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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 1,531 records · Page 85
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Influence of chemical disorder on energy dissipation and defect evolution in advanced alloys

We report that historically, alloy development with better radiation performance has been focused on traditional alloys with one or two principal element(s) and minor alloying elements, where enhanced radiation resistance depends on microstructural or nanoscale features to mitigate displacement damage. In sharp contrast to traditional alloys, recent advances of single-phase concentrated solid solution alloys (SP-CSAs) have opened up new frontiers in materials research. In these alloys, a random arrangement of multiple elemental species on a crystalline lattice results in disordered local chemical environments and unique site-to-site lattice distortions. Based on closely integrated computational and experimental studies using a novel set of SP-CSAs in a face-centered cubic structure, we have explicitly demonstrated that increasing chemical disorder can lead to a substantial reduction in electron mean free paths, as well as electrical and thermal conductivity, which results in slower heat dissipation in SP-CSAs. The chemical disorder also has a significant impact on defect evolution under ion irradiation. Considerable improvement in radiation resistance is observed with increasing chemical disorder at electronic and atomic levels. Finally, the insights into defect dynamics may provide a basis for understanding elemental effects on evolution of radiation damage in irradiated materials and may inspire new design principles of radiation-tolerant structural alloys for advanced energy systems.

36 MATERIALS SCIENCE↗
DOE OSTI2016

The enhancement in dielectric and magnetic property in Na and Mn co substituted lanthanum ferrite

Nanocrystalline solid solutions of La{sub 1-x}Na{sub x}Fe{sub 1-y}Mn{sub y}O{sub 3} (x=y=0.00 and 0.25) were prepared via modified Pechini route. No evidence of secondary or impurity phase has been detected up to the detection of error limit of high power X-ray diffractometer. Dielectric property of the samples has been investigated in the frequency range 100 Hz-4MHz at temperature ranging 300–450K. The value of relative permittivity (ε{sub r}) increases drastically and shows colossal dielectric response (∼10{sup 4}) by cosubstitution of Na and Mn as compared to pure LaFeO{sub 3}. Dielectric relaxation peak in loss tangent in both samples have been found and shift towards higher frequency region as temperature increases. Magnetization-Field (M-H) loop of the calcined sample have been recorded at room temperature (300K) at field ±60kOe. Magnetic property also enhanced by co substitution of Na and Mn. The change in Fe/Mn-O-Fe/Mn angle by co-substitution of Na and Mn in LaFeO{sub 3} and indirect exchange interaction between two different magnetic sub lattices Fe and Mn might be responsible for drastic change. Saturation/maximum magnetic moment increase ∼four times in LNFM25 (5.335emu/g) as compared to pure LaFeO{sub 3} (1.302emu/g).

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Contrasting SnTe–NaSbTe 2 and SnTe–NaBiTe 2 Thermoelectric Alloys: High Performance Facilitated by Increased Cation Vacancies and Lattice Softening

Defect chemistry is critical to designing high performance thermoelectric materials. In SnTe, the naturally large density of cation vacancies results in excessive hole doping and frustrates the ability to control the thermoelectric properties. Yet, recent work also associates the vacancies with suppressed sound velocities and low lattice thermal conductivity, underscoring the need to understand the interplay between alloying, vacancies, and the transport properties of SnTe. Here, we report solid solutions of SnTe with NaSbTe 2 and NaBiTe 2 (NaSn m SbTe m +2 and NaSn m BiTe m +2 , respectively) and focus on the impact of the ternary alloys on the cation vacancies and thermoelectric properties. We find introduction of NaSbTe 2 , but not NaBiTe 2 , into SnTe nearly doubles the natural concentration of Sn vacancies. Furthermore, DFT calculations suggest that both NaSbTe 2 and NaBiTe 2 facilitate valence band convergence and simultaneously narrow the band gap. These effects improve the power factors but also make the alloys more prone to detrimental bipolar diffusion. Indeed, the performance of NaSn m BiTe m +2 is limited by strong bipolar transport and only exhibits modest maximum ZTs ≈ 0.85 at 900 K. In NaSn m SbTe m +2 however, the doubled vacancy concentration raises the charge carrier density and suppresses bipolar diffusion, resulting in superior power factors than those of the Bi-containing analogues. Lastly, NaSbTe 2 incorporation lowers the sound velocity of SnTe to give glasslike lattice thermal conductivities. Facilitated by the favorable impacts of band convergence, vacancy-augmented hole concentration, and lattice softening, NaSn m SbTe m +2 reaches high ZT ≈ 1.2 at 800–900 K and a competitive average ZT avg of 0.7 over 300–873 K. The difference in ZT between two chemically similar compounds underscores the importance of intrinsic defects in engineering high-performance thermoelectrics.

