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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 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Interlayer Coupling Controlled Ordering and Phases in Polar Vortex Superlattices

The recent discovery of polar topological structures has opened the door for exciting physics and emergent properties. There is, however, little methodology to engineer stability and ordering in these systems, properties of interest for engineering emergent functionalities. Notably, when the surface area is extended to arbitrary thicknesses, the topological polar texture becomes unstable. Here we show that this instability of the phase is due to electrical coupling between successive layers. We demonstrate that this electrical coupling is indicative of an effective screening length in the dielectric, similar to the conductor–ferroelectric interface. Controlling the electrostatics of the superlattice interfaces, the system can be tuned between a pure topological vortex state and a mixed classical-topological phase. This coupling also enables engineering coherency among the vortices, not only tuning the bulk phase diagram but also enabling the emergence of a 3D lattice of polar textures.

3D ordering↗
DOE OSTI2020

Phase evolution and amorphous stability upon solid-state reaction in superlattice like Ge–Sb–Te combinatorial thin-film

In this paper, the superlattice-like (SLL) Ge–Sb–Te combinatorial thin films were prepared by using a high-throughput ion beam sputtering system. The phase evolution and amorphous stability of such films undergoing heat treatment as a function of the coating sequence and modulation period were systematically studied. The composition structure diagram was constructed via an automated process of data obtained by high-throughput synchrotron micro-X-ray diffraction and lab-based micro-X-ray fluorescence. Furthermore, the element distribution and microstructure in the depth direction of the SLL thin films were characterized with time-of-flight secondary ion mass spectrometry and transmission electron microscopy, respectively. These studies demonstrated that the coating sequence has a significant effect on the element distribution in the as-deposited SLL thin films and the structure of the final product upon solid-state reaction. Reducing the modulation period of the SLL thin film improves the stability of the amorphous Ge–Sb–Te phase. This work lays a solid foundation for the rational design of SLL Ge–Sb–Te thin films to improve their performance.

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

All-Perovskite Multicomponent Nanocrystal Superlattices

Nanocrystal superlattices (NC SLs) have long been sought as promising metamaterials, with nanoscale-engineered properties arising from collective and synergistic effects among the constituent building blocks. Lead halide perovskite (LHP) NCs come across as outstanding candidates for SL design, as they demonstrate collective light emission, known as superfluorescence, in single- and multicomponent SLs. Thus far, LHP NCs have only been assembled in single-component SLs or coassembled with dielectric NC building blocks acting solely as spacers between luminescent NCs. Here, we report the formation of multicomponent LHP NC-only SLs, i.e., using only CsPbBr 3 NCs of different sizes as building blocks. The structural diversity of the obtained SLs encompasses the ABO 6 , ABO 3 , and NaCl structure types, all of which contain orientationally and positionally locked NCs. For the selected model system, the ABO 6 -type SL, we observed efficient NC coupling and Förster-like energy transfer from strongly confined 5.3 nm CsPbBr 3 NCs to weakly confined 17.6 nm CsPbBr 3 NCs, along with characteristic superfluorescence features at cryogenic temperatures. Spatiotemporal exciton dynamics measurements reveal that binary SLs exhibit enhanced exciton diffusivity compared to single-component NC assemblies across the entire temperature range (from 5 to 298 K). The observed coherent and incoherent NC coupling and controllable excitonic transport within the solid NC SLs hold promise for applications in quantum optoelectronic devices.

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

Symmetry-Protected Moiré Band Engineering and Enhanced Electron–Phonon Coupling in Xe/Bi 2 Se 3 Superlattices: Path to Topological Superconductivity

Observation of superconductivity, magnetism, and correlated insulating phases driven by the moiré potential in twisted graphene bilayer has opened the exciting new field of “twistronics”. Even richer physics is expected if moiré superlattice could be generated on topological insulators; however, until now, experimental studies have been scarce. Here, we demonstrate topological moirés generated by adsorbing a monolayer of noble gas on a topological insulator. By angle-resolved photoemission spectroscopy, we show that the moiré potential replicates the topological surface state and affects it in a way fundamentally different from the trivial states. Replicated Dirac cones generally avoid crossings, except at the time-reversal invariant momenta that remain gapless. This creates van Hove singularities at the moiré Brillouin zone corners, providing the mechanism of enhancing correlations. Indeed, we observe a strong enhancement of the electron–phonon coupling strength that, if properly tuned, might lead to topological superconductivity and Majorana Fermions.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Improved lifetime of a high spin polarization superlattice photocathode

