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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Origins of Electrostriction in Poly(vinylidene fluoride)-Based Ferroelectric Polymers

Although electrostriction is ubiquitous for dielectric polymers, giant electrostriction has not been observed until relaxor ferroelectric (RFE) poly(vinylidene fluoride) (PVDF)-based polymers are achieved. However, the exact origin for giant electrostriction in these polymers has not been fully understood. By studying the electrostriction in the uniaxially stretched films of a ferroelectric poly(VDF-co-trifluoroethylene) [P(VDF-TrFE)] random copolymer and an RFE poly(VDF-co-TrFE-co-chlorotrifluoroethylene) [P(VDF-TrFE-CTFE)] random terpolymer in this work, we confirmed that ferroelectric switching with large hysteresis, such as in the case of P(VDF-TrFE), was not genuine electrostriction. By decreasing large ferroelectric domains to the nanometer scale (i.e., 2–3 nm), such as in the case of the P(VDF-TrFE-CTFE) terpolymer, electrostriction with low hysteresis could be achieved. Here, two origins of the large electrostriction in these polymers were identified. The first was the mechano-electrostriction due to the poling field-induced conformation transformation of oriented polymer chains. The second was the electric repulsion of electrically aligned nanodomains. These effects could occur in both crystals and the oriented amorphous fraction, which links between the nanocrystals and the isotropic amorphous fraction. When the poling field was relatively low (e.g., <40 MV/m), the mechano-electrostriction was the major contribution and the electric repulsion effect was a minor contribution to electrostriction. Meanwhile, a strong temperature dependence of the low-field electrostriction coefficient was observed. Finally, we found an empirical inverse relationship between the electrostriction coefficient and the product of Young’s modulus and dielectric constant. The knowledge obtained from this study provides an insightful understanding of the electrostriction mechanism in PVDF-based electroactive polymers, which will find potential applications in sensors and actuators for wearable electronics and soft robotics.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Mesophase Structure-Enabled Electrostrictive Property in Nylon-12-Based Poly(ether- block -amide) Copolymers

In this work, to search for alternative electrostrictive polymers and to understand the underlying mechanism, the structure-ferroelectric/electrostrictive property relationship for nylon-12-based poly(ether-b-amide) multiblock copolymers (PEBAX) is investigated. Two PEBAX samples are studied, namely, P6333 and P7033 with 37 and 25 mol.% of soft poly(tetramethylene oxide) (PTMO) blocks, respectively. In both samples, poorly hydrogen-bonded mesophase facilitates electric field-induced ferroelectric switching. Meanwhile, the longitudinal electrostrictive strain (S 1 )–electric field (E) loops are obtained at 2 Hz. Different from conventional poly(vinylidene fluoride-co-trifluoroethylene) [P(VDF-TrFE)]-based terpolymers, uniaxially stretched nylon-12-based PEBAX samples exhibit negative S 1 , that is, shrinking rather than elongation in the longitudinal direction. Additionally, this is attributed to the unique conformation transformation of nylon-12 crystals during ferroelectric switching. Namely, at a zero electric field, crystalline nylon-12 chains adopt a more or less antiparallel arrangement of amide groups. Upon high-field poling, ferroelectric domains are enforced with more twisted chains adopting a parallel arrangement of amide groups. Meanwhile, extensional S 1 is observed for P6333 at electric fields above 150 MV m -1 . This is attributed to the elongation of the amorphous phases (i.e., amorphous nylon-12 and PTMO). Therefore, competition between shrinking S 1 from mesomorphic nylon-12 crystals (i.e., nanoactuation) and elongational S 1 from amorphous phases determines the ultimate electrostriction behavior in stretched PEBAX films.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Giant Electrostriction via Nanodomain Engineering in Relaxor Ferroelectric Polymers