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

Electro-chemo-mechanically Driven Ni Exsolution from (Pr,Ce,Ni)O 2−δ : Controlled Nucleation Density and Enhanced Electrode Kinetics

In situ exsolution of metal nanoparticles is a promising strategy to prepare electrocatalysts with enhanced activity and resistance to agglomeration for efficient chemical transformations and energy conversion. Achieving a high nucleation density of nanoparticles under mild conditions and understanding how to tailor the process is important for performance of these electrodes in electrochemical cells. In this work, we demonstrate facile exsolution of Ni nanoparticles using fluorite-structured (Pr,Ce)O 2−δ as the support oxide, driven by electrochemical potential and aided by the metastability of Ni in the solid solution (elastic driving force). We prepare single-phase oriented thin films of (Pr,Ce,Ni)O 2−δ (NPCO) on (Zr,Y)O 2−δ (YSZ) substrates by pulsed laser deposition. With the aid of a high-throughput electrochemical cell that provides a lateral gradient in Nernst voltage, we apply in situ near-ambient pressure synchrotron X-ray photoelectron spectroscopy and ex situ atomic force microscopy to investigate the impact of electrochemical potential on Ni nucleation density. We find that metallic Ni can be successfully exsolved at 550 °C upon cathodic biasing in 20 mTorr O 2 , and its nucleation density increases with increasing electrochemical driving force/decreasing oxygen chemical potential. We further evaluate the electrochemical performance under highly reducing (fuel electrode) conditions by electrochemical impedance spectroscopy. With the exsolved Ni nanoparticles, the surface exchange coefficient of the NPCO is found to be ∼4× higher than for PCO without exsolution. This work confirms mixed conducting fluorites as beneficial host lattices for facile transition-metal exsolution and suggests the possibility for constructing an all ceria-based electrochemical cell with PCO serving as both the cathode and the anode.

36 MATERIALS SCIENCE↗
DOE OSTI2014

The effects of glass doping, temperature and time on the morphology, composition, and iron redox of spinel crystals

Precipitation of large crystals/agglomerates of spinel and their accumulation in the pour spout riser of a Joule-heated ceramic melter during idling can plug the melter and prevent pouring of molten glass into canisters. Thus, there is a need to understand the effects of spinel-forming components, temperature, and time on the growth of crystals in connection with an accumulation rate. In our study, crystals of spinel [Fe, Ni, Mn, Zn, Sn][Fe, Cr]₂O₄ were precipitated from simulated high-level waste borosilicate glasses containing different concentrations of Ni, Fe, and Cr by heat treating at 850 and 900°C for different times. These crystals were extracted from the glasses and analyzed with scanning electron microscopy and image analysis for size and shape, with inductively coupled plasma-atomic emission spectroscopy and atom probe tomography for concentration of spinel-forming components, and with wet colorimetry and Mössbauer spectroscopy for Fe²⁺/Fe total ratio. High concentrations of Ni, Fe, and Cr in glasses resulted in the precipitation of crystals larger than 100 µm in just two days. Crystals were a solid solution of NiFe₂O₄, NiCr₂O₄, and -Fe₂O₃ (identified only in the high-Ni-Fe glass) and also contained small concentrations of less than 1 at% of Li, Mg, Mn, and Al.

chemical analysis↗
DOE OSTI2020

Phase‐Dependent Band Gap Engineering in Alloys of Metal‐Semiconductor Transition Metal Dichalcogenides

