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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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Superconductivity in Oxides Generated by Percolating Electron or Hole Bipolarons

It is remarkable that in over three decades since the discovery of high-temperature superconductivity (HTS) in cuprates, no other class of materials has been found to exhibit this property above the liquid nitrogen boiling point at ambient pressure. Here, we describe the conformation of hole and electron bipolarons in doped cuprates and tungstates. Important similarities and differences between them are discussed. Both hole and electron bipolarons can percolate forming filaments or clusters in the bulk or on the surfaces as well. Upon cooling, these electronic objects can show superconducting properties. It is proposed that oxygen-reduced tungsten oxide WO{sub 3−x} in bulk or thin film form is a promising material to explore the HTS. Such material would be another example of bipolaronic superconductivity similar to cuprates. However, there is also an important difference: in the cuprates, holes predominantly enter the oxygen orbitals and hole bipolarons are composed of three-spin polarons, whereas in the tungstates, doped electrons are located on tungsten ions and W{sup 5+}–O{sup 2−}–W{sup 5+}electron bipolarons form from 5d{sup 1} W{sup 5+} polarons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Dimensional Crossover in Anisotropic Percolation on ℤ{sup d+s}

We consider bond percolation on ℤ{sup d}×ℤ{sup s} where edges of ℤ{sup d} are open with probability p<p{sub c}(ℤ{sup d}) and edges of ℤ{sup s} are open with probability q, independently of all others. We obtain bounds for the critical curve in (p, q), with p close to the critical threshold p{sub c}(ℤ{sup d}). The results are related to the so-called dimensional crossover from ℤ{sup d} to ℤ{sup d+s}.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Regularity of the Speed of Biased Random Walk in a One-Dimensional Percolation Model

We consider biased random walks on the infinite cluster of a conditional bond percolation model on the infinite ladder graph. Axelson-Fisk and Häggström established for this model a phase transition for the asymptotic linear speed v̄ of the walk. Namely, there exists some critical value λ{sub c}>0 such that v̄>0 if λ∈(0,λ{sub c}) and v̄=0 if λ≥λ{sub c}. We show that the speed v̄ is continuous in λ on (0,∞) and differentiable on (0,λ{sub c}/2). Moreover, we characterize the derivative as a covariance. For the proof of the differentiability of v̄ on (0,λ{sub c}/2), we require and prove a central limit theorem for the biased random walk. Additionally, we prove that the central limit theorem fails to hold for λ≥λ{sub c}/2.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Hyperscaling for Oriented Percolation in 1+1 Space–Time Dimensions

Consider nearest-neighbor oriented percolation in d+1 space–time dimensions. Let ρ,η,ν be the critical exponents for the survival probability up to time t, the expected number of vertices at time t connected from the space–time origin, and the gyration radius of those vertices, respectively. We prove that the hyperscaling inequality dν≥η+2ρ, which holds for all d≥1 and is a strict inequality above the upper-critical dimension 4, becomes an equality for d=1, i.e., ν=η+2ρ, provided existence of at least two among ρ,η,ν. The key to the proof is the recent result on the critical box-crossing property by Duminil-Copin et al. [6].

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Structural Correlations and Percolation in Twisted Perylene Diimides Using a Simple Anisotropic Coarse-Grained Model

Large, twisted, and fused conjugated molecular architectures have begun to appear more prominently in the organic semiconductor literature. From a modeling perspective, such structures present a challenge to conventional simulation techniques; atomistic resolutions are computationally inefficient, while traditional isotropic coarse-grained models do not capture the inherent anisotropies of the molecules. In this work, we develop a simple coarse-grained model that explicitly incorporates the anisotropy of these molecular architectures, thereby providing a route toward analyzing pi-stacking, and thus qualitative electronic structure, at a computationally efficient coarse-grained resolution. Our simple coarse-grained model maintains relative orientations of conjugated rings, as well as inter-ring dihedrals, that are critical for understanding electronic and excitonic transport in bulk systems. We apply this model to understand structural correlations in several recently synthesized perylene diimide (PDI)-based organic semiconductors. Twisted and nonplanar molecular architectures are found to promote amorphous morphologies while maintaining local pi-stacking. In conclusion, a graph theoretical network analysis demonstrates that these twisted molecules are more likely to form percolating three-dimensional pathways for charge motion than strictly planar molecules, which show connectivity in only one dimension.

