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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Domain wall enabled steep slope switching in MoS2 transistors towards hysteresis-free operation

Abstract The device concept of ferroelectric-based negative capacitance (NC) transistors offers a promising route for achieving energy-efficient logic applications that can outperform the conventional semiconductor technology, while viable operation mechanisms remain a central topic of debate. In this work, we report steep slope switching in MoS 2 transistors back-gated by single-layer polycrystalline PbZr 0.35 Ti 0.65 O 3 . The devices exhibit current switching ratios up to 8 × 10 6 within an ultra-low gate voltage window of $$V_{{{\mathrm{g}}}} = \pm \! 0.5$$ V g = ± 0.5 V and subthreshold swing (SS) as low as 9.7 mV decade −1 at room temperature, transcending the 60 mV decade −1 Boltzmann limit without involving additional dielectric layers. Theoretical modeling reveals the dominant role of the metastable polar states within domain walls in enabling the NC mode, which is corroborated by the relation between SS and domain wall density. Our findings shed light on a hysteresis-free mechanism for NC operation, providing a simple yet effective material strategy for developing low-power 2D nanoelectronics.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Tip-based proximity ferroelectric switching and piezoelectric response in wurtzite multilayers

Proximity ferroelectricity is a paradigm for inducing ferroelectricity when a nonferroelectric polar material (such as Al⁢ N), which is unswitchable with an external field below the dielectric breakdown field, becomes a practically switchable ferroelectric in direct contact with a thin switchable ferroelectric layer (such as Al 1−𝑥 ⁢Sc 𝑥 ⁢N). Here, we develop a Landau-Ginzburg-Devonshire approach to study the proximity effect of local piezoelectric response and polarization reversal in wurtzite ferroelectric multilayers under a sharp electrically biased tip. Using finite-element modeling, we analyze the probe-induced nucleation of nanodomains, the features of local polarization hysteresis loops and coercive fields in the Al 1−𝑥 ⁢Sc 𝑥 ⁢N/Al⁢ N bilayers and three-layers. Similar to the wurtzite multilayers sandwiched between two parallel electrodes, the regimes of “proximity switching” (when all layers collectively switch) and the regime of “proximity suppression” (when they collectively do not switch) are the only two possible regimes in the probe-electrode geometry. However, the parameters and asymmetry of the local piezoresponse and polarization hysteresis loops depend significantly on the sequence of the layers with respect to the probe. The physical mechanism of proximity ferroelectricity in the local probe geometry is a depolarizing electric field determined by the polarization of the layers and their relative thickness. The field, whose direction is opposite to the polarization vector in the layer(s) with the larger spontaneous polarization (such as Al⁢ N), renormalizes the double-well ferroelectric potential to lower the steepness of the switching barrier in the “otherwise unswitchable” polar layers. Tip-based control of domains in otherwise nonferroelectric layers using proximity ferroelectricity can provide nanoscale control of domain reversal in memory, actuation, sensing, and optical applications. The ability of the tip-induced proximity switching to differentially switch multilayers, based on the order of the layers, provides a powerful tool for selective domain engineering.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Solvent and Temperature Effects on Photoinduced Proton-Coupled Electron Transfer in the Marcus Inverted Region

