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At least 1,549 records · Page 86
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Synthesis and exceptional operational durability of polyaniline-inspired conductive ladder polymers

Ladder-type structures can impart exceptional stability to polymeric electronic materials. This article introduces a new class of conductive polymers featuring a fully ladder-type backbone. A judicious molecular design strategy enables the synthesis of a low-defect ladder polymer, which can be efficiently oxidized and acid-doped to achieve its conductive state. The structural elucidation of this polymer and the characterization of its open-shell nature are facilitated with the assistance of studies on small molecular models. An autonomous robotic system is used to optimize the conductivity of the polymer thin film, achieving over 7 mS cm −1 . Impressively, this polymer demonstrates unparalleled stability in strong acid and under harsh UV-irradiation, significantly surpassing commercial benchmarks like PEDOT:PSS and polyaniline. Moreover, it displays superior durability across numerous redox cycles as the active material in an electrochromic device and as the pseudocapacitive material in a supercapacitor device. This work provides structural design guidance for durable conductive polymers for long-term device operation.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Ultrathin electron and proton-conducting membranes for nanoscale integrated artificial photosystems

Reducing the thickness of separation membranes without compromising their selectivity and robustness is the most effective way of maximizing the areal conductivity. This is especially important for the integration of visible light-driven water oxidation and carbon dioxide (or proton) reduction into a complete artificial photosystem on the shortest possible length scale – the nanoscale – because of the efficiency advantages over macroscale photosystems. In addition to their excellent separation property, ultrathin membranes of 10 nm thickness or less need to exhibit sufficient electrical and proton conductivity in order for the photocatalytic rates to keep up with the photon flux at maximum solar intensity. Furher, two materials, graphene and amorphous silica with embedded molecular wires, have emerged as promising ultrathin membranes for the development of nanoscale integrated solar-fuel systems. Moreover, electrically conducting metal–organic or covalent–organic frameworks can be used to fabricate high surface area-supports that enable the use of molecular catalysts and/or light absorbers at an adequate areal density for nanoscale integration with graphene membranes. Following an overview of the electron and proton conductivity of these ultrathin materials and recent examples of photoelectrocatalytic applications that take advantage of some but not all the properties that constitute a complete functional membrane, the status and future opportunities for complete nanoscale integrated photosystems featuring an ultrathin membrane are discussed.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Ion concentration polarization causes a nearly pore-length-independent conductance of nanopores

There has been a great amount of interest in nanopores as the basis for sensors and templates for preparation of biomimetic channels as well as model systems to understand transport properties at the nanoscale. The presence of surface charges on the pore walls has been shown to induce ion selectivity as well as enhance ionic conductance compared to uncharged pores. Here, using three-dimensional continuum modeling, we examine the role of the length of charged nanopores as well as applied voltage for controlling ion selectivity and ionic conductance of single nanopores and small nanopore arrays. First, we present conditions where the ion current and ion selectivity of nanopores with homogeneous surface charges remain unchanged, even if the pore length decreases by a factor of 6. This length-independent conductance is explained through the effect of ion concentration polarization (ICP), which modifies local ionic concentrations, not only at the pore entrances but also in the pore in a voltage-dependent manner. We describe how voltage controls the ion selectivity of nanopores with different lengths and present the conditions when charged nanopores conduct less current than uncharged pores of the same geometrical characteristics. The manuscript provides different measures of the extent of the depletion zone induced by ICP in single pores and nanopore arrays, including systems with ionic diodes. In conclusion, the modeling shown here will help design selective nanopores for a variety of applications where single nanopores and nanopore arrays are used.

