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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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Structure and ferroelectric studies of (Ba{sub 0.85}Ca{sub 0.15})(Ti{sub 0.9}Zr{sub 0.1})O{sub 3} piezoelectric ceramics

Graphical abstract: - Highlights: • (Ba{sub 0.85}Ca{sub 0.15})(Ti{sub 0.9}Zr{sub 0.1})O{sub 3} (BCTZO) ceramic was synthesized by the ceramic method. • In situ XRD and Raman spectra showed the phase transition of BCTZO around 360 K. • The ceramics showed a tunability of 82% at 40 kV cm{sup −1} electric field. • BCTZO exhibited good quality factor of 111 at microwave frequencies. • Piezoforce microscopy studies indicated the switchability of ferroelectric domains. - Abstract: We have synthesized and studied the structural and ferroelectric properties of lead-free 0.5(Ba{sub 0.7}Ca{sub 0.3})TiO{sub 3}–0.5Ba(Zr{sub 0.2}Ti{sub 0.8})O{sub 3} ceramics in the temperature region of its ferroelectric transition. The synthesized material showed high dielectric constant, low loss and good pyroelectric figure of merit. From the temperature dependent X-ray diffraction measurements, we determined the tricritical point to be in the temperature range of 303–400 K. The dielectric measurements indicate a diffuse ferroelectric phase transition (DPT) around 360 K in agreement with the X-ray measurements. We studied the evolution of Raman spectra with temperature to understand the nature of phase transition in BaTiO{sub 3} (BTO) and the BCTZO. The results indicates that the transition of ferroelectric–paraelectric state is not sharp as in the case of BTO and the polar state persists through the paraelectric state. In general, our study indicates that there are ferroelectric domains of nanometer size beyond the commonly defined transition temperature. The observation of local piezoelectric hysteresis loop indicated the existence of intrinsic ferroelectric property of the ceramic at the nanoscale. The ceramics exhibited electric field tunable dielectric properties with a tunability of 82% at an applied DC field of 40 kV cm{sup −1}, low dielectric loss of 0.001 and room temperature pyroelectric coefficient of 6 × 10{sup −8} C cm{sup −2} K{sup −1} and the detectivity of 1.9 × 10{sup −8} C cm{sup −1} J{sup −1}; larger than those reported for other BaTiO{sub 3}-based materials. Overall, our results indicate that BCTZO ceramics with coexistence of rhombohedral–tetragonal phases is a promising candidate for lead-free ferroelectric applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Broad Distribution of Local Polar States Generates Large Electrothermal Properties in Pb-Free Relaxor Ferroelectrics

Electrothermal energy conversion provides attractive solutions for global energy management, such as energy harvesting from waste heat using pyroelectric energy conversion (PEC) and efficient cooling of portable electronics or data servers using the electrocaloric effect. Relaxor ferroelectrics are attractive for electrothermal energy conversion because of their large pyroelectric coefficients over a wide temperature range. Although Pb-based relaxors are well-known, toxicity concerns have mandated the intense search for Pb-free alternatives. Here, we engineered (Ba,Ca)TiO 3 -based relaxors based on a multisite doping strategy, which show promising electrothermal performance, viz. a maximum PEC efficiency of 14% and electrocaloric refrigeration capacity of 115 J/kg. Using local-scale structural analysis, we provide an atomistic model for large electrothermal properties in the newly designed Pb-free ferroelectrics, whereby a temperature-independent continuous distribution of cation displacement directions creates easy pathways for microscopic polarization reorientation. This research provides key structural insight for future atomic-scale engineering of environmentally sustainable ferroelectrics in energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