Negative Electron Affinity (NEA) activated surfaces are required to extract highly spin-polarized electron beams from GaAs-based photocathodes, but they suffer extreme sensitivity to poor vacuum conditions that results in rapid degradation of quantum efficiency. We report on a series of unconventional NEA activations on surfaces of bulk GaAs with Cs, Sb, and O 2 using different methods of oxygen exposure for optimizing photocathode performance. Additionally, one order of magnitude improvement in lifetime with respect to the standard Cs–O 2 activation is achieved without significant loss of electron spin polarization and quantum efficiency by codepositing Cs, Sb, and O 2 . A strained GaAs/GaAsP superlattice sample activated with the codeposition method demonstrated similar enhancement in lifetime near the photoemission threshold while maintaining 90% spin polarization.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Emergent behavior of LaNiO 3 in short-periodic nickelate superlattices

Heterostructure engineering provides an efficient way to obtain several emergent phases of LaNiO 3 , as demonstrated in recent works. In this work, a new class of short periodic superlattices, consisting of LaNiO 3 and EuNiO 3 have been grown by pulsed laser interval deposition to investigate the effect of structural symmetry mismatch on the electronic and magnetic behaviors. Using synchrotron based soft and hard x-ray resonant scattering experiments, we have found that these heterostructures undergo simultaneous electronic and magnetic transitions. Most importantly, LaNiO 3 within these artificial structures exhibits a new antiferromagnetic, charge ordered insulating phase, which may be a potential candidate to achieve high temperature superconductivity.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Low-frequency Raman spectrum of 2D layered perovskites: Local atomistic motion or superlattice modes?

We report the low-frequency Raman spectrum (ω = 10 cm -1 –150 cm -1 ) of a wide variety of alkylammonium iodide based 2D lead halide perovskites (2D LHPs) as a function of A-site cation (MA = methylammonium and FA = formamidinium), octahedral layer thickness (n = 2–4), organic spacer chain length (butyl-, pentyl-, hexyl-), and sample temperature (T = 77 K–293 K). Using density functional theory calculations under the harmonic approximation for n = 2 BA:MAPbI, we assign several longitudinal/transverse optical phonon modes between 30 cm -1 and 100 cm -1 , the eigen displacements of which are analogous to that observed previously for octahedral twists/distortions in bulk MAPbI. Additionally, we propose an alternative assignment for low-frequency modes below this band (<30 cm -1 ) as zone-folded longitudinal acoustic phonons corresponding to the periodicity of the entire layered structure. Furthermore, we compare measured spectra to predictions of the Rytov elastic continuum model for zone-folded dispersion in layered structures. Our results are consistent across the various 2D LHPs studied herein, with energetic shifts of optical phonons corresponding to microscopic structural differences between materials and energetic shifts of acoustic phonons according to changes in the periodicity and elastic properties of the perovskite/organic subphases. This study highlights the importance of both the local atomic order and the superlattice structure on the vibrational properties of layered 2D materials.

2D materials↗
DOE OSTI2023

Controlling quantum phases of electrons and excitons in moiré superlattices

Moiré lattices formed in twisted and lattice-mismatched van der Waals heterostructures have emerged as a platform to engineer the novel electronic and excitonic states at the nanoscale. This Perspective reviews the materials science of moiré heterostructures with a focus on the structural properties of the interface and its structural–property relationships. We first review the studies of the atomic relaxation and domain structures in moiré superlattices and how these structural studies provide critical insights into understanding the behaviors of quantum-confined electrons and excitons. We discuss the general frameworks to manipulate moiré structures and how such control can be harnessed for engineering new phases of matter and simulating various quantum phenomena. Lastly, we discuss routes toward large-scale moiré heterostructures and give an outlook on their applications in quantum electronics and optoelectronics. Special emphasis will be placed on the challenges and opportunities of the reliable fabrication and dynamical manipulation of moiré heterostructures.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Multiscale electric-field imaging of polarization vortex structures in PbTiO 3 /SrTiO 3 superlattices

In ferroelectric heterostructures, the interaction between intrinsic polarization and the electric field generates a rich set of localized electrical properties. The local electric field is determined by several connected factors, including the charge distribution of individual unit cells, the interfacial electromechanical boundary conditions, and chemical composition of the interfaces. However, especially in ferroelectric perovskites, a complete description of the local electric field across micro-, nano-, and atomic-length scales is missing. Here, by applying four-dimensional scanning transmission electron microscopy (4D STEM) with multiple probe sizes matching the size of structural features, we directly image the electric field of polarization vortices in (PbTiO 3 ) 16 /(SrTiO 3 ) 16 superlattices and reveal different electric field configurations corresponding to the atomic scale electronic ordering and the nanoscale boundary conditions. The separability of two different fields probed by 4D STEM offers the possibility to reveal how each contributes to the electronic properties of the film.

