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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 757 records · Page 42
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Chiral recognition and selection during the self-assembly process of protein-mimic macroanions

The research on chiral recognition and chiral selection is not only fundamental in resolving the puzzle of homochirality, but also instructive in chiral separation and stereoselective catalysis. Here we report the chiral recognition and chiral selection during the self-assembly process of two enantiomeric wheel-shaped macroanions, [Fe28(μ3-O)8(Tart)16(HCOO)24]20- (Tart=D- or L-tartaric acid tetra-anion). The enantiomers are observed to remain self-sorted and self-assemble into their individual assemblies in their racemic mixture solution. The addition of chiral co-anions can selectively suppress the self-assembly process of the enantiomeric macroanions, which is further used to separate the two enantiomers from their mixtures on the basis of the size difference between the monomers and the assemblies. We believe that delicate long-range electrostatic interactions could be responsible for such high-level chiral recognition and selection.

Yin, Panchao↗
DOE OSTI2017

Experimental realization of two-dimensional Dirac nodal line fermions in monolayer Cu 2 Si

Topological nodal line semimetals, a novel quantum state of materials, possess topologically nontrivial valence and conduction bands that touch at a line near the Fermi level. The exotic band structure can lead to various novel properties, such as long-range Coulomb interaction and flat Landau levels. Recently, topological nodal lines have been observed in several bulk materials, such as PtSn 4 , ZrSiS, TlTaSe 2 and PbTaSe 2 . However, in two-dimensional materials, experimental research on nodal line fermions is still lacking. Here, we report the discovery of two-dimensional Dirac nodal line fermions in monolayer Cu 2 Si based on combined theoretical calculations and angle-resolved photoemission spectroscopy measurements. The Dirac nodal lines in Cu 2 Si form two concentric loops centred around the Γ point and are protected by mirror reflection symmetry. In conclusion, our results establish Cu 2 Si as a platform to study the novel physical properties in two-dimensional Dirac materials and provide opportunities to realize high-speed low-dissipation devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Superconductivity from energy fluctuations in dilute quantum critical polar metals

Abstract Superconductivity in low carrier density metals challenges the conventional electron-phonon theory due to the absence of retardation required to overcome Coulomb repulsion. Here we demonstrate that pairing mediated by energy fluctuations, ubiquitously present close to continuous phase transitions, occurs in dilute quantum critical polar metals and results in a dome-like dependence of the superconducting T c on carrier density, characteristic of non-BCS superconductors. In quantum critical polar metals, the Coulomb repulsion is heavily screened, while the critical transverse optical phonons decouple from the electron charge. In the resulting vacuum, long-range attractive interactions emerge from the energy fluctuations of the critical phonons, resembling the gravitational interactions of a chargeless dark matter universe. Our estimates show that this mechanism may explain the critical temperatures observed in doped SrTiO 3 . We provide predictions for the enhancement of superconductivity near polar quantum criticality in two- and three-dimensional materials that can be used to test our theory.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Imaging moiré flat bands in three-dimensional reconstructed WSe 2 /WS 2 superlattices

Moiré superlattices in transition metal dichalcogenide (TMD) heterostructures can host novel correlated quantum phenomena due to the interplay of narrow moiré flat bands and strong, long-range Coulomb interactions. However, microscopic knowledge of the atomically reconstructed moiré superlattice and resulting flat bands is still lacking, which is critical for fundamental understanding and control of the correlated moiré phenomena. Here we quantitatively study the moiré flat bands in three-dimensional (3D) reconstructed WSe 2 /WS 2 moiré superlattices by comparing scanning tunnelling spectroscopy (STS) of high-quality exfoliated TMD heterostructure devices with ab initio simulations of TMD moiré superlattices. A strong 3D buckling reconstruction accompanied by large in-plane strain redistribution is identified in our WSe 2 /WS 2 moiré heterostructures. STS imaging demonstrates that this results in a remarkably narrow and highly localized K-point moiré flat band at the valence band edge of the heterostructure. A series of moiré flat bands are observed at different energies that exhibit varying degrees of localization. Our observations contradict previous simplified theoretical models but agree quantitatively with ab initio simulations that fully capture the 3D structural reconstruction. Furthermore, our results reveal that the strain redistribution and 3D buckling in TMD heterostructures dominate the effective moiré potential and the corresponding moiré flat bands at the Brillouin zone K points.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Dynamic crystallography reveals spontaneous anisotropy in cubic GeTe

