogen bond acceptor (HBA), hydrogen bond donor (HBD), and a metal halide salt. These DESs can be easily manipulated by an external magnet and employed in numerous applications including liquid–liquid extractions and catalysis. In this work, a total of forty-six (46) HMDESs were prepared and their physicochemical properties studied. Six structurally unique ionic and non-ionic HBAs were combined with lanthanide and transition metal halide salts and twelve different HBDs to prepare room temperature eutectic solvents. The viscosities of HMDESs ranged from 46 centipoise (cP) to 124,600 cP at 23 °C. Their magnetic susceptibilities, studied by superconducting quantum interference device (SQUID) magnetometry and a magnetic susceptibility balance, varied from 3.03 Bohr magnetons (μB) to 9.32 μB when the type of metal halide salt and its molar ratio were varied. Thermal stabilities ranged from 151.1 °C to 308.5 °C at 5% mass loss. Further, all HMDESs comprised of ionic HBA were observed to be insoluble in hexane. This study demonstrates that the physicochemical properties of HMDESs can easily be tailored by varying the DES constituents as well as their molar ratio. The structural tunability of these solvents make them highly attractive candidates for a plethora of applications ranging from extractions to electrochromic applications, where HMDESs can be easily manipulated by an external magnetic field.

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

Measurement of the impact-parameter dependent azimuthal anisotropy in coherent $ρ$ 0 photoproduction in Pb–Pb collisions at $\sqrt{s_{NN}}$ = 5.02 TeV

This Letter presents the first measurement of the impact-parameter dependent angular anisotropy in the decay of coherently photoproduced $ρ$ 0 mesons. The $ρ$ 0 mesons are reconstructed through their decay into pion pairs. The measured anisotropy corresponds to the amplitude of the cos(2φ) modulation, where φ is the angle between the two vectors formed by the sum and the difference of the transverse momenta of the pions, respectively. The measurement was performed by the ALICE Collaboration at the LHC using data from ultraperipheral Pb–Pb collisions at a center-of-mass energy of $\sqrt{s_{NN}}$ = 5.02 TeV per nucleon pair. Different impact-parameter regions are selected by classifying the events in nuclear-breakup classes. The amplitude of the cos(2φ) modulation is found to increase by about one order of magnitude from large to small impact parameters. Theoretical calculations describe the measured cos(2φ) anisotropy and its impact-parameter dependence as the result of a quantum interference effect at the femtometer scale, arising from the ambiguity regarding which of the nuclei is the photon source in the interaction.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Structure–property relationships in atomic-scale junctions: Histograms and beyond

Over the past 10 years, there has been tremendous progress in the measurement, modeling and understanding of structure–function relationships in single molecule junctions. Numerous research groups have addressed significant scientific questions, directed both to conductance phenomena at the single molecule level and to the fundamental chemistry that controls junction functionality. Many different functionalities have been demonstrated, including single-molecule diodes, optically and mechanically activated switches, and, significantly, physical phenomena with no classical analogues, such as those based on quantum interference effects. Experimental techniques for reliable and reproducible single molecule junction formation and characterization have led to this progress. In particular, the scanning tunneling microscope based break-junction (STM-BJ) technique has enabled rapid, sequential measurement of large numbers of nanoscale junctions allowing a statistical analysis to readily distinguish reproducible characteristics. Furthermore, harnessing fundamental link chemistry has provided the necessary chemical control over junction formation, enabling measurements that revealed clear relationships between molecular structure and conductance characteristics.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Comprehensive Magnetic Study of Nanostructured Mesoporous Manganese Oxide Materials and Implications for Catalytic Behavior

