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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Ion Accumulation and Migration Effects on Redox Cycling in Nanopore Electrode Arrays at Low Ionic Strength

Ion permselectivity can lead to accumulation in zero-dimensional nanopores, producing a significant increase in ion concentration, an effect which may be combined with unscreened ion migration to improve sensitivity in electrochemical measurements, as demonstrated by the enormous current amplification (~2000-fold) previously observed in nanopore electrode arrays (NEA) in the absence of supporting electrolyte. Ionic strength is a key experimental factor that governs the magnitude of the additional current amplification (AF ad ) beyond simple redox cycling through both ion accumulation and ion migration effects. Here, separate contributions from ion accumulation and ion migration to the overall AF ad were identified by studying NEAs with varying geometries, with larger AF ad values being achieved in NEAs with smaller pores. In addition, larger AF ad values were observed for Ru(NH 3 ) 6 3/2+ than for ferrocenium/ferrocene (Fc + /Fc) in aqueous solution, indicating that coupling efficiency in redox cycling can significantly affect AF ad . While charged species are required to observe migration effects or ion accumulation, poising the top electrode at an oxidizing potential converts neutral species to cations, which can then exhibit current amplification similar to starting with the cation. The electrical double layer effect was also demonstrated for Fc/Fc + in acetonitrile and 1,2-dichloroethane, producing AF ad up to 100× at low ionic strength. The pronounced AF ad effects demonstrate the advantage of coupling redox cycling with ion accumulation and migration effects for ultrasensitive electrochemical measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Facet control of gold nanorods

While great success has been achieved in fine-tuning the aspect ratios and thereby the plasmon resonances of cylindrical Au nanorods, facet control with atomic level precision on the highly curved nanorod surfaces has long been a significantly more challenging task. The intrinsic structural complexity and lack of precise facet control of the nanorod surfaces remain the major obstacles for the atomic-level elucidation of the structure–property relationships that underpin the intriguing catalytic performance of Au nanorods. Here we demonstrate that the facets of single-crystalline Au nanorods can be precisely tailored using cuprous ions and cetyltrimethylammonium bromide as a unique pair of surface capping competitors to guide the particle geometry evolution during nanorod overgrowth. By deliberately maneuvering the competition between cuprous ions and cetyltrimethylammonium bromide, we have been able to create, in a highly controllable and selective manner, an entire family of nanorod-derived anisotropic multifaceted geometries whose surfaces are enclosed by specific types of well-defined high-index and low-index facets. This facet-controlled nanorod overgrowth approach also allows us to fine-tune the particle aspect ratios while well-preserving all the characteristic facets and geometric features of the faceted Au nanorods. Furthermore, taking full advantage of the combined structural and plasmonic tunability, we have further studied the facet-dependent heterogeneous catalysis on well-faceted Au nanorods using surface-enhanced Raman spectroscopy as an ultrasensitive spectroscopic tool with unique time-resolving and molecular finger-printing capabilities.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Tellurene Photodetector with High Gain and Wide Bandwidth

Two-dimensional (2D) semiconductors have been extensively explored as a new class of materials with great potential. In particular, black phosphorus (BP) has been considered to be a strong candidate for applications such as high-performance infrared photodetectors. However, the scalability of BP thin film is still a challenge, and its poor stability in the air has hampered the progress of the commercialization of BP devices. Herein, we report the use of hydrothermal-synthesized and air-stable 2D tellurene nanoflakes for broadband and ultrasensitive photodetection. The tellurene nanoflakes show high hole mobilities up to 458 cm 2 /V·s at ambient conditions, and the tellurene photodetector presents peak extrinsic responsivity of 383 A/W, 19.2 mA/W, and 18.9 mA/W at 520 nm, 1.55 μm, and 3.39 μm light wavelength, respectively. Because of the photogating effect, high gains up to 1.9 × 10 3 and 3.15 × 10 4 are obtained at 520 nm and 3.39 μm wavelength, respectively. At the communication wavelength of 1.55 μm, the tellurene photodetector exhibits an exceptionally high anisotropic behavior, and a large bandwidth of 37 MHz is obtained. The photodetection performance at different wavelength is further supported by the corresponding quantum molecular dynamics (QMD) simulations. Our approach has demonstrated the air-stable tellurene photodetectors that fully cover the short-wave infrared band with ultrafast photoresponse.

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

Highly Stable Fe/Co-TPY-MIL-88(NH 2 ) Metal–Organic Framework (MOF) in Enzymatic Cascade Reactions for Chemiluminescence-Based Detection of Extracellular Vesicles

Metal-Organic Frameworks (MOFs) can deliver many advantages when acting as enzyme mimics to assist with signal amplification in molecular detection: they have abundant active catalytic sites per unit volume of the material; their structures and elemental compositions are highly tunable, and their high specific surface area and porous property can assist with target separation and enrichment. In the present work, we have demonstrated that, by adding the pore partition agent, 2,4,6-tris(4-pyridyl)pyridine (TPY) during synthesis of the bimetallic Fe/Co-MIL-88(NH 2 ) MOF to block the open metal sites, a highly porous MOF of Fe/Co-TPY-MIL-88(NH 2 ) can be produced. This material also exhibits high stability in basic solutions and biofluids and possesses high peroxidase-mimicking activity, which can be utilized to produce long-lasting chemiluminescence (CL) from luminol and H 2 O 2 . Moreover, acting as the peroxidase-mimic, the Fe/Co-TPY-MIL-88(NH 2 ) MOF can form the enzymatic cascade with glucose oxidase (GOx) for biomarker detection. Further, when applied to detect extracellular vesicles (EVs), the MOF material and GOx are brought to the proximity on the EVs through two surface proteins, which triggers the enzyme cascade to produce high CL from glucose and luminol. EVs within the concentration range of 5 × 10 5 - 4 ×10 7 particles/mL can be detected, and the method can be used to analyze EV contents in human serum without sample preparation and EV purification. Overall, our work demonstrates that the high versatility and tunability of the MOF structures could bring in significant benefits to biosensing and enable ultrasensitive detection of biomarkers with judicious material designs.

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

Hexagonal boron nitride nanomechanical resonators with spatially visualized motion

Atomic layers of hexagonal boron nitride (h-BN) crystal are excellent candidates for structural materials as enabling ultrathin, two-dimensional (2D) nanoelectromechanical systems (NEMS) due to the outstanding mechanical properties and very wide bandgap (5.9 eV) of h-BN. In this work, we report the experimental demonstration of h-BN 2D nanomechanical resonators vibrating at high and very high frequencies (from ~ 5 to ~ 70 MHz), and investigations of the elastic properties of h-BN by measuring the multimode resonant behavior of these devices. First, we demonstrate a dry-transferred doubly clamped h-BN membrane with ~ 6.7 nm thickness, the thinnest h-BN resonator known to date. In addition, we fabricate circular drumhead h-BN resonators with thicknesses ranging from ~ 9 to 292 nm, from which we measure up to eight resonance modes in the range of ~ 18 to 35 MHz. Combining measurements and modeling of the rich multimode resonances, we resolve h-BN’s elastic behavior, including the transition from membrane to disk regime, with built-in tension ranging from 0.02 to 2 N m -1 . The Young’s modulus of h-BN is determined to be EY≈392 GPa from the measured resonances. The ultrasensitive measurements further reveal subtle structural characteristics and mechanical properties of the suspended h-BN diaphragms, including anisotropic built-in tension and bulging, thus suggesting guidelines on how these effects can be exploited for engineering multimode resonant functions in 2D NEMS transducers.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Plasmon mediated coherent population oscillations in molecular aggregates

The strong coherent coupling of quantum emitters to vacuum fluctuations of the light field offers opportunities for manipulating the optical and transport properties of nanomaterials, with potential applications ranging from ultrasensitive all-optical switching to creating polariton condensates. Often, ubiquitous decoherence processes at ambient conditions limit these couplings to such short time scales that the quantum dynamics of the interacting system remains elusive. Prominent examples are strongly coupled exciton-plasmon systems, which, so far, have mostly been investigated by linear optical spectroscopy. Here, we use ultrafast two-dimensional electronic spectroscopy to probe the quantum dynamics of J-aggregate excitons collectively coupled to the spatially structured plasmonic fields of a gold nanoslit array. We observe rich coherent Rabi oscillation dynamics reflecting a plasmon-driven coherent exciton population transfer over mesoscopic distances at room temperature. This opens up new opportunities to manipulate the coherent transport of matter excitations by coupling to vacuum fields.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Reversible parts-per-trillion-level detection of perfluorooctane sulfonic acid in tap water using field-effect transistor sensors

Widespread, persistent and toxic per- and polyfluoroalkyl substances (PFAS) pose a major threat to water systems and human health. Current detection methods are relatively expensive, slow and complex, underscoring the need for more accessible alternatives to meet increasingly stringent PFAS regulations. Here, in this study, we present an ultrasensitive sensing platform for perfluorooctane sulfonic acid detection in tap water with a reporting limit ( ~ 250 parts per quadrillion) lower than the US Environmental Protection Agency’s regulatory standard (4 parts per trillion), using a remote gate field-effect transistor featuring β-cyclodextrin (β-CD)-modified reduced graphene oxide as the sensing membrane. The sensor exhibits excellent selectivity against common inorganic ions, natural organic matter and select organic pollutants in tap water. The reversible and rapid response ( < 2 min) indicates the potential of remote gate field-effect transistor for continuous in-line monitoring. Mechanistic studies using quartz crystal microbalance and molecular dynamics simulations reveal key roles of analyte adsorption and charge properties in sensing performance and offer insights for designing more selective PFAS capture probes.

Wang, Yuqin [University of Chicago, IL (United Sta↗
DOE OSTI2015

Self-induced redox cycling coupled luminescence on nanopore recessed disk-multiscale bipolar electrodes

Self-induced redox cycling at nanopore ring-disk electrodes is coupled, through a bipolar electrode, to a remote fluorigenic reporter reaction. We present a new configuration for coupling fluorescence microscopy and voltammetry using self-induced redox cycling for ultrasensitive electrochemical measurements. An array of nanopores, each supporting a recessed disk electrode separated by 100 nm in depth from a planar multiscale bipolar top electrode, was fabricated using multilayer deposition, nanosphere lithography, and reactive-ion etching. Self-induced redox cycling was induced on the disk electrode producing ~30× current amplification, which was independently confirmed by measuring induced electrogenerated chemiluminescence from Ru(bpy) 3 2/3+ /tri-n-propylamine on the floating bipolar electrode. In this design, redox cycling occurs between the recessed disk and the top planar portion of a macroscopic thin film bipolar electrode in each nanopore. Electron transfer also occurs on a remote (mm-distance) portion of the planar bipolar electrode to maintain electroneutrality. This couples the electrochemical reactions of the target redox pair in the nanopore array with a reporter, such as a potential-switchable fluorescent indicator, in the cell at the distal end of the bipolar electrode. Oxidation or reduction of reversible analytes on the disk electrodes were accompanied by reduction or oxidation, respectively, on the nanopore portion of the bipolar electrode and then monitored by the accompanying oxidation of dihydroresorufin or reduction of resorufin at the remote end of the bipolar electrode, respectively. In both cases, changes in fluorescence intensity were triggered by the reaction of the target couple on the disk electrode, while recovery was largely governed by diffusion of the fluorescent indicator. Reduction of 1 nM of Ru(NH 3 ) 6 3+ on the nanoelectrode array was detected by monitoring the fluorescence intensity of resorufin, demonstrating high sensitivity fluorescence-mediated electrochemical sensing coupled to self-induced redox cycling.

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

Potential-induced wetting and dewetting in pH-responsive block copolymer membranes for mass transport control

Wetting and dewetting behavior in channel-confined hydrophobic volumes is used in biological membranes to effect selective ion/molecular transport. Artificial biomimetic hydrophobic nanopores have been devised utilizing wetting and dewetting, however, tunable mass transport control utilizing multiple transport modes is required for applications such as controllable release/transport, water separation/purification and energy conversion. Here, we investigate the potential-induced wetting and dewetting behavior in a pH-responsive membrane composed of a polystyrene-b-poly(4-vinylpyridine) (PS-b-P4VP) block copolymer (BCP) when fabricated as a hierarchically-organized sandwich structure on a nanopore electrode array (NEA), i.e. BCP@NEA. At pH < pK a (P4VP) (pK a ~ 4.8), the BCP acts as an anion-exchange membrane due to the hydrophilic, protonated P4VP cylindrical nanodomains, but at pH > pK a (P4VP), the P4VP domains exhibit charge-neutral, hydrophobic and collapsed structures, blocking mass transport via the hydrophobic membrane. However, when originally prepared in a dewetted condition, mass transport in the BCP membrane may be switched on if sufficiently negative potentials are applied to the BCP@NEA architecture. When the hydrophobic BCP membrane is introduced on top of 2-electrode-embedded nanopore arrays, electrolyte solution in the nanopores is introduced, then isolated, by exploiting the potential-induced wetting and dewetting transitions in the BCP membrane. The potential-induced wetting/dewetting transition and the effect on cyclic voltammetry in the BCP@NEA structures is characterized as a function of the potential, pH and ionic strength. Additionally chronoamperometry and redox cycling experiments are used to further characterize the potential response. The multi-modal mass transport system proposed in this work will be useful for ultrasensitive sensing and single-molecule studies, which require long-time monitoring to explore reaction dynamics as well as molecular heterogeneity in nanoconfined volumes.

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

Rational design of a genetically encoded NMR zinc sensor

Elucidating the biochemical roles of the essential metal ion, Zn 2+ , motivates detection strategies that are sensitive, selective, quantitative, and minimally invasive in living systems. Fluorescent probes have identified Zn 2+ in cells but complementary approaches employing nuclear magnetic resonance (NMR) are lacking. Recent studies of maltose binding protein (MBP) using ultrasensitive 129 Xe NMR spectroscopy identified a switchable salt bridge which causes slow xenon exchange and elicits strong hyperpolarized 129 Xe chemical exchange saturation transfer (hyper-CEST) NMR contrast. To engineer the first genetically encoded, NMR-active sensor for Zn 2+ , we converted the MBP salt bridge into a Zn 2+ binding site, while preserving the specific xenon binding cavity. The zinc sensor (ZS) at only 1 μM achieved ‘turn-on’ detection of Zn 2+ with pronounced hyper-CEST contrast. This made it possible to determine different Zn 2+ levels in a biological fluid via hyper-CEST. ZS was responsive to low-micromolar Zn 2+ , only modestly responsive to Cu 2+ , and nonresponsive to other biologically important metal ions, according to hyper-CEST NMR spectroscopy and isothermal titration calorimetry (ITC). Protein X-ray crystallography confirmed the identity of the bound Zn 2+ ion using anomalous scattering: Zn 2+ was coordinated with two histidine side chains and three water molecules. Penta-coordinate Zn 2+ forms a hydrogen-bond-mediated gate that controls the Xe exchange rate. Metal ion binding affinity, 129 Xe NMR chemical shift, and exchange rate are tunable parameters via protein engineering, which highlights the potential to develop proteins as selective metal ion sensors for NMR spectroscopy and imaging.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Synthesis and characterization of 10 nm thick piezoelectric AlN films with high c-axis orientation for miniaturized nanoelectromechanical devices

The scaling of piezoelectric nanoelectromechanical systems (NEMS) is challenged by the synthesis of ultrathin and high quality piezoelectric films on very thin electrodes. We report the synthesis and characterization of the thinnest piezoelectric aluminum nitride (AlN) films (10 nm) ever deposited on ultrathin platinum layers (2–5 nm) using reactive sputtering. X-ray diffraction, high-resolution transmission electron microscopy, and fast Fourier transform analyses confirmed the proper crystal orientation, fine columnar texture, and the continuous lattice structure within individual grains in the deposited AlN nanometer thick films. The average extracted d{sub 31} piezoelectric coefficient for the synthesized films is −1.73 pC/N, which is comparable to the reported values for micron thick and highly c-axis oriented AlN films. The 10 nm AlN films were employed to demonstrate two different types of optimized piezoelectric nanoactuators. The unimorph actuators exhibit vertical displacements as large as 1.1 μm at 0.7 V for 25 μm long and 30 nm thick beams. These results have a great potential to realize miniaturized NEMS relays with extremely low voltage, high frequency resonators, and ultrasensitive sensors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

“Rings of saturn-like” nanoarrays with high number density of hot spots for surface-enhanced Raman scattering

The Ag nanoparticles (NPs) surrounding triangular nanoarrays (TNAs) with high number density of surface-enhanced Raman scattering (SERS) hot spots (SERS hot spots ring) are prepared by a combination of NPs deposition and subsequent colloid lithography processing. Owing to the SERS hot spots ring, the Ag NPs surrounding TNAs have been proved an excellent candidate for ultrasensitive molecular sensing for their high SERS signal enhancing capacity in experiments and theories. The Ag NPs surrounding TNAs can be readily used for the quick detection of low concentrations of molecules related to food safety; herein, detection of melamine is discussed.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2014

Optical re-injection in cavity-enhanced absorption spectroscopy

Non-mode-matched cavity-enhanced absorption spectrometry (e.g., cavity ringdown spectroscopy and integrated cavity output spectroscopy) is commonly used for the ultrasensitive detection of trace gases. These techniques are attractive for their simplicity and robustness, but their performance may be limited by the reflection of light from the front mirror and the resulting low optical transmission. Although this low transmitted power can sometimes be overcome with higher power lasers and lower noise detectors (e.g., in the near-infrared), many regimes exist where the available light intensity or photodetector sensitivity limits instrument performance (e.g., in the mid-infrared). In this article, we describe a method of repeatedly re-injecting light reflected off the front mirror of the optical cavity to boost the cavity's circulating power and deliver more light to the photodetector and thus increase the signal-to-noise ratio of the absorption measurement. We model and experimentally demonstrate the method's performance using off-axis cavity ringdown spectroscopy (OA-CRDS) with a broadly tunable external cavity quantum cascade laser. The power coupled through the cavity to the detector is increased by a factor of 22.5. The cavity loss is measured with a precision of 2 × 10{sup −10} cm{sup −1}/√(Hz;) an increase of 12 times over the standard off-axis configuration without reinjection and comparable to the best reported sensitivities in the mid-infrared. Finally, the re-injected CRDS system is used to measure the spectrum of several volatile organic compounds, demonstrating the improved ability to resolve weakly absorbing spectroscopic features.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Ferroelectric-ferromagnetic multilayers: A magnetoelectric heterostructure with high output charge signal

Multiferroic composites and heterostructures comprising ferroelectric and ferromagnetic materials exhibit room-temperature magnetoelectric (ME) effects greatly exceeding those of single-phase magnetoelectrics known to date. Since these effects are mediated by the interfacial coupling between ferroic constituents, the ME responses may be enhanced by increasing the density of interfaces and improving their quality. A promising material system providing these features is a ferroelectric-ferromagnetic multilayer with epitaxial interfaces. In this paper, we describe theoretically the strain-mediated direct ME effect exhibited by free-standing multilayers composed of single-crystalline ferroelectric nanolayers interleaved by conducting ferromagnetic slabs. Using a nonlinear thermodynamic approach allowing for specific mechanical boundary conditions of the problem, we first calculate the polarization states and dielectric properties of ferroelectric nanolayers in dependence on the lattice mismatch between ferroic constituents and their volume fractions. In these calculations, the ferromagnetic component is described by a model which combines linear elastic behavior with magnetic-field-dependent lattice parameters. Then the quasistatic ME polarization and voltage coefficients are evaluated using the theoretical strain sensitivity of ferroelectric polarization and measured effective piezomagnetic coefficients of ferromagnets. For Pb(Zr₀.₅Ti₀.₅)O₃-FeGaB and BaTiO₃-FeGaB multilayers, the ME coefficients are calculated numerically as a function of the FeGaB volume fraction and used to evaluate the output charge and voltage signals. It is shown that the multilayer geometry of a ferroelectric-ferromagnetic nanocomposite opens the way for a drastic enhancement of the output charge signal. This feature makes biferroic multilayers advantageous for the development of ultrasensitive magnetