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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 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Giant spontaneous polarization for enhanced ferroelectric properties of biaxially oriented poly(vinylidene fluoride) by mobile oriented amorphous fractions

Poly(vinylidene fluoride) (PVDF) and its random copolymers exhibit the most distinctive ferroelectric properties; however, their spontaneous polarization (60–105 mC m -2 ) is still inferior to those (>200 mC m -2 ) of the ceramic counterparts. In this work, we report an unprecedented spontaneous polarization ( P s = 140 mC m -2 ) for a highly poled biaxially oriented PVDF (BOPVDF) film, which contains a pure β crystalline phase. Given the crystallinity of ~0.52, the P s for the β phase ( P s,β ) is calculated to be 279 mC m -2 , if a simple two-phase model of semicrystalline polymers is assumed. This high P s,β is invalid, because the theoretical limit of P s,β is 185 mC m -2 , as calculated by density functional theory. To explain such a high P s for the poled BOPVDF, a third component in the amorphous phase must participate in the ferroelectric switching to contribute to the P s . Namely, an oriented amorphous fraction (OAF) links the lamellar crystal and the mobile amorphous fraction. From the hysteresis loop study, the OAF content was determined to be ~0.28, more than 50% of the amorphous phase. Because of the high polarizability of the OAFs, the dielectric constant of the poled BOPVDF reached nearly twice the value of conventional PVDF. Overall, the fundamental knowledge obtained from this study will provide a solid foundation for the future development of PVDF-based high performance electroactive polymers for wearable electronics and soft robotic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Spin filtering and spin separation in 2D materials by topological spin Hall effect

The needs of high speed performance electronic devices for various applications require novel materials and new physical phenomena. For these purposes we propose to study new physical effects based on electron scattering on magnetic skyrmions and vortices distributed in a 2D ferromagnetic material. Herein, we show that the topological spin Hall effect can be efficiently employed for the filtering, switching, and separation of spin currents. For some values of the parameters (conduction electron concentrations, and skyrmion/vortex sizes) it is possible to separate Hall currents for different electron spin projections as it is like for different carrier charges (electrons and holes) in the normal Hall effect. The calculations are performed using the Boltzmann kinetic equation for the nonequilibrium distribution function and the Lippmann–Schwinger equation for the transition matrix in the whole range of the adiabaticity parameter. The spin filtering due to the skyrmion/vortex scattering can be several orders of magnitude more efficient in the narrow range of the electron concentrations than that of the ordinary ferromagnetic spin polarization in spintronics.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Terahertz electric-field-driven dynamical multiferroicity in SrTiO 3

The emergence of collective order in matter is among the most fundamental and intriguing phenomena in physics. In recent years, the dynamical control and creation of novel ordered states of matter not accessible in thermodynamic equilibrium is receiving much attention. The theoretical concept of dynamical multiferroicity has been introduced to describe the emergence of magnetization due to time-dependent electric polarization in non-ferromagnetic materials. In simple terms, the coherent rotating motion of the ions in a crystal induces a magnetic moment along the axis of rotation. Here we provide experimental evidence of room-temperature magnetization in the archetypal paraelectric perovskite SrTiO 3 due to this mechanism. We resonantly drive the infrared-active soft phonon mode with an intense circularly polarized terahertz electric field and detect the time-resolved magneto-optical Kerr effect. A simple model, which includes two coupled nonlinear oscillators whose forces and couplings are derived with ab initio calculations using self-consistent phonon theory at a finite temperature, reproduces qualitatively our experimental observations. A quantitatively correct magnitude was obtained for the effect by also considering the phonon analogue of the reciprocal of the Einstein–de Haas effect, which is also called the Barnett effect, in which the total angular momentum from the phonon order is transferred to the electronic one. Our findings show a new path for the control of magnetism, for example, for ultrafast magnetic switches, by coherently controlling the lattice vibrations with light.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Dynamic Manipulation in Piezoresponse Force Microscopy: Creating Nonequilibrium Phases with Large Electromechanical Response