Magnetic behavior of nanostructured mesoporous manganese oxide materials, designated UCT-1 and UCT-18, were studied using a combination of superconducting quantum interference device (SQUID) magnetometry and 55 Mn zero-field spin–echo nuclear magnetic resonance (NMR). Curie–Weiss fits to the magnetic susceptibility for the UCT-1 and UCT-18 samples calcined at 550 °C yielded paramagnetic moment values consistent with spin-only Mn 3+ ions in the α-Mn 2 O 3 phase ( S = 2, 4.90 μ B ). However, the magnetization and NMR results reported here clearly identify a small amount of the Mn 3 O 4 second phase (ferrimagnetic with T C ≈ 43 K) that does not appear in X-ray diffraction (XRD). We report the study resulted in the observation of fascinating magnetic behavior: (1) exchange bias, which occurs in cases where a ferromagnetic (or ferrimagnetic) phase forms a boundary with an antiferromagnetic phase and (2) a magnetic contribution attributed to uncompensated spins on the surfaces of the α-Mn 2 O 3 nanoparticles. The presence of Mn 3 O 4 and the interplay of Mn 3+ and Mn 2+ impact the catalytic properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Ground State and Excited State Tuning in Ferric Dipyrrin Complexes Promoted by Ancillary Ligand Exchange

Three ferric dipyrromethene complexes featuring different ancillary ligands were synthesized by one electron oxidation of ferrous precursors. Four-coordinate iron complexes of the type ( Ar L)FeX 2 [ Ar L = 1,9-(2,4,6-Ph 3 C 6 H 2 ) 2 -5-mesityldipyrromethene] with X = Cl or t BuO were prepared and found to be high-spin (S = 5/2), as determined by superconducting quantum interference device magnetometry, electron paramagnetic resonance, and 57 Fe Mössbauer spectroscopy. The ancillary ligand substitution was found to affect both ground state and excited properties of the ferric complexes examined. While each ferric complex displays reversible reduction and oxidation events, each alkoxide for chloride substitution results in a nearly 600 mV cathodic shift of the Fe III/II couple. The oxidation event remains largely unaffected by the ancillary ligand substitution and is likely dipyrrin-centered. While the alkoxide substituted ferric species largely retain the color of their ferrous precursors, characteristic of dipyrrin-based ligand-to-ligand charge transfer (LLCT), the dichloride ferric complex loses the prominent dipyrrin chromophore, taking on a deep green color. Time-dependent density functional theory analyses indicate the weaker-field chloride ligands allow substantial configuration mixing of ligand-to-metal charge transfer into the LLCT bands, giving rise to the color changes observed. Furthermore, the higher degree of covalency between the alkoxide ferric centers is manifest in the observed reactivity. Delocalization of spin density onto the tert-butoxide ligand in ( Ar L)FeCl(O t Bu) is evidenced by hydrogen atom abstraction to yield ( Ar L)FeCl and HOtBu in the presence of substrates containing weak C–H bonds, whereas the chloride ( Ar L)FeCl 2 analogue does not react under these conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Nanoscale Metastable ε-Fe 3 N Ferromagnetic Materials by Self-Sustained Reactions

A single-step method for the preparation of metastable ε-Fe 3 N nanoparticles by combustion of reactive gels containing iron nitrate (Fe(NO 3 ) 3 ) and hexamethylenetetramine (C 6 H 12 N 4 ) in an inert atmosphere is reported. The results of Fourier transform infrared spectroscopy (FTIR) and thermal analysis coupled with dynamic mass spectrometry revealed that the exothermic decomposition of a coordination complex formed between Fe(NO 3 ) 3 and HMTA is responsible for the formation of ε-Fe 3 N nanoscale particles with sizes of 5-15 nm. The magnetic properties between 5 and 350 K are characterized using a superconducting quantum interference device (SQUID) magnetometer, revealing a ferromagnetic behavior with a low-temperature magnetic moment of 1.09 μB/Fe, high room temperature saturation magnetization (~80 emu/g), and low remanent magnetization (~15 emu/g). The obtained value for the Curie temperature of ~522 K is close to that (~575 K) for bulk ε-Fe 3 N reported in the literature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Probing Charge Ordering in Fractional Mixed-Valence Charge Density Wave Systems with Oriented HERFD-XANES Spectroscopy