Concerted proton-coupled electron transfer (PCET) in the Marcus inverted region was recently demonstrated. Understanding the requirements for such reactivity is fundamentally important and holds promise as a design principle for solar energy conversion systems. Herein, we investigate the solvent polarity and temperature dependence of photoinduced proton-coupled charge separation (CS) and charge recombination (CR) in anthracene–phenol–pyridine triads: 1 (10-(4-hydroxy-3-(4-methylpyridin-2-yl)benzyl)anthracene-9-carbonitrile) and 2 (10-(4-hydroxy-3-(4-methoxypyridin-2-yl)benzyl)anthracene-9-carbonitrile). Both the CS and CR rate constants increased with increasing polarity in acetonitrile:n-butyronitrile mixtures. The kinetics were semi-quantitatively analyzed where changes in dielectric and refractive index, and thus consequently changes in driving force (–ΔG°) and reorganization energy (λ), were accounted for. The results were further validated by fitting the temperature dependence, from 180 to 298 K, in n-butyronitrile. The analyses support previous computational work where transitions to proton vibrational excited states dominate the CR reaction with a distinct activation free energy (ΔG* CR ~ 140 meV). However, the solvent continuum model fails to accurately describe the changes in ΔG° and λ with temperature via changes in dielectric constant and refractive index. Satisfactory modeling was obtained using the results of a molecular solvent model, which predicts that λ decreases with temperature, opposite to that of the continuum model. To further assess the solvent polarity control in the inverted region, the reactions were studied in toluene. Nonpolar solvents decrease both ΔG° CR and λ, slowing CR into the nanosecond time regime for 2 in toluene at 298 K. This demonstrates how PCET in the inverted region may be controlled to potentially use proton-coupled CS states for efficient solar fuel production and photoredox catalysis.

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

Chemical control of polarization in thin strained films of a multiaxial ferroelectric: Phase diagrams and polarization rotation

The emergent behaviors in thin films of a multiaxial ferroelectric (FE) due to electrochemical coupling between the rotating polarization and surface ions are explored within the framework of the 2–4 Landau-Ginzburg-Devonshire (LGD) thermodynamic potential combined with the Stephenson-Highland (SH) approach. The combined LGD-SH approach allows us to describe the electrochemical switching and rotation of a polarization vector in a multiaxial ferroelectric film covered by surface ions with a charge density defined by the oxygen pressure. In this work, we calculate phase diagrams, analyze the dependence of polarization components on the applied voltage, and discuss the peculiarities of quasistatic ferroelectric, dielectric, and piezoelectric hysteresis loops in thin strained multiaxial ferroelectric films. The nonlinear surface screening by oxygen ions makes the diagrams very different from the known diagrams of, e.g., strained BaTiO 3 films. Quite unexpectedly, we predict the appearance of ferroelectric reentrant phases. The obtained results point to the possibility to control the appearance and features of ferroelectric, dielectric, and piezoelectric hysteresis in multiaxial FE films covered with surface ions by varying their concentration via the partial oxygen pressure. The LGD-SH description of a multiaxial FE film can be further implemented within the Bayesian optimization framework, paving the way toward predictive materials optimization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Photoinduced charge transfer in Zn(II) and Au(III)-ligated symmetric and asymmetric bacteriochlorin dyads: A computational study

The excited-state properties and photoinduced charge-transfer (CT) kinetics in a series of symmetrical and asymmetrical Zn- and Au-ligated meso–meso-connected bacteriochlorin (BChl) complexes are studied computationally. BChl derivatives, which are excellent near-IR absorbing chromophores, are found to play a central role in bacterial photosynthetic reaction centers but are rarely used in artificial solar energy harvesting systems. The optical properties of chemically linked BChl complexes can be tuned by varying the linking group and involving different ligated metal ions. We investigate charge transfer in BChl dyads that are either directly linked or through a phenylene ring (1,4- phenylene) and which are ligating Zn or Au ions. The directly linked dyads with a nearly perpendicular arrangement of the BChl units bear markedly different properties than phenylene linked dyads. In addition, we find that the dielectric dependence of the intramolecular CT rate is very strong in neutral Zn-ligated dyads, whereas cationic Au-ligated dyads show negligible dielectric dependence of the CT rate. Rate constants of the photo induced CT process are calculated at the semiclassical Marcus level and are compared to fully quantum mechanical Fermi’s golden rule based values. The rates are calculated using a screened range separated hybrid functional that offers a consistent framework for addressing environment polarization. We study solvated systems in two solvents of a low and a high scalar dielectric constant.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Asymmetric ferroelectricity by design in atomic-layer superlattices with broken inversion symmetry