36 MATERIALS SCIENCE↗
DOE OSTI2021

GdN/SmN superlattices; influence of a Zeeman/exchange conflict

GdN and SmN are two of the lanthanide nitrides, most of which are intrinsic ferromagnetic semiconductors. Superlattices comprising the pair offer a unique opportunity to investigate heterojunctions that feature simultaneous conductivity and magnetic interface influences. In this work, we report an investigation of these influences, using magnetisation and X-ray magnetic circular dichroism for magnetic effects, and magnetoresistance and Hall effect studies of their electrical conductance. Magnetic data show clear signatures of a conflicting Zeeman vs. interfacial exchange and the magnetic disruption that results, while resistivity and Hall measurements show conduction in both GdN and SmN.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Improving luminescence response in ZnGeN 2 /GaN superlattices: defect reduction through composition control

Abstract Color-mixed (cm) light-emitting diodes (LEDs) are theoretically the most efficient white light emitters, projected to improve white light luminous efficacy by 34% compared to incumbent phosphor converted LEDs. Since white light technology is pervasive and essential, small improvements in LED technology can result in energy savings. However, cm-LEDs are not yet realized due to poor efficacy in green and amber emitting materials, a spectral region colloquially referred to as the Green Gap. ZnGeN 2 is nearly isostructural and closely lattice-matched to GaN and can be heteroepitaxially integrated with existing GaN devices; ZnGeN 2 /GaN hybrid structures are theorized to emit green (~530 nn) light with a spontaneous emission rate 4.6–4.9 times higher than traditional InGaN LEDs when incorporated into III-N LED structures. In this report we demonstrate the molecular beam epitaxy (MBE) growth of GaN and ZnGeN 2 superlattices, an important step towards realizing multiple quantum well structures required for efficient LEDs. Elemental analysis, including atom probe tomography, shows that Ga and Ge are observed in both ZnGeN 2 and GaN layers, degrading the structural uniformity. The lack of elemental abruptness also leads to increased defect luminescence and reabsorption of band edge luminescence. The source of unintentional Ga distributed throughout the ZnGeN 2 layers was identified as excess flux escaping from around the closed MBE shutter. The source of unintentional Ge, which tended to incorporate as a single delta-doped layer in GaN, was identified as Ge riding along the cyclical metal-rich Ga adlayer used for high quality GaN, incorporating during subsequent nitrogen-rich growth step. Modifying the growth strategy results in improved structural quality, elemental abruptness, and luminescence response. This realization of structurally and elementally abrupt interfaces demonstrates the potential of heteroepitaxially integrated binary and ternary nitrides for energy-relevant devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Dimensionality-Induced Change in Topological Order in Multiferroic Oxide Superlattices

We construct ferroelectric (LuFeO 3 ) m /(LuFe 2 O 4 ) superlattices with varying index m to study the effect of confinement on topological defects. We observe a thickness-dependent transition from neutral to charged domain walls and the emergence of fractional vortices. In thin LuFeO 3 layers, the volume fraction of domain walls grows, lowering the symmetry from P6 3 cm to P3c1 before reaching the nonpolar P6 3 /mmc state, analogous to the group-subgroup sequence observed at the high-temperature ferroelectric to paraelectric transition. Our study shows how dimensional confinement stabilizes textures beyond those in bulk ferroelectric systems.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Quantum Anomalous Hall Crystal at Fractional Filling of Moiré Superlattices

We predict the emergence of a state of matter with intertwined ferromagnetism, charge order, and topology in fractionally filled moiré superlattice bands. Remarkably, these quantum anomalous Hall crystals exhibit a quantized integer Hall conductance that is different than expected from the filling and Chern number of the band. Microscopic calculations show that this phase is robustly favored at half-filling (𝜈 =1/2) at larger twist angles of the twisted semiconductor bilayer 𝑡⁢MoTe 2 .

Exact diagonalization↗
DOE OSTI2022

Record Efficiency Multijunction Solar Cells with Strain-Balanced Quantum Well Superlattices

The absorption edge of a GaAs solar cell can be tuned to longer wavelengths with strain-balanced quantum wells, as an alternative to metamorphic epitaxy. For one-sun photovoltaic applications, an optimum bandgap for both single and multijunction solar cells is near the broad water absorption peak at 930 nm and can be accessed by a Ga0.9In0.1As alloy. This alloy is strained with respect to the GaAs substrate, and so only very thin ~10 nm layers can be grown without relaxation via dislocation formation. However, solar cells require significant thickness for complete absorption of the incoming solar spectrum, requiring many such layers. We have designed quantum well superlattices with up to 300 sets of carefully tuned strain-balanced GaInAs/GaAsP pairs by limiting composition modulation and material degradation. We have incorporated quantum well solar cells into multijunction devices to achieve record 32.9% two-junction and 39.5% three-junction solar cells under standard one-sun illumination. We will describe the physics of the quantum well devices and the growth conditions that lead to sharp interfaces and good material quality, as well as the characterization of the efficiencies.