In this paper, we present oriented Pt L III edge high energy resolution fluorescence detected X-ray absorption near edge structure (HERFD-XANES) measurements on a series of structurally tunable quasi-one-dimensional mixed-valence platinum-halide linear chain materials, [Pt(en) 2 ][Pt(en) 2 X 2 ](ClO 4 ) 4 with X = Cl, Br, I, together with ab initio modeling of the spectral components and electronic structure. The materials exhibit a commensurate charge density wave (CDW) with an amplitude controlled by the bridging halide ion, giving rise to fractional mixed valence states. Ab initio FEFF9 modeling of the spectra and the associated angular momentum projected density of states (lDOS) are used to interpret the results, revealing systematic changes in the platinum orbital occupancy through the series of materials that reflect the fractional mixed valence states of the CDW. A significant contribution to a post-edge feature in the oriented spectra is identified as resulting from quantum interference between the final states of the X-ray absorption transition.

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

In Situ Local Imaging of Ferromagnetism and Superconductivity in RbEuFe 4 As 4

The coexistence of superconductivity and ferromagnetism is an intrinsically interesting research focus in condensed matter physics but the study is limited by low superconducting (T c ) and magnetic (T m ) transition temperatures in related materials. Here, we used a scanning superconducting quantum interference device to image the in-situ diamagnetic and ferromagnetic responses of RbEuFe 4 As 4 with high T c and T m . We observed significant suppression of superfluid density in vicinity of the magnetic phase transition, signifying fluctuation-enhanced magnetic scatterings between Eu spins and Fe 3d conduction electrons. Intriguingly, we observed multiple ferromagnetic domains which should be absent in an ideal magnetic helical phase. The formation of these domains demonstrates a weak c-axis ferromagnetic component probably arising from Eu spin-canting effect, indicative of possible superconductivity-driven domain Meissner and domain vortex-antivortex phases as revealed in EuFe 2 (As 0.79 P 0.21 ) 2 . Finally, our observations highlight RbEuFe 4 As 4 is a unique system which includes multiple interplay channels between superconductivity and ferromagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Current-Phase Relations of Superconducting PtSi Constriction Josephson Junctions

Here, we study the current-phase relations of superconductor–constriction–superconductor Josephson junctions made from platinum silicide thin films by fabricating dc-superconducting quantum interference devices incorporating pairs of junctions and measuring their magnetic-field-dependent electrical transport. By comparing the supercurrent interference patterns with numerical Ginzburg–Landau simulations, we extract the current-phase relations of individual junctions and quantify the degree of nonlinearity. These measurements show that while the constrictions themselves sustain substantial nonlinearity, the effect is moderated by the kinetic inductance of the device leads, which is an important consideration for practical superconducting circuit applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

Non-Altermagnetic Origin of Exchange Bias Behaviors in Incoherent RuO 2 /Fe Bilayer Heterostructures

Initially identified as a promising altermagnetic (AM) candidate, rutile RuO 2 has since become embroiled in controversy due to contradictory findings of modeling and measurements of the magnetic properties of bulk crystals and thin films. For example, despite observations of a bulk nonmagnetic state using density functional theory, neutron scattering, and muon spin resonance measurements, patterned RuO 2 Hall bars and film heterostructures display magnetotransport signatures of magnetic ordering. Among the characteristics routinely cited as evidence for AM is the observation of exchange bias (EB) in an intimately contacted Fe-based ferromagnetic (FM) layer, which can arise due to interfacial coupling with a compensated antiferromagnet. Here, within this work, the origins of this EB coupling in Ru-capped RuO 2 /Fe bilayers are investigated using polarized neutron diffraction, polarized neutron reflectometry, cross-sectional transmission electron microscopy, and super conducting quantum interference device measurements. These experiments reveal that the EB behavior is driven by the formation of an iron oxide interlayer containing Fe 3 O 4 that undergoes a magnetic transition and pins interfacial moments within Fe at low temperature. These findings are confirmed by comparable measurements of Ni-based heterostructures, which do not display EB coupling, as well as magnetometry of additional Fe/Ru bilayers that display oxide-driven EB coupling despite the absence of the epitaxial RuO 2 layer. While these results do not directly refute the possibility of AM ordering in RuO 2 thin films, they reveal that EB, and related magnetotransport phenomena, cannot alone be considered evidence of this characteristic in the rutile structure due to interfacial chemical disorder.