Relaxor ferroelectric (RFE) polymers hold great promise for artificial muscles due to their high actuation strain, high loading stress, and fast response. However, the structural origin underlying their large electrostrictive deformation remains elusive. In this study, we investigate poly(vinylidene fluoride-co-trifluoroethylene) [P(VDF-TrFE)]-based RFE terpolymers, incorporating 1,1-chlorofluoroethylene (CFE) or chlorotrifluoroethylene (CTFE) (the terpolymers are denoted as terP-CFE and terP-CTFE, respectively) as termonomers. Although both terpolymers show similar semicrystalline morphology, drastically different electrostrictive properties are observed. Specifically, the terP-CFE annealed at 100 °C achieves a record-high transverse strain of ∼10.6%, whereas 100 °C-annealed terP-CTFE only shows a much lower actuation strain of ∼4.2% at the same poling field of 190 MV/m. To elucidate the origin of this difference, time-resolved wide-angle X-ray diffraction, small-angle X-ray scattering, and Fourier transform infrared experiments are performed during in situ electric poling. An RFE-to-ferroelectric (FE) crystal phase transition is observed for terP-CFE but is absent for terP-CTFE. Beyond the contribution of the crystalline phase, the oriented amorphous fraction and crystalline defects (e.g., taut-tie molecules) also play significant roles in enhancing electrostriction. In conclusion, this mechanistic insight provides a valuable foundation for the rational design of next-generation RFE polymers with tunable properties through defect engineering of their semicrystalline structures.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Correlated Displacement of Dynamic Elastic Dipoles Produces Nonclassical Electrostriction in Zr-Doped Ceria

By combining experimental data with density functional theory-based ab initio molecular dynamics modeling, this work provides evidence that nonclassical electrostriction in isovalent Zr-doped ceria is due to the correlated anharmonic motion of dynamic elastic dipoles associated with multiple [ZrO 8 ]-local bonding units with a high Zr concentration (Zr 0.1 Ce 0.9 O 2 ). Introduction of 0.5 mol % trivalent or divalent codopants (Sc, Yb, La, or Ca) reduces the longitudinal electrostriction strain coefficient by more than a factor of 10, produces a 3-fold decrease in the relative dielectric permittivity, and increases the elastic modulus. Since these changes depend neither on the radius nor on the valency of the codopant, we conclude that the responsible species are charge-compensating oxygen vacancies (VO). For trivalent dopants (Do 0.005 Zr 0.1 Ce 0.895 O 1.9975 ), oxygen vacancies are present at a concentration ratio 1:40 with respect to Zr, giving, for random distribution, a characteristic interaction distance of ≤2.3 unit cells (1.2 nm). Oxygen vacancies participate in [ZrO 7 -V O ] local bonding units, disrupting the correlated dynamic displacements of the connected [ZrO 8 ]-local bonding units. Finally, such correlated motion of dynamic elastic dipoles may also explain the exponential increase in the longitudinal electrostriction strain coefficient with an increase in Zr concentration to <0.2 mole fraction and must be taken into account for further development of nonclassical electrostrictors based on Zr-doped ceria.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Lead-free Zr-doped ceria ceramics with low permittivity displaying giant electrostriction

Electrostrictors, materials developing mechanical strain proportional to the square of the applied electric field, present many advantages for mechanical actuation as they convert electrical energy into mechanical, but not vice versa. Both high relative permittivity and reliance on Pb as the key component in commercial electrostrictors pose serious practical and health problems. Here we describe a low relative permittivity (<250) ceramic, Zr x Ce 1-x O 2 (x < 0.2), that displays electromechanical properties rivaling those of the best performing electrostrictors: longitudinal electrostriction strain coefficient ~10 -16 m 2 /V 2 ; relaxation frequency ≈ a few kHz; and strain ≥0.02%. Combining X-ray absorption spectroscopy, atomic-level modeling and electromechanical measurements, here we show that electrostriction in Zr x Ce 1-x O 2 is enabled by elastic dipoles produced by anharmonic motion of the smaller isovalent dopant (Zr). Unlike the elastic dipoles in aliovalent doped ceria, which are present even in the absence of an applied elastic or electric field, the elastic dipoles in Zr x Ce 1-x O 2 are formed only under applied anisotropic field. The local descriptors of electrostrictive strain, namely, the cation size mismatch and dynamic anharmonicity, are sufficiently versatile to guide future searches in other polycrystalline solids.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Improved ferroelectric, piezoelectric and electrostrictive properties of dense BaTiO{sub 3} ceramic

