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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 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Conjugated Polymer Controlled Morphology and Charge Transport of Small-Molecule Organic Semiconductors

In this study, we report an efective approach to tune the crystallization, microstructure and charge transport of solution-processed organic semiconductors by blending with a conjugated polymer additive poly(3-hexylthiophene) (P3HT). When 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS pentacene) was used as a model semiconductor material to mix with diferent amount of P3HT, their intermolecular interactions led to distinctive TIPS pentacene flm morphologies, including randomly-oriented crystal ribbons, elongated needles with enhanced long-range order, and grasslike curved microwires with interlinkages. Each type of morphology was found to further correlate to considerably diferent charge transport and device performance. As compared to pristine TIPS pentacene devices, bottom-gate, top-contact OTFTs with 2% in weight P3HT additive showed a 2-fold and 5-fold improvement of average feld-efect mobility and performance consistency (defned as the ratio of average mobility to the standard deviation), respectively. The improvement in transistor electrical performance can be attributed to the combined efect of enhanced crystal orientation and uniformity, as well as increased areal coverage. This work can be applied beyond the particular example demonstrated in this study and to tune the charge transport of other small-molecule organic semiconductors in general.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Charge Transport Properties of Lithium Superoxide in Li–O 2 Batteries

The theoretical energy density of lithium–oxygen (Li–O 2 ) batteries is extremely high, although there are many challenges that must be overcome to achieve high energy density in a manufactured cell. For example, little is known about the properties of one of the key intermediates, lithium superoxide (LiO 2 ), which until recently had not been stabilized in bulk form. In this work, lithium superoxide was deposited onto iridium–reduced graphene oxide (Ir–rGO) cathodes in a Li–O 2 system under a flow of O 2 . Lithium peroxide (Li 2 O 2 ) was subsequently produced on the cathode surface in an inert Ar atmosphere. Based on a detailed analysis of electrochemical impedance spectroscopy data, it was demonstrated experimentally for the first time that the charge transport resistance through LiO 2 was much lower than for Li 2 O 2 and correlated with lower LiO 2 charge overpotentials. We report this result indicates that LiO 2 has good electronic conductivity and confirms previous theoretical predictions that bulk LiO 2 has better charge transport properties than Li 2 O 2 . In addition, impedance and other characterization of Li 2 O 2 formation from LiO 2 in an Ar atmosphere revealed that when surface-mediated Li 2 O 2 formation occurs, it has a significantly lower discharge potential than when it forms through a solution-phase-mediated process. These significant findings will contribute to the development of Li–O 2 batteries through better understanding of LiO 2 properties and formation mechanisms.

25 ENERGY STORAGE↗
DOE OSTI2020

Enhanced Electron-Phonon Coupling for Charge-Density-Wave Formation in La 1.8-$x$ Eu 0.2 Sr $x$ CuO 4+$δ$

Charge density wave (CDW) correlations are prevalent in all copper-oxide superconductors. While CDWs in conventional metals are driven by coupling between lattice vibrations and electrons, the role of the electron-phonon coupling (EPC) in cuprate CDWs is strongly debated. Using Cu L 3 edge resonant inelastic x-ray scattering, we study the CDW and Cu-O bond-stretching phonons in the stripe-ordered cuprate La 1.8-x Eu 0.2 Sr x CuO 4+δ . In this work, we investigate the interplay between charge order and EPC as a function of doping and temperature and find that the EPC is enhanced in a narrow momentum region around the CDW ordering vector. By detuning the incident photon energy from the absorption resonance, we extract an EPC matrix element at the CDW ordering vector of M ≃ 0.36 eV , which decreases to M ≃ 0.30 eV at high temperature in the absence of the CDW. Our results suggest a feedback mechanism in which the CDW enhances the EPC which, in turn, further stabilizes the CDW.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Study of the interaction between $Ξ$ baryons and light mesons via femtoscopy at the LHC