RuO2↗
DOE OSTI2019

Understanding Active Sites in Pyrolyzed Fe–N–C Catalysts for Fuel Cell Cathodes by Bridging Density Functional Theory Calculations and 57 Fe Mössbauer Spectroscopy

Pyrolyzed Fe–N–C materials are promising platinum-group-metal-free catalysts for proton-exchange membrane fuel cell cathodes. However, the detailed structure, oxidation, and spin states of their active sites are still undetermined. As such, 57 Fe Mössbauer spectroscopy has identified FeN x moieties as the most active sites, with their fingerprint being a doublet in low-temperature Mössbauer spectra. However, the interpretation of the doublets for such materials has lacked theoretical basis. Here, we applied density functional theory to calculate the quadrupole splitting energy of doublets (Δ E QS ) for a range of FeN x structures in different oxidation and spin states. The calculated and experimental values are then compared for a reference Fe–N–C catalyst, whereas further information on the Fe oxidation and spin states was obtained from electron paramagnetic resonance, superconducting quantum interference device, and 57 Fe Mössbauer spectroscopy under external magnetic field. The combined theoretical and experimental results identify the main presence of FeN x moieties in Fe(II) low-spin and Fe(III) high-spin states, whereas a minor fraction of sites could exist in the Fe(II) S = 1 state. From the analysis of the 57 Fe Mössbauer spectrum under the external magnetic field and the comparison of calculated and measured Δ E QS values, we assign the experimental doublet D1 with a mean Δ E QS value of around 0.9 mm·s –1 to Fe(III)N 4 C 12 moieties in high-spin state and the experimental doublet D2 with a mean Δ E QS value of around 2.3 mm·s –1 to Fe(II)N 4 C 10 moieties in low and medium spin. These conclusions indicate that D1 corresponds to surface-exposed sites, whereas D2 may correspond either to bulk sites that are inaccessible to O 2 or to surface sites that bind O 2 weaker than D1.

fuel cell↗
DOE OSTI2018

Gate-Controlled Metal–Insulator Transition in TiS 3 Nanowire Field-Effect Transistors

We explore the electrical characteristics of TiS 3 nanowire field-effect transistor (FETs), over the wide temperature range from 3 to 350 K. These nanomaterials have a quasi-one-dimensional (1D) crystal structure and exhibit a gate-controlled metal–insulator transition (MIT) in their transfer curves. Their room-temperature mobility is ~20–30 cm 2 /(V s), 2 orders of magnitude smaller than predicted previously, a result that we explain quantitatively in terms of the influence of polar-optical phonon scattering in these materials. In the insulating state (<~220 K), the transfer curves exhibit unusual mesoscopic fluctuations and a current suppression near zero bias that is common to charge-density wave (CDW) systems. The fluctuations have a nonmonotonic temperature dependence and wash out at a temperature close to that of the bulk MIT, suggesting they may be a feature of quantum interference in the CDW state. Overall, our results demonstrate that quasi-1D TiS 3 nanostructures represent a viable candidate for FET realization and that their functionality is influenced by complex phenomena.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Magnetic Blocking in Fluoflavine Radical-Bridged Dilanthanide Complexes