Cain, DaVante↗
DOE OSTI2025

Thermal Conductivity of Graphene Coated Copper Under Uniaxial Tensile Mechanical Strain

Graphene continues to demonstrate promise as a highly effective barrier coating, even at only one atom thick. The thermal properties of this coating are also promising to allow diffusion of heat across the surface, as the isolated graphene is an intrinsically good thermal conductor, yet this and its behavior under mechanical deformation has been less extensively studied. This report demonstrates that the in-plane thermal conductivity and interfacial thermal conductance of graphene coatings on copper are affected by mechanical strain. By inducing a strain in the copper substrate, the Raman-active 2D peak exhibits a change in position as well as a change in laser power dependence as the copper substrate is uniaxially elongated to a maximum of 0.5%. Non-linear trends in thermal conductivity are observed with tensile strain in samples with differing strain transfer rates from the substrate, indicating the close correlation between intrinsic thermal conduction and interfacial properties in atomically thin coatings transferred onto metals.

36 MATERIALS SCIENCE↗
DOE OSTI2025

A single-ion-conducting polymer and high-entropy Li-garnet composite electrolyte with simultaneous enhancement in ion transport and mechanical properties

Enabling the lithium metal anode has been the holy grail for improving the energy density for the next generation advanced batteries. Developing electrolytes that will suppress Li dendrite growth and provide sufficient ionic conductivity remains a major challenge in this field. In this study, we develop a polymer–ceramic composite electrolyte for lithium metal batteries. The polymer matrix is a vinyl ethylene carbonate (VEC) based single-ion-conducting polymer electrolyte. The ceramic filler is a Li 7 La 3 Zr 0.5 Nb 0.5 Ta 0.5 Hf 0.5 O 12 high-entropy Li-garnet (HE Li-garnet) ceramic, which is less prone to surface Li 2 CO 3 formation compared to Al-doped Li garnets. The addition of HE Li-garnet leads to a 7-fold increase in the ionic conductivity (8.6 × 10 −5 S cm −1 at 30 °C) compared to the pure polymer, while maintaining a high Li + transference of 0.73. Proton nuclear magnetic resonance and thermogravimetric analysis results suggest that the addition of HE Li-garnet results in a lower degree of polymerization of VEC, leaving more unpolymerized VEC monomers in the matrix, serving as the governing mechanism for conductivity enhancement. The favorable interactions between HE Li-garnet particles and the polymer matrix lead to a stable and well-mixed composite with 2-fold enhancement of storage modulus at 40 °C. The simultaneous ion transport and mechanical property enhancement significantly improves the composite electrolyte's dendrite resistance and cycle life in Li symmetric cells. This work highlights the positive role HE Li-garnet can play in improving polymer electrolytes to enable lithium metal anodes.

Ock, Ji-young [Oak Ridge National Laboratory (ORNL↗
DOE OSTI2013

Conductance of ferro- and antiferro-magnetic single-atom contacts: A first-principles study

We present a first-principles study on the spin dependent conductance of five single-atom magnetic junctions consisting of a magnetic tip and an adatom adsorbed on a magnetic surface, i.e., the Co-Co/Co(001) and Ni-X/Ni(001) (X = Fe, Co, Ni, Cu) junctions. When their spin configuration changes from ferromagnetism to anti-ferromagnetism, the spin-up conductance increases while the spin-down one decreases. For the junctions with a magnetic adatom, there is nearly no spin valve effect as the decreased spin-down conductance counteracts the increased spin-up one. For the junction with a nonmagnetic adatom (Ni-Cu/Ni(001)), a spin valve effect is obtained with a variation of 22% in the total conductance. In addition, the change in spin configuration enhances the spin filter effect for the Ni-Fe/Ni(001) junction but suppresses it for the other junctions.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Conductance modulation in topological insulator Bi{sub 2}Se{sub 3} thin films with ionic liquid gating

A Bi{sub 2}Se{sub 3} topological insulator field effect transistor is investigated by using ionic liquid as an electric double layer gating material, leading to a conductance modulation of 365% at room temperature. We discuss the role of charged impurities on the transport properties. The conductance modulation with gate bias is due to a change in the carrier concentration, whereas the temperature dependent conductance change is originated from a change in mobility. Large conductance modulation at room temperature along with the transparent optical properties makes topological insulators as an interesting (opto)electronic material.

