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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 541 records · Page 30
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Using Molecular Structure to Tune Intrachain and Interchain Charge Transport in Indacenodithiophene-Based Copolymers

Here, in this work, we compare two structurally near-amorphous rigid-rod polymers-poly(indacenodithiophene-co-benzothiadiazole), p(IDT-BT), and poly(indacenodithiophene-co-benzopyrollodione), p(IDT-BPD)-with orders of magnitude different mobilities to understand the effect charge carrier intrachain delocalization has on electronic transport. Quantum chemical calculations show that p(IDT-BPD) has a barrier to torsion that is significantly lower than that of p(IDT-BT) and is thus more likely to have reduced conjugation lengths. We utilize absorption and photoluminescence spectroscopy to characterize energetic disorder and show that p(IDT-BPD) has higher energetic disorder. Charge modulation spectroscopy (CMS) and model calculations are used to show that charge carriers are substantially delocalized in p(IDT-BT) and occupy near-uniform energetic environments. We find that mobility activated hopping barriers are similar in these two materials. Electronic structure calculations show that both intrachain and interchain couplings of monomer units are poor enough in p(IDT-BPD) that charge carriers collapse to single IDT units and transport via a through-space tunneling mechanism. This work highlights the remarkable charge transport properties of p(IDT-BT) by showing that high mobilities are achievable on device-relevant length scales with only 1D carrier delocalization.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Enhanced charge density wave with mobile superconducting vortices in La 1.885 Sr 0.115 CuO 4

Superconductivity in the cuprates is found to be intertwined with charge and spin density waves. Determining the interactions between the different types of order is crucial for understanding these important materials. Here, we elucidate the role of the charge density wave (CDW) in the prototypical cuprate La 1.885 Sr 0.115 CuO 4 , by studying the effects of large magnetic fields (H) up to 24 Tesla. At low temperatures (T), the observed CDW peaks reveal two distinct regions in the material: a majority phase with short-range CDW coexisting with superconductivity, and a minority phase with longer-range CDW coexisting with static spin density wave (SDW). With increasing magnetic field, the CDW first grows smoothly in a manner similar to the SDW. However, at high fields we discover a sudden increase in the CDW amplitude upon entering the vortex-liquid state. Our results signify strong coupling of the CDW to mobile superconducting vortices and link enhanced CDW amplitude with local superconducting pairing across the H -T phase diagram.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Fractionalization of subsystem symmetries in two dimensions

The fractionalization of global symmetry charges is a striking hallmark of topological quantum order. Here, we discuss the fractionalization of subsystem symmetries in two-dimensional topological phases. In line with previous no-go arguments, we show that subsystem symmetry fractionalization is not possible in many cases due to the additional rigid geometric structure of the symmetries. However, we identify a mechanism that allows fractionalization, involving global relations between macroscopically many symmetry generators. We find that anyons can fractionalize such relations, meaning that the total charge carried under all generators involved in the global relation is nontrivial, despite the fact that these generators multiply to the identity. We first discuss the general algebraic framework needed to characterize this type of fractionalization, and then explore this framework using a number of exactly solvable models with Z 2 topological order, including models having line and fractal symmetries. These models all showcase another necessary property of subsystem symmetry fractionalization: Fractionalized anyons must have restricted mobility when the symmetry is enforced, such that they are confined to a single line or point in the case of line and fractal symmetries, respectively. Looking forward, we expect that our identification of the importance of global relations in fractionalization will hold significance for the classification of phases with subsystem symmetries in all dimensions.

2-dimensional systems↗
DOE OSTI2020

Perfect short-range ordered alloy with line-compound-like properties in the ZnSnN 2 :ZnO system

We present a new solid-state material phase which is a disordered solid solution but offers many ordered line-compound features. The emergent physical phenomena are rooted in the perfect short-range order which conserves the local octet rule. We model the dual-sublattice-mixed semiconductor alloy (ZnSnN 2 ) 1-x (ZnO) 2x using first-principles calculations, Monte-Carlo simulations with a model Hamiltonian, and an extension of the regular solution model by incorporating short-range order. We demonstrate that this unique solid solution, occurring at a “magic” composition, can provide an electronically pristine character without disorder-induced charge localization and, therefore, a superior carrier transport similar to ordered phases. Interestingly, this phase shows singularities that are absent in the conventional solid-solution models, such as the regular solution and band-gap bowing model. Thermodynamically, this alloy phase has a sharply reduced enthalpy at its composition (like a line compound), but it still requires the entropy from long-range disorder to be stabilized at experimentally accessible temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2023