Abstract Bandgap engineering plays a critical role in optimizing the electrical, optical and (photo)‐electrochemical applications of semiconductors. Alloying has been a historically successful way of tuning bandgaps by making solid solutions of two isovalent semiconductors. In this work, a novel form of bandgap engineering involving alloying non‐isovalent cations in a 2D transition metal dichalcogenide (TMDC) is presented. By alloying semiconducting MoSe 2 with metallic NbSe 2 , two structural phases of Mo 0.5 Nb 0.5 Se 2 , the 1T and 2H phases, are produced each with emergent electronic structure. At room temperature, it is observed that the 1T and 2H phases are semiconducting and metallic, respectively. For the 1T structure, scanning tunneling microscopy/spectroscopy (STM/STS) is used to measure band gaps in the range of 0.42–0.58 at 77 K. Electron diffraction patterns of the 1T structure obtained at room temperature show the presence of a nearly commensurate charge density wave (NCCDW) phase with periodic lattice distortions that result in an uncommon 4 × 4 supercell, rotated approximately 4° from the lattice. Density‐functional‐theory calculations confirm that local distortions, such as those in a NCCDW, can open up a band gap in 1T ‐Mo 0.5 Nb 0.5 Se 2 , but not in the 2H phase. This work expands the boundaries of alloy‐based bandgap engineering by introducing a novel technique that facilitates CDW phases through alloying.

Wang, Shuxi↗
DOE OSTI2022

Unprecedented Multifunctionality in 1D Nb 1- x Ta x S 3 Transition Metal Trichalcogenide Alloy

One-dimensional (1D) van der Waals materials, such as nanofibers or nanoribbons are considered as the future ultimate limit of downscaling for modern electrical and electrochemical devices. Here, for the first time, we successfully synthesize nanofibers of a solid solution transition metal trichalcogenide (TMTC), Nb 1-x Ta x S 3 , with outstanding electrical, thermal, and electrochemical characteristics rivaling the performance of the-state-of-the art materials for each application. This material shows nearly unchanged sheet resistance (≈740 Ω/sq -1 ) versus bending cycles tested up to 90 cycles, stable sheet resistance in ambient conditions tested up to 60 days, remarkably high electrical breakdown current density of ≈ 30 MA cm -2 , strong evidence of successive charge density wave (CDW) transitions, and outstanding thermal stability up to ≈900 K. Additionally, this material demonstrates excellent activity and selectivity for CO2 conversion to CO reaching ≈ 350 mA cm -2 at – 0.8 V vs RHE with an outstanding turnover frequency number of 25 for CO formation. It also exhibits an excellent performance in a high-rate Li-air battery with the specific capacity of 3000 mAhg -1 at a high current density of 0.3 mAcm -2 . This study uncovers the multifunctionality in 1D TMTC alloys for a wide range of high-impact applications and opens a new direction for the design of the next generation of low-dimensional materials with high performance.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Lattice-Distortion-Enhanced Yield Strength in a Refractory High-Entropy Alloy

Severe distortion is one of the four core effects in single-phase high-entropy alloys (HEAs) and contributes significantly to the yield strength. However, the connection between the atomic-scale lattice distortion and macro-scale mechanical properties through experimental verification has yet to be fully achieved, owing to two critical challenges: 1) the difficulty in the development of homogeneous single-phase solid-solution HEAs and 2) the ambiguity in describing the lattice distortion and related measurements and calculations. Here, a single-phase body-centered-cubic (BCC) refractory HEA, NbTaTiVZr, using thermodynamic modeling coupled with experimental verifications, is developed. Compared to the previously developed single-phase NbTaTiV HEA, the NbTaTiVZr HEA shows a higher yield strength and comparable plasticity. The increase in yield strength is systematically and quantitatively studied in terms of lattice distortion using a theoretical model, first-principles calculations, synchrotron X-ray/neutron diffraction, atom-probe tomography, and scanning transmission electron microscopy techniques. These results demonstrate that severe lattice distortion is a core factor for developing high strengths in refractory HEAs.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Enhancing the Reversibility of Lattice Oxygen Redox Through Modulated Transition Metal–Oxygen Covalency for Layered Battery Electrodes

Utilizing reversible lattice oxygen redox (OR) in battery electrodes is an essential strategy to overcome the capacity limitation set by conventional transition metal redox. However, lattice OR reactions are often accompanied with irreversible oxygen oxidation, leading to local structural transformations and voltage/capacity fading. Herein, it is proposed that the reversibility of lattice OR can be remarkably improved through modulating transition metal-oxygen covalency for layered electrode of Na-ion batteries. By developing a novel layered P2-Na 0.6 Mg 0.15 Mn 0.7 Cu 0.15 O 2 electrode, it is demonstrated that the highly electronegative Cu dopants can improve the lattice OR reversibility to 95% compared to 73% for Cu-free counterpart, as directly quantified through high-efficiency mapping of resonant inelastic X-ray scattering. Crucially, the large energetic overlap between Cu 3d and O 2p states dictates the rigidity of oxygen framework, which effectively mitigates the structural distortion of local oxygen environment upon (de)sodiation and leads to the enhanced lattice OR reversibility. The electrode also exhibits a completely solid-solution reaction with an ultralow volume change of only 0.45% and a reversible metal migration upon cycling, which together ensure the improved electrochemical performance. Finally, these results emphasize the critical role of transition metal-oxygen covalency for enhancing the reversibility of lattice OR toward high-capacity electrodes employing OR chemistry.

25 ENERGY STORAGE↗
DOE OSTI2022

Strain‐Driven Mixed‐Phase Domain Architectures and Topological Transitions in Pb 1− x Sr x TiO 3 Thin Films

Abstract The potential for creating hierarchical domain structures, or mixtures of energetically degenerate phases with distinct patterns that can be modified continually, in ferroelectric thin films offers a pathway to control their mesoscale structure beyond lattice‐mismatch strain with a substrate. Here, it is demonstrated that varying the strontium content provides deterministic strain‐driven control of hierarchical domain structures in Pb 1− x Sr x TiO 3 solid‐solution thin films wherein two types, c / a and a 1 / a 2 , of nanodomains can coexist. Combining phase‐field simulations, epitaxial thin‐film growth, detailed structural, domain, and physical‐property characterization, it is observed that the system undergoes a gradual transformation (with increasing strontium content) from droplet‐like a 1 / a 2 domains in a c / a domain matrix, to a connected‐labyrinth geometry of c / a domains, to a disconnected labyrinth structure of the same, and, finally, to droplet‐like c / a domains in an a 1 / a 2 domain matrix. A relationship between the different mixed‐phase modulation patterns and its topological nature is established. Annealing the connected‐labyrinth structure leads to domain coarsening forming distinctive regions of parallel c / a and a 1 / a 2 domain stripes, offering additional design flexibility. Finally, it is found that the connected‐labyrinth domain patterns exhibit the highest dielectric permittivity.

Kavle, Pravin↗
DOE OSTI2023

Engineering Relaxor Behavior in (BaTiO 3 ) n /(SrTiO 3 ) n Superlattices

Complex-oxide superlattices provide a pathway to numerous emergent phenomena because of the juxtaposition of disparate properties and the strong interfacial interactions in these unit-cell-precise structures. This is particularly true in superlattices of ferroelectric and dielectric materials, wherein new forms of ferroelectricity, exotic dipolar textures, and distinctive domain structures can be produced. Here, in this study, relaxor-like behavior, typically associated with the chemical inhomogeneity and complexity of solid solutions, is observed in (BaTiO 3 ) n /(SrTiO 3 ) n (n = 4–20 unit cells) superlattices. Dielectric studies and subsequent Vogel–Fulcher analysis show significant frequency dispersion of the dielectric maximum across a range of periodicities, with enhanced dielectric constant and more robust relaxor behavior for smaller period n. Bond-valence molecular-dynamics simulations predict the relaxor-like behavior observed experimentally, and interpretations of the polar patterns via 2D discrete-wavelet transforms in shorter-period superlattices suggest that the relaxor behavior arises from shape variations of the dipolar configurations, in contrast to frozen antipolar stripe domains in longer-period superlattices (n = 16). Moreover, the size and shape of the dipolar configurations are tuned by superlattice periodicity, thus providing a definitive design strategy to use superlattice layering to create relaxor-like behavior which may expand the ability to control desired properties in these complex systems.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Tuning the Spin Transition and Carrier Type in Rare-Earth Cobaltates via Compositional Complexity