36 MATERIALS SCIENCE↗
DOE OSTI2014

The role of band alignment in p-type conductivity of Na-doped ZnMgO: Polar versus non-polar

We investigate the electrical properties of polar and non-polar ZnMgO:Na films that have been fabricated on c-plane and r-plane sapphire substrates using intervened ZnO layers (10–30 nm thick) by pulsed laser deposition. Hall-effect measurements indicate that the a-plane ZnMgO:Na film exhibits p-type conductivity with a carrier concentration of about 3.5 × 10{sup 16} cm{sup −3}, while the polar film shows a compensatory conductivity. Meanwhile, the dependence of the band alignment on the orientation of the ZnMgO/ZnO heterojunctions has been investigated using photoelectron spectroscopy. The heterojunctions form in the type-I straddling alignment with valence band offsets of 0.07 (0.02) eV for the (non-)polar heterojunction. The difference in valence band offsets is primarily attributed to the spontaneous polarization effect. We propose that the smaller valence band offsets and larger conduction band offsets would reduce the Na{sub Zn} acceptor level and enhance the relative intrinsic donor levels. Such effects consequently lead to p-type conductivity in non-polar ZnMgO:Na films. The band alignment of non-polar ZnMgO/ZnO can be used to facilitate p-type doping with a shallower acceptor state in the ZnO-like alloy.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Microstructure and conductance-slope of InAs/GaSb tunnel diodes

InAs/GaSb and similar materials systems have generated great interest as a heterojunction for tunnel field effect transistors (TFETs) due to favorable band alignment. However, little is currently understood about how such TFETs are affected by materials defects and nonidealities. We present measurements of the conductance slope for various InAs/GaSb heterojunctions via two-terminal electrical measurements, which removes three-terminal parasitics and enables direct study on the effect of microstructure on tunnelling. Using this, we can predict how subthreshold swings in TFETs can depend on microstructure. We also demonstrate growth and electrical characterization for structures grown by metalorganic chemical vapor deposition (MOCVD)—a generally more scalable process compared with molecular beam epitaxy (MBE). We determine that misfit dislocations and point defects near the interface can lead to energy states in the band-gap and local band bending that result in trap-assisted leakage routes and nonuniform band alignment across the junction area that lower the steepness of the conductance slope. Despite the small lattice mismatch, misfit dislocations still form in InAs on GaSb due to relaxation as a result of large strain from intermixed compositions. This can be circumvented by growing GaSb on InAs, straining the GaSb underlayer, or lowering the InAs growth temperature in the region of the interface. The conductance slope can also be improved by annealing the samples at higher temperatures, which we believe acts to annihilate point defects and average out major fluctuations in band alignment across the interface. Using a combination of these techniques, we can greatly improve the steepness of the conductance slope which could result in steeper subthreshold swings in TFETs in the future.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Origin of the current discretization in deep reset states of an Al{sub 2}O{sub 3}/Cu-based conductive-bridging memory, and impact on state level and variability

In this paper, we develop a Quantum-Point-Contact (QPC) model describing the state conduction in a W/Al{sub 2}O{sub 3}/TiW/Cu Conductive-Bridging Memory cell (CBRAM). The model allows describing both the voltage- and the temperature-dependence of the conduction. For deep current levels, a resistance component is added in series to the point-contact constriction to account for electron scattering in the residual filament. The fitting of single-particle perturbation also allowed to estimate the number and effective size of the conduction-controlling particles in the QPC constriction. The results clearly point to smaller particles for CBRAM (Cu particles) as compared to oxide-based resistive RAM involving oxygen-vacancy defects, which is discussed as a possible origin of deeper reset level obtained in CBRAM. We also evidence a beneficial impact of this smaller particle size on lower Random-Telegraph-Noise amplitude measured on CBRAM devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Fourier analysis of conductive heat transfer for glazed roofing materials