A novel large-scale EV charging scheduling algorithm considering V2G and reactive power management based on ADMM

Electric vehicle aggregators (EVAs) that utilize vehicle-to-grid (V2G) technologies can function as both controllable loads and virtual power plants, providing key energy management services to the distribution system operator (DSO). EVAs can also balance the grid’s reactive power as a virtual static VAR compensator (SVC) and provide voltage stability by utilizing advanced electric vehicle (EV) chargers that are capable of four-quadrant operations to provide reactive power management. Finally, managed charging can benefit EVAs themselves by minimizing power factor penalties in their electricity bills. In this paper, we propose a novel EV charging scheduling algorithm based on a hierarchical distributed optimization framework that minimizes peak load and provides reactive power compensation for the DSO by collaboration with EVAs that manage both the active and the reactive charging and discharging power of participating EVs. Utilizing the alternative direction method of multipliers (ADMM), the proposed distributed optimization approach scales well with increased EV charging infrastructure by balancing active and reactive power while decreasing computational burden. In our proposed hierarchical approach, each EVA schedules the active and reactive EV charging and discharging power for 1) reactive power compensation in order to minimize power factor penalty and electricity cost accrued by the EVA, 2) satisfaction of each EV’s energy demand at minimal charging cost, and 3) peak shaving and load management for the DSO. When compared with an uncoordinated charging model, the efficacy of this proposed model is successfully demonstrated through a 300% decreased peak EV load for the DSO, 28% lower electricity costs for EV users, and 98.55% smaller power factor penalty, along with 17.58% lower overall electricity costs, for EVAs. The performance of our approach is validated in a case study with 50 EVs at multiple EVAs in an IEEE 13-bus test case and compared the results with uncoordinated EV charging.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2021

Bias-dependent displacement damage effects in a silicon avalanche photodiode

Radiation effects studies on a commercial beveled-edge avalanche photodiode (APD) showed that applying reverse bias to the device during irradiation enhanced the severity of apparent damage. Proton microbeam irradiations were made using a proton beam energy of 2 MeV and fluence ranging from 2.0 × 10 10 to 5.1 × 10 12 cm -2 . Charge collection measurements using the ion beam induced charge (IBIC) technique showed that relative losses increased by up to an order of magnitude when the reverse bias applied during irradiation increased from 50 to 1500 V. The presence of reverse bias also led to equivalent losses in charge collection that would only be seen in irradiations with an order of magnitude higher fluence in unbiased APDs. The results demonstrate that bias-enhanced irradiation damage is insufficiently understood and must be accounted for in characterizations of radiation effects.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Photoinduced Halide Segregation in Ruddlesden–Popper 2D Mixed Halide Perovskite Films

2D lead halide perovskites, which exhibit bandgap tunability and increased chemical stability, have been found to be useful for designing optoelectronic devices. Reducing dimensionality with decreasing number of layers (n = 10–1) also imparts resistance to light-induced ion migration as seen from the halide ion segregation and dark recovery in mixed halide (Br:I = 50:50) perovskite films. The light-induced halide ion segregation efficiency, as determined from difference absorbance spectra, decreases from 20% to <1% as the dimensionality is decreased for 2D perovskite film from n = 10 to 1. The segregation rate constant (ksegregation), which decreases from 5.9 × 10 –3 s –1 (n = 10) to 3.6 × 10 –4 s –1 (n = 1), correlates well with nearly an order of magnitude decrease observed in charge-carrier lifetime (τ average = 233 ps for n = 10 vs τ avg = 27 ps for n = 1). The tightly bound excitons in 2D perovskites make charge separation less probable, which in turn decreases the halide mobility and resulting phase segregation. Furthermore, the importance of controlling the dimensionality of the 2D architecture in suppressing halide ion mobility is discussed.