The ferroelectric, piezoelectric and electrostrictive properties of BaTiO{sub 3} (BT) dense ceramic synthesized by solid-state reaction were investigated. X-ray diffraction study confirmed tetragonal crystal structure having c/a ~1.0144. The dense microstructure was evidenced from morphological studies with an average grain size ~7.8 µm. Temperature dependent dielectric measurement showed the maximum values of dielectric constant, ε{sub r} = 5617 at Curie temperature, T{sub c} = 125 °C. The saturation and remnant polarization, P{sub sat.} = 24.13 µC/cm{sup 2} and P{sub r} =10.42 µC/cm{sup 2} achieved respectively for the first time with lower coercive field of E{sub c}=2.047 kV/cm. The polarization current density-electric field measurement exhibits the peaking characteristics, confirms the saturation state of polarization for BT. The strain-electric field measurements revealed the “sprout” shape nature instead of typical “butterfly loop”. This shows the excellent converse piezoelectric response with remnant strain ~ 0.212% and converse piezoelectric constant d*{sub 33} ~376.35 pm/V. The intrinsic electrostrictive coefficient was deduced from the variation of strain with polarization with electrostrictive coefficient Q{sub 33}~ 0.03493m{sup 4}/C{sup 2}.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Characterizing Hygroscopic Films of Polyzwitterions in Electric Fields Using Neutron and X-ray Reflectometries: Electrostriction or Mass Loss?

Herein we study responses of thermally annealed ultrathin films deposited on silicon substrates and containing polyzwitterions to applied electric fields by using specular neutron reflectometry (NR). In particular, we applied 7 kV under vacuum at 150 °C on the films containing poly(1-(3-sulfonatopropyl)-2-vinylpyridinium) (P2VPPS) and its blends with either a deuterated ionic liquid (EMIMBF 4 - d 11 ), potassium bromide (KBr), or deuterated sodium polystyrenesulfonate (NaPSS-d 7 ). The voltage was applied over an air gap, and the in situ neutron reflectivity measurements allowed us to measure changes in the films. In all the cases, we measured decreases in thicknesses of the films, which varied up to ~8% depending on the added salt. Posteriori X-ray reflectivity (XRR) measurements on the same films at room temperature reveal that these films were highly hygroscopic, which led to the presence of water in these films. Analysis of the NR and the XRR revealed that the decrease in the thickness of the films in the neutron reflectivity experiments on heating resulted from the loss of water and the ionic liquid but not from electrostrictive effects. The in situ NR and posteriori XRR experiments revealed not only the hygroscopic nature of these films but also depth-resolved structural rearrangements due to the applied electric fields in the films containing electrolytes and polyelectrolytes. This work shows that a combination of NR and XRR can be used to distinguish between mass loss and electrostriction in films containing charged polymers such as polyzwitterions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

CO 2 solubility in aqueous solutions containing Na + , Ca 2+ , Cl - , SO 4 2- and HCO 3 - : The effects of electrostricted water and ion hydration thermodynamics

Dissolution of CO 2 into deep subsurface brines for carbon sequestration is regarded as one of the few viable means of reducing the amount of CO 2 entering the atmosphere. Ions in solution partially control the amount of CO 2 that dissolves, but the mechanisms of the ion's influence are not clearly understood and thus CO 2 solubility is difficult to predict. Here in this study, CO 2 solubility was experimentally determined in water, NaCl, CaCl 2 , Na 2 SO 4 , and NaHCO 3 solutions and a mixed brine similar to the Bravo Dome natural CO 2 reservoir; ionic strengths ranged up to 3.4 molal, temperatures to 140 °C, and CO 2 pressures to 35.5 MPa. Increasing ionic strength decreased CO 2 solubility for all solutions when the salt type remained unchanged, but ionic strength was a poor predictor of CO 2 solubility in solutions with different salts. A new equation was developed to use ion hydration number to calculate the concentration of electrostricted water molecules in solution. Dissolved CO 2 was strongly correlated (R 2 = 0.96) to electrostricted water concentration. Strong correlations were also identified between CO 2 solubility and hydration enthalpy and hydration entropy. These linear correlation equations predicted CO 2 solubility within 1% of the Bravo Dome brine and within 10% of two mixed brines from literature (a 10 wt % NaCl + KCl + CaCl 2 brine and a natural Na + , Ca 2+ , Cl - type brine with minor amounts of Mg 2+ , K + , Sr 2+ and Br - ).