In atomic-layer superlattices constructed using three constituent phases, CaTiO 3 , SrTiO 3 , and BaTiO 3 , the stacking sequence of the atomic layers is found to control the symmetry of the high-temperature dielectric response. In such a superlattice when a nanostructured asymmetric strain is programmed into the lattice via the stacking order, the natural symmetry at high temperatures is removed and a polarized sample is obtained in which the polarization increases as the temperature is lowered. Here, in contrast to a ferroelectric characterized by a bistable ground state with two equal and opposite electronic polarizations, our experiments show evidence of asymmetric ferroelectric correlations that set in when such a sample becomes hysteretic below a temperature T x , with two unequal polarization states. We further show that both the magnitude and direction of this ferroelectric asymmetry can be controlled by the engineered atomic-layer stacking order and periodicity of the superlattice.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Ferroelectricity in Si-Doped Hafnia: Probing Challenges in Absence of Screening Charges

The ability to develop ferroelectric materials using binary oxides is critical to enable novel low-power, high-density non-volatile memory and fast switching logic. The discovery of ferroelectricity in hafnia-based thin films, has focused the hopes of the community on this class of materials to overcome the existing problems of perovskite-based integrated ferroelectrics. However, both the control of ferroelectricity in doped-HfO2 and the direct characterization at the nanoscale of ferroelectric phenomena, are increasingly difficult to achieve. The main limitations are imposed by the inherent intertwining of ferroelectric and dielectric properties, the role of strain, interfaces and electric field-mediated phase, and polarization changes. In this work, using Si-doped HfO2 as a material system, we performed a correlative study with four scanning probe techniques for the local sensing of intrinsic ferroelectricity on the oxide surface. Putting each technique in perspective, we demonstrated that different origins of spatially resolved contrast can be obtained, thus highlighting possible crosstalk not originated by a genuine ferroelectric response. By leveraging the strength of each method, we showed how intrinsic processes in ultrathin dielectrics, i.e., electronic leakage, existence and generation of energy states, charge trapping (de-trapping) phenomena, and electrochemical effects, can influence the sensed response. We then proceeded to initiate hysteresis loops by means of tip-induced spectroscopic cycling (i.e., “wake-up”), thus observing the onset of oxide degradation processes associated with this step. Finally, direct piezoelectric effects were studied using the high pressure resulting from the probe’s confinement, noticing the absence of a net time-invariant piezo-generated charge. Our results are critical in providing a general framework of interpretation for multiple nanoscale processes impacting ferroelectricity in doped-hafnia and strategies for sensing it.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Liberating a hidden antiferroelectric phase with interfacial electrostatic engineering

Antiferroelectric materials have seen a resurgence of interest because of proposed applications in a number of energy-efficient technologies. Unfortunately, relatively few families of antiferroelectric materials have been identified, precluding many proposed applications. Here, we propose a design strategy for the construction of antiferroelectric materials using interfacial electrostatic engineering. We begin with a ferroelectric material with one of the highest known bulk polarizations, BiFeO 3 . By confining thin layers of BiFeO 3 in a dielectric matrix, we show that a metastable antiferroelectric structure can be induced. Application of an electric field reversibly switches between this new phase and a ferroelectric state. The use of electrostatic confinement provides an untapped pathway for the design of engineered antiferroelectric materials with large and potentially coupled responses.

