Showing papers by "Sandia National Laboratories published in 2014"

MOF-based electronic and opto-electronic devices.

Abstract: Metal–organic frameworks (MOFs) are a class of hybrid materials with unique optical and electronic properties arising from rational self-assembly of the organic linkers and metal ions/clusters, yielding myriads of possible structural motifs. The combination of order and chemical tunability, coupled with good environmental stability of MOFs, are prompting many research groups to explore the possibility of incorporating these materials as active components in devices such as solar cells, photodetectors, radiation detectors, and chemical sensors. Although this field is only in its incipiency, many new fundamental insights relevant to integrating MOFs with such devices have already been gained. In this review, we focus our attention on the basic requirements and structural elements needed to fabricate MOF-based devices and summarize the current state of MOF research in the area of electronic, opto-electronic and sensor devices. We summarize various approaches to designing active MOFs, creation of hybrid material systems combining MOFs with other materials, and assembly and integration of MOFs with device hardware. Critical directions of future research are identified, with emphasis on achieving the desired MOF functionality in a device and establishing the structure–property relationships to identify and rationalize the factors that impact device performance.

Tunable electrical conductivity in metal-organic framework thin film devices

Abstract: A composition including a porous metal organic framework (MOF) including an open metal site and a guest species capable of charge transfer that can coordinate with the open metal site, wherein the composition is electrically conductive. A method including infiltrating a porous metal organic framework (MOF) including an open metal site with a guest species that is capable of charge transfer; and coordinating the guest species to the open metal site to form a composition including an electrical conductivity greater than an electrical conductivity of the MOF.

Review of High-Temperature Central Receiver Designs for Concentrating Solar Power

Abstract: This paper reviews central receiver designs for concentrating solar power applications with high-temperature power cycles Desired features include low-cost and durable materials that can withstand high concentration ratios (~1000 suns), heat-transfer fluids that can withstand temperatures >650 °C, high solar absorptance, and low radiative and convective heat losses leading to a thermal efficiency >90% Different receiver designs are categorized and evaluated in this paper: (1) gas receivers, (2) liquid receivers, and (3) solid particle receivers For each design, the following information is provided: general principle and review of previous modeling and testing activities, expected outlet temperature and thermal efficiency, benefits, perceived challenges, and research needs Emerging receiver designs that can enable higher thermal-to-electric efficiencies (50% or higher) using advanced power cycles such as supercritical CO 2 closed-loop Brayton cycles include direct heating of CO 2 in tubular receiver designs (external or cavity) that can withstand high internal fluid pressures (~20 MPa) and temperatures (~700 °C) Indirect heating of other fluids and materials that can be stored at high temperatures such as advanced molten salts, liquid metals, or solid particles are also being pursued, but challenges include stability, heat loss, and the need for high-temperature heat exchangers

Oxygen Vacancy Enhanced Photocatalytic Activity of Pervoskite SrTiO3

Abstract: A facile and general method has been developed to fabricate oxygen vacancies on perovskite SrTiO3 (STO) nanocrystals through a controllable solid-state reaction of NaBH4 and SrTiO3 nanocrystals. STO samples with tunable color, oxygen vacancy concentration on nanocrystal surface have been synthesized. TEM results reveal that these STO samples have a crystalline core/amorphous shell structure (SrTiO3@SrTiO3–x). XPS and EPR results disclose that the oxygen vacancy concentration increases with the increase of reaction time and temperature. The concentration of oxygen vacancies calculated from TGA data, could reach 5.07% (atom) in this study. UV–vis spectra and photocatalytic results indicate that oxygen vacancies on STO surface play an important role in influencing the light absorption and photocatalytic performance. However, an excess amount of oxygen vacancies leads to a decrease of photocatalytic performance. The optimal photocatalytic activity for H2 production under UV–vis irradiation is up to 2.2 mmol h...

Enhanced Third-Harmonic Generation in Silicon Nanoparticles Driven by Magnetic Response

Abstract: We observe enhanced third-harmonic generation from silicon nanodisks exhibiting both electric and magnetic dipolar resonances. Experimental characterization of the nonlinear optical response through third-harmonic microscopy and spectroscopy reveals that the third-harmonic generation is significantly enhanced in the vicinity of the magnetic dipole resonances. The field localization at the magnetic resonance results in two orders of magnitude enhancement of the harmonic intensity with respect to unstructured bulk silicon with the conversion efficiency limited only by the two-photon absorption in the substrate.