58 GEOSCIENCES↗
DOE OSTI2018

Giant thermally-enhanced electrostriction and polar surface phase in L a 2 M o 2 O 9 oxygen ion conductors

Ferroelectrics possess spontaneous electric polarization at macroscopic scales which nonetheless imposes strict limitations on the material classes. Recent discoveries of untraditional symmetry-breaking phenomena in reduced material dimensions have indicated feasibilities to extend polar properties to broader types of materials, potentially opening up the freedom for designing materials with hybrid functionalities. Here in this paper, we report the unusual electromechanical properties of La 2 Mo 2 O 9 (LAMOX) oxygen ion conductors, systematically investigated at both bulk and surface length levels. We first observed giant electrostriction effects in La 2 Mo 2 O 9 bulk ceramics that are thermally enhanced in concert with their low-energy oxygen-vacancy hopping dynamics. Moreover, while no clear bulk polarization was detected, the surface phases of LAMOX were found to be manifestly polar, likely originating from the coupling between the intrinsic structural flexibilities with strain gradients (i.e., flexoelectricity) and/or chemical heterogeneities present in the materials. These findings identify La 2 Mo 2 O 9 as a promising electromechanical material system and suggest that the flexible structural and chemical configurations in ionically active materials could enable fundamentally different venues to accommodate electric polarization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Stress-induced phase transitions in nanoscale CuInP 2 S 6

Using the Landau-Devonshire approach and available experimental results, we constructed multiwell thermodynamic potential of the layered ferroelectric CuInP 2 S 6 (CIPS). The analysis of temperature dependences of the dielectric permittivity and lattice constants for different applied pressures unexpectedly reveals the critically important role of a nonlinear electrostriction in this material. With the nonlinear electrostriction included we calculated the temperature and pressure phase diagrams and spontaneous polarization of a bulk CIPS, within the assumed range of applicable temperatures and applied pressures. Using the developed thermodynamic potential, we revealed the strain-induced phase transitions in thin epitaxial СIPS films, as well as the stress-induced phase transitions in СIPS nanoparticles, the shape of which varies from prolate needles to oblate disks. Furthermore, w also revealed the strong influence of a mismatch strain, elastic stress, and shape anisotropy on the phase diagrams and polar properties of a nanoscale CIPS, and derived analytical expressions allowing for elastic control of the nanoscale CIPS polar properties. Hence obtained results can be of particular interest for the strain engineering of nanoscale layered ferroelectrics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Enhanced Curie temperature and piezoelectric properties of (Ba0.85Ca0.15)(Zr0.10Ti0.90)O3 lead-free ceramics after the addition of LiTaO3

