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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Phonon-Driven Femtosecond Dynamics of Excitons in Crystalline Pentacene from First Principles

Nonradiative exciton relaxation processes are critical for energy transduction and transport in optoelectronic materials, but how these processes are connected to the underlying crystal structure and the associated electron, exciton, and phonon band structures, as well as the interactions of all these particles, is challenging to understand. Here, in this work, we present a first-principles study of exciton-phonon relaxation pathways in pentacene, a paradigmatic molecular crystal and optoelectronic semiconductor. We compute the momentum- and band-resolved exciton-phonon interactions, and use them to analyze key scattering channels. We find that both exciton intraband scattering and interband scattering to parity-forbidden dark states occur on the same ~100 fs timescale as a direct consequence of the longitudinal-transverse splitting of the bright exciton band. Consequently, exciton-phonon scattering exists as a dominant nonradiative relaxation channel in pentacene. We further show how the propagation of an exciton wave packet is connected with crystal anisotropy, which gives rise to the longitudinal-transverse exciton splitting and concomitant anisotropic exciton and phonon dispersions. Our results provide a framework for understanding the role of exciton-phonon interactions in exciton nonradiative lifetimes in molecular crystals and beyond.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

High-field/high-frequency electron spin resonances of Fe-doped β − Ga 2 O 3 by terahertz generalized ellipsometry: Monoclinic symmetry effects

We demonstrate detection and measurement of electron paramagnetic spin resonances (EPR) of iron defects in β − Ga 2 O 3 utilizing generalized ellipsometry at frequencies between 110 and 170 GHz. The experiments are performed on an Fe-doped single crystal in a free-beam configuration in reflection at 45 ∘ and magnetic fields between 3 and 7 T. In contrast with low-field, low-frequency EPR measurements, we observe all five transitions of the s = 5 / 2 high-spin state Fe 3 + simultaneously. We confirm that ferric Fe 3 + is predominantly found at octahedrally coordinated Ga sites. We obtain the full set of fourth-order monoclinic zero-field splitting parameters for both octahedrally and tetrahedrally coordinated sites by employing measurements at multiple sample azimuth rotations. The capability of high-field EPR allows us to demonstrate that simplified second-order orthorhombic spin Hamiltonians are insufficient, and fourth-order terms as well as consideration of the monoclinic symmetry are needed. These findings are supported by computational approaches based on density-functional theory for second-order and on ligand-field theory for fourth-order parameters of the spin Hamiltonian. Terahertz ellipsometry is a way to measure spin resonances in a cavity-free setup. Its possibility of varying the probe frequency arbitrarily without otherwise changing the experimental setup offers unique means of truly disentangling different components of highly anisotropic spin Hamiltonians. Published by the American Physical Society 2024

Materials Science↗
DOE OSTI2025

Time evolution of a pumped molecular magnet—A time-resolved inelastic neutron scattering study

Introducing an experimental technique of time-resolved inelastic neutron scattering (TRINS), we explore the time-dependent effects of resonant pulsed microwaves on the molecular magnet Cr 8 F 8 Piv 16 . The octagonal rings of magnetic Cr 3+ atoms with antiferromagnetic interactions form a singlet ground state with a weakly split triplet of excitations at 0.8 meV. A 4.6 tesla field was applied to tune the splitting between two members of the triplet excited level |1$\rangle$ ↔ |2$\rangle$ to resonance with 105 GHz (0.434 meV) microwaves. The time-dependent occupations of the ground state |0$\rangle$, lower lying levels |1$\rangle$ and |2$\rangle$, and higher energy states |λ ≥ 3$\rangle$ were extracted during and after 20 s long microwave pulses incident along the (101) direction of a Cr 8 F 8 Piv 16 crystal held at 1.9 K. At significantly elevated spin temperatures, we found underpopulation relative to thermal equilibrium of |2$\rangle$ and spin-lattice thermalization time scales ranging from 1.6(2) s to 5.7(2) s depending on the power level. This contrasts with the relaxation time τ 1 (T → 0) = 27(5) 𝛍 s inferred for |2$\rangle$ from in situ Electron Spin Resonance measurements. By probing a broad range of excited states during intense microwave pumping, TRINS thus provides a first view of long lived excited states in a molecular antiferromagnet.