Meson-baryon systems with strangeness content provide a unique laboratory for investigating the strong interaction and testing theoretical models of hadron structure and dynamics. In this work, the measured correlation functions for oppositely charged $Ξ$-K and $Ξ$ − 𝜋 pairs obtained in high-multiplicity pp collisions at $\sqrt{𝑠}$ = 13 TeV at the LHC are presented. For the first time, high-precision data on the $Ξ$-K interaction are delivered at small relative momenta. The scattering lengths, extracted via the Lednický–Lyuboshits expression of the pair wavefunction, indicate a repulsive and a shallow attractive strong interaction for the $Ξ$-K and $Ξ$ − 𝜋 systems, respectively. The $Ξ$(1620) and $Ξ$(1690) states are observed in the $Ξ$ − 𝜋 correlation function and their properties, mass and width, are determined. These measurements are in agreement with other available results. Such high-precision data can help refine the understanding of these resonant states, provide stronger constraints for chirally motivated potentials, and address the key challenge of describing the coupled-channel dynamics that may give rise to molecular configurations .

Femtoscopy↗
DOE OSTI2022

Electronic Raman scattering in the 2D antiferromagnet NiPS 3

Correlated-electron systems have long been an important platform for various interesting phenomena and fundamental questions in condensed matter physics. As a pivotal process in these systems, d-d transitions have been suggested as a key factor toward realizing optical spin control in two-dimensional (2D) magnets. However, it remains unclear how d-d excitations behave in quasi-2D systems with strong electronic correlation and spin-charge coupling. Here, we present a systematic electronic Raman spectroscopy investigation on d-d transitions in a 2D antiferromagnet—NiPS 3 , from bulk to atomically thin samples. Two electronic Raman modes originating from the scattering of incident photons with d electrons in Ni 2+ ions are observed at ~1.0 eV. This electronic process persists down to trilayer flakes and exhibits insensitivity to the spin ordering of NiPS 3 . Our study demonstrates the utility of electronic Raman scattering in investigating the unique electronic structure and its coupling to magnetism in correlated 2D magnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Direct Spectroscopic Observation of the Hole Polaron in Lead Halide Perovskites

Intrinsic photophysical origin of lead halide perovskites (LHPs) succeeding in optolectronic applications still remains hotly debated. In this study, by using the ultrafast X-ray transient absorption spectroscopy, we successfully tracked the fate of photogenerated charge carriers at room temperature within the thin films of two classic LHPs, namely MAPbBr 3 (MA: CH 3 NH 3 ) and FAPbBr 3 (FA: CH(NH 2 ) 2 ). We clearly observed in both thin films that the hole polaron is formed by localizing the photogenerated hole at Br 4p orbital and concurrently distorting the local structure surrounding Br atom after the photoexcitation. Furthermore, the bigger cation FA in the cavity of [PbBr 6 ] 4- octahedral framework induces larger hole polaron effect due to its p orbital hybridization into valence and conduction bands, correlating with the slower charge carrier recombination dynamics. Our direct experimental observation of the localized hole polaron in perovskites should advance the fundamental comprehension of charge carrier behavior within LHPs and their related devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Measurement of D 0 -meson + hadron two-dimensional angular correlations in Au + Au collisions at s N N = 200 GeV

Open heavy flavor hadrons provide unique probes of the medium produced in ultra-relativistic heavy-ion collisions. Due to their increased mass relative to light-flavor hadrons, long lifetime, and early production in hard-scattering interactions, they provide access to the full evolution of the partonic medium formed in heavy-ion collisions. This paper reports two-dimensional (2D) angular correlations between neutral D-mesons and unidentified charged particles produced in minimum-bias Au+Au collisions at s N N = 200 GeV. D 0 and D 0 ¯ mesons are reconstructed via their weak decay to K ∓ π ± using the Heavy Flavor Tracker (HFT) in the Solenoidal Tracker at RHIC (STAR) experiment. Correlations on relative pseudorapidity and azimuth (Δη,ΔΦ) are presented for peripheral, mid-central and central collisions with D 0 transverse momentum from 2 to 10 GeV/c. Attention is focused on the 2D peaked correlation structure near the triggered D 0 -meson, the {\em near-side} (NS) peak, which serves as a proxy for a charm-quark containing jet. The correlated NS yield of charged particles per D 0 -meson and the 2D widths of the NS peak increase significantly from peripheral to central collisions. These results are compared with similar correlations using unidentified charged particles, consisting primarily of light-flavor hadrons, at similar trigger particle momenta. Similar per-trigger yields and widths of the NS correlation peak are observed. Here, the present results provide additional evidence that D 0 -mesons undergo significant interactions with the medium formed in heavy-ion collision and show, for the first time, significant centrality evolution of the NS 2D peak in the correlations of particles associated with a heavy-flavor hadron produced in these collisions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Compressing Hamiltonians with ab initio downfolding for simulating strongly-correlated materials on quantum computers

The accurate first-principles description of strongly correlated materials is an important and challenging problem in condensed matter physics. Ab initio downfolding has emerged as a way of deriving compressed many-body Hamiltonians that maintain the essential physics of strongly correlated materials. The solution of these material-specific models is still exponentially difficult to generate on classical computers, but quantum algorithms allow for a significant speed-up in obtaining the ground states of these compressed Hamiltonians. Here, we demonstrate that using quantum algorithms to obtain the properties of downfolded Hamiltonians can indeed yield high-fidelity solutions. By combining ab initio downfolding and variational quantum eigensolvers, we correctly predict the antiferromagnetic state of one-dimensional cuprate Ca 2 Cu O 3 , the excitonic ground state of monolayer W Te 2 , and the charge-ordered state of correlated metal Sr VO 3 . Numerical simulations using a classical tensor network implementation of variational quantum eigensolvers allow us to simulate large models with up to 54 qubits and encompassing up to four bands in the correlated subspace, which is indicative of the complexity that our framework can address. Through these methods we demonstrate the potential of classical preoptimization and downfolding techniques for enabling efficient materials simulation using quantum algorithms.

Alvertis, Antonios M. [NASA, Ames; LBNL, Berkeley]↗
DOE OSTI2021

Re-entrance to a ferromagnetic insulator with oxygen-vacancy ordering in the La 0.7 Sr 0.3 MnO 3 /SrTiO 3 superlattice

The charge-density wave is correlated with the properties in transition metal oxides, and regulating this state is important to explore the potential of oxides. Defects could modulate the local environment, in which the effect is subject to the concentration and arrangement, and an artificial arrangement of defect-ordering is highly expected to design the material properties. In this work, the ordering of oxygen vacancies with a preferred location on the (001) La/SrO plane by self-structural optimization was induced in La 0.7 Sr 0.3 MnO 3 /SrTiO 3 superlattices with medium oxygen pressure during SrTiO 3 deposition, and then the ferromagnetic charge-ordering (CO)/charge-density-wave (CDW) state was formed in La 0.7 Sr 0.3 MnO 3 with susceptibility to magnetic field, temperature, and superlattice configuration. In addition, re-entrance to the ferromagnetic insulator CO/CDW could be induced by a high magnetic field. The selective occupancy of oxygen vacancies on the (001) La/SrO plane and the phase fluctuation around the CO/CDW-to-ferromagnetic metal phase transition were critical to the above properties. The interfacial diffusion with atomic-level resolution to control oxygen vacancies could be used in other magnetoelectric systems and corresponding device applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Structuring, stochastic behavior, and charge storage capacity of redox-active microemulsions formulated with mixtures of toluene and ionic liquid as oil phase