Cubic energy materials such as thermoelectrics or hybrid perovskite materials are often understood to be highly disordered. In GeTe and related IV–VI compounds, this is thought to provide the low thermal conductivities needed for thermoelectric applications. Since conventional crystallography cannot distinguish between static disorder and atomic motions, we develop the energy-resolved variable-shutter pair distribution function technique. This collects structural snapshots with varying exposure times, on timescales relevant for atomic motions. In disagreement with previous interpretations, we find the time-averaged structure of GeTe to be crystalline at all temperatures, but with anisotropic anharmonic dynamics at higher temperatures that resemble static disorder at fast shutter speeds, with correlated ferroelectric fluctuations along the <100> c direction. We show that this anisotropy naturally emerges from a Ginzburg–Landau model that couples polarization fluctuations through long-range elastic interactions. By accessing time-dependent atomic correlations in energy materials, we resolve the long-standing disagreement between local and average structure probes and show that spontaneous anisotropy is ubiquitous in cubic IV–VI materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Mapping charge excitations in generalized Wigner crystals

Transition metal dichalcogenide-based moiré superlattices exhibit strong electron-electron correlations, thus giving rise to strongly correlated quantum phenomena such as generalized Wigner crystal states. Evidence of Wigner crystals in transition metal dichalcogenide moire superlattices has been widely reported from various optical spectroscopy and electrical conductivity measurements, while their microscopic nature has been limited to the basic lattice structure. Theoretical studies predict that unusual quasiparticle excitations across the correlated gap between upper and lower Hubbard bands can arise due to long-range Coulomb interactions in generalized Wigner crystal states. However, the microscopic proof of such quasiparticle excitations is challenging because of the low excitation energy of the Wigner crystal. Here, in this study, we describe a scanning single-electron charging spectroscopy technique with nanometre spatial resolution and single-electron charge resolution that enables us to directly image electron and hole wavefunctions and to determine the thermodynamic gap of generalized Wigner crystal states in twisted WS 2 moiré heterostructures. High-resolution scanning single-electron charging spectroscopy combines scanning tunnelling microscopy with a monolayer graphene sensing layer, thus enabling the generation of individual electron and hole quasiparticles in generalized Wigner crystals. We show that electron and hole quasiparticles have complementary wavefunction distributions and that thermodynamic gaps of ~50 meV exist for the 1/3 and 2/3 generalized Wigner crystal states in twisted WS 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2021

Imaging local discharge cascades for correlated electrons in WS 2 /WSe 2 moiré superlattices

Transition metal dichalcogenide moiré heterostructures provide an ideal platform to explore the extended Hubbard model, where long-range Coulomb interactions play a critical role in determining strongly correlated electron states. This has led to experimental observations of Mott insulator states at half filling as well as a variety of extended Wigner crystal states at different fractional fillings. However, a microscopic understanding of these emerging quantum phases is still lacking. Here we describe a scanning tunnelling microscopy (STM) technique for the local sensing and manipulation of correlated electrons in a gated WS 2 /WSe 2 moiré superlattice, which enables the experimental extraction of fundamental extended Hubbard model parameters. We demonstrate that the charge state of the local moiré sites can be imaged by their influence on the STM tunnelling current. In addition to imaging, we are also able to manipulate the charge state of correlated electrons. When we ramp the bias on the STM tip, there is a local discharge cascade of correlated electrons in the moiré superlattice, which allows us to estimate the nearest-neighbour Coulomb interaction. Two-dimensional mapping of the moiré electron charge states also enables us to determine the on-site energy fluctuations at different moiré sites. Furthermore, our technique should be broadly applicable to many semiconductor moiré systems, offering a powerful tool for the microscopic characterization and control of strongly correlated states in moiré superlattices.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Continuous symmetry breaking in a two-dimensional Rydberg array