Science & Technology - Other Topics↗
NASA NTRS2019

Global Ecosystem Dynamics Investigation (GEDI) Instrument Alignment and Test

NASA's Global Ecosystem Dynamics Investigation (GEDI) instrument was launched Dec. 5, 2018, and installed on the International Space Station 419 km from Earth. The GEDI is a Light Detection and Ranging (LIDAR) instrument; measuring the time of flight of transmitted laser beams to the Earth and back to determine altitude for geospatial mapping of forest canopy heights. The need for very dense cross track sampling for slope measurements of canopy height is accomplished by using three individual laser transmitter systems, where each beam is split into two beams by a birefringent crystal. Furthermore, one transmitter is equipped with a diffractive optical element splitting the two beams into four, for a total of 8 beams. The beams are reflected off of the features and imaged by an 800 mm diameter Receiver Telescope Assembly, composed of a Ritchey-Chretien telescope, a refractive aft optics assembly and focal plane array which collects and focuses the light from the 8 probe beams into the 8 science fibers, each with a field of view on the Earth subtending 300 mu rad. The dense cross-track sampling mandated a custom designed dual-fiber interface. The science fibers had to be aligned to the nominal, projected laser spots. The alignment was highly dependent on optimization and co-positioning of the fibers pair-wise due to mechanical constraints. This paper presents the end-to-end alignment and metrology of the full optical system from transmitter elements through receiver telescope, aft-optics, focal plane and receiver fibers performed at NASA Goddard Space Flight Center.[GRAPHICS]

Bente Eegholm↗
DOE OSTI2024

Controlling magnon-photon coupling in a planar geometry

Abstract The tunability of magnons enables their interaction with various other quantum excitations, including photons, paving the route for novel hybrid quantum systems. Here, we study magnon-photon coupling using a high-quality factor split-ring resonator and single-crystal yttrium iron garnet (YIG) sphere at room temperature. We investigate the dependence of the coupling strength on the size of the sphere and find that the coupling is stronger for spheres with a larger diameter as predicted by theory. Furthermore, we demonstrate strong magnon-photon coupling by varying the position of the YIG sphere within the resonator. Our experimental results reveal the expected correlation between the coupling strength and the rf magnetic field. These findings demonstrate the control of coherent magnon-photon coupling through the theoretically predicted square-root dependence on the spin density in the ferromagnetic medium and the magnetic dipolar interaction in a planar resonator.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Determining the nature of magnetism in altermagnetic candidate RuO 2

The terminology “altermagnetism” has recently been adopted to describe collinear magnetic order with no net magnetization and nonrelativisitic, momentum-dependent spin splitting. The archetypal material used to theoretically explore altermagnetism is RuO 2 , but there has been significant debate as to whether RuO 2 possesses magnetic, let alone altermagnetic, order. To address questions surrounding the nature of magnetism in RuO 2 , we combine symmetry-sensitive torque magnetometry and magnetization measurements in single crystals up to 31 T. The data are inconsistent with collinear magnetic order possessing a Néel vector along the 𝑐 axis. Torque magnetometry further demonstrates an isotropic, field-independent magnetic susceptibility within the 𝑎⁢𝑏 plane, indicative of neither a Néel vector within the 𝑎⁢𝑏 plane nor a field-induced Néel vector reorientation. Magnetic quantum oscillations from both techniques reveal a nearly spherical Fermi surface pocket at the Brillouin zone center, in agreement with paramagnetic electronic structure calculations. Taken together, these data indicate that high-quality RuO 2 single crystals are itinerant paramagnets with no detectable long-range magnetic order and, by extension, no altermagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Topological behavior and Zeeman splitting in trigonal PtBi2-x single crystals