Oil/water microemulsions (µEs) are promising electrolytes for redox flow batteries (RFBs) as they simultaneously improve charge capacity and ionic conductivity. Here, we report the successful formulation of bicontinuous µEs where the oil phase is a solution of trihexyltetradecylphosphonium bis(trifluoromethylsulfonyl)amide ionic liquid in toluene with redox-active ferrocene. We examined the effect of supporting electrolyte anion (NO 3 – , Cl – , ClO 4 – ) on the structure, reactivity, transport, and electrolytic performance of redox-active µEs. Neutron scattering and nuclear magnetic resonance showed that the domain size increased as Cl – > NO 3 – > ClO 4 – while the ferrocene diffusion coefficient increased as NO 3 – > Cl – > ClO 4 – . Scanning electrochemical microscopy indicated anion-dependent current fluctuations during electrolysis, with ClO 4 – exhibiting the least high-frequency oscillations, which correlate to the highest charge and discharge capacity and reversibility. All ionic liquid containing systems improved the performance of toluene-based µEs, highlighting new design principles for these electrolytes.

diffusion↗
DOE OSTI2024

Luther-Emery liquid and dominant singlet superconductivity in the hole-doped Haldane spin-1 chain

We investigate the pairing tendencies in the hole-doped Haldane spin-1 chain. To allow for doping, we extend the original spin chain Hamiltonian into a fermionic model involving a two-orbital Hubbard chain at intermediate or strong repulsive interaction strengths U and for degenerate orbitals. At half filling and large U, the ferromagnetic Hund's coupling, J H , generates effective spin-1 moments, with antiferromagnetic correlations between sites. Using large-scale density matrix renormalization group calculations, we accurately study the system's behavior under light hole-doping. For U = 1.6 in units of the noninteracting bandwidth and for J H /U ≳ 0.275, we find that singlet pairing dominates the long-distance physics, establishing this system as a promising platform for repulsively mediated superconductivity. We provide concrete examples of materials that could realize the physics described here. We also provide evidence that the system approaches a Luther-Emery liquid state at large system sizes, reminiscent of the behavior of doped one-orbital two-leg ladders at weak coupling, which also have superconducting tendencies. The numerically calculated central charge approaches one in the thermodynamic limit, indicating a single gapless mode as is expected for the Luther-Emery state. Exponents characterizing the power-law decays of singlet pair-pair and charge density-density correlations are determined, and found to approximately satisfy the Luther-Emery identity.

1-dimensional systems↗
DOE OSTI2021

Scaling Theory of Neutral Sequence-Specific Polyampholytes

The primary sequence of charged monomers in a polyampholyte has a profound effect on its conformational properties. In this work, theory and simulations are used to predict how the sequence influences the single-chain behavior of globally neutral polyampholytes (PAs) under salt-free conditions. We consider PAs with Markov statistics of charges, where charge “blockiness” is defined by the correlation λ along the chain. These PAs cover a wide spectrum of primary sequences ranging from alternating (λ = –1) to ideally random (λ = 0) to diblock (λ → 1). In a theta solvent, sufficiently long PAs of any primary sequence form globules, but their internal structure, as well as the position and sharpness of the coil–globule transition, crucially depends on λ. Further, using scaling arguments, we demonstrate that the excess charge of the globule correlation volume (blob) increases with increasing λ, thereby inducing stronger Coulomb attractions between neighboring blobs of opposite charge and leading to higher density PA globules. Scaling predictions are supported by the results of the random phase approximation (RPA) and coarse-grained molecular dynamics simulations. A generalization to good and poor solvents is presented that enables the construction of the resulting scaling diagram of PA conformations in terms of solvent quality and charge blockiness, thereby providing a comprehensive molecular understanding of the role of the PA primary sequence in the chain structure.

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

Charge Condensation and Lattice Coupling Drives Stripe Formation in Nickelates

Revealing the predominant driving force behind symmetry breaking in correlated materials is sometimes a formidable task due to the intertwined nature of different degrees of freedom. This is the case for La 2–x Sr x NiO 4+δ , in which coupled incommensurate charge and spin stripes form at low temperatures. Here, we use resonant x-ray photon correlation spectroscopy to study the temporal stability and domain memory of the charge and spin stripes in La 2–x Sr x NiO 4+δ . Although spin stripes are more spatially correlated, charge stripes maintain a better temporal stability against temperature change. More intriguingly, charge order shows robust domain memory with thermal cycling up to 250 K, far above the ordering temperature. Furthermore, these results demonstrate the pinning of charge stripes to the lattice and that charge condensation is the predominant factor in the formation of stripe orders in nickelates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Resolving the Solvation Structure and Transport Properties of Aqueous Zinc Electrolytes from Salt-in-Water to Water-in-Salt Using Neural Network Potential