42 ENGINEERING↗
DOE OSTI2021

3D printing of High Precision Radiation Filters for next generation Cosmic Background (CMB) studies (Final Report)

The terahertz (THz) spectral range is the part of the electromagnetic spectrum between 0.1–10 THz or 0.03–3 mm wavelength. For a long period, the terahertz band was relatively unexplored due to the unavailability of cost-effective and powerful sources. Due to the evolution of these devices in the mid-1980s, however, terahertz radiation has attracted much more attention. Since this part of the spectrum is between the infrared (IR) and microwave frequency ranges, the development of waveguides, filters, polarizers, lenses, and other optical components. Since terahertz waves to penetrate most dielectric materials offers the possibility of many applications. Since terahertz radiation can pass through organic tissue without causing damage, and it can be safely applied for biomedical applications. Radio astronomy and wireless communication are also fields with great interest in this spectral range. For example, terahertz waves could be used to detect cold bodies and debris in space or to increase data transmission using the larger bandwidth of the terahertz band.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Prototyping of 2D and 3D photonic nanodevices by Electron Beam Lithography (CRADA Final Report)

Team developed a large area and fast electron beam lithographic for patterning visible wavelength optical materials to create 2 or 3 dimensional gratings and metasurfaces. Metasurfaces,are arrays of nanoantennas or optical resonators, are dielectric or plasmonic structures that allow control of the amplitude, phase, and polarization of light by locally modulating its wavefront The team was able to write a 1cm2 pattern with resolution better than 30 nm without visible discontinuities in the pattern. Performance to this specification allowed prototyping of optical lenses for production applications such as augmented reality goggles (optical displays) and other applications for visible light manipulations

36 MATERIALS SCIENCE↗
DOE OSTI2024

Comparison of interband related optical transitions and excitons in ZnGeN 2 and GaN

The optical dielectric function of ZnGeN 2 is calculated from the interband transitions using the energy bands calculated in the quasiparticle self-consistent (QS)GW^ method using two different levels of approximation: the independent particle approximation (IPA) and the Bethe-Salpeter Equation (BSE) approach. The first allows us to relate peaks in ε 2 to specific bands and k-points but does not include electron-hole interaction effects. The second includes electron-hole interaction or excitonic effects. The corresponding changes in the shape of ε 2 (ω) are found to be similar to those in GaN. The screened Coulomb interaction W^ is here calculated including electron-hole interactions in the polarization function and gives a band structure already going beyond the random phase approximation. The static dielectric constants including only electronic screening, commonly referred to as ε∞ , were calculated separately by extrapolating the wave vector dependent macroscopic dielectric function in the long-wavelength limit. Below the quasiparticle gap, we find three bound excitons optically active for different polarization. The convergence of these bound excitons with respect to the density of the k-mesh used in the BSE is studied and found to require a fine mesh. It is also found that these bound excitons originate from only the lowest conduction band and the top three valence bands. To incorporate the lattice screening, we include a scaling factor (ε∞/ε 0 ) 2 , which allows us to obtain exciton binding energies of the correct order of magnitude similar to those in GaN. Here, the excitons are related to each of the three fold split valence bands and the splittings of the latter are also studied as function of strain. Finally, a relation between the anisotropic effective masses and the valence band splitting is pointed out and explained.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Enhancements of electric field and afterglow of non-equilibrium plasma by Pb(ZrxTi1−x)O3 ferroelectric electrode

Abstract Manipulating surface charge, electric field, and plasma afterglow in a non-equilibrium plasma is critical to control plasma-surface interaction for plasma catalysis and manufacturing. Here, we show enhancements of surface charge, electric field during breakdown, and afterglow by ferroelectric barrier discharge. The results show that the ferroelectrics manifest spontaneous electric polarization to increase the surface charge by two orders of magnitude compared to discharge with an alumina barrier. Time-resolved in-situ electric field measurements reveal that the fast polarization of ferroelectrics enhances the electric field during the breakdown in streamer discharge and doubles the electric field compared to the dielectric barrier discharge. Moreover, due to the existence of surface charge, the ferroelectric electrode extends the afterglow time and makes discharge sustained longer when alternating the external electric field polarity. The present results show that ferroelectric barrier discharge offers a promising technique to tune plasma properties for efficient plasma catalysis and electrified manufacturing.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Enhanced dielectric insulation of biaxially oriented high temperature polyester films for capacitive energy storage