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

Nonlocal Effect of Percolated Particle Networks on Viscoelasticity of Polymer–Filler Nanocomposites: A Mesoscale Simulation Study

With nanoparticles (NPs) as fillers, polymer nanocomposites (PNCs) usually exhibit enhanced mechanical properties. However, a direct connection between the microscopic structural relaxation and macroscopic mechanical properties of PNCs remains to be established. To investigate the micro-to-macro connection, we develop a mesoscale model, in which the NPbridging polymer chains are represented by a dynamic bonded interaction between NPs, and the bulk polymer matrix is implicitly modeled by overdamped Langevin dynamics. Extensive equilibrium simulations are performed to quantify the microscopic dynamics of model PNCs. Systematic analyses of modified Rouse dynamics, dynamic structure factor, and relaxation modulus uncover that the microscopic relaxation dynamics of PNCs are significantly decelerated across different length scales because of nonlocal effects of percolated particle networks a phenomenon that has not been adequately captured in prior simulation studies. We find that NPvolume- fraction and NP-bonding-energy barrier are the two critical variables that affect bulk viscoelasticity the most. The proposed mesoscale model is versatile and provides a powerful framework for studying structure−property relations of different PNCs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Carbon Coating Influence on the Formation of Percolating Electrode Networks for Silicon Anodes

Previous studies have demonstrated that chemical vapor deposition carbon coating on silicon (Si@C) can enhance the electrochemical performance of lithium-ion batteries with Si-based anodes. However, the underlying mechanisms contributing to this improvement have not been fully explored. Here, we address this knowledge gap by applying a suite of characterization methods to evaluate Si@C anodes prepared by reducing acetylene on ball-milled Si particles. Raman mapping measurements show that the C coating (<5 nm thick) enables a homogeneous Si and carbon distribution during the slurry casting process, thereby promoting Si utilization during cycling. The coating’s microstructure and morphology were evaluated using X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy, and neutron reflectivity experiments. Electrochemical impedance spectroscopy measurements upon cycling indicate that carbon coating also reduces the overall resistance as benchmarked against bare Si anodes. Galvanostatic cycling in half-cell studies revealed higher initial Coulombic efficiency and specific capacities with increasing carbon coating time. However, solid electrolyte interphase (SEI) investigations using XPS showed that the coated and uncoated samples have very similar characteristics, suggesting that the SEI may only play a minor role in enhancing the performance of Si@C. Full-cell evaluation of the Si electrodes was consistent with half-cell results relating to performance and SEI properties, further supporting the conclusion that electronic and ionic percolation, enabled by effective electrode manufacturing, are the dominant factors contributing to the favorable performance of Si@C.

25 ENERGY STORAGE↗
DOE OSTI2017

Efficient Steplike Carrier Multiplication in Percolative Networks of Epitaxially Connected PbSe Nanocrystals

Here, carrier multiplication (CM) is a process in which a single photon excites two or more electrons. CM is of interest to enhance the efficiency of a solar cell. Until now, CM in thin films and solar cells of semiconductor nanocrystals (NCs) has been found at photon energies well above the minimum required energy of twice the band gap. The high threshold of CM strongly limits the benefits for solar cell applications. We show that CM is more efficient in a percolative network of directly connected PbSe NCs. The CM threshold is at twice the band gap and increases in a steplike fashion with photon energy. A lower CM efficiency is found for a solid of weaker coupled NCs. This demonstrates that the coupling between NCs strongly affects the CM efficiency. According to device simulations, the measured CM efficiency would significantly enhance the power conversion efficiency of a solar cell.

14 SOLAR ENERGY↗
DOE OSTI2025

Effect of Sulfonation Level on the Percolated Morphology and Proton Conductivity of Hydrated Fluorine-Free Copolymers: Experiments and Simulations

Using all-atom molecular dynamics simulations and a variety of experimental methods, we previously reported on a linear polyethylene with pendant phenyl sulfonated groups precisely on every fifth carbon along the backbone. With increasing relative humidity this fluorine-free polymer self-assembled to form nanoscale water channels and exhibited exceptional proton conductivity. Expanding upon those findings, here we explore partially sulfonated random copolymers, referred to as p 5PhSH-Y. Using either acetyl sulfate or sulfuric acid, a wide range of sulfonation levels were prepared ( Y = 34−98%) corresponding to ion-exchange capacities (IEC) of 2.0−4.4 mmol/g. Combining experimental techniques and all-atom molecular dynamics simulations, we study the effect of Y on water uptake, nanoscale morphology, and the proton/water transport properties of p5PhSH- Y . The proton conductivity of p 5PhSH- Y increases with relative humidity and with Y and achieves values in excess of 0.1 S/cm. These high conductivities are attributed to high IEC and welldeveloped nanoscale percolated hydrophilic domains made possible by the flexible backbone. We quantitatively describe the nature of the water channels using the characteristic distance, channel width distribution, the area per sulfonate group at the hydrophilic/ hydrophobic interface, and the fractal dimension. Notably, the channel widths and the areas per sulfonate group are nominally independent of the level of sulfonation, while depending significantly on the level of hydration. The fractal dimension of the water channels correlates strongly with the water diffusion coefficients calculated from the molecular dynamics (MD) simulations. These findings demonstrate that the p 5PhSH- Y hydrocarbon copolymers can be modified to tune properties, particularly proton conductivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Evidence for percolation diffusion of cations and reordering in disordered pyrochlore from accelerated molecular dynamics