14 SOLAR ENERGY↗
DOE OSTI2026

Shifting Defect Self-Regulation via Disordered Vacancies in Hollow Tin Perovskites

Tin(II)-based hybrid halide perovskites typically suffer from severe self-doping behavior as a result of facile oxidation of Sn(II) to Sn(IV), leading to high carrier densities (holes) and metallic-like conductivities that limit their applications. In this contribution, we describe how substituting the large ethylenediammonium cation for methylammonium in the intentionally defective “hollow” perovskite family, MA 1−x en x Sn 1−0.7x I 3−0.4x (MA = methylammonium, en = ethylenediammonium), where 0 ≤ x ≤ 0.38, effectively minimizes the intrinsic self-doping behavior. The use of a solvent-free, mechanochemical synthesis route further circumvents oxidative side reactions typical in solution processing, enabling more precise control and understanding of both composition and defect chemistry. Dark and time-resolved microwave conductivity measurements of these materials as a function of “x” reveal two regimes of conductivity suppression: at low x incorporation (x ≤ 0.15), the carrier density decreases by an order of magnitude via defect-mediated charge compensation, while higher substitution (0.15 < x ≤ 0.38) greatly reduces the carrier mobility. At these lower substitution levels, the observations suggest that intrinsic equilibrium tin vacancies are compensated instead by ionic defects in lieu of mobile holes. For the higher substitution levels, the less mobile carriers exhibit long recombination lifetimes, consistent with polaron-mediated transport. These findings establish a strategy for relatively low iodine chemical potential synthesis and defect-driven control of the carrier concentration in tin halide perovskites, advancing the rational discovery of dopable hybrid semiconductors.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Interactions between Per- and Polyfluoroalkyl Substances (PFAS) at the Water–Air Interface

Per- and polyfluoroalkyl substances (PFAS)--so-called “forever chemicals”--contaminate the drinking water of about 100 million people in the U.S. alone and are inefficiently removed by standard treatment techniques. A key property of these compounds that underlies their fate and transport and the efficacy of several promising remediation approaches is that they accumulate at the water−air interface. This phenomenon remains incompletely understood, particularly under conditions relevant to natural and treatment systems where water−air interfaces often carry significant loads of other organic contaminants or natural organic matter. To understand the impact of organic loading on PFAS adsorption, we carried out molecular dynamics simulations of PFAS at varying interfacial densities. We find that adsorbed PFAS form strong mutual interactions (attraction between perfluoroalkyl chains and electrostatic interactions among charged head groups) that give rise to ordered interfacial coatings. Furthermore, these interactions often involve near-cancellation of hydrophobic attraction and Coulomb repulsion. Our findings explain an apparent paradox whereby PFAS adsorption isotherms often suggest minimal mutual interactions while simultaneously displaying a high sensitivity to the composition and density of interfacial coatings. Consideration of the compounds present with PFAS at the interface has the potential to allow for more accurate predictions of fate and transport and the design of more efficient remediation approaches.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Understanding Hydrogenation Chemistry at MgB 2 Reactive Edges from Ab Initio Molecular Dynamics

Solid-state hydrogen storage materials often operate via transient, multistep chemical reactions at complex interfaces that are difficult to capture. Here, we use direct ab initio molecular dynamics simulations at accelerated temperatures and hydrogen pressures to probe the hydrogenation chemistry of the candidate material MgB 2 without a priori assumption of reaction pathways. Focusing on highly reactive ($10\overline{1}0$) edge planes where initial hydrogen attack is likely to occur, we track mechanistic steps toward the formation of hydrogen-saturated BH 4 – units and key chemical intermediates, involving H 2 dissociation, generation of functionalities and molecular complexes containing BH 2 and BH 3 motifs, and B–B bond breaking. Further, the genesis of higher-order boron clustering is also observed. Different charge states and chemical environments at the B-rich and Mg-rich edge planes are found to produce different chemical pathways and preferred speciation, with implications for overall hydrogenation kinetics. The reaction processes rely on B–H bond polarization and fluctuations between ionic and covalent character, which are critically enabled by the presence of Mg 2+ cations in the nearby interphase region. Our results provide guidance for devising kinetic improvement strategies for MgB 2 -based hydrogen storage materials, while also providing a template for exploring chemical pathways in other solid-state energy storage reactions.