There is growing interest in material candidates with properties that can be engineered beyond traditional design limits. Compositionally complex oxides (CCO), often called high entropy oxides, are excellent candidates, wherein a lattice site shares more than four cations, forming single-phase solid solutions with unique properties. However, the nature of compositional complexity in dictating properties remains unclear, with characteristics that are difficult to calculate from first principles. Here, in this study, compositional complexity is demonstrated as a tunable parameter in a spin-transition oxide semiconductor La 1- x (Nd, Sm, Gd, Y) x/4 CoO 3 , by varying the population x of rare earth cations over 0.00≤ x≤ 0.80. Across the series, increasing complexity is revealed to systematically improve crystallinity, increase the amount of electron versus hole carriers, and tune the spin transition temperature and on-off ratio. At high a population (x = 0.8), Seebeck measurements indicate a crossover from hole-majority to electron-majority conduction without the introduction of conventional electron donors, and tunable complexity is proposed as new method to dope semiconductors. First principles calculations combined with angle resolved photoemission reveal an unconventional doping mechanism of lattice distortions leading to asymmetric hole localization over electrons. Thus, tunable complexity is demonstrated as a facile knob to improve crystallinity, tune electronic transitions, and to dope semiconductors beyond traditional means.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Control of Two Solid Electrolyte Interphases at the Negative Electrode of an Anode‐Free All Solid‐State Battery based on Argyrodite Electrolyte

Abstract Anode‐free all solid‐state batteries (AF‐ASSBs) employ “empty” current collector with three active interfaces that determine electrochemical stability; lithium metal – Solid electrolyte (SE) interphase (SEI‐1), lithium – current collector interface, and collector – SE interphase (SEI‐2). Argyrodite Li 6 PS 5 Cl (LPSCl) solid electrolyte (SE) displays SEI‐2 containing copper sulfides, formed even at open circuit. Bilayer of 140 nm magnesium/30 nm tungsten (Mg/W‐Cu) controls the three interfaces and allows for state‐of‐the‐art electrochemical performance in half‐cells and fullcells. AF‐ASSB with NMC811 cathode achieves 150 cycles with Coulombic efficiency (CE) above 99.8%. With high mass‐loading cathode (8.6 mAh cm −2 ), AF‐ASSB retains 86.5% capacity after 45 cycles at 0.2C. During electrodeposition of Li, gradient Li‐Mg solid solution is formed, which reverses upon electrodissolution. This promotes conformal wetting/dewetting by Li and stabilizes SEI‐1 by lowering thermodynamic driving force for SE reduction. Inert refractory W underlayer is required to prevent ongoing formation of SEI‐2 that also drives electrochemical degradation. Inert Mo and Nb layers likewise protect Cu from corroding, while Li‐alloying layers (Mg, Sn) are less effective due to ongoing volume changes and associated pulverization. Mechanistic explanation for observed Li segregation within alloying Li x Mg layer is provided through mesoscale modelling, considering opposing roles of diffusivity differences and interfacial stresses.

Wang, Yixian [Materials Science and Engineering Pr↗
DOE OSTI2025

Creating Favorable Pt/Co Interfaces via a Two‐Step Approach for Constructing Highly Durable PtCo Intermetallic Fuel Cell Catalysts

Structurally ordered PtCo intermetallics are one of the most promising oxygen-reduction catalysts in proton exchange membrane fuel cells (PEMFCs) due to their intrinsically improved catalytic activity and stability relative to PtCo solid-solution alloys. However, increasing the heating temperature to achieve a desirable high degree of ordering results in severe particle agglomeration and low mass activity and stability. Herein, a two-step synthesis approach is developed to create an L1 2 -Pt 3 Co intermetallic structure with an increased ordering degree and well-dispersed ultrafine particles. The first step of the synthesis yields ultrafine Pt nanoparticles that are well-dispersed on the ZIF-8-derived carbon support. The second adsorption step enables us to fine-tune the Pt and Co interfaces, assisted by optimal amino acids, to establish a favorable Co-rich environment around fine Pt nanoparticles, facilitating Co diffusion into the Pt crystalline under mild thermal conditions (<800 °C). In conclusion, this two-step ordered L1 2 -Pt 3 Co catalyst is systematically evaluated using membrane electrode assemblies under heavy-duty vehicle (HDV) conditions and demonstrated exceptional performance and durability, retaining 1.35 A cm -2 only a 7% loss in current density at 0.7 V after an extensive accelerated stress test of 150,000 voltage cycles.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2017