Magnetic exchange coupling is difficult to foster in polynuclear lanthanide (Ln) complexes and poorly understood. While coupling Ln ions through closed-shell ligands is inherently weak due to the contracted 4f orbitals, placing open-shell ligands instead has proven to promote orders of magnitude stronger coupling, giving rise to single-molecule magnets (SMMs) innate to real magnetic memory effect in the case of the anisotropic Ln ions. Notably, the impact of radical bridges with differing oxidation states on magnetic blocking remains unexplored due to lack of Ln SMMs with radicals in two distinct charge states. Herein, the first dilanthanide complexes (Ln = Gd, Dy) containing fluoflavine (flv) bridges, [(Cp* 2 Ln) 2 (μ-flv z )]X, (where X = [Al(OC{CF 3 } 3 ) 4 ] − (z = 1−•), 1-Ln; X = 0 (z = 2−), 2-Ln; X =[K(crypt-222)] + (z = 3−•), 3-Ln) are reported. 1-Ln and 3-Ln, comprising the flv 1−• and flv 3−• radical bridges, were investigated via single-crystal X-ray diffraction (SCXRD), ultraviolet−visible (UV−vis) spectroscopy, Superconducting Quantum Interference Device (SQUID) magnetometry, high-field electron paramagnetic resonance (HF-EPR) spectroscopy and broken-symmetry density functional theory (BS-DFT) calculations. 1-Dy and 3-Dy constitute the first SMMs innate to radicals in two differing oxidation states. 1-Dy exhibits a spin-reversal barrier U eff of 28.36 cm −1 and open magnetic hysteresis loops below 3 K. By contrast, 3-Dy displays a much higher U eff of 143(2) cm −1 and open hysteresis loops until 9.5 K, representing a record for dilanthanide SMMs containing an organic radical bridge. The boost in SMM properties in 3-Dy is attributed to spin-phonon coupling and improved frontier orbital structure. This study paves the way for advanced design strategies of polynuclear Ln SMMs.

Benner, Florian [Michigan State Univ., East Lansin↗
DOE OSTI2019

Synthesis and Characterization of Single Phase Metal Dodecaboride Solid Solutions: Zr 1-x Y x B 12 and Zr 1-x U x B 12

Single-phase metal dodecaboride solid solutions, Zr 0.5 Y 0.5 B 12 and Zr 0.5 U 0.5 B 12 , were arranged by arc melting from pure elements. The phase purity and composition were established by powder X-ray diffraction (PXRD), energy-dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), and 10 B and 11 B solid-state nuclear magnetic resonance (NMR) spectroscopy. The effects of carbon addition to Zr 1-x Y x B 12 were studied and it was found that carbon causes fast cooling and as a result rapid nucleation of grains, as well as “templating” and patterning effects of the surface morphology. The hardness of the Zr 0.5 Y 0.5 B 12 phase is 47.6 ± 1.7 GPa at 0.49 N load, which is ~17% higher than that of its parent compounds, ZrB 12 and YB 12 , with hardness values of 41.6 ± 2.6 and 37.5 ± 4.3 GPa, respectively. The hardness of Zr 0.5 U 0.5 B 12 is ~54% higher than that of its UB 12 parent. The dodecaborides were confirmed to be metallic by band structure calculations, diffuse reflectance UV–vis, and solid-state NMR spectroscopies. The nature of the dodecaboride colors—violet for ZrB 12 and blue for YB 12 —can be applied to charge-transfer. XPS indicates that the metals are in the following oxidation states: Y 3+ , Zr 4+ , and U$^{{5+}/^{6+}}$. The superconducting transition temperatures (T c ) of the dodecaborides were determined to be 4.5 and 6.0 K for YB 12 and ZrB 12 , respectively, as shown by resistivity and superconducting quantum interference device (SQUID) measurements. The T c of the Zr 0.5 Y 0.5 B 12 solid solution was suppressed to 2.5 K.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Molecular physics: Breaking up is hard to do [Molecular physics: Asymmetric separation]