Spontaneous symmetry breaking underlies much of our classification of phases of matter and their associated transitions. The nature of the underlying symmetry being broken determines many of the qualitative properties of the phase; this is illustrated by the case of discrete versus continuous symmetry breaking. Indeed, in contrast to the discrete case, the breaking of a continuous symmetry leads to the emergence of gapless Goldstone modes controlling, for instance, the thermodynamic stability of the ordered phase. Here, we realize a two-dimensional dipolar XY model that shows a continuous spin-rotational symmetry using a programmable Rydberg quantum simulator. We demonstrate the adiabatic preparation of correlated low-temperature states of both the XY ferromagnet and the XY antiferromagnet. In the ferromagnetic case, we characterize the presence of a long-range XY order, a feature prohibited in the absence of long-range dipolar interaction. In conclusion, our exploration of the many-body physics of XY interactions complements recent works using the Rydberg-blockade mechanism to realize Ising-type interactions showing discrete spin rotation symmetry.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Visualizing interfacial collective reaction behaviour of Li–S batteries

Benefiting from high energy density (2,600 Wh kg -1 )) and low cost, lithium-sulfur (Li-S) batteries are considered promising candidates for advanced energy-storage systems. Despite tremendous efforts in suppressing the long-standing shuttle effect of lithium polysulfides, understanding of the interfacial reactions of lithium polysulfides at the nanoscale remains elusive. This is mainly because of the limitations of in situ characterization tools in tracing the liquid-solid conversion of unstable lithium polysulfides at high temporal-spatial resolution. There is an urgent need to understand the coupled phenomena inside Li-S batteries, specifically, the dynamic distribution, aggregation, deposition and dissolution of lithium polysulfides. Here, by using in situ liquid-cell electrochemical transmission electron microscopy, we directly visualized the transformation of lithium polysulfides over electrode surfaces at the atomic scale. Notably, an unexpected gathering-induced collective charge transfer of lithium polysulfides was captured on the nanocluster active-centre-immobilized surface. It further induced an instantaneous deposition of nonequilibrium Li2S nanocrystals from the dense liquid phase of lithium polysulfides. Without mediation of active centres, the reactions followed a classical single-molecule pathway, lithium polysulfides transforming into Li 2 S 2 and Li 2 S step by step. Molecular dynamics simulations indicated that the long-range electrostatic interaction between active centres and lithium polysulfides promoted the formation of a dense phase consisting of Li + and S n 2- (2 < n ≤ 6), and the collective charge transfer in the dense phase was further verified by ab initio molecular dynamics simulations. Finally, the collective interfacial reaction pathway unveils a new transformation mechanism and deepens the fundamental understanding of Li-S batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Integrative analysis of the 3D genome and epigenome in mouse embryonic tissues

While a rich set of putative cis-regulatory sequences involved in mouse fetal development have been annotated recently on the basis of chromatin accessibility and histone modification patterns, delineating their role in developmentally regulated gene expression continues to be challenging. To fill this gap, here we mapped chromatin contacts between gene promoters and distal sequences across the genome in seven mouse fetal tissues and across six developmental stages of the forebrain. We identified 248,620 long-range chromatin interactions centered at 14,138 protein-coding genes and characterized their tissue-to-tissue variations and developmental dynamics. Integrative analysis of the interactome with previous epigenome and transcriptome datasets from the same tissues revealed a strong correlation between the chromatin contacts and chromatin state at distal enhancers, as well as gene expression patterns at predicted target genes. We predicted target genes of 15,098 candidate enhancers and used them to annotate target genes of homologous candidate enhancers in the human genome that harbor risk variants of human diseases. We present evidence that schizophrenia and other adult disease risk variants are frequently found in fetal enhancers, providing support for the hypothesis of fetal origins of adult diseases.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Magnetic ground states of honeycomb lattice Wigner crystals

Lattice Wigner crystal states stabilized by long-range Coulomb interactions have recently been realized in two-dimensional moiré materials. We employ large-scale unrestricted Hartree-Fock techniques to unveil the magnetic phase diagrams of honeycomb lattice Wigner crystals. For the three lattice filling factors with the largest charge gaps, $n=2/3,1/2,1/3$, the magnetic phase diagrams contain multiple phases, including ones with non-collinear and non-coplanar spin arrangements. We discuss magnetization evolution with external magnetic field, which has potential as an experimental signature of exotic spin states. Our theoretical results could potentially be validated in moiré materials formed from group VI transition metal dichalcogenide twisted homobilayers.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Electronic transport in two-dimensional high dielectric constant nanosystems