High Entropy Oxide Relaxor Ferroelectrics

Relaxor ferroelectrics are important in technological applications due to strong electromechanical response, energy storage capacity, electrocaloric effect, and pyroelectric energy conversion properties. Current efforts to discover and design materials in this class generally rely on substitutional doping as slight changes to local compositional order can significantly affect the Curie temperature, morphotropic phase boundary, and electromechanical responses. In this work, we demonstrate that moving to the strong limit of compositional complexity in an ABO 3 perovskite allows stabilization of relaxor responses that do not rely on a single narrow phase transition region. Entropy-assisted synthesis approaches are utilized to synthesize single-crystal Ba(Ti 0.2 Sn 0.2 Zr 0.2 Hf 0.2 Nb 0.2 )O 3 [Ba(5B)O] films. The high levels of configurational disorder present in this system are found to influence dielectric relaxation, phase transitions, nanopolar domain formation, and Curie temperature. Temperature-dependent dielectric, Raman spectroscopy, and second-harmonic generation measurements reveal multiple phase transitions, a high Curie temperature of 570 K, and the relaxor ferroelectric nature of Ba(5B)O films. The first-principles theory calculations are used to predict possible combinations of cations to design relaxor ferroelectrics and quantify the relative feasibility of synthesizing these highly disordered single-phase perovskite systems. Further, the ability to stabilize single-phase perovskites with various cations on the B-sites offers possibilities for designing high-performance relaxor ferroelectric materials for piezoelectric, pyroelectric, and electrocaloric applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Resolving the Heat of Trimethylaluminum and Water Atomic Layer Deposition Half-Reactions

We report that atomic layer deposition (ALD) is a surface synthesis technique that is characterized by self-limiting reactions between gas-phase precursors and a solid substrate. Although ALD processes have been demonstrated that span the periodic table, a greater understanding of the surface chemistry that affords ALD is necessary to enable greater precision, including area- and site-selective growth. We offer new insight into the thermodynamics and kinetics of the trimethylaluminum (TMA) and H 2 O ALD half-reactions with calibrated and time-resolved in situ pyroelectric calorimetry. The half-reactions produce 3.46 and 2.76 eV/Al heat, respectively, which is greater than the heat predicted by computational models based on crystalline Al 2 O 3 substrates and closely aligned with the heat predicted by standard heats of formation. The pyroelectric thin-film calorimeter offers submilisecond temporal resolution that uniquely and clearly resolves precursor delivery and reaction kinetics. Both half-reactions are observed to exhibit multiple kinetic rates, with average TMA half-reaction rates at least 2 orders of magnitude faster than the H 2 O half-reaction kinetics. Comparing the experimental heat with published computational literature and additional first-principles modeling highlights the need to refine our models and mechanistic understanding of even the most ubiquitous ALD reactions.

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

Atomic lift-off of epitaxial membranes for cooling-free infrared detection

Recent breakthroughs in ultrathin, single-crystalline, freestanding complex oxide systems have sparked industry interest in their potential for next-generation commercial devices. However, the mass production of these ultrathin complex oxide membranes has been hindered by the challenging requirement of inserting an artificial release layer between the epilayers and substrates. Here we introduce a technique that achieves atomic precision lift-off of ultrathin membranes without artificial release layers to facilitate the high-throughput production of scalable, ultrathin, freestanding perovskite systems. Leveraging both theoretical insights and empirical evidence, we have identified the pivotal role of lead in weakening the interface. This insight has led to the creation of a universal exfoliation strategy that enables the production of diverse ultrathin perovskite membranes less than 10 nm. Our pyroelectric membranes demonstrate a record-high pyroelectric coefficient of 1.76 × 10 −2 C m −2 K −1 , attributed to their exceptionally low thickness and freestanding nature. Moreover, this method offers an approach to manufacturing cooling-free detectors that can cover the full far-infrared spectrum, marking a notable advancement in detector technology.

nanoscale materials↗
DOE OSTI2015

Evidence of large magneto-dielectric effect coupled to a metamagnetic transition in Yb{sub 2}CoMnO{sub 6}

The double perovskite Yb{sub 2}CoMnO{sub 6} has been synthesized with an almost perfect checkerboard arrangement of Co{sup 2+} and Mn{sup 4+} cations in the B-sublattice of the perovskite cell. It presents an anomaly in the electric capacitance and a strong magneto-dielectric effect at about 40 K whose interplay with the microscopic magnetic behavior has been investigated by means of neutron diffraction, magnetization, pyroelectric, and relative dielectric permittivity measurements. We show that the onset of an E-type antiferromagnetic ordering of Co{sup 2+} and Mn{sup 4+} moments monitored by neutron diffraction provokes the noticeable jump of the relative dielectric permittivity (∼9%) at about 40 K. It is also shown that this jump can be totally suppressed by application of a magnetic field of μ{sub 0}H = 5 T. Neutron experiments and magnetic measurements confirm that such a suppression leading to a significant magneto-dielectric effect is driven by a metamagnetic phase transition from the peculiar E-type ordering of 3d moments into a collinear ferromagnetic order. Pyroelectric current measurements do not show any spontaneous electric polarization, so the large dielectric anomaly at zero field cannot be ascribed to a ferroelectric ordering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Effect of the out-of-plane stress on the properties of epitaxial SrTiO{sub 3} films with nano-pillar array on Si-substrate

A nonlinear thermodynamic formalism has been proposed to calculate the physical properties of the epitaxial SrTiO{sub 3} films containing vertical nano-pillar array on Si-substrate. The out-of-plane stress induced by the mismatch between film and nano-pillars provides an effective way to tune the physical properties of ferroelectric SrTiO{sub 3} films. Tensile out-of-plane stress raises the phase transition temperature and increases the out-of-plane polarization, but decreases the out-of-plane dielectric constant below Curie temperature, pyroelectric coefficient, and piezoelectric coefficient. These results showed that by properly controlling the out-of-plane stress, the out-of-plane stress induced paraelectric-ferroelectric phase transformation will appear near room temperature. Excellent dielectric, pyroelectric, piezoelectric properties of these SrTiO{sub 3} films similar to PZT and other lead-based ferroelectrics can be expected.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Short range ferromagnetic, magneto-electric, and magneto-dielectric effect in ceramic Co{sub 3}TeO{sub 6}

We report observation of magneto-electric and magneto-dielectric couplings along with short range ferromagnetic order in ceramic Cobalt Tellurate (Co{sub 3}TeO{sub 6}, CTO) using magnetic, structural, dielectric, pyroelectric, and polarization studies. DC magnetization along with dielectric constant measurements indicate a coupling between magnetic order and electrical polarization. A strong anomaly in the dielectric constant at ∼17.4 K in zero magnetic field indicates spontaneous electric polarization, consistent with a recent neutron diffraction study. Observation of weak short range ferromagnetic order at lower temperatures is attributed to the Griffiths-like ferromagnetism. Furthermore, magnetic field dependence of the ferroelectric transition follows earlier theoretical predictions, applicable to single crystal CTO. Finally, combined dielectric, pyroelectric, and polarization measurements suggest that the ground state of CTO may possess spontaneous symmetry breaking in the absence of magnetic field.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Pyro-paraelectric and flexocaloric effects in barium strontium titanate: A first principles approach

Inhomogeneous strain allows the manifestation of an unexplored component of stress-driven caloric effect (flexocaloric effect) and enhanced pyroelectric performance, obtainable significantly beyond the Curie point. A peak temperature change of 1.5 K (at 289 K) was predicted from first-principles-based simulations for Ba{sub 0.5}Sr{sub 0.5}TiO{sub 3} under the application of a strain gradient of 1.5 μm{sup −1}. Additionally, enhanced pyro-paraelectric coefficient (pyroelectric coefficient in paraelectric phase) and flexocaloric cooling 11 × 10{sup −4} C m{sup −2 }K{sup −1} and 1.02 K, respectively, could be obtained (at 330 K and 1.5 μm{sup −1}). A comparative analysis with prevailing literature indicates huge untapped potential and warrants further research.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Electrocaloric Effect in a Lead Magnoniobate–Scandoniobate Relaxor

The electrocaloric effect and also the dielectric, pyroelectric, acoustic, and piezoelectric properties of a lead magnoniobate–scandoniobate solid solution in a biasing electric field have been studied. The dielectric and electromechanical contributions to the pyroelectric and electrocaloric effects are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Relaxor behavior and electrothermal properties of Sn- and Nb-modified (Ba,Ca)TiO 3 Pb-free ferroelectric

Relaxor ferroelectrics have drawn attention for possible applications in solid-state cooling and thermal energy harvesting, owing to their electrothermal energy conversion properties. Here, we have synthesized and characterized the structure–property correlations of a new Sn- and Nb-doped (Ba,Ca)TiO 3 relaxor ferroelectric with large pyroelectric and electrocaloric effects over a broad temperature range. We observed two peaks for the temperature-dependent pyroelectric coefficient: (i) -(∂P/∂T) ~ 563 µC/(m 2 K) at T~ 270 K and (ii) -(∂P/∂T) ~ 1021 µC/(m 2 K) at T~ 320 K. In addition, a broad peak for electrocaloric temperature change is observed near 320 K with a relative cooling power of ~17 J/kg. These properties could be correlated to structural changes observed using X-ray diffraction at two different temperature ranges in the material. Analysis of high-energy X-ray scattering and specific heat capacity data revealed a transition from the cubic to tetragonal phase near T m ~ 320 K, whereas an additional increase in the tetragonality (c/a) of the polar phase is observed below T s ~ 270 K.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Zero-Power Radio Device.

This report describes an unpowered radio receiver capable of detecting and responding to weak signals transmit ted from comparatively long distances . This radio receiver offers key advantages over a short range zero - power radio receiver previously described in SAND2004 - 4610, A Zero - Power Radio Receiver . The device described here can be fabricated as an integrated circuit for use in portable wireless devices, as a wake - up circuit, or a s a stand - alone receiver operating in conjunction with identification decoders or other electroni cs. It builds on key sub - components developed at Sandia National Laboratories over many years. It uses surface acoustic wave (SAW) filter technology. It uses custom component design to enable the efficient use of small aperture antennas. This device uses a key component, the pyroelectric demodulator , covered by Sandia owned U.S. Patent 7397301, Pyroelectric Demodulating Detector [1] . This device is also described in Sandia owned U.S. Patent 97266446, Zero Power Receiver [2].

47 OTHER INSTRUMENTATION↗
DOE OSTI2014

Quantum state specific reactant preparation in a molecular beam by rapid adiabatic passage

Highly efficient preparation of molecules in a specific rovibrationally excited state for gas/surface reactivity measurements is achieved in a molecular beam using tunable infrared (IR) radiation from a single mode continuous wave optical parametric oscillator (cw-OPO). We demonstrate that with appropriate focusing of the IR radiation, molecules in the molecular beam crossing the fixed frequency IR field experience a Doppler tuning that can be adjusted to achieve complete population inversion of a two-level system by rapid adiabatic passage (RAP). A room temperature pyroelectric detector is used to monitor the excited fraction in the molecular beam and the population inversion is detected and quantified using IR bleaching by a second IR-OPO. The second OPO is also used for complete population transfer to an overtone or combination vibration via double resonance excitation using two spatially separated RAP processes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

One-step fabrication of free-standing flexible membranes reinforced with self-assembled arrays of carbon nanotubes

Here, we report on a single step approach for fabricating free-standing polymer membranes reinforced with arrayed self-assembled carbon nanotubes (CNTs). The CNTs are self-assembled spontaneously by electrode-free DC dielectrophoresis based on surface charge templates. The electrical charge template is generated through the pyroelectric effect onto periodically poled lithium niobate ferroelectric crystals. A thermal stimulus enables simultaneously the self-assembly of the CNTs and the cross-linking of the host polymer. Examples of thin polydimethylsiloxane membranes reinforced with CNT patterns are shown.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Giant magnetostriction and nonsaturating electric polarization up to 60 T in the polar magnet $\mathrm{CaBaCo_4O_7}$

Giant magnetostriction in insulating magnetic materials is highly required for applications but is rarely observed. Here we show that giant magnetostriction (> 1500 ppm) can be achieved in an insulating transition metal oxide CaBaCo 4 O 7 where the ferrimagnetic ordering at T c ~ 62K is associated with a huge change in the lattice. Moreover, because this material is pyroelectric with a nonswitchable electric polarization (P), the giant magnetostriction results in a pronounced magnetoelectric effect—a huge change of electric polarization (ΔP ~ 1.6μC/cm 2 ) in response to the applied magnetic field up to 60 T. Geometric frustration as well as the orbital instability of Co 2+ /Co 3+ ions is believed to play a crucial role in the giant magnetostriction. Here our study provides insights on how to achieve both giant magnetostriction and pronounced magnetoelectric effect in insulating transition metal oxides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Piezosuperconductivity: Novel effects in noncentrosymmetric superconductors

Here we study effects in noncentrosymmetric superconductors arising from their unique coupling of Cooper-pair condensate and elasticity. We show that although the much discussed Lifshitz coupling is not observable in a uniform bulk state, it strikingly endows dislocations with a fractional magnetic flux. We also predict a generation of voltage-free strain by a DC current in a P- and T-breaking Josephson junction. Viewing superconductors through the lens of higher-form symmetries we identify the Lifshitz coupling as a chemical potential for the approximately conserved winding number, drawing an analogy with pyroelectric insulators.

36 MATERIALS SCIENCE↗
DOE OSTI2018

A Charge Sensitive Pre-Amplifier for Smart Point-of-Care Devices Employing Polymer Based Lab-on-a-Chip

With increasing emphasis on implantable and portable medical devices, low-power, small-chip-area sensor readout system realized in lab-on-a-chip (LOC) platform is gaining more and more importance these days. The main building blocks of the LOC system include a front-end transducer that generates an electrical signal in response to the presence of an analyte of interest, signal processing electronics to process the signal to comply with a specific transmission protocol and a low-power transmitter, all realized in a single integrated circuit platform. Low power consumption and compactness of the components are essential requirements of the LOC system. This paper presents a novel charge sensitive pre-amplifier developed in a standard 180-nm CMOS process suitable for implementing in an LOC platform. The pre-amplifier converts the charge generated by a pyroelectric transducer into a voltage signal, which provides a measurement of the temperature variation in biological fluids. The proposed design is capable of providing 0.8-mV/pC gain while consuming only 2.1 μW of power. Finally, the pre-amplifier composed of integrated components occupies an area of 0.038 mm 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2018

A Review on Low-Grade Thermal Energy Harvesting: Materials, Methods and Devices

Combined rejected and naturally available heat constitute an enormous energy resource that remains mostly untapped. Thermal energy harvesting can provide a cost-effective and reliable way to convert available heat into mechanical motion or electricity. This extensive review analyzes the literature covering broad topical areas under solid-state low temperature thermal energy harvesting. These topics include thermoelectricity, pyroelectricity, thermomagneticity, and thermoelasticity. For each topical area, a detailed discussion is provided comprising of basic physics, working principle, performance characteristics, state-of-the-art materials, and current generation devices. Technical advancements reported in the literature are utilized to analyze the performance, identify the challenges, and provide guidance for material and mechanism selection. The review provides a detailed analysis of advantages and disadvantages of each energy harvesting mechanism, which will provide guidance towards designing a hybrid thermal energy harvester that can overcome various limitations of the individual mechanism.

36 MATERIALS SCIENCE↗