GaAs↗
DOE OSTI2021

Manipulation of the Electronic State of Mott Iridate Superlattice through Protonation Induced Electron-Filling

Spin-orbit-coupled Mott iridates show great similarity with parent compounds of superconducting cuprates, attracting extensive research interest especially for their electron-doped states. However, previous experiments have been largely limited within a small doping range due to the absence of effective dopants, and therefore the electron-doped phase diagram remains elusive. Here, an ionic-liquid-gating-induced protonation method is utilized to achieve electron-doping into a 5d Mott-insulator built with a SrIrO 3 /SrTiO 3 superlattice (SL), and a systematic mapping of its electron-doped phase diagram is achieved with the evolution of the iridium valence state from 4+ to 3+, equivalent to doping of one electron per iridium ion. Along increasing doping level, the parent Mott-insulator is first turned into a localized metallic state with gradually suppressed magnetic ordering, and then further evolves into a nonmagnetic band insulating state. This work forms an important step forward for the study of electron-doped Mott iridate systems, and the strategy of manipulating the band filling in an artificially designed SL structure can be readily extended into other systems with more exotic states to explore.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Crystal Symmetry Engineering in Epitaxial Perovskite Superlattices

Interface plays a critical role in determining the physical properties and device performance of heterostructures. Traditionally, lattice mismatch, resulting from the different lattice constants of the heterostructure, can induce epitaxial strain. Over past decades, strain engineering has been demonstrated as a useful strategy to manipulate the functionalities of the interface. However, mismatch of crystal symmetry at the interface is relatively less studied due to the difficulty of atomically structural characterization, particularly for the epitaxy of low symmetry correlated materials on the high symmetry substrates. Overlooking those phenomena restrict the understanding of the intrinsic properties of the as- determined heterostructure, resulting in some long-standing debates including the origin of magnetic and ferroelectric dead layers. Here, perovskite LaCoO 3 -SrTiO 3 superlattice (SL) is used as a model system to show that the crystal symmetry effect can be isolated by the existing interface strain. Combining the state-of-art diffraction and electron microscopy, it is found that the symmetry mismatch of LaCoO 3 -SrTiO 3 SL can be tuned by manipulating the SrTiO 3 layer thickness to artificially control the magnetic properties. Furthermore, the work suggests that crystal symmetry mismatch can also be designed and engineered to act as an effective strategy to generate functional properties of perovskite oxides.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Transient Terahertz Oscillations During Photoinduced Polarization Topology Reconfiguration in Ferroelectric Superlattices

Terahertz resonances embedded in crystalline heterostructures could close a spectral gap between conventional electronics and photonics while opening new windows on non-equilibrium lattice dynamics. We show that femtosecond optical screening of the depolarization field in epitaxial PbTiO3/SrTiO3 superlattices launches a collective polar mode that oscillates near 1 THz and coherently spans the entire mini-Brillouin zone. Wave-vector-resolved pump–probe X-ray diffraction resolves a nearly dispersion-less oscillation at 0.87 THz and 0.94 THz at the zone boundary and zone center, respectively, persisting for ~2.5 ps, corresponding to a weakly damped resonance. Dynamical phase-field simulations reveal the origin of the mode to mesoscopic rotation of closure-domain textures during the photo-excited transition from an unscreened to a screened electrostatic state. Varying the PbTiO3 and SrTiO3 ratio tunes the mode frequency continuously from 0.9 to 1.4 THz, providing a quantitative design rule for frequency-selectable THz oscillators in ferroelectric heterostructures. By coupling nanoscale polarization reconfiguration to long-wavelength coherent dynamics, this work establishes depolarization-field engineering to topology-driven THz functionality and expanding the landscape of collective lattice dynamics.

Sri Gyan, Deepankar [Univ. of Wisconsin, Madison, ↗
DOE OSTI2021

Low‐Density 2D Superlattices Assembled via Directional DNA Bonding

Abstract It is critical to assemble nanoparticles (NPs) into superlattices with controlled symmetries and spacings on substrates for metamaterials applications, where such structural parameters dictate their properties. Here, we use DNA to assemble anisotropic NPs of three shapes—cubes, octahedra, and rhombic dodecahedra—on substrates and investigate their thermally induced reorganization into two‐dimensional (2D) crystalline films. We report two new low‐density 2D structures, including a honeycomb lattice based on octahedral NPs. The low‐density lattices favored here are not usually seen when particles are crystallized via other bottom‐up assembly techniques. Furthermore, we show that, consistent with the complementary contact model, a primary driving force for crystallization is the formation of directional, face‐to‐face DNA bonds between neighboring NPs and between NPs and the substrate. Our results can be used to deliberately prepare crystalline NP films with novel morphologies.

Miao, Ziyi↗