Molecular dissociation is one of the most fundamental chemical reactions, but its physics is by no means simple. In many cases it defies a classical explanation and can only be accurately described using quantum mechanics. This need not be detrimental, as quantum effects can also induce modified dynamics that may even be exploited for finer control over chemical reactions. Now, writing in Nature Physics , E. Krishnakumar and co-workers have found an asymmetry in dissociative electron attachment to hydrogen molecules, which amounts to symmetry breaking due to quantum interference.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Imaging of super-fast dynamics and flow instabilities of superconducting vortices

Quantized magnetic vortices driven by electric current determine key electromagnetic properties of superconductors. And while the dynamic behavior of slow vortices has been thoroughly investigated, the physics of ultrafast vortices under strong currents remains largely unexplored. Here, we use a nanoscale scanning superconducting quantum interference device to image vortices penetrating into a superconducting Pb film at rates of tens of GHz and moving with velocities of up to tens of km/s, which are not only much larger than the speed of sound but also exceed the pair-breaking speed limit of superconducting condensate. These experiments reveal formation of mesoscopic vortex channels which undergo cascades of bifurcations as the current and magnetic field increase. Our numerical simulations predict metamorphosis of fast Abrikosov vortices into mixed Abrikosov-Josephson vortices at even higher velocities. Our work offers an insight into the fundamental physics of dynamic vortex states of superconductors at high current densities, crucial for many applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Room-temperature intrinsic ferromagnetism in epitaxial CrTe 2 ultrathin films

While the discovery of two-dimensional (2D) magnets opens the door for fundamental physics and next-generation spintronics, it is technically challenging to achieve the room-temperature ferromagnetic (FM) order in a way compatible with potential device applications. Here in this paper, we report the growth and properties of single- and few-layer CrTe 2 , a van der Waals (vdW) material, on bilayer graphene by molecular beam epitaxy (MBE). Intrinsic ferromagnetism with a Curie temperature (TC) up to 300 K, an atomic magnetic moment of ~0.21 μ B /Cr and perpendicular magnetic anisotropy (PMA) constant (K u ) of 4.89 × 10 5 erg/cm 3 at room temperature in these few-monolayer films have been unambiguously evidenced by superconducting quantum interference device and X-ray magnetic circular dichroism. This intrinsic ferromagnetism has also been identified by the splitting of majority and minority band dispersions with ~0.2 eV at Г point using angle-resolved photoemission spectroscopy. The FM order is preserved with the film thickness down to a monolayer (T C ~ 200 K), benefiting from the strong PMA and weak interlayer coupling. The successful MBE growth of 2D FM CrTe 2 films with room-temperature ferromagnetism opens a new avenue for developing large-scale 2D magnet-based spintronics devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Tunable room-temperature ferromagnetism in Co-doped two-dimensional van der Waals ZnO

The recent discovery of ferromagnetism in two-dimensional van der Waals crystals has provoked a surge of interest in the exploration of fundamental spin interaction in reduced dimensions. However, existing material candidates have several limitations, notably lacking intrinsic room-temperature ferromagnetic order and air stability. Here, motivated by the anomalously high Curie temperature observed in bulk diluted magnetic oxides, we demonstrate room-temperature ferromagnetism in Co-doped graphene-like Zinc Oxide, a chemically stable layered material in air, down to single atom thickness. Through the magneto-optic Kerr effect, superconducting quantum interference device and X-ray magnetic circular dichroism measurements, we observe clear evidences of spontaneous magnetization in such exotic material systems at room temperature and above. Transmission electron microscopy and atomic force microscopy results explicitly exclude the existence of metallic Co or cobalt oxides clusters. X-ray characterizations reveal that the substitutional Co atoms form Co 2+ states in the graphitic lattice of ZnO. By varying the Co doping level, we observe transitions between paramagnetic, ferromagnetic and less ordered phases due to the interplay between impurity-band-exchange and super-exchange interactions. Our discovery opens another path to 2D ferromagnetism at room temperature with the advantage of exceptional tunability and robustness.

36 MATERIALS SCIENCE↗