There has been remarkable recent progress in engineering high-dielectric constant two dimensional (2D) materials, which are being actively pursued for applications in nanoelectronics in capacitor and memory devices, energy storage, and high-frequency modulation in communication devices. Yet many of the unique properties of these systems are poorly understood and remain unexplored. Here we report a numerical study of hopping conductivity of the lateral network of capacitors, which models two-dimensional insulators, and demonstrate that 2D long-range Coulomb interactions lead to peculiar size effects. We find that the characteristic energy governing electronic transport scales logarithmically with either system size or electrostatic screening length depending on which one is shorter. Our results are relevant well beyond their immediate context, explaining, for example, recent experimental observations of logarithmic size dependence of electric conductivity of thin superconducting films in the critical vicinity of superconductor-insulator transition where a giant dielectric constant develops. Our findings mark a radical departure from the orthodox view of conductivity in 2D systems as a local characteristic of materials and establish its macroscopic global character as a generic property of high-dielectric constant 2D nanomaterials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Control of chemical reactivity by transition-state and beyond

It has been long established that the transition state for an activated reaction controls the overall reactivity, serving as the bottleneck for reaction flux. However, the role of the transition state in regulating quantum state resolved reactivity has only been addressed more recently, thanks to advances in both experimental and theoretical techniques. Here in this perspective, we discuss some recent advances in understanding mode-specific reaction dynamics in bimolecular reactions, mainly focusing on the X + H 2 O/CH 4 (X = H, F, Cl, and O( 3 P)) systems, extensively studied in our groups. These advances shed valuable light on the importance of the transition state in mode-specific and steric dynamics of these prototypical reactions. It is shown that many mode-specific phenomena can be understood in terms of a transition-state based model, which assumes in the sudden limit that the ability of a reactant mode for promoting the reaction stems from its coupling with the reaction coordinate at the transition state. Yet, in some cases the long-range anisotropic interactions in the entrance (or exit) valley, which govern how the trajectories reach (or leave) the transition state, also come into play, thus modifying the reactive outcomes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Near Surface Nucleation and Particle Mediated Growth of Colloidal Au Nanocrystals

During non-classical growth of nanostructures via assembly of primary nuclei, nucleation and assembly are assumed to be distinct processes: nanoparticles nucleate randomly and aggregate to form extended structures through Brownian motion in the presence of long-range attractive interactions. Here we investigate the relationship between these two processes by using in situ AFM, in situ, ex situ and cryo TEM and UV-Vis spectroscopy to observe growth of colloidal gold and simulations to develop a mechanistic model of the process. Our results reveal an inexorable link between nucleation and assembly with nuclei forming almost exclusively within a ~ 1 nm interfacial region of existing particles. The new particles immediately close the gap either through a diffusive jump or via growth of a neck between the seed and new particle, generating aggregates exhibiting features commonly attributed to oriented attachment of independently nucleated particles. The results demonstrate that creation of initial particle interfaces leads to local environments that redirect growth towards non-classical processes.

Cheng, Yingwen↗
DOE OSTI2020

Conversion between triplet pair states is controlled by molecular coupling in pentadithiophene thin films