Highlights: • The Curie temperature and piezoelectric properties of BCZT ceramics can be obviously enhanced by the addition of LiTaO{sub 3}. • The Curie temperature of (Ba{sub 0.85}Ca{sub 0.15})(Zr{sub 0.10}Ti{sub 0.90})O{sub 3} ceramics improved from 93 ℃ to 102 ℃. • (Ba{sub 0.85}Ca{sub 0.15})(Zr{sub 0.10}Ti{sub 0.90})O{sub 3} ceramic with x = 0.3 mol.% LiTaO{sub 3} demonstrates optimal piezoelectric properties. • The giant electrostrictive coefficients (Q{sub 33} ≈ 0.040-0.050 m{sup 4}/C{sup 2}) were also obtained in LT-doped BCZT ceramics. - Abstract: Polycrystalline (Ba{sub 0.85}Ca{sub 0.15})(Zr{sub 0.10}Ti{sub 0.90})O{sub 3}–xLiTaO{sub 3} ceramics were designed and synthesized using a solid-state reaction to improve both the Curie temperature and the electrical properties of (Ba{sub 0.85}Ca{sub 0.15})(Zr{sub 0.10}Ti{sub 0.90})O{sub 3} lead-free piezoelectric ceramics. The effect that the addition of LiTaO{sub 3} has on the structure and electrical properties of BCZT ceramics was studied systemically. The results show that the Curie temperature and the piezoelectric properties of BCZT can be substantially enhanced by adding LiTaO{sub 3.} The Curie temperature increased from 93 °C to 102 °C after adding LT of 0.3 mol.%. X-ray diffraction and Raman spectral analysis of the ceramics reveal the coexistence of orthorhombic (O) and tetragonal (T) phases. This coexistence of O and T phases at room temperature helps improve the ferroelectric and piezoelectric properties. The ceramic with x = 0.3 mol.% exhibits the highest values for d{sub 33} = 433 pC/N, d{sub 33}{sup *} = 858 pm/V (at 1 kV/mm) and k{sub p} = 44.6%. Furthermore, giant electrostrictive coefficients (Q{sub 33} ≈ 0.040–0.050 m{sup 4}/C{sup 2}) were also obtained for these LT-doped BCZT ceramics. These properties confirm that BCZT-xLT is a promising candidate system for lead-free piezoelectric ceramic materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Role of Solvent Rearrangement on Mg2+ Solvation Structures in Dimethoxyethane Solutions Using Multimodal NMR Analysis

One of the main impediments faced for predicting important emergent properties of a multivalent electrolyte (such as conductivity and electrochemical stability) is the lack of quantitative analysis of ion-ion and ion-solvent interactions, which manifest in solvation structures and dynamics. In particular, the role of ion-solvent interactions is still unclear in cases where the strong electric field from multivalent cations can influence structural evolution of lower permittivity organic solvent molecules on solvation structure. These influences are commonly refered to as electrostriction pheonmena. Using quantitative 1H, 19F, 17O, and 25Mg NMR together with 19F nuclear spin relaxation and diffusion measurments, we find an unusual correlation between ion concentration and solvation structure of Mg(TFSI)2 salt in dimethoxyethane (DME) solution. The domiant solvation structure evolves from contact ion pairs (i.e. [Mg(TFSI)(DME)1-2]+) to fully solvated clusters (i.e. [Mg(DME)3]2+) as salt concentration increases or as temperature decreases. This transition is coupled to a phase separation, which we study here between 0.06 M and 0.36 M. Subsequent analysis is based on an explanation of the electrostriction phenomena and the competion between solvent molecules and TFSI anions for cation coordination.

Chen, Ying↗
DOE OSTI2020

Piezoresponse amplitude and phase quantified for electromechanical characterization

Piezoresponse force microscopy (PFM) is a powerful characterization technique to readily image and manipulate the ferroelectric domains. PFM gives an insight into the strength of local piezoelectric coupling and polarization direction through PFM amplitude and phase, respectively. Converting measured arbitrary units into units of effective piezoelectric constant remains a challenge, and insufficient methods are often used. While most quantification efforts have been spent on quantifying the PFM amplitude signal, little attention has been given to the PFM phase, which is often arbitrarily adjusted to fit expectations. This is problematic when investigating materials with unknown or negative sign of the probed effective electrostrictive coefficient or strong frequency dispersion of electromechanical responses, because assumptions about the PFM phase cannot be reliably made. The PFM phase can, however, provide important information on the polarization orientation and the sign of the effective electrostrictive coefficient probed by PFM. Most notably, the orientation of the PFM hysteresis loop is determined by the PFM phase. Moreover, when presenting PFM data as a combined signal, the resulting response can be artificially lowered or asymmetric if the phase data have not been correctly processed. Here, we explain the PFM amplitude quantification process and demonstrate a path to identify the phase offset required to extract correct meaning from the PFM phase data. We explore different sources of phase offsets including the experimental setup, instrumental contributions, and data analysis. We discuss the physical working principles of PFM and develop a strategy to extract physical meaning from the PFM amplitude and phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