Regulation and Function of Adult Neurogenesis: From Genes to Cognition

Abstract: Adult neurogenesis in the hippocampus is a notable process due not only to its uniqueness and potential impact on cognition but also to its localized vertical integration of different scales of neu...

MaxBin: an automated binning method to recover individual genomes from metagenomes using an expectation-maximization algorithm.

Abstract: Background: Recovering individual genomes from metagenomic datasets allows access to uncultivated microbial populations that may have important roles in natural and engineered ecosystems. Understanding the roles of these uncultivated populations has broad application in ecology, evolution, biotechnology and medicine. Accurate binning of assembled metagenomic sequences is an essential step in recovering the genomes and understanding microbial functions. Results: We have developed a binning algorithm, MaxBin, which automates the binning of assembled metagenomic scaffolds using an expectation-maximization algorithm after the assembly of metagenomic sequencing reads. Binning of simulated metagenomic datasets demonstrated that MaxBin had high levels of accuracy in binning microbial genomes. MaxBin was used to recover genomes from metagenomic data obtained through the Human Microbiome Project, which demonstrated its ability to recover genomes from real metagenomic datasets with variable sequencing coverages. Application of MaxBin to metagenomes obtained from microbial consortia adapted to grow on cellulose allowed genomic analysis of new, uncultivated, cellulolytic bacterial populations, including an abundant myxobacterial population distantly related to Sorangium cellulosum that possessed a much smaller genome (5 MB versus 13 to 14 MB) but has a more extensive set of genes for biomass deconstruction. For the cellulolytic consortia, the MaxBin results were compared to binning using emergent self-organizing maps (ESOMs) and differential coverage binning, demonstrating that it performed comparably to these methods but had distinct advantages in automation, resolution of related genomes and sensitivity. Conclusions: The automatic binning software that we developed successfully classifies assembled sequences in metagenomic datasets into recovered individual genomes. The isolation of dozens of species in cellulolytic microbial consortia, including a novel species of myxobacteria that has the smallest genome among all sequenced aerobic myxobacteria, was easily achieved using the binning software. This work demonstrates that the processes required for recovering genomes from assembled metagenomic datasets can be readily automated, an important advance in understanding the metabolic potential of microbes in natural environments. MaxBin is available at https://sourceforge. net/projects/maxbin/.

Heteroepitaxial Growth of Two-Dimensional Hexagonal Boron Nitride Templated by Graphene Edges

Abstract: By adapting the concept of epitaxy to two-dimensional space, we show the growth of a single-atomic-layer, in-plane heterostructure of a prototypical material system--graphene and hexagonal boron nitride (h-BN). Monolayer crystalline h-BN grew from fresh edges of monolayer graphene with atomic lattice coherence, forming an abrupt one-dimensional interface, or boundary. More important, the h-BN lattice orientation is solely determined by the graphene, forgoing configurations favored by the supporting copper substrate.

Spectrally selective chiral silicon metasurfaces based on infrared Fano resonances

Abstract: Metamaterials and metasurfaces represent a remarkably versatile platform for light manipulation, biological and chemical sensing, and nonlinear optics Many of these applications rely on the resonant nature of metamaterials, which is the basis for extreme spectrally selective concentration of optical energy in the near field In addition, metamaterial-based optical devices lend themselves to considerable miniaturization because of their subwavelength features This additional advantage sets metamaterials apart from their predecessors, photonic crystals, which achieve spectral selectivity through their long-range periodicity Unfortunately, spectral selectivity of the overwhelming majority of metamaterials that are made of metals is severely limited by high plasmonic losses Here we propose and demonstrate Fano-resonant all-dielectric metasurfaces supporting optical resonances with quality factors Q>100 that are based on CMOS-compatible materials: silicon and its oxide We also demonstrate that these infrared metasurfaces exhibit extreme planar chirality, opening exciting possibilities for efficient ultrathin circular polarizers and narrow-band thermal emitters of circularly polarized radiation

Addressing failures in exascale computing

Abstract: We present here a report produced by a workshop on 'Addressing failures in exascale computing' held in Park City, Utah, 4-11 August 2012. The charter of this workshop was to establish a common taxonomy about resilience across all the levels in a computing system, discuss existing knowledge on resilience across the various hardware and software layers of an exascale system, and build on those results, examining potential solutions from both a hardware and software perspective and focusing on a combined approach. The workshop brought together participants with expertise in applications, system software, and hardware; they came from industry, government, and academia, and their interests ranged from theory to implementation. The combination allowed broad and comprehensive discussions and led to this document, which summarizes and builds on those discussions.