Abstract Transition-metal dipnictide PtBi 2 exhibits rich structural and physical properties with topological semimetallic behavior and extremely large magnetoresistance (XMR) at low temperatures. We have investigated the electrical and magnetic properties of trigonal-phase PtBi 2 -x single crystals with x ~ 0.4. Profound de Haas–van Alphen (dHvA) and Shubnikov-de Haas (SdH) oscillations are observed. Through fast Fourier transformation (FFT) analyses, four oscillation frequencies are extracted, which result from α, β, γ, and δ bands. By constructing the Landau fan diagram for each band, the Berry phase is extracted demonstrating the non-trivial nature of the α, β, and δ bands. Despite Bi deficiency, we observe the Zeeman splitting in dHvA and SdH oscillations under moderate magnetic field and the moderate Landé g factor (4.97–6.48) for the α band. Quantitative analysis of the non-monotonic field dependence including the sign change of the Hall resistivity suggests that electrons and holes in our system are not perfectly compensated thus not responsible for the XMR effect.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Azimuthal Anchoring Strength in Photopatterned Alignment of a Nematic

Spatially-varying director fields have become an important part of research and development in liquid crystals. Characterization of the anchoring strength associated with a spatially-varying director is difficult, since the methods developed for a uniform alignment are seldom applicable. Here we characterize the strength of azimuthal surface anchoring produced by the photoalignment technique based on plasmonic metamsaks. The measurements used photopatterned arrays of topological point defects of strength +1 and −1 in thin layers of a nematic liquid crystal. The integer-strength defects split into pairs of half-integer defects with lower elastic energy. The separation distance between the split pair is limited by the azimuthal surface anchoring, which allows one to determine the strength of the latter. The strength of the azimuthal anchoring is proportional to the UV exposure time during the photoalignment of the azobenzene layer.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Slow magnetic relaxation in a europium(II) complex

Single-ion anisotropy is vital for the observation of Single-Molecule Magnet (SMM) properties (i.e., a slow dynamics of the magnetization) in lanthanide-based systems. In the case of europium, the occurrence of this phenomenon has been inhibited by the spin and orbital quantum numbers that give way to J = 0 in the trivalent state and the half-filled population of the 4f orbitals in the divalent state. Herein, by optimizing the local crystal field of a quasi-linear bis(silylamido) Eu II complex, the [Eu II (N{SiMePh 2 } 2 ) 2 ] SMM is described, providing an example of a europium complex exhibiting slow relaxation of its magnetization. This behavior is dominated by a thermally activated (Orbach-like) mechanism, with an effective energy barrier of approximately 8 K, determined by bulk magnetometry and electron paramagnetic resonance. Ab initio calculations confirm second-order spin-orbit coupling effects lead to non-negligible axial magnetic anisotropy, splitting the ground state multiplet into four Kramers doublets, thereby allowing for the observation of an Orbach-like relaxation at low temperatures.

36 MATERIALS SCIENCE↗
NASA NTRS2007

Comparison of CALIPSO-Like, LaRC, and MODIS Retrievals of Ice Cloud Properties over SIRTA in France and Florida during CRYSTAL-FACE

This study compares cirrus particle effective radius retrieved by a CALIPSO-like method with two similar methods using MODIS, MODI Airborne Simulator (MAS), and GOES imagery. The CALIPSO-like method uses lidar measurements coupled with the split-window technique that uses the infrared spectral information contained at the 8.65-micrometer, 11.15-micrometer and 12.05-micrometer bands to infer the microphysical properties of cirrus clouds. The two other methods, sing passive remote sensing at visible and infrared wavelengths, are the operational MODIS cloud products (referred to by its archival product identifier MOD06 for MODIS Terra) and MODIS retrievals performed by the CERES team at LaRC (Langley Research Center) in support of CERES algorithms; the two algorithms will be referred to as MOD06- and LaRC-method, respectively. The three techniques are compared at two different latitudes: (i) the mid-latitude ice clouds study uses 18 days of observations at the Palaiseau ground-based site in France (SIRTA: Site Instrumental de Recherche par Teledetection Atmospherique) including a ground-based 532 nm lidar and the Moderate Resolution Imaging Spectrometer (MODIS) overpasses on the Terra Platform, (ii) the tropical ice clouds study uses 14 different flight legs of observations collected in Florida, during the intensive field experiment CRYSTAL-FACE (Cirrus Regional Study of Tropical Anvils and cirrus Layers-Florida Area Cirrus Experiment), including the airborne Cloud Physics Lidar (CPL) and the MAS. The comparison of the three methods gives consistent results for the particle effective radius and the optical thickness, but discrepancies in cloud detection and altitudes. The study confirms the value of an active remote-sensing method (CALIPSO-like) for the study of sub-visible ice clouds, in both mid-latitudes and tropics. Nevertheless, this method is not reliable in optically very thick tropical ice clouds.

Chiriaco, M.↗
DOE OSTI2026

Magnetic field induced modification of a first-order ferromagnetic transition in Eu 2 ⁢In

Here, we present a comprehensive study of the temperature-and magnetic-field-dependent magnetization, specific heat, and local crystal structure across the first-order ferromagnetic–paramagnetic transition in Eu 2 ⁢In. Anomalies in the magnetocaloric response are observed near 𝐻 ≈ 25 kOe, including changes in field scaling of magnetic entropy, local entropy exponent, and universal master curve, which suggest an apparent weakening of the first-order character of the transition. However, quantitative analysis of the magnetocaloric parameters together with modified Arrott plots demonstrates that the transition remains first order up to at least 70 kOe. Specific-heat measurements reveal a field-induced splitting of the sharp zero-field anomaly into a doublet, providing a natural explanation for the change in the magnetocaloric response. Magnetic-field-dependent extended x-ray absorption fine structure (EXAFS) measurements show no detectable field-induced changes in the local coordination environment of Eu. We therefore attribute these observations to a magnetic-field-induced two-step transition process in Eu 2 ⁢In.

Kumar, Ajay [Ames Laboratory (AMES), Ames, IA (Uni↗
DOE OSTI2025

Orbital-spin locking and its optical signatures in altermagnets

Altermagnets, magnetic materials with zero magnetization and spin-split band structure, have gained tremendous attention recently for their rich physics and potential applications. Here, we report on a microscopic tight-binding model that unveils a unique coupling between orbitals and spins in d-wave altermagnets, which gives rise to momentum-dependent and spin-selective optical absorption. This coupling promotes the controlled optical excitation of up or down spins depending on the polarization direction of linearly polarized light. Such an effect originates from the coupling of orbitals to the sublattice degree of freedom through the crystal field, which is then coupled to spins through the antiferromagnetic interaction. Our crystal field analysis, which is general to any type of altermagnet, helps understand the onset of altermagnetism from a microscopic point of view, and we use our results to propose clear magneto-optical signatures of our predictions. Our findings shine light on the interplay between orbitals and spins in altermagnets, thus paving the way towards novel orbitronic and optospintronic devices.