We discuss how domain walls and topological defects in ferroelectric materials have emerged as a powerful tool for functional electronic devices including memory and logic. Similarly, wall interactions and dynamics underpin a broad range of mesoscale phenomena ranging from giant electromechanical responses to memory effects. Exploring the functionalities of individual domain walls, their interactions, and controlled modifications of the domain structures is crucial for applications and fundamental physical studies. However, the dynamic nature of these features severely limits studies of their local physics since application of local biases or pressures in piezoresponse force microscopy induce wall displacement as a primary response. Here, we introduce an approach for the control and modification of domain structures based on automated experimentation, whereby real-space image-based feedback is used to control the tip bias during ferroelectric switching, allowing for modification routes conditioned on domain states under the tip. This automated experiment approach is demonstrated for the exploration of domain wall dynamics and creation of metastable phases with large electromechanical response.

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

Ferroelectric Al1 − xBxN thin films integrated on Si

Ferroelectric Al0.93B0.07N thin films are prepared (100) Si substrates. The necessary c-axis out-of-plane orientation to observe macroscopic ferroelectric switching was achieved by implementing an initial Ar/N2 plasma treatment, followed by a thin layer of AlN to initiate the desired texture and a 150 nm W layer. The plasma treatment facilitates crystallinity enhancement of the AlN template layer, allowing for subsequent growth of highly oriented W and Al0.93B0.07N layers. The W layer exhibits random in-plane orientation and exclusive (110) out-of-plane orientation with a rocking curve width of 1.4°. When grown on these W surfaces, 175 nm thick Al0.93B0.07N films exhibit random in-plane orientation and exclusive (001) texture with rocking curve full-width-half-max values of 1.6° and RMS roughness values less than 1 nm. Polarization hysteresis measurements show robust hysteresis with coercive field values of 5.4 MV/cm and remanent polarization values of 136 μC/cm2. XPS depth profile analysis suggests that the plasma treatment converts the existing native oxide to a nitrogen rich oxynitride with approximate composition Si3O0.5N3.67. Cross-sectional TEM reveals that the oxynitride interlayer is amorphous and ∼3.4 nm thick, more than double the native oxide thickness measured by multiwavelength ellipsometry, implying that (oxy)nitride growth continues after conversion of the native oxide. This new family of ferroelectric wurtzites is interesting from an integration perspective given their chemical compatibility with mainstream semiconductors. Developing synthesis routes that promote needed texture while preserving compatible processing windows is an important step toward practical integration.

Physics↗
DOE OSTI2021

Charged Ferroelectric Domain Walls for Deterministic ac Signal Control at the Nanoscale

The direct current (dc) conductivity and emergent functionalities at ferroelectric domain walls are closely linked to the local polarization charges. Depending on the charge state, the walls can exhibit unusual dc conduction ranging from insulating to metallic-like, which is leveraged in domain-wall-based memory, multilevel data storage, and synaptic devices. In contrast to the functional dc behaviors at charged walls, their response to alternating currents (ac) remains to be resolved. Here, we reveal ac characteristics at positively and negatively charged walls in ErMnO 3 , distinctly different from the response of the surrounding domains. By combining voltage-dependent spectroscopic measurements on macroscopic and local scales, we demonstrate a pronounced nonlinear response at the electrode-wall junction, which correlates with the domain-wall charge state. The dependence on the ac drive voltage enables reversible switching between uni- and bipolar output signals, providing conceptually new opportunities for the application of charged walls as functional nanoelements in ac circuitry.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Electrochemical Switching of a Fluorescent Molecular Rotor Embedded within a Bistable Rotaxane

We report how the nanoconfined environment, introduced by the mechanical bonds within an electrochemically switchable bistable [2]rotaxane, controls the rotation of a fluorescent molecular rotor, namely, an 8-phenyl-substituted boron dipyrromethene (BODIPY). The electrochemical switching of the bistable [2]rotaxane induces changes in the ground-state coconformation and in the corresponding excited-state properties of the BODIPY rotor. In the starting redox state, when no external potential is applied, the cyclobis(paraquat-p-phenylene) (CBPQT4+) ring component encircles the tetrathiafulvalene (TTF) unit on the dumbbell component, leaving the BODIPY rotor unhindered and exhibiting low fluorescence. Upon oxidation of the TTF unit to a TTF2+ dication, the CBPQT4+ ring is forced toward the molecular rotor, leading to an increased energy barrier for the excited state to rotate the rotor into the state with a high nonradiative rate constant, resulting in an overall 3.4-fold fluorescence enhancement. On the other hand, when the solvent polarity is high enough to stabilize the excited charge-transfer state between the BODIPY rotor and the CBPQT4+ ring, movement of the ring toward the BODIPY rotor produces an unexpectedly strong fluorescence signal decrease as the result of photoinduced electron transfer from the BODIPY rotor to the CBPQT4+ ring. The nanoconfinement effect introduced by mechanical bonding can effectively lead to modulation of the physicochemical properties as observed in this bistable [2]rotaxane. On account of the straightforward synthetic strategy and the facile modulation of switchable electrochromic behavior, our approach could pave the way for the development of new stimuli-responsive materials based on mechanically interlocked molecules for future electro-optical applications, such as sensors, molecular memories, and molecular logic gates.

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

Direct Imaging of Asymmetric Interfaces and Electrostatic Potentials inside a Hafnia–Zirconia Ferroelectric Nanocapacitor

In hafnia-based thin-film ferroelectric devices, chemical phenomena during growth and processing, such as oxygen vacancy formation and interfacial reactions, appear to strongly affect device performance. However, the correlation between the structure, chemistry, and electrical potentials at the nanoscale in these devices is not fully known, making it difficult to understand their influence on device properties. Here, we directly image the composition and electrostatic potential with nanometer resolution in the cross section of a nanocrystalline W/Hf 0.5 Zr 0.5 O 2−δ (HZO)/W ferroelectric capacitor using multimodal electron microscopy. This reveals a 1.4 nm wide tungsten suboxide interfacial layer formed at the bottom interface during fabrication, which introduces a potential dip and leads to asymmetric switching fields. Additionally, we compare the measured potentials to DFT calculations and find it is nearly 3 V lower than expected in the HZO, which appears to be caused by oxygen vacancies and a resulting negative built-in potential. In conclusion, these chemical and electrostatic details are important to characterize and tune to achieve high-performance ferroelectric devices.

Defects in solids↗
DOE OSTI2022

Smectic C Self‐Assembly in Mesogen‐Free Liquid Crystalline Chiral Polyethers with Sulfonylated Methyl‐Branched Side Chains

Abstract To realize advanced electrical applications for ferroelectric liquid crystalline polymers, high spontaneous polarization ( P s ) is highly desired. However, current ferroelectric liquid crystalline polymers usually exhibit a low P s . In this work, mesogen‐free, chiral polyethers containing sulfonylated methyl‐branched alkyl side chains with a (CH 2 ) 3 O spacer between the sulfonyl and the branched alkyl groups are designed and synthesized. In contrast to the linear n ‐alkyl side chains, the methyl‐branched alkyl side chains induce chain tilting in the smectic layers. When double chirality exists in both the main chain and the side chains, a crystalline structure is observed after mechanical stretching. Intriguingly, when single chirality exists in either the backbone or the side chains, a liquid crystalline smectic C phase is obtained. The electric displacement–electric field study, however, does not show typical ferroelectric switching, although the dielectric constants are relatively high for these liquid crystalline polymers. This is likely because the dipole–dipole interactions among neighboring sulfonyl groups along the main chain are so strong that the ferroelectric switching is hindered in the samples. For the future work, it is desired to weaken the dipole–dipole interaction to achieve ferroelectricity in these mesogen‐free liquid crystalline polymers.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Direct experimental evidence of tunable charge transfer at the LaNiO 3 / CaMnO 3 ferromagnetic interface

Interfacial charge transfer in oxide heterostructures gives rise to a rich variety of electronic and magnetic phenomena. Designing heterostructures where one of the thin-film components exhibits a metal-insulator transition opens a promising avenue for controlling such phenomena both statically and dynamically. In this work, we utilize a combination of depth-resolved soft x-ray standing-wave and hard x-ray photoelectron spectroscopies in conjunction with polarization-dependent x-ray absorption spectroscopy to investigate the effects of the metal-insulator transition in LaNiO 3 on the electronic and magnetic states at the LaNiO 3 /CaMnO 3 interface. Here, we report a direct observation of the reduced effective valence state of the interfacial Mn cations in the metallic superlattice with an above-critical LaNiO 3 thickness (6 unit cells, u.c.) facilitated by the charge transfer of itinerant Ni 3d e g electrons into the interfacial CaMnO 3 layer. Conversely, in an insulating superlattice with a below-critical LaNiO 3 thickness of 2 u.c., a homogeneous effective valence state of Mn is observed throughout the CaMnO 3 layers due to the blockage of charge transfer across the interface. The ability to switch and tune interfacial charge transfer enables precise control of the emergent ferromagnetic state at the LaNiO 3 /CaMnO 3 interface and, thus, has far-reaching consequences on the future strategies for the design of next-generation spintronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Fabrication and characterization of net-shaped iron nitride-amine-epoxy soft magnetic composites

Soft magnetic composites (SMCs) offer a promising alternative to electrical steels and soft ferrites in high performance motors and power electronics. They are ideal for incorporation into passive electronic components such as inductors and transformers, which require a non-permanent magnetic core to rapidly switch magnetization. As a result, there is a need for materials with the right combination of low coercivity, low magnetic remanence, high relative permeability, and high saturation magnetization to achieve these goals. Iron nitride is an attractive soft magnetic material for incorporation into an amine/epoxy resin matrix. This permits the synthesis of net-shaped SMCs using a “bottom-up” approach for overcoming the limitations of current state-of-the-art SMCs made via conventional powder metal processing techniques. In this work we present the fabrication of various net-shaped, iron nitride-based SMCs using two different amine/epoxy resin systems and their magnetic characterization. The maximum volume loading of iron nitride reached was ~77% via hot pressing, which produced SMCs with a saturation magnetic polarization (J s ) of ~0.9 T, roughly 2–3 times the J s of soft ferrites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Optimal filtering and generation of entangled photons for quantum applications in the presence of noise

Filtering is commonly used in quantum optics to reject noise photons, and also to enable interference between independent photons. However, filtering the joint spectrum of photon pairs can reduce the inherent coincidence probability or loss-independent heralding efficiency. Here we investigate filtering for multiphoton applications based on entanglement and interference (e.g., quantum teleportation). We multiplex C-band entangled photons and C-band classical communications into the same long-distance fibers, which enables scalable low-loss quantum networking but requires filtering of spontaneous Raman scattering noise from classical light. Using tunable-bandwidth filters, low-jitter detectors, and polarization filters, we distribute wavelength-degenerate time-bin entangled photons in the C band (1536.5 nm) over 25 km/25 km standard fibers (50 km) each carrying 10 Gbit/s C-band classical data signals. Narrow filtering enables milliwatt-level C-band power, which exceeds the power achieved by comparable studies by roughly an order of magnitude and could feasibly support terabit per second classical rates. We evaluate how performance depends on pump and filter bandwidths, multipair emission, filter shapes, loss, phase matching, and how quantum information is measured. We find a trade-off between reducing noise impact and increasing single-mode purity, and discuss mitigation methods toward optimal multiphoton applications. Importantly, these results apply to noise in free space and in quantum devices (sources, frequency converters, switches, detectors, etc.) and provide insight into filter-induced degradation of single-photon purity and rates even in noise-free environments.

Thomas, Jordan M. [Fermilab; Northwestern U.]↗
DOE OSTI2021

Disorder-induced time effect in the antiferromagnetic domain state of Fe 1+ y Te

Herein we report on temperature-dependent soft X-ray absorption spectroscopy (XAS) measurements utilizing linearly polarized synchrotron radiation to probe magnetic phase transitions in iron-rich Fe 1+y Te (y ≈ 0.12). X-ray magnetic linear dichroism (XMLD) signals, which sense magnetic ordering processes at surfaces, start to increase monotonically below the Néel temperature T N = 57 K. This increase is due to a progressive bicollinear antiferromagnetic (AFM) alignment of Fe spins of the monoclinic Fe 1+y Te parent phase. This AFM alignment was achieved by a [1 0 0]-oriented biasing field favoring a single-domain state during cooling across T N . Our specific heat and magnetization measurements confirm the bulk character of this AFM phase transition. On longer time scales, however, we observe that the field-biased AFM state is highly unstable even at the lowest temperature of T = 3 K. After switching off the biasing field, the XMLD signal decays exponentially with a time constant τ = 1506 s. The initial XMLD signal is restored only upon repeating a cycle consisting of heating and field-cooling through T N . We explain the time effect by a gradual formation of a multi-domain state with 90° rotated AFM domains, promoted by structural disorder, facilitating the motion of twin-domains. Significant disorder in our Fe 1+y Te sample is evident from our X-ray diffraction and specific heat data. The stability of magnetic phases in Fe-chalcogenides is an important material property, since the Fe(Te 1-x Se x ) phase diagram shows magnetism intimately connected with superconductivity.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Magnetoelectric effect arising from a field-induced pseudo Jahn-Teller distortion in a rare-earth magnet

Magnetoelectric materials are attractive for several applications, including actuators, switches, and magnetic field sensors. Typical mechanisms for achieving a strong magnetoelectric coupling are rooted in transition metal magnetism. In sharp contrast, here we identify CsEr(MoO 4 ) 2 as a magnetoelectric material without magnetic transition metal ions, thus ensuring that the Er ions play a key role in achieving this interesting property. Our detailed study includes measurements of the structural, magnetic, and magnetoelectric properties of this material. Bulk characterization and neutron powder diffraction show no evidence for structural phase transitions down to 0.3 K and therefore CsEr(MoO 4 ) 2 maintains the room temperature P2/c space group over a wide temperature range without external magnetic field. These same measurements also identify collinear antiferromagnetic ordering of the Er 3+ moments below T N =0.87K. Complementary dielectric constant and pyroelectric current measurements reveal that a ferroelectric phase with a maximum polarization P~0.6 nC/cm 2 emerges when applying a modest external magnetic field, which indicates that this material has a strong magnetoelectric coupling. Finally, we argue that the magnetoelectric coupling in this system arises from a pseudo Jahn-Teller distortion induced by the magnetic field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Dual Emission Bands of a 2D Perovskite Single Crystal with Charge Transfer State Characteristics

Several hybrid halide 2D-perovskite species emit light with an emergent and controversial broadband emission Stokes-shifted down from the narrow band emission. This work uncovers the sub- and above-bandgap emission and absorption characteristics of PEA 2 PbI 4 prepared with gap states introduced during single crystal growth. Here, gap states led to coexistent intrinsic and heterostructured electronic frameworks that are selectively accessible with ultraviolet (UV) and infrared (IR) light, respectively, resulting in the phenomenon of photoluminescence (PL) switching from narrowband green to broadband red. Electron-energy dependent cathodoluminescence shows a relative increase in the broadband red PL intensity as the electron penetration depth increases from 30 nm to 2 μm, confirming the heterostructured framework is formed in the bulk of the crystal. Excitation–emission power slope of 2.5 and up-conversion pump transient absorption (TA) spectra suggest that the IR up-conversion excitation with red photoluminescence, peaked at 655 nm, is a multiphoton process occurring in the heterostructured framework through a nonlinear optical response. The energetic pathways toward the dual emission bands are revealed by pump–probe transient absorption spectroscopy, showing energetically broad gap states with high sensitivity to an IR pump are upconverted and subsequently quickly relax from high to low energy levels within 4 ps. Furthermore, the up-conversion red PL demonstrates a linear polarization with magnetic field effects, thus affirming that the band-like heterostructured framework is crystallographically aligned with characteristics of spatially extended charge-transfer states.

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

Circularly Polarized Optical Stark Effect in CdSe Colloidal Quantum Wells

Colloidal quantum wells, or nanoplatelets, exhibit large, circularly polarized optical Stark effects under sub-band-gap femtosecond illumination. The optical Stark effect is measured for CdSe colloidal quantum wells of several thicknesses and separately as a measure of pump photon energy, pump fluence, and temperature. These measurements show that optical Stark effects in colloidal quantum wells shift the absorption features up to 5 meV, at the intensities up to 2.9 GW.cm -2 and large detuning (>400 meV) of the pump photon energy from the band edge absorption. Optical Stark shifts are underpinned by large transition dipoles of the colloidal quantum wells (mu = 15-23 D), which are larger than those of any reported colloidal quantum dots or epitaxial quantum wells. The rapid (<500 fs), narrow band blue shift of the excitonic features under circular excitation indicates the viability of these materials beyond light emission such as spintronics or all-optical switching.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Coupled magnetostructural continuum model for multiferroic BiFeO 3

Here, a continuum approach to study magnetoelectric multiferroic BiFeO 3 (BFO) is proposed. Our modeling effort marries the ferroelectric (FE) phase field method and micromagnetic simulations to describe the entire multiferroic order parameter sector (polarization, oxygen antiphase tilts, strain, and magnetism) self-consistently on the same time- and length scale. In this paper, we discuss our choice of FE and magnetic energy terms and demonstrate benchmarks against known behavior. We parametrize the lowest order couplings of the structural distortions against previous predictions from density functional theory calculations giving access to simulations of the FE domain wall (DW) topology. This allows us to estimate the energetic hierarchy and thicknesses of the numerous structural DWs. We then extend the model to the canted antiferromagnetic order and demonstrate how the FE domain boundaries influence the resulting magnetic DWs. We also highlight some capabilities of this model by providing two examples relevant for applications. We demonstrate spin-wave transmission through the multiferroic domain boundaries which identify rectification in qualitative agreement with recent experimental observations. As a second example of application, we model fully dynamical magnetoelectric switching, where we find a sensitivity on the Gilbert damping with respect to switching pathways. We envision that this modeling effort will set the basis for further work on properties of arbitrary 3D nanostructures of BFO (and related multiferroics) at the mesoscale.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Synthesis and Properties of Bulk Mg 3 WN 4 in a Wurtzite-Derived Structure

Experimental synthesis of theoretically predicted materials with controlled elemental coordination environments can lead to the realization of useful properties, such as facile ion transport or ferroelectric switching. Among such materials are ternary nitrides in the Mg−W−N composition space, where several stable and metastable compounds have been predicted and synthesized recently in bulk and film forms. Here, we report for the first time on the bulk synthesis of Mg 3 WN 4 in a wurtzite-derived crystal structure via a solid-state metathesis reaction. In situ synchrotron powder X-ray diffraction shows how the ion exchange proceeds from Li 6 WN 4 + MgCl 2 precursors to Mg 3 WN 4 + LiCl products, with the reaction starting slowly near 380 °C and completing by 600 °C, including the presence of a competing disordered rocksalt-derived phase (Mg,W)N above 440 °C. The follow-up ex situ powder synthesis at 400 °C for 0.5 h with 10% excess MgCl 2 reveals the cation-ordered nature of the wurtzite-derived Mg 3 WN 4 structure with polar symmetry confirmed by second-harmonic generation measurements. Optical absorption spectra, chemical composition analysis, and electron microscopy imaging suggest that bulk Mg 3 WN 4 obtained via metathesis reaction is prone to defect formation. Overall, this study shows that selective ex situ synthesis of the phase-pure ternary nitrides, informed by in situ measurements, is possible by carefully controlling the thermal budget of the reaction and paves the way toward property characterization of the Mg 3 WN 4 wurtzite-derived material.

36 MATERIALS SCIENCE↗