Heterogeneous Two-Phase Pillars in Epitaxial NiFe 2 O 4 -LaFeO 3 Nanocomposites

Self-assembled epitaxial oxide nanocomposites have been explored for a wide range of applications, including multiferroic and magnetoelectric properties, plasmonics, and catalysis. These so-called “vertically aligned nanocomposites” form spontaneously during the deposition process when segregation into two phases is energetically favorable as compared to a solid solution. However, there has been surprisingly little work understanding the driving forces that govern the synthesis of these materials, which can include point defect energetics, surface diffusion, and interfacial energies. To explore these factors, La-Ni-Fe-O films have been synthesized by molecular beam epitaxy and it is shown that these phase segregate into spinel-perovskite nanocomposites. Using complementary scanning transmission electron microscopy and atom-probe tomography, the elemental composition of each phase is examined and found that Ni ions are exclusively found in the spinel phase. From correlative analysis, a model for the relative favorability of the Ni2+ and Ni3+ valences under the growth conditions is developed. It is shown that multidimensional characterization techniques provide previously unobserved insight into the growth process and complex driving forces for phase segregation.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Strain-Induced Structural Deformation Study of 2D Mo x W (1- x ) S 2

The potential ability of tuning properties and its possible applications in the fields of optoelectronics and/or flexible electronics, has increased the demand for 2D alloys in recent times. Understanding the mechanical performance of 2D materials under extreme conditions, such as strain, stress, and fracture is essential for the reliable electronic devices based on these structures. Here, combined molecular dynamics (MD) simulations and in situ Raman spectroscopic techniques are used to study the mechanical performance of a 2D alloy system, MoxW (1- x ) S 2 . It is determined that W substitution in MoS 2 causes solid-solution strengthening and increase in the Young's modulus values. Higher W content decreases failure strain for MoS 2 . Due to spatially resolved Raman spectroscopy and MD simulations results, a detailed model to explain failure mechanisms in MoxW (1- x ) S 2 alloys is proposed.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Mechanochemistry of Phosphorus and Arsenic Alloys for Visible and Infrared Photonics

Incorporating few‐layer 2D phosphorus–arsenic alloys (PAs) into optoelectronic devices requires a synthesis technique that allows control of the alloy composition while producing volumes of material suitable for application development such as photodetectors, solar cells, and lasers. With that goal in mind, high‐energy ball milling allows production of both orthorhombic (o‐PAs) and trigonal (t‐PAs) alloys by reacting red phosphorus and metallic arsenic powders. The synthesis follows a two‐step process in which arsenic rapidly reacts with red phosphorus to first produce t‐PAs followed by a slower phase transformation into o‐PAs; synthesis time and overall conversion rate are slightly enhanced by the presence of arsenic. Optical measurements on exfoliated alloys at the few‐layer atomic limit of the 2D PAs reveal emission spanning from the visible (≈1.9 eV) into the near‐infrared region, covering a broad application space. Rapid powder synthesis within a closed system for stochiometric control of the solid‐solution PAs alloys combined with solution‐based exfoliation opens up opportunities for a whole new class of optoelectronic devices based on PA nanomaterials.

Pedersen, Samuel V.↗
DOE OSTI2019

Accelerated Search for BaTiO 3 -Based Ceramics with Large Energy Storage at Low Fields Using Machine Learning and Experimental Design

The problem that is considered is that of maximizing the energy storage density of Pb-free BaTiO3-based dielectrics at low electric fields. It is demonstrated that how varying the size of the combinatorial search space influences the efficiency of material discovery by comparing the performance of two machine learning based approaches where different levels of physical insights are involved. It is started with physics intuition to provide guiding principles to find better performers lying in the crossover region in the composition–temperature phase diagram between the ferroelectric phase and relaxor ferroelectric phase. Such an approach is limiting for multidopant solid solutions and motivates the use of two data-driven machine learning and design strategies with a feedback loop to experiments. Strategy I considers learning and property prediction on all the compounds, and strategy II learns to preselect compounds in the crossover region on which prediction is carried out. By performing only two active learning loops via strategy II, the compound (Ba0.86Ca0.14)(Ti0.79Zr0.11Hf0.10)O3 is synthesized with the largest energy storage density ≈73 mJ cm-3 at a field of 20 kV cm-1 , and an insight into the relative performance of the strategies using varying levels of knowledge is provided.

36 MATERIALS SCIENCE↗