Diffusion in complex oxides is critical to ionic transport, radiation damage evolution, sintering, and aging. In complex oxides such as pyrochlores, anionic diffusion is dramatically affected by cation disorder. However, little is known about how disorder influences cation transport. Here, we report results from classical and accelerated molecular dynamics simulations of vacancy-mediated cation diffusion in Gd 2 Ti 2 O 7 pyrochlore, on the microsecond timescale. We find that diffusion is slow at low levels of disorder, while higher disorder allows for fast diffusion, which is then accompanied by antisite annihilation and reordering, and thus a slowing of cation transport. Cation diffusivity is therefore not constant, but decreases as the material reorders. We also show that fast cation diffusion is triggered by the formation of a percolation network of antisites. This is in contrast with observations from other complex oxides and disordered media models, suggesting a fundamentally different relation between disorder and mass transport.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Emergence of superconductivity in the cuprates via a universal percolation process

Abstract A pivotal step toward understanding unconventional superconductors would be to decipher how superconductivity emerges from the unusual normal state. In the cuprates, traces of superconducting pairing appear above the macroscopic transition temperature T c , yet extensive investigation has led to disparate conclusions. The main difficulty has been to separate superconducting contributions from complex normal-state behaviour. Here we avoid this problem by measuring nonlinear conductivity, an observable that is zero in the normal state. We uncover for several representative cuprates that the nonlinear conductivity vanishes exponentially above T c , both with temperature and magnetic field, and exhibits temperature-scaling characterized by a universal scale Ξ 0 . Attempts to model the response with standard Ginzburg-Landau theory are systematically unsuccessful. Instead, our findings are captured by a simple percolation model that also explains other properties of the cuprates. We thus resolve a long-standing conundrum by showing that the superconducting precursor in the cuprates is strongly affected by intrinsic inhomogeneity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Percolative nature of the direct-current paraconductivity in cuprate superconductors

Abstract Despite extraordinary scientific efforts over the past three decades, the cuprate high-temperature superconductors continue to pose formidable challenges. A pivotal problem, essential for understanding both the normal and superconducting states, is to clarify the nature of the superconducting pre-pairing above the bulk transition temperature T c . Different experimental probes have given conflicting results, in part due to difficulties in discerning the superconducting response from the complex normal-state behavior. Moreover, it has proven challenging to separate common properties of the cuprates from compound-specific idiosyncrasies. Here we investigate the paraconductivity—the superconducting contribution to the direct-current (dc) conductivity—of the simple-tetragonal model cuprate material HgBa 2 CuO 4+ δ . We are able to separate the superconducting and normal-state responses by taking advantage of the Fermi-liquid nature of the normal state in underdoped HgBa 2 CuO 4+ δ ; the robust and simple quadratic temperature-dependence of the normal-state resistivity enables us to extract the paraconductivity above the macroscopic T c with great accuracy. We find that the paraconductivity exhibits unusual exponential temperature dependence, and that it can be quantitatively explained by a simple superconducting percolation model. Consequently, the emergence of superconductivity in this model system is dominated by the underlying intrinsic gap inhomogeneity. Motivated by these insights, we reanalyze published results for two other cuprates and find exponential behavior as well, with nearly the same characteristic temperature scale. The universal intrinsic gap inhomogeneity is not only essential for understanding the supercoducting precursor, but will also have to be taken into account in the analysis of other bulk measurements of the cuprates.

Popčević, Petar↗
DOE OSTI2023

Edge mode percolation and equilibration in the topological insulator cadmium arsenide

Two-dimensional topological insulators can feature one-dimensional charge transport via edge modes, which offer a rich ground for studying exotic quasi-particles and for quantum materials applications. In this work, we use lateral junction devices, defined by nanoscale finger gates, to study edge mode transport in the two-dimensional topological insulator Cd 3 As 2 . The finger gate can be tuned to transmit an integer number of quantum Hall edge modes and exhibits full equilibration in the bipolar regime. When the Fermi level of the channel crosses a Landau level, reflected modes percolate through the channel, resulting in an anomalous conductance peak. The device does not fully pinch off when the channel is tuned into the topological gap, which is a sign of remnant modes in the channel. These modes are expected from band inversion, while residual bulk conduction associated with the disorder potential may also play a role.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A percolation theory for designing corrosion-resistant alloys