Terahertz laser frequency combs

Abstract: Frequency combs based on terahertz quantum cascade lasers, which combine the high power of lasers with the broadband capabilities of pulsed sources, are demonstrated. The frequency combs generate 5 mW of terahertz power covering a frequency range of almost 500 GHz and produce more than 70 lines at 3.5 THz.

Experimental Demonstration of Fusion-Relevant Conditions in Magnetized Liner Inertial Fusion

Abstract: This Letter presents results from the first fully integrated experiments testing the magnetized liner inertial fusion concept [S. A. Slutz et al., Phys. Plasmas 17, 056303 (2010)], in which a cylinder of deuterium gas with a preimposed 10 Taxial magnetic field is heated by Z beamlet, a 2.5 kJ, 1 TW laser, and magnetically imploded by a 19 MA, 100 ns rise time current on the Z facility. Despite a predicted peak implosion velocity of only 70 km = s, the fuel reaches a stagnation temperature of approximately 3 keV, with T(e) ≈ T(i), and produces up to 2 x 10(12) thermonuclear deuterium-deuterium neutrons. X-ray emission indicates a hot fuel region with full width at half maximum ranging from 60 to 120 μm over a 6 mm height and lasting approximately 2 ns. Greater than 10(10) secondary deuterium-tritium neutrons were observed, indicating significant fuel magnetization given that the estimated radial areal density of the plasma is only 2 mg = cm(2).

Review: Down Conversion Materials for Solid‐State Lighting

Abstract: The wavelength down conversion approach to solid-state lighting (SSL) uses down conversion materials to produce visible light when excited by near-UV or blue emission from InGaN LEDs. This review discusses two classes of down conversion materials: phosphors and semiconductor quantum dots (QDs). Strong absorption of the excitation wavelength; high luminous efficacy of radiation, which enables white light with a high color rendering index and a low correlated color temperature; high quantum efficiency; and thermal and chemical stability are some of the criteria for down converters used in SSL. This review addresses the challenges in the development of down converters that satisfy all these criteria. We will discuss the advantages and disadvantages of several phosphor compositions for blue and near-UV LEDs. The use of core/shell architectures to improve the photoluminescence and moisture resistance of phosphors is presented. QDs are another class of down conversion materials for near-UV and blue LEDs. Strategies to improve the photostability and reduce the thermal quenching of QDs include strain-graded core/shell interfaces and alloying. We discuss Cd-containing II–VI QDs, and Cd-free III–V and I–III–VI QDs and their potential for SSL applications. Finally, a description of different methods to integrate the phosphors and QDs with the LED is given.

Quantum control and process tomography of a semiconductor quantum dot hybrid qubit

Abstract: The similarities between gated quantum dots and the transistors in modern microelectronics--in fabrication methods, physical structure and voltage scales for manipulation--have led to great interest in the development of quantum bits (qubits) in semiconductor quantum dots. Although quantum dot spin qubits have demonstrated long coherence times, their manipulation is often slower than desired for important future applications, such as factoring. Furthermore, scalability and manufacturability are enhanced when qubits are as simple as possible. Previous work has increased the speed of spin qubit rotations by making use of integrated micromagnets, dynamic pumping of nuclear spins or the addition of a third quantum dot. Here we demonstrate a qubit that is a hybrid of spin and charge. It is simple, requiring neither nuclear-state preparation nor micromagnets. Unlike previous double-dot qubits, the hybrid qubit enables fast rotations about two axes of the Bloch sphere. We demonstrate full control on the Bloch sphere with π-rotation times of less than 100 picoseconds in two orthogonal directions, which is more than an order of magnitude faster than any other double-dot qubit. The speed arises from the qubit's charge-like characteristics, and its spin-like features result in resistance to decoherence over a wide range of gate voltages. We achieve full process tomography in our electrically controlled semiconductor quantum dot qubit, extracting high fidelities of 85 per cent for X rotations (transitions between qubit states) and 94 per cent for Z rotations (phase accumulation between qubit states).