08 HYDROGEN↗
DOE OSTI2020

Strong Differential Monovalent Anion Selectivity in Narrow Diameter Carbon Nanotube Porins

Inner pores of carbon nanotubes combine extremely fast water transport and ion selectivity that could potentially be useful for high-performance water desalination and separation applications. In this study, we used dye-quenching halide assays and stopped-flow spectrometry to determine intrinsic permeability of three small monovalent halide anions (chloride, bromide, iodide) and one pseudohalide anion (thiocyanate) through narrow 0.8 nm-diameter carbon nanotube porins (CNTPs). These measurements revealed unexpectedly strong differential ion selectivity with permeabilities of different ions varying by up to two orders of magnitude. Removal of the negative charge from the nanotube entrance increased anion permeability by only a relatively small factor, indicating that electrostatic repulsion was not a major determinant of CNTP selectivity. First principle molecular dynamics simulations revealed that the origin of this strong differential ion selectivity is partial dehydration of anions upon entry into the narrow CNTP channels.

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

Chiral structures of electric polarization vectors quantified by X-ray resonant scattering

Resonant elastic X-ray scattering (REXS) offers a unique tool to investigate solid-state systems providing spatial knowledge from diffraction combined with electronic information through the enhanced absorption process, allowing the probing of magnetic, charge, spin, and orbital degrees of spatial order together with electronic structure. A new promising application of REXS is to elucidate the chiral structure of electrical polarization emergent in a ferroelectric oxide superlattice in which the polarization vectors in the REXS amplitude are implicitly described through an anisotropic tensor corresponding to the quadrupole moment. Here, we present a detailed theoretical framework and analysis to quantitatively analyze the experimental results of Ti L-edge REXS of a polar vortex array formed in a PbTiO 3 /SrTiO 3 superlattice. Based on this theoretical framework, REXS for polar chiral structures can become a useful tool similar to x-ray resonant magnetic scattering (XRMS), enabling a comprehensive study of both electric and magnetic REXS on the chiral structures.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Mott and generalized Wigner crystal states in WSe 2 /WS 2 moiré superlattices

Moiré superlattices can be used to engineer strongly correlated electronic states in two-dimensional van der Waals heterostructures, as recently demonstrated in the correlated insulating and superconducting states observed in magic-angle twisted-bilayer graphene and ABC trilayer graphene/boron nitride moiré superlattices. Transition metal dichalcogenide moiré heterostructures provide another model system for the study of correlated quantum phenomena because of their strong light–matter interactions and large spin–orbit coupling. However, experimental observation of correlated insulating states in this system is challenging with traditional transport techniques. Here we report the optical detection of strongly correlated phases in semiconducting WSe 2 /WS 2 moiré superlattices. We use a sensitive optical detection technique and reveal a Mott insulator state at one hole per superlattice site and surprising insulating phases at 1/3 and 2/3 filling of the superlattice, which we assign to generalized Wigner crystallization on the underlying lattice. Furthermore, the spin–valley optical selection rules of transition metal dichalcogenide heterostructures allow us to optically create and investigate low-energy excited spin states in the Mott insulator. We measure a very long spin relaxation lifetime of many microseconds in the Mott insulating state, orders of magnitude longer than that of charge excitations. Here, our studies highlight the value of using moiré superlattices beyond graphene to explore correlated physics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Design, synthesis and characterization of fused bithiazole- and dithiophene-based low bandgap thienylenevinylene copolymers

The structural rigidity of fused units in the polymer backbone, in addition to the resulting stabilizing effect of the quinoidal structure, and tunable electronic properties have played a key role in promoting highly-ordered π-stacking moieties, exhibiting promising charge carrier mobilities. The electron-deficient thiazole moiety shows high planarity and effective π–π stacking, which leads to the reduction in the energy levels of the highest occupied and lowest unoccupied molecular orbitals (HOMO/LUMO), and ideally enhances the electron charge mobility. Four heterocycle-based monomers BTzS, BTzSe, DTS, and DTG based on fused bithiazole and dithiophene units incorporated with sulfur, selenium, silicon, and germanium as the bridging atoms were synthesized and characterized. Here, the monomers were copolymerized with the electron-rich alkylated thienylenevinylene (TV) unit to afford copolymers P1–P4. The thermal, optical, and electrochemical properties and crystallinity of the copolymers were thoroughly investigated. Extensive OFET device optimization using different solvents and annealing temperatures resulted in the best charge mobility of 0.09 cm2 V –1 s –1 for the electron-deficient bithiazole BTzS copolymer P1 and 0.36 cm2 V –1 s –1 for the DTS copolymer P3.