For low-rise buildings, roof is the most exposed surface to solar radiation. The main mode of heat transfer from outdoor via the roof is conduction. The rate of heat transfer and the thermal impact is dependent on the thermophysical properties of roofing materials. Thus, it is important to analyze the heat distribution for the various types of roofing materials. The objectives of this paper are to obtain the Fourier series for the conductive heat transfer for two types of glazed roofing materials, namely polycarbonate and polyfilled, and also to determine the relationship between the ambient temperature and the conductive heat transfer for these materials. Ambient and surface temperature data were collected from an empirical field investigation in the campus of Universiti Teknologi MARA Shah Alam. The roofing materials were installed on free-standing structures in natural ventilation. Since the temperature data are generally periodic, Fourier series and numerical harmonic analysis are applied. Based on the 24-point harmonic analysis, the eleventh order harmonics is found to generate an adequate Fourier series expansion for both glazed roofing materials. In addition, there exists a linear relationship between the ambient temperature and the conductive heat transfer for both glazed roofing materials. Based on the gradient of the graphs, lower heat transfer is indicated through polyfilled. Thus polyfilled would have a lower thermal impact compared to polycarbonate.

42 ENGINEERING↗
DOE OSTI2014

Luminescence quenching of conductive Si nanocrystals via “Linkage emission”: Hopping-like propagation of infrared-excited Auger electrons

Phosphorus (P) is an n-type dopant for conductive silicon nanocrystals (Si-nc's), the electrical activation of which may be monitored through a non-radiative Auger recombination process that quenches the Si-nc luminescence. We investigated this quenching mechanism through electrical measurements of Si-nc's. Infrared-excited Auger electron emission as the non-radiative process was directly probed and the dynamics of the process are determined from a frequency response analysis. To explain the dynamics, we propose a model in which Auger electrons with a low kinetic energy establish a local inter-nanocrystal conductance and the repetition of this local conductance results in a constant photocurrent (“linkage emission”). This emission becomes significant by electron filling in the Si-nc's owing to the electrical activation of P, which is consistent with observed luminescence quenching behavior. We found that the IR photo-excited emission is distinct from the thermally induced hopping conduction and show that confined, rather than trapped, charges are the source of the Auger electrons. Thus, the process consumes both confined charges and the recombination energy for Auger emission, which explains the luminescence quenching mechanism of Si-nc:P.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Resistive switching and conductance quantization in Ag/SiO{sub 2}/indium tin oxide resistive memories

The Ag/SiO{sub 2}/indium tin oxide (ITO) devices exhibit bipolar resistive switching with a large memory window of ∼10{sup 2}, satisfactory endurance of >500 cycles, good retention property of >2000 s, and fast operation speed of <100 ns, thus being a type of promising resistive memory. Under slow voltage sweep measurements, conductance plateaus with a conductance value of integer or half-integer multiples of single atomic point contact have been observed, which agree well with the physical phenomenon of conductance quantization. More importantly, the Ag/SiO{sub 2}/ITO devices exhibit more distinct quantized conductance plateaus under pulse measurements, thereby showing the potential for realizing ultra-high storage density.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Metallic to hopping conduction transition in Ta{sub 2}O{sub 5−x}/TaO{sub y} resistive switching device

In this Letter, a comprehensive analysis of how the metallic behavior transition to hopping was presented by studying the transport mechanisms of low resistance states (LRS) in Ta{sub 2}O{sub 5−x}/TaO{sub y} resistive switching devices at very low temperatures. Three types of conduction behaviors were reported through temperature-dependent measurements ranging from 5 K to 250 K. Memory cells at low LRS show metallic behavior due to the formation of metallic filament. The temperature dependence of resistance at medium LRS exhibits an interesting phenomenon that a positive temperature coefficient transfers into a negative one at temperature of 20 K. Detailed analysis reveals that this phenomenon is caused by the coexistence of extended and localized states, with metallic conduction at higher temperatures and variable-range hopping at lower temperatures. Carrier transport at high LRS is dominated by electrons hopping conduction with nearest-neighboring hopping conduction changing into variable-range hopping as temperature decreases.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Sheath oscillation characteristics and effect on near-wall conduction in a krypton Hall thruster