Toward Smart and Ultra-Efficient Solid-State Lighting

Abstract: Solid-state lighting has made tremendous progress this past decade, with the potential to make much more progress over the coming decade. In this article, the current status of solid-state lighting relative to its ultimate potential to be “smart” and ultra-efficient is reviewed. Smart, ultra-efficient solid-state lighting would enable both very high “effective” efficiencies and potentially large increases in human performance. To achieve ultra-efficiency, phosphors must give way to multi-color semiconductor electroluminescence: some of the technological challenges associated with such electroluminescence at the semiconductor level are reviewed. To achieve smartness, additional characteristics such as control of light flux and spectra in time and space will be important: some of the technological challenges associated with achieving these characteristics at the lamp level are also reviewed. It is important to emphasise that smart and ultra-efficient are not either/or, and few compromises need to be made between them. The ultimate route to ultra-efficiency brings with it the potential for smartness, the ultimate route to smartness brings with it the potential for ultra-efficiency, and the long-term ultimate route to both might well be color-mixed RYGB lasers.

Efficient biomass pretreatment using ionic liquids derived from lignin and hemicellulose

Abstract: Ionic liquids (ILs), solvents composed entirely of paired ions, have been used in a variety of process chemistry and renewable energy applications. Imidazolium-based ILs effectively dissolve biomass and represent a remarkable platform for biomass pretreatment. Although efficient, imidazolium cations are expensive and thus limited in their large-scale industrial deployment. To replace imidazolium-based ILs with those derived from renewable sources, we synthesized a series of tertiary amine-based ILs from aromatic aldehydes derived from lignin and hemicellulose, the major by-products of lignocellulosic biofuel production. Compositional analysis of switchgrass pretreated with ILs derived from vanillin, p-anisaldehyde, and furfural confirmed their efficacy. Enzymatic hydrolysis of pretreated switchgrass allowed for direct comparison of sugar yields and lignin removal between biomass-derived ILs and 1-ethyl-3-methylimidazolium acetate. Although the rate of cellulose hydrolysis for switchgrass pretreated with biomass-derived ILs was slightly slower than that of 1-ethyl-3-methylimidazolium acetate, 90–95% glucose and 70–75% xylose yields were obtained for these samples after 72-h incubation. Molecular modeling was used to compare IL solvent parameters with experimentally obtained compositional analysis data. Effective pretreatment of lignocellulose was further investigated by powder X-ray diffraction and glycome profiling of switchgrass cell walls. These studies showed different cellulose structural changes and differences in hemicellulose epitopes between switchgrass pretreatments with the aforementioned ILs. Our concept of deriving ILs from lignocellulosic biomass shows significant potential for the realization of a “closed-loop” process for future lignocellulosic biorefineries and has far-reaching economic impacts for other IL-based process technology currently using ILs synthesized from petroleum sources.

Analysis of a consumer survey on plug-in hybrid electric vehicles

Abstract: Plug-in Hybrid Electric Vehicles (PHEVs) show potential to reduce greenhouse gas (GHG) emissions, increase fuel efficiency, and offer driving ranges that are not limited by battery capacity. However, these benefits will not be realized if consumers do not adopt this new technology. Several agent-based models have been developed to model potential market penetration of PHEVs, but gaps in the available data limit the usefulness of these models. To address this, we administered a survey to 1000 stated US residents, using Amazon Mechanical Turk, to better understand factors influencing the potential for PHEV market penetration. Our analysis of the survey results reveals quantitative patterns and correlations that extend the existing literature. For example, respondents who felt most strongly about reducing US transportation energy consumption and cutting greenhouse gas emissions had, respectively, 71 and 44 times greater odds of saying they would consider purchasing a compact PHEV than those who felt least strongly about these issues. However, even the most inclined to consider a compact PHEV were not generally willing to pay more than a few thousand US dollars extra for the sticker price. Consistent with prior research, we found that financial and battery-related concerns remain major obstacles to widespread PHEV market penetration. We discuss how our results help to inform agent-based models of PHEV market penetration, governmental policies, and manufacturer pricing and marketing strategies to promote consumer adoption of PHEVs.