Vila, Marc↗
DOE OSTI2020

Enhancing easy-plane anisotropy in bespoke Ni(II) quantum magnets

We examine the crystal structures and magnetic properties of several S = 1 Ni(II) coordination compounds, molecules and polymers, that include the bridging ligands HF 2 - , A F 6 2- ( A = Ti, Zr) and pyrazine or non-bridging ligands F - , SiF 6 2- , glycine, H 2 O, 1-vinylimidazole, 4-methylpyrazole and 3-hydroxypyridine. Pseudo-octahedral NiN 4 F 2 , NiN 4 O 2 or NiN 4 OF cores consist of equatorial Ni-N bonds that are equal to or slightly longer than the axial Ni- L ax bonds. By design, the zero-field splitting ( D ) is large in these systems and, in the presence of substantial exchange interactions ( J ), can be difficult to discriminate from magnetometry measurements on powder samples. Thus, we relied on pulsed-field magnetization in those cases and employed electron-spin resonance (ESR) to confirm D when J ← D . The anisotropy of each compound was found to be easy-plane ( D > 0) and range from ≈ 8–25 K. This work reveals a linear correlation between the ratio d (Ni- L ax )/ d (Ni-N eq ) and D although the ligand spectrochemical properties may play an important role. We assert that this relationship allows us to predict the type of magnetocrystalline anisotropy in tailored Ni(II) quantum magnets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Asymmetric equilibrium core structures of pyramidal-II < c + a > dislocations in ten hexagonal-close-packed metals

The structures of pyramidal-II < c + a > dislocations, one of the most important defects in structural hexagonal-close-packed (HCP) metals, have not been fully characterized for many of the HCP metals in use today. Here, we employ ab initio informed phase-field dislocation dynamics to determine the minimum energy structure of pyramidal {1¯1¯22} < 11¯23 > dislocations in ten HCP metals, including Be, Co, Mg, Re, Ti, Zn, Cd, Hf, Y, and Zr. As input for the simulations, we calculate, using first-principles density functional theory, the {1¯1¯22} generalized stacking fault energy (GSFE) curves for all ten metals. From these calculations, it is found that magnetism in Co is necessary for achieving a local minimum in the GSFE curve. We observe in simulations that edge and screw character dislocations split into two partials separated by a low-energy intrinsic stacking fault. The splitting distance is shown to scale inversely with the local minimum energy normalized by the product of its shear modulus and Burgers vector. Interestingly, some HCP metals exhibit an asymmetric structure, with either unequal partial Burgers vectors or widths, in contrast to the symmetric configuration expected from linear elastic dislocation theory. We explain these structures by properties of the local maxima in their GSFE curves. Metals with larger degrees of elastic anisotropy result in dislocations with larger splitting distances than would be expected under the commonly used assumption of elastic isotropy. Furthermore, these findings on the sizes and asymmetry in the structures of pyramidal-II < c + a > dislocations are fundamental to understanding how these dislocations glide and interact or react with other defects when these metals are mechanically strained.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Enabling room-temperature ferromagnetism in few-layered MoS 2 films via strain engineering

Strain engineering presents a promising pathway for modulating the physical properties of two-dimensional (2D) transition metal dichalcogenides materials. Here, in this study, we investigate the strain-induced magnetic behavior of diamagnetic MoS 2 films prepared by the DC magnetron sputtering technique. By applying +1% tensile strain to few-layered MoS 2 films (∼3.5 nm), we observe the emergence of room-temperature ferromagnetism with a magnetization saturation of about ∼130 emu/cm 3 , in stark contrast to bulk films (∼40 nm), which remain diamagnetic under similar conditions. Raman spectroscopy reveals a pronounced reduction in the intensity and the splitting of the E′ mode in 1% strained few-layered films, indicating a possible bond elongation and symmetry breaking under tensile stress. Additionally, x-ray absorption spectroscopy at the Mo M 3 edge further confirms a strain-induced electronic structure modification in few-layered films, with no corresponding shift observed in bulk counterparts. Moreover, the strain-induced magnetic and structural changes are largely reversible upon strain release. We attribute the origin of ferromagnetism in few-layered films to the combined influence of tensile strain and defect-assisted bond weakening, which facilitates crystal field transitions within the Mo 4d orbitals. These findings demonstrate that strain engineering can effectively induce and modulate magnetism in 2D materials, providing opportunities for developing strain-controlled spintronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Spin–orbit coupling proximity effect in MoS 2 /Fe 3 GeTe 2 heterostructures