Iron-chromium and nickel-chromium binary alloys containing sufficient quantities of chromium serve as the prototypical corrosion-resistant metals owing to the presence of a nanometre-thick protective passive oxide film. Should this film be compromised by a scratch or abrasive wear, it reforms with little accompanying metal dissolution, a key criterion for good passive behaviour. This is a principal reason that stainless steels and other chromium-containing alloys are used in critical applications ranging from biomedical implants to nuclear reactor components. Unravelling the compositional dependence of this electrochemical behaviour is a long-standing unanswered question in corrosion science. Herein, we develop a percolation theory of alloy passivation based on two-dimensional to three-dimensional crossover effects that accounts for selective dissolution and the quantity of metal dissolved during the initial stage of passive film formation. We validate this theory both experimentally and by kinetic Monte Carlo simulation. Our results reveal a path forward for the design of corrosion-resistant metallic alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Plasmon-Enhanced Light Harvesting of Chlorophylls on Near-Percolating Silver Films via One-Photon Anti-Stokes Upconversion

There exists a wealth of means of efficient utilization of solar energy in nature, with photosynthesis of chlorophylls as a prime example. Separately, artificially structured plasmonic materials are versatile in light harvesting and energy conversion. Using a simple and scalable design of near-percolating silver nanostructures, we demonstrate that the light-harvesting efficiency of chlorophylls can be drastically enhanced by tuning the plasmon frequency of the constituent silver nanoparticles to coincide with the maximal photon flux of sunlight. In particular, we show that the photon upconversion efficiency can be readily enhanced by over 20 folds, with the room-temperature fluorescence quantum yield increased by a factor of 2.63. The underlying mechanism for the upconversion enhancement is attributed to a one-electron-per-photon anti-Stokes process, involving absorption of a characteristic phonon mode of the chlorophylls. These findings suggest that chlorophylls can serve as molecular building blocks for high-efficiency light harvesting and solar energy conversion.

14 SOLAR ENERGY↗
DOE OSTI2017

Transition of temporal scaling behavior in percolation assisted shear-branching structure during plastic deformation

This study explores the temporal scaling behavior induced shear-branching structure in response to variant temperatures and strain rates during plastic deformation of Zr-based bulk metallic glass (BMG). The data analysis based on the compression tests suggests that there are two states of shear-branching structures: the fractal structure with a long-range order at an intermediate temperature of 223 K and a larger strain rate of 2.5 × 10 –2 s –1 ; the disordered structure dominated at other temperature and strain rate. It can be deduced from the percolation theory that the compressive ductility, ec, can reach the maximum value at the intermediate temperature. Furthermore, a dynamical model involving temperature is given for depicting the shear-sliding process, reflecting the plastic deformation has fractal structure at the temperature of 223 K and strain rate of 2.5 × 10 –2 s –1 .

36 MATERIALS SCIENCE↗
DOE OSTI2019

Visualizing percolation and ion transport in hybrid solid electrolytes for Li–metal batteries

Hybrid solid electrolytes are composed of organic (polymer) and inorganic (ceramic) ion conducting materials, and are promising options for large-scale production of solid state lithium–metal batteries. Hybrid solid electrolytes containing 15 vol% Al-LLZO demonstrate optimal ionic conductivity properties. Ionic conductivity is shown to decrease at high inorganic loadings. This optimum is most obvious above the melting temperature of polyethylene oxide where the polymer is amorphous. Structural analysis using synchrotron nanotomography reveals that the inorganic particles are highly aggregated. The aggregation size grows with inorganic content and the largest percolating clusters measured for 5 vol%, 15 vol% and 50 vol% were ~12 μm 3 , 206 μm 3 , and 324 μm 3 , respectively. Enhanced transport in hybrid electrolytes is shown to be due to polymer|particle (Al-LLZO) interactions and ionic conductivity is directly related to the accessible surface area of the inorganic particles within the electrolyte. Finally, ordered and well-dispersed structures are ideal for next generation hybrid solid electrolytes.

25 ENERGY STORAGE↗
DOE OSTI2014

Ag nanowire percolating network embedded in indium tin oxide nanoparticles for printable transparent conducting electrodes

Solution-based printable transparent conducting electrodes consisting of Ag nanowire (NW) and indium tin oxide (ITO) nanoparticles (NPs) were fabricated by simple brush painting at room temperature under atmospheric ambient conditions. Effectively embedding the Ag NW percolating network into the ITO NPs provided a conduction path, led to a metallic conduction behavior of the ITO NPs/Ag NW/ITO NPs multilayer and supplied electrons into the ITO NPs. The optimized ITO NPs/Ag NW/ITO NPs multilayer showed a sheet resistance of 16.57 Ω/sq and an optical transparency of 79.50% without post annealing. Based on high resolution transmission electron microscope analysis, we investigated the microstructure and interface structure of the ITO NPs/Ag NW/ITO NPs multilayer electrodes and suggested a possible mechanism to explain the low resistivity of the multilayers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