In singlet fission (SF) the initially formed correlated triplet pair state, 1 (TT), may evolve toward independent triplet excitons or higher spin states of the (TT) species. The latter result is often considered undesirable from a light harvesting perspective but may be attractive for quantum information sciences (QIS) applications, as the final exciton pair can be spin-entangled and magnetically active with relatively long room temperature decoherence times. In this study we use ultrafast transient absorption (TA) and time-resolved electron paramagnetic resonance (TR-EPR) spectroscopy to monitor SF and triplet pair evolution in a series of alkyl silyl-functionalized pentadithiophene (PDT) thin films designed with systematically varying pairwise and long-range molecular interactions between PDT chromophores. The lifetime of the (TT) species varies from 40 ns to 1.5 μs, the latter of which is associated with extremely weak intermolecular coupling, sharp optical spectroscopic features, and complex TR-EPR spectra that are composed of a mixture of triplet and quintet-like features. On the other hand, more tightly coupled films produce broader transient optical spectra but simpler TR-EPR spectra consistent with significant population in 5 (TT) 0 . These distinctions are rationalized through the role of exciton diffusion and predictions of TT state mixing with low exchange coupling J versus pure spin substate population with larger J. The connection between population evolution using electronic and spin spectroscopies enables assignments that provide a more detailed picture of triplet pair evolution than previously presented and provides critical guidance for designing molecular QIS systems based on light-induced spin coherence.

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

Directing the far-from-equilibrium assembly of nanoparticles in confined liquid crystals by hydrodynamic fields

The assembly of nematic colloids relies on long-range elastic interactions that can be manipulated through external stimuli. Confinement and the presence of a hydrodynamic field alter the defect structures and the energetic interactions between the particles. Here, the assembly landscape of nanoparticles embedded in a nematic liquid crystal confined in a nanochannel under a pressure-driven flow is determined. The dynamics of the liquid crystal tensor alignment field is determined through a Poisson-Bracket framework, namely the Stark–Lubensky equations, coupled with the zero-Reynolds momentum equations and the liquid crystal Landau-de Gennes free energy functional. A second order semi-implicit time integration and a three-dimensional Galerkin finite element method are used to resolve flow and nematic fields under several conditions. In general, the zero Reynolds flow displaces the defects around the particles in the upstream direction and renders the surface anchoring ineffective when the flow strength dominates over the nematic elasticity. More importantly, the potential of mean force for particle assembly is non-monotonic independent of surface anchoring. Our results show that the confinement length scale determines the repulsion/attraction transition between colloids, while the flow strength modifies the static defect structure surrounding the particles and determines the magnitude of the energetic barrier for successful assembly. In the attractive regime, the particles move at different rates through the nematic until one particle eventually catches up with the other. This process occurs against or along the direction of flow depending on the flow strength. Ultimately, these results provide a template for engineering and controlling the transport and assembly of nanoparticles under far-from equilibrium conditions in anisotropic media.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Microscopic magnetic properties of an oxygen-doped Tb-Fe thin film by magnetic Compton scattering

The magnetic Compton scattering of a Tb{sub 32}Fe{sub 55}O{sub 13} film was measured in order to investigate the microscopic magnetization processes (i.e., the spin moment, orbital moment, and element specific moments). The trend of the spin magnetic moment was the same as that of the total magnetic moment but opposite to the orbital magnetic moment. In the low magnetic field region, the magnetic moments were not perfectly aligned perpendicular to the film surface, and the perpendicular components were found to mainly arise from the magnetic moment of Tb. Oxygen atoms hinder long range magnetic interaction and hence also affect the magnetization process of the magnetic moments of Tb and Fe.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Membrane formation by preferential solvation of ions in mixture of water, 3-methylpyridine, and sodium tetraphenylborate

The structure and dynamics of a ternary system composed of deuterium oxide (D{sub 2}O), 3-methylpyridine (3MP), and sodium tetraphenylborate (NaBPh{sub 4}) are investigated by means of small-angle neutron scattering (SANS) and neutron spin echo (NSE) techniques. In the SANS experiments, a structural phase transition is confirmed between a disordered-phase and an ordered-lamellar-phase upon variation of the composition and/or temperature of the mixture. The characteristic lengths of the structures is on the sub-micrometer scale. A dispersion relation of the structure is measured through NSE experiments, which shows that the relaxation rate follows a cubic relation with momentum transfer. This implies that the dynamics of the system are determined predominantly by membrane fluctuations. The present results indicate that 3MP-rich domains are microscopically separated from bulk water in the presence of NaBPh{sub 4}, and that the layers behave as membranes. These results are interpreted that preferential solvation of salt in each solvent induces a microphase separation between the solvents, and the periodic structure of 3MP-rich domains is stabilized by the long-range electrostatic interaction arising from Na{sup +} ions in D{sub 2}O-rich domains.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