Layered two-dimensional (2D) magnet/semiconductor heterostructures combine spintronic and optoelectronic properties of constituent materials, leading to new magneto-optical and magnetoelectric phenomena such as spontaneous emission of helical light and enhanced Zeeman splitting in single photon emission. While prior focus was mostly on the magnetic proximity effect, where properties of 2D magnets are transferred to nonmagnetic 2D materials, the inverse effect of 2D semiconductors altering 2D magnets is much less understood. Here, we fabricated and studied van der Waals (vdW) heterostructures of 2D magnet Fe 3 GeTe 2 (FGT) and 2D semiconductor MoS 2 . With reflectance magnetic circular dichroism, we found that the coercive field of MoS 2 -covered FGT reduces compared with uncovered FGT, agreeing well with our first-principles calculations. With its strong spin–orbit coupling (SOC), MoS 2 effectively alters the crystal field of the adjacent FGT and its magnetic anisotropy. Furthermore, an unconventional two-step hysteresis loop emerges in MoS 2 /FGT as a result of the superposition of two regions of FGT: at the interface and away from the interface. Our experimental elucidation of the SOC proximity effect that MoS 2 exerts on FGT provides fundamental understanding for the rational development of 2D magnet/semiconductor heterostructures.

2D materials↗
DOE OSTI2026

Frequency reproducibility of solid-state thorium-229 nuclear clocks

Solid-state thorium-229 ( 229 Th) nuclear clocks are set to provide new opportunities for precision metrology and fundamental physics. Taking advantage of inherent low sensitivity of a nuclear transition to its environment, orders of magnitude more emitters can be hosted in a solid-state crystal compared with current optical lattice atomic clocks. Furthermore, solid-state systems needing only simple thermal control are key to the development of field-deployable compact clocks. Here we explore and characterize the frequency reproducibility of the 229 Th:CaF 2 nuclear clock transition, a key performance metric for all clocks. We measure the transition linewidth and centre frequency as a function of the doping concentration, temperature and time. We report the concentration-dependent inhomogeneous linewidth of the nuclear transition, limited by the intrinsic host crystal properties. We determine an optimal working temperature for the 229 Th:CaF 2 nuclear clock at 196(5) K, at which the first-order thermal sensitivity vanishes. This would enable in situ temperature co-sensing using different quadrupole-split lines, reducing the temperature-induced systematic shift below the 10 −18 fractional frequency uncertainty level. At 195 K, the reproducibility of the nuclear transition frequency is 220 Hz (fractionally 1.1 × 10 −13 ) for two differently doped 229 Th:CaF 2 crystals over 7 months. Furthermore, these results form the foundation for understanding, controlling and harnessing the coherent nuclear excitation of 229 Th in solid-state hosts and for their applications in constraining temporal variations of fundamental constants.

Atomic and molecular physics↗
NASA NTRS1972

An EPR investigation of the dynamic Jahn-Teller effect in SrCl2:y(2 plus) and SrCl2:Sc(2 plus)

EPR spectra have been observed for SrCl2:Y(2+) and SrCl2:Sc(2+) at liquid helium temperatures. At 1.2 K the spectra were dominated by anisotropic hyperfine patterns whose lineshapes and angular dependences were explained using second order solutions of the effective Hamiltonian for an isolated 2Eg state split by large random internal strains. Pronounced asymmetries in some of the strin produced lineshapes for Srcl2:Sc(2+) are shown to result from second order terms in the solution of the effective Hamiltonian. Coexisting with the anisotropic hyperfine patterns are weak nearly isotropic hyperfine patterns with typical lineshapes. Variations in the apparent intensity of lines in these weak hyperfine patterns as functions of the applied magnetic field direction and temperature imply that these lines result from averaging by vibronic relaxation of a portion of the anisotropic pattern. The effective Hamiltonian parameters for SrCl2:La(2+), SrCl2:y(2+), and SrCl2:SC(2+) are analyzed in terms of crystal field theory modified to include a dynamic Jahn-Teller effect.

Herrington, J. R.↗