Despite its affordability, the krypton Hall-effect thruster in applications always had problems in regard to performance. The reason for this degradation is studied from the perspective of the near-wall conductivity of electrons. Using the particle-in-cell method, the sheath oscillation characteristics and its effect on near-wall conduction are compared in the krypton and xenon Hall-effect thrusters both with wall material composed of BNSiO{sub 2}. Comparing these two thrusters, the sheath in the krypton-plasma thruster will oscillate at low electron temperatures. The near-wall conduction current is only produced by collisions between electrons and wall, thereby causing a deficiency in the channel current. The sheath displays spatial oscillations only at high electron temperature; electrons are then reflected to produce the non-oscillation conduction current needed for the krypton-plasma thruster. However, it is accompanied with intensified oscillations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Optical conductivity of topological insulator thin films

We present a detailed theoretical study on the optoelectronic properties of topological insulator thin film (TITFs). The k·p approach is employed to calculate the energy spectra and wave functions for both the bulk and surface states in the TITF. With these obtained results, the optical conductivities induced by different electronic transitions among the bulk and surface states are evaluated using the energy-balance equation derived from the Boltzmann equation. We find that for Bi{sub 2}Se{sub 3}-based TITFs, three characteristic regimes for the optical absorption can be observed. (i) In the low radiation frequency regime (photon energy ℏω<200 meV), the free-carrier absorption takes place due to intraband electronic transitions. An optical absorption window can be observed. (ii) In the intermediate radiation frequency regime (200<ℏω<300 meV), the optical absorption is induced mainly by interband electronic transitions from surface states in the valance band to surface states in the conduction band and an universal value σ{sub 0}=e{sup 2}/(8ℏ) for the optical conductivity can be obtained. (iii) In the high radiation frequency regime (ℏω>300 meV), the optical absorption can be achieved via interband electronic transitions from bulk and surface states in the valance band to bulk and surface states in the conduction band. A strong absorption peak can be observed. These interesting findings indicate that optical measurements can be applied to identify the energy regimes of bulk and surface states in the TITF.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

An origin of good electrical conduction in La{sub 4}BaCu{sub 5}O{sub 13+δ}

We have prepared a set of polycrystalline samples of the metallic copper oxide La{sub 4}BaCu{sub 5−x}Co{sub x}O{sub 13+δ} (0 ≤ x ≤ 0.35) and have measured the resistivity from 4 to 800 K. All the resistivities show metallic temperature dependence with a small magnitude less than 2 mΩ cm at 800 K, indicating that the metallic conduction is robust against impurities. The robust metallic conduction further suggests that this class of oxide is a promising candidate for electrical leads at high temperature, which might replace platinum. A detailed measurement and analysis on the Hall resistivity have revealed that at least two components are responsible for the electrical conduction, in which a large number of electrons of moderate mobility coexist with a much smaller number of holes of extremely high mobility. This large electron density well screens the impurity potential and retains the metallic conduction against 7% impurity doping.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Dipolar resonances in conductive carbon micro-fibers probed by near-field terahertz spectroscopy

In this study, we observe dipole resonances in thin conductive carbon micro-fibers by detecting an enhanced electric field in the near-field of a single fiber at terahertz (THz) frequencies. Time-domain analysis of the electric field shows that each fiber sustains resonant current oscillations at the frequency defined by the fiber's length. Strong dependence of the observed resonance frequency and degree of field enhancement on the fibers' conductive properties enable direct non-contact probing of the THz conductivity in single carbon micro-fibers. We find the conductivity of the fibers to be within the range of 1– 5∙10 4 S/m. This approach is suitable for experimental characterization of individual doped semiconductor resonators for THz metamaterials and devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