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

Positive charging of grains in an afterglow plasma is enhanced by ions drifting in an electric field

In a plasma, the polarity of a dust grain's charge is typically negative, but it can reverse and become positive in an afterglow, when the power sustaining the plasma is switched off. This positive charging, which occurs in the afterglow's first few milliseconds, is studied for grains much larger than a few nm. It is hypothesized that the positive charging is enhanced by the presence of a dc electric field, which causes ions to drift through the neutral gas. A larger value of the reduced electric field E/N leads to a larger ion kinetic energy and thus a greater collection of positive charge on a grain. The maximum possible positive charge is attained if the grain's surface potential rises to match the ion kinetic energy, at a time before ions have departed and the grain's charge becomes frozen. Thereafter, when vacuum conditions prevail, the grain will retain its positive residual charge. In an experiment, dust grains were electrically levitated in a capacitively coupled plasma until the power was abruptly turned off. In the afterglow, grains fell faster than expected due to gravity alone, indicating a downward electric force, in the presence of a remaining dc electric field. Acceleration measurements yielded repeatable results for the residual charge's value, which was of the order +10 4 e and increased with E/N, supporting the hypothesis.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Ion-driven destabilization of a toroidal electron plasma—A 3D3V PIC simulation

Ion-driven destabilization of a toroidal electron plasma in a small aspect ratio axisymmetric toroidal device is reported for A r + ions of different initial density values using a high fidelity 3D3V PIC solver. Stability of a recently discovered quiescent quasi-steady state (QQS) of a toroidal electron plasma obtained from “seed” solution as a result of entropy extremization at zero inertia is addressed in the presence of a small ion population. An initial value (f0) of the ion fraction (f = n i / n e) and the corresponding secondary electrons are “preloaded” into the system after the electron plasma attains a QQS state. This procedure is regarded as a proxy to the conventional production of ions in the experimental devices via impact ionization. The resulting electron plasma exhibits destabilized “center of charge motion” (m = 1) along with higher order harmonics with dominant power in the second harmonic. Gradual loss of ions (and also electrons) is observed resulting in time varying f values. Beyond a certain value of f0 (≥ 0.005), growth in wall probe current is observed, which saturates at later simulation time due to the loss of particles. In conclusion, trajectories of ion particles indicate ion trapping in the potential well, which is qualitatively similar to the ion resonance instability in pure electron plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Particle-hole asymmetric phases in doped twisted bilayer graphene

Twisted bilayer graphene (TBG) has emerged as a paradigmatic platform for exploring the interplay between strong interactions in a multi-band system with nearly flat bands, while offering unprecedented control over the filling fraction of electron/hole carriers. Despite much theoretical work, developing a comprehensive ab initio model for this system has proven challenging due to the inherent trade-off between accurately describing the band structure and incorporating the interactions within the Hamiltonian. Here, we constructed an extended multi-orbital Hubbard model, and performed Hartree-Fock (HF) calculations to explore its phase diagram across commensurate fillings. We found several nearly-degenerate insulating states at charge neutrality, all of which exhibit orbital orders. We also observed that most of the Hartree–Fock ground states exhibit a generalized valley Hund’s-like rule, resulting in valley polarization. Importantly, we show that the incorporation of the intra-valley and inter-valley exchange interactions is crucial to properly stabilize the ordered symmetry-broken states. In agreement with experiments, we find significant particle-hole asymmetry, which underscores the importance of using particle-hole asymmetric models.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Forward doubly-virtual Compton scattering off an unpolarized deuteron in pionless effective field theory

In this work, we calculate the forward unpolarised doubly-virtual Compton scattering (VVCS) off the deuteron in the framework of pionless effective field theory, up to next-to-next-to-next-to-leading order (N3LO) for the longitudinal and next-to-leading order (NLO) for the transverse amplitude. The charge elastic form factor of the deuteron, obtained from the residue of the longitudinal VVCS amplitude, is used to extract the value of the single unknown two-nucleon one-photon contact coupling that enters the longitudinal amplitude at N3LO. We also study the lowest spin-independent generalised polarisabilities of the deuteron. The calculated unpolarised VVCS amplitude provides a high-precision model-independent input for a future calculation of the two-photon-exchange correction to the Lamb shift of muonic deuterium.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