Observation of measurement-induced entanglement and quantum trajectories of remote superconducting qubits

Abstract: The creation of a quantum network requires the distribution of coherent information across macroscopic distances. We demonstrate the entanglement of two superconducting qubits, separated by more than a meter of coaxial cable, by designing a joint measurement that probabilistically projects onto an entangled state. By using a continuous measurement scheme, we are further able to observe single quantum trajectories of the joint two-qubit state, confirming the validity of the quantum Bayesian formalism for a cascaded system. Our results allow us to resolve the dynamics of continuous projection onto the entangled manifold, in quantitative agreement with theory.

Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes

Abstract: Many battery electrodes contain ensembles of nanoparticles that phase-separate on (de)intercalation. In such electrodes, the fraction of actively intercalating particles directly impacts cycle life: a vanishing population concentrates the current in a small number of particles, leading to current hotspots. Reports of the active particle population in the phase-separating electrode lithium iron phosphate (LiFePO4; LFP) vary widely, ranging from near 0% (particle-by-particle) to 100% (concurrent intercalation). Using synchrotron-based X-ray microscopy, we probed the individual state-of-charge for over 3,000 LFP particles. We observed that the active population depends strongly on the cycling current, exhibiting particle-by-particle-like behaviour at low rates and increasingly concurrent behaviour at high rates, consistent with our phase-field porous electrode simulations. Contrary to intuition, the current density, or current per active internal surface area, is nearly invariant with the global electrode cycling rate. Rather, the electrode accommodates higher current by increasing the active particle population. This behaviour results from thermodynamic transformation barriers in LFP, and such a phenomenon probably extends to other phase-separating battery materials. We propose that modifying the transformation barrier and exchange current density can increase the active population and thus the current homogeneity. This could introduce new paradigms to enhance the cycle life of phase-separating battery electrodes.

In situ transmission electron microscopy study of electrochemical sodiation and potassiation of carbon nanofibers.

Abstract: Carbonaceous materials have great potential for applications as anodes of alkali-metal ion batteries, such as Na-ion batteries and K-ion batteries (NIB and KIBs). We conduct an in situ study of the electrochemically driven sodiation and potassiation of individual carbon nanofibers (CNFs) by transmission electron microscopy (TEM). The CNFs are hollow and consist of a bilayer wall with an outer layer of disordered-carbon (d-C) enclosing an inner layer of crystalline-carbon (c-C). The d-C exhibits about three times volume expansion of the c-C after full sodiation or potassiation, thus suggesting a much higher storage capacity of Na or K ions in d-C than c-C. For the bilayer CNF-based electrode, a steady sodium capacity of 245 mAh/g is measured with a Coulombic efficiency approaching 98% after a few initial cycles. The in situ TEM experiments also reveal the mechanical degradation of CNFs through formation of longitudinal cracks near the c-C/d-C interface during sodiation and potassiation. Geometrical changes...

Entropy Stable Spectral Collocation Schemes for the Navier--Stokes Equations: Discontinuous Interfaces

Abstract: Nonlinear entropy stability and a summation-by-parts framework are used to derive provably stable, polynomial-based spectral collocation element methods of arbitrary order for the compressible Navier--Stokes equations. The new methods are similar to strong form, nodal discontinuous Galerkin spectral elements but conserve entropy for the Euler equations and are entropy stable for the Navier--Stokes equations. Shock capturing follows immediately by combining them with a dissipative companion operator via a comparison approach. Smooth and discontinuous test cases are presented that demonstrate their efficacy.