Biaxially oriented polypropylene (BOPP) films are widely used in dielectric capacitors due to their ultralow loss, high breakdown strength, and long lifetime. However, their poor temperature tolerance limits applications in emerging high-temperature environments such as wide-band-gap power electronics in electric vehicles. Here, we report significantly enhanced dielectric insulation properties of biaxially oriented poly(ethylene 2,6-naphthalate) (BOPEN) films compared to biaxially oriented poly(ethylene terephthalate) (BOPET) films, despite their similar semicrystalline morphologies. BOPEN exhibits higher DC and AC breakdown strengths and markedly extended lifetimes at elevated temperatures. For instance, at 120 °C, the DC Weibull lifetime of BOPEN exceeded that of BOPET by over two orders of magnitude and even surpassed that of BOPP. Through comprehensive analyses—leakage current, electric displacement-electric field loops, and thermally stimulated depolarization current—we attribute this superior performance to suppressed homocharge injection and conduction losses, enabled by the rigid naphthalene-based backbone in BOPEN that reduces dipole mobility and chain polarity. These findings underscore the potential of BOPEN as a next-generation polymer dielectric for high-temperature capacitor applications.

25 ENERGY STORAGE↗
DOE OSTI2024

Analytical model and dynamical phase-field simulation of terahertz transmission across ferroelectrics

Here, we theoretically investigate the steady-state transmission of continuous terahertz (THz) wave across a freestanding ferroelectric slab. Based on the Landau-Ginzburg-Devonshire theory of ferroelectrics and the coupled equations of motion for polarization and electromagnetic (EM) waves, we derive the analytical expressions of the frequency- and thickness-dependent dielectric susceptibility and transmission coefficient at the thin slab limit in the harmonic excitation regime. When the slab thickness is much smaller than the THz wavelength in the ferroelectric, the analytical predictions agree well with the numerical simulations from a dynamical phase-field model that incorporates the coupled dynamics of strain, polarization, and EM wave in multiphase systems. At larger thicknesses, the transmission is mainly determined by the frequency-dependent attenuation of THz waves in the ferroelectric and the formation of a standing polarization/THz wave. Our results advance the understanding of the interaction between THz wave and ferroelectrics and suggest the potential of exploiting ferroelectrics to achieve low-heat-dissipation, nonvolatile voltage modulation of THz transmission for high-data-rate wireless communication.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Relaxation dynamics of water in the vicinity of cellulose nanocrystals

Water molecules near cellulose nanocrystals (CNCs; produced via the sulfuric acid-catalyzed hydrolysis of wood pulp) are believed to relax slower than those in the bulk liquid, which may result in unique properties of CNC aqueous dispersions. Herein this study analyzed the polarization behavior of water molecules in CNC aqueous dispersions and other reference samples using a dielectric relaxation spectroscopy (DRS) technique in the microwave frequency range (0.2–20 GHz). As the CNC concentration increases, two slow relaxation components become prominent. The comparison with DRS data of aqueous dispersions of nanoporous silica, polyvinyl alcohol (PVA), and hairy CNC (HCNC) with amorphous chains protruding from both ends suggested that these slow relaxation modes of water near CNC surfaces cannot be attributed to direct hydrogen bonding interactions with the hydroxyl (OH) groups exposed and immobilized at the solid surface. Instead, they are similar to the water molecules interacting with OH groups attached to flexible polymer chains. Molecular dynamics (MD) simulations of the polarization behavior of water near the (110) facet of cellulose Iβ crystals confirmed that the interactions of water molecules with the cellulose crystal surface do not cause slower relaxations in the frequency range studied via the DRS. These results indicated that the CNC surface cannot be depicted with the crystallographic facets of cellulose Iβ; instead, it resembles a polymer-brush surface on which the short glucan residues or fragments of the strong acid-catalyzed hydrolysis process are swollen and extended into the aqueous phase.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2026