Zn Cl 2 solutions are promising electrolytes for aqueous zinc-ion batteries. Here, we report a joint computational and experimental study of the structural and dynamic properties of aqueous Zn Cl 2 electrolytes with concentrations ranging from salt-in-water to water-in-salt (WIS). By developing a neural network potential (NNP) model, we perform molecular dynamics (MD) simulations with accuracy but at much larger lengths and longer timescales. The NNP predicted structures are validated by the structure factors measured by X-ray total scattering experiments. The MD trajectories provide a comprehensive and quantitative picture of the Zn 2 + solvation shell structures. Additionally, we find that the O − H covalent bonds in water are strengthened with increasing salt concentration, thus expanding the electrochemical stability window of aqueous electrolytes. In terms of dynamic properties, the calculated and experimentally measured conductivities are in good agreement. Through the analysis of the calculated cation transference number, we propose a three-stage charge carrier transport mechanism with increasing concentration: independent ion transport, strongly correlated ion transport, and small positive charge carrier diffusion through negatively charged polymeric clusters. Our study provides fundamental atomic scale insights into the structure and transport properties of the Zn Cl 2 electrolyte that can aid the optimization and development of WIS electrolytes. Published by the American Physical Society 2025

25 ENERGY STORAGE↗
DOE OSTI2020

One Structure, Two Elements—LuGe 2 Superconductor vs Ordinary Metallic Conductor LuSn 2 . A Case Study on How Site-Selective Germanium for Tin Atom Substitution Leads to Modulating of the Charge Distribution

The substitution of chemically similar elements in a given crystal structure is an effective way to enhance physical properties, but the understanding on such improvements is usually impeded because the substitutions are random, and the roles of the different atoms cannot be distinguished by crystallographic symmetry. Herein, we provide a detailed crystallographic analysis and property measurements for the continuous solid solutions LuGe x Sn 2–x (0 < x < 2). The results show that there is no apparent change of the global symmetry, with the end-members LuGe 2 and LuSn 2 , as well as the intermediate LuGe x Sn 2–x compositions adopting the ZrSi 2 type structure (space group Cmcm, Pearson index oC12). Yet, the refinements of the crystal structures from single-crystal X-ray diffraction data show that Ge–Sn atom substitutions are not random, but occur preferentially at the zig-zag chain. The patterned distribution of two group 14 elements leads to a significant variation in chemical bonding and charge ordering within the other structural fragment, the 2D square nets, thereby resulting in tuned electron transport. The enhancement is greater than the typical Bloch-Gruneisen model, and more akin to the parallel-resistor model. Magnetization measurements on single crystals show bulk superconductivity in all LuGe x Sn 2–x samples with shielding fractions as high as 90%. Specific heat data confirm the effect to originate from residual metallic tin in the material, indicating that Sn atom substitutions in the 2D square nets cause disruptions of the hypervalent bonding and local anisotropy, which ultimately leads to vanishing of the superconducting state in the end-member LuGe 2 . This work sheds light on how the complexity in chemical interactions by two different carbon congeners leads to changes in the physical properties and how they can be correlated with the induced charge distribution. Furthermore, these studies also provide a general approach to modulation of charge density, and thus, of emerging physical properties in other classes of intermetallic systems based on the main-group elements of groups 13 to 15.

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

Nature of Excitons and Their Ligand-Mediated Delocalization in Nickel Dihalide Charge-Transfer Insulators

The fundamental optical excitations of correlated transition-metal compounds are typically identified with multielectronic transitions localized at the transition-metal site, such as d d transitions. In this vein, intense interest has surrounded the appearance of sharp, below-band-gap optical transitions, i.e., excitons, within the magnetic phase of correlated Ni 2 + van der Waals magnets. The interplay of magnetic and charge-transfer insulating ground states in Ni 2 + systems raises intriguing questions on the roles of long-range magnetic order and of metal-ligand charge transfer in the exciton nature, which inspired microscopic descriptions beyond typical d d excitations. Here we study the impact of charge transfer and magnetic order on the excitation spectrum of the nickel dihalides ( Ni X 2 , X = Cl , Br, and I) using Ni- L 3 edge resonant inelastic x-ray scattering (RIXS). In all compounds, we detect sharp excitations, analogous to the recently reported excitons, and assign them to spin-singlet multiplets of octahedrally coordinated Ni 2 + stabilized by intra-atomic Hund’s exchange. Additionally, we demonstrate that these excitons are dispersive using momentum-resolved RIXS. Our data evidence a ligand-mediated multiplet dispersion, which is tuned by the charge-transfer gap and independent of the presence of long-range magnetic order. This reveals the mechanisms governing nonlocal interactions of on-site d d excitations with the surrounding crystal or magnetic structure, in analogy to ground-state superexchange. These measurements thus establish the roles of magnetic order, self-doped ligand holes, and intersite-coupling mechanisms for the properties of d d excitations in charge-transfer insulators. Published by the American Physical Society 2024

2-dimensional systems↗
DOE OSTI2025

Unveiling the role of halide mixing in the crystallization kinetics and charge transfer mechanisms of wide-bandgap organic–inorganic halide perovskites

Understanding the crystallization kinetics of Br–I mixed-halide WBG perovskite films, and their correlation to the crystallographic structure and charge transfer dynamics, is critical for advancing WBG perovskite devices. Despite many efforts to increase the photovoltaic performances of wide-bandgap (WBG, with a Br content above 20%) perovskite solar cells based on bromine–iodine (Br–I) mixed-halide perovskites, understanding the crystallization kinetics of WBG perovskite films, as well as the role of Br mixing in the crystallization kinetics, is still lacking. Furthermore, an overlooked aspect is the correlation of the halide compositions, crystallization kinetics, crystallographic structure, and charge transfer dynamics. Here, we unveil that Br–I mixed-halide WBG perovskite films undergo two intrinsically different crystallization kinetic processes. One is the intermediate solvent-complex phase-assisted growth (I-rich), and the other is top-to-bottom downward growth (Br-rich). Such downward growth (including high Br concentrations) correlates with the formation of a highly vertically oriented perovskite film, which is accompanied by defect formation caused by a dissolving and recrystallization process coupled with halide homogenization. Consequently, Br-rich WBG perovskite films exhibit enhanced charge carrier transport, but are concurrently plagued by non-radiative charge recombination. Addressing this fundamental perspective is critical to precisely tailor Br-related crystallization, which significantly affects the structure and optoelectronic properties of WBG perovskite films and devices.

Li, Nian↗
DOE OSTI2026

Measuring pH Changes Inside a Bipolar Membrane Junction

Here, the local pH environment within bipolar membrane (BPM) junctions is complex and not well understood, yet it is important to control for advancing the performance of BPM-based electrochemical systems. We report a voltammetric strategy using an ultrathin Ni mesh pH probe to spatially resolve pH changes in the BPM junction during model BPM electrolyzer operation. Under reverse bias, we observe depletion of OH – at the anion-exchange layer (AEL) interface, with a degree diminishing with increasing distance from the AEL. These gradients correlate with current-dependent water dissociation (WD) and are modulated by the electric field and the surface charge state of the catalyst. By correlating spatial pH profiles with the surface-charging behavior of WD catalysts, we explore a mechanism of catalyst-mediated H + and OH – transfer facilitated by hydrogen-bonding networks. These findings highlight the role of local chemistry and electrostatics in BPM performance and offer new methods to probe and engineer catalytic junctions in electrochemical energy devices.

Hou, Shujin [University of California, Berkeley, C↗