Evaluating the performance of parallel subsurface simulators: An illustrative example with PFLOTRAN

Abstract: [1] To better inform the subsurface scientist on the expected performance of parallel simulators, this work investigates performance of the reactive multiphase flow and multicomponent biogeochemical transport code PFLOTRAN as it is applied to several realistic modeling scenarios run on the Jaguar supercomputer. After a brief introduction to the code's parallel layout and code design, PFLOTRAN's parallel performance (measured through strong and weak scalability analyses) is evaluated in the context of conceptual model layout, software and algorithmic design, and known hardware limitations. PFLOTRAN scales well (with regard to strong scaling) for three realistic problem scenarios: (1) in situ leaching of copper from a mineral ore deposit within a 5-spot flow regime, (2) transient flow and solute transport within a regional doublet, and (3) a real-world problem involving uranium surface complexation within a heterogeneous and extremely dynamic variably saturated flow field. Weak scalability is discussed in detail for the regional doublet problem, and several difficulties with its interpretation are noted.

Chloroaluminate-Doped Conducting Polymers as Positive Electrodes in Rechargeable Aluminum Batteries

Abstract: Demonstrated here is the use of conducting polymers as active materials in the positive electrodes of rechargeable aluminum-based batteries operating at room temperature. The battery chemistry is based on chloroaluminate ionic liquid electrolytes, which allow reversible stripping and plating of aluminum metal at the negative electrode. Characterization of electrochemically synthesized polypyrrole films revealed doping of the polymers with chloroaluminate anions. Cycling of the conducting polymer electrodes occurred via the electrochemical insertion and removal of these anions. Stable galvanostatic cycling of polypyrrole and polythiophene cells was demonstrated, with electrode capacities at near-theoretical levels (30–100 mAh g–1) and Coulombic efficiencies approaching 100%. The energy density of a sealed sandwich-type cell with polythiophene at the positive electrode was estimated to be 44 Wh kg–1 relative to the total mass of active components. This energy density is competitive with state-of-the-art bat...

Carbon Nanotube Terahertz Detector

Abstract: Terahertz (THz) technologies are promising for diverse areas such as medicine, bioengineering, astronomy, environmental monitoring, and communications. However, despite decades of worldwide efforts, the THz region of the electromagnetic spectrum still continues to be elusive for solid state technology. Here, we report on the development of a powerless, compact, broadband, flexible, large-area, and polarization-sensitive carbon nanotube THz detector that works at room temperature. The detector is sensitive throughout the entire range of the THz technology gap, with responsivities as high as ∼2.5 V/W and polarization ratios as high as ∼5:1. Complete thermoelectric and opto-thermal characterization together unambiguously reveal the photothermoelectric origin of the THz photosignal, triggered by plasmonic absorption and collective antenna effects, and suggest that judicious design of thermal management and quantum engineering of Seebeck coefficients will lead to further enhancement of device performance.

High-efficiency thermodynamic power cycles for concentrated solar power systems

Abstract: This paper provides a review of high-efficiency thermodynamic cycles and their applicability to concentrating solar power systems, primarily focusing on high-efficiency single and combined cycles. Novel approaches to power generation proposed in the literature are also highlighted. The review is followed by analyses of promising candidates, including regenerated He-Brayton, regenerated CO2-Brayton, CO2 recompression Brayton, steam Rankine, and CO2–ORC combined cycle. Steam Rankine is shown to offer higher thermal efficiencies at temperatures up to about 600 °C but requires a change in materials for components above this temperature. Above this temperature, CO2 recompression Brayton cycles are shown to have very high thermal efficiency, potentially even exceeding 60% at 30 MPa maximum pressure and above 1000 °C maximum temperature with wet cooling. An estimate of a combined receiver and power cycle operating temperature is provided for the cycles considered and compared to the traditional approach of optimization based on the Carnot efficiency. It is shown that the traditional approach to optimizing the receiver and turbine inlet temperatures based on Carnot is generally not sufficient, leading to an optimum temperature shift of more than 100 °C from the Carnot case under various conditions.

Research frontiers in the chemistry of Criegee intermediates and tropospheric ozonolysis

Abstract: The chemistry of carbonyl oxides, known as Criegee intermediates, is central to many aspects of tropospheric chemistry. For decades it has been known that these reactive species, whose electronic structure contains zwitterionic and biradical character, are formed in the ozonolysis of alkenes. However it is only recently that direct measurements of their reaction kinetics have become possible. In this perspective we describe the most recent progress in understanding the reactivity of these historically elusive molecules, explore the atmospheric chemistry implications of new experimental discoveries, and propose important new areas for investigation.