Proximity Ferroelectricity in Compositionally Graded Structures

Proximity ferroelectricity is a novel paradigm for inducing ferroelectricity in a non-ferroelectric polar material, such as AlN or ZnO that are typically unswitchable with an external field below their dielectric breakdown field. When placed in direct contact with a thin switchable ferroelectric layer (such as Al 1-x Sc x N or Zn 1-x Mg x O), they become a practically switchable ferroelectric. Using the thermodynamic Landau-Ginzburg-Devonshire theory, in this work, we perform the finite element modeling of the polarization switching in the compositionally graded AlN-Al 1-x Sc x N, ZnO-Zn 1-x Mg x O, and MgO-Zn 1-x Mg x O structures sandwiched in both a parallel-plate capacitor geometry as well as in a sharp probe-planar electrode geometry. We reveal that the compositionally graded structure allows the simultaneous switching of spontaneous polarization in the whole system by a coercive field significantly lower than the electric breakdown field of unswitchable polar materials. The physical mechanism is the depolarization electric field determined by the gradient of chemical composition “x”. The field lowers the steepness of the switching barrier in the otherwise unswitchable parts of the compositionally graded AlN-Al 1-x Sc x N and ZnO-Zn 1-x Mg x O structures. In the MgO-like regions of the compositionally graded MgO-Zn 1-x Mg x O structure, a shallow double-well free energy potential emerges. Proximity ferroelectric switching of the compositionally graded structures placed in the probe-electrode geometry occurs due to nanodomain formation under the tip. We predict that a gradient of chemical composition “x” significantly lowers effective coercive fields of the compositionally graded AlN-Al 1-x Sc x N and ZnO-Zn 1-x Mg x O structures compared to the coercive fields of the corresponding multilayers with a uniform chemical composition in each layer. A tip-induced switching further lowers the coercive field, enabling control of ferroelectric domains in otherwise unswitchable compositionally graded structures, which can provide nanoscale domain control for memory, actuation, sensing, and optical applications.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Microwave-Absorbing Foams with Adjustable Absorption Frequency and Structural Coloration

Microwave-absorbing materials with regulatable absorption frequency and optical camouflage hold great significance in intelligent electronic devices and advanced stealth technology. Herein, we present an innovative microwave-absorbing foam that can dynamically tune microwave absorption frequencies via a simple mechanical compression while in parallel enabling optical camouflage over broad spectral ranges by adjusting the structural colors. In this study, the vivid colors spanning different color categories generated from thin-film interference can be precisely regulated by adjusting the thickness of the conformal TiO 2 coatings on Ni/melamine foam. Enhanced interfacial and defect-induced polarizations resulting from the introduction of TiO 2 coating synergistically contribute to the dielectric attenuation performance. Consequently, such a foam exhibits exceptional microwave absorption capabilities, and the absorption frequency can be dynamically tuned from the S band to the Ku band by manipulating its compression ratio. Additionally, simulation calculations validate the adjustable electromagnetic wave loss behavior, offering valuable insights for the development of next-generation intelligent electromagnetic devices across diverse fields.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ultrafast and Highly Collimated Radially Polarized Photons at Room Temperature from a Colloidal Quantum Dot Coupled to a Hybrid Nanoantenna

To harness the potential of radially polarized photons for classical and quantum communication applications, we demonstrate an on-chip, room-temperature device, which generates highly directional radially polarized photons at very high rates. The photons are emitted from a giant CdSe/CdS colloidal quantum dot (gQD) accurately positioned at the tip of a metal nanocone centered inside a hybrid metal-dielectric bullseye antenna. We show that due to the large and selective Purcell enhancement specifically for the out-of-plane optical dipole of the gQD, the emitted photons can have a very high degree of radial polarization (>93%), based on a quantitative metric. Our study emphasizes the importance of accurate gQD positioning for optimal radial polarization purity through extensive experiments and simulations, which contribute to the fundamental understanding of radial polarization in nanostructured devices and pave the way for implementation of such systems in practical applications using structured quantum light.

36 MATERIALS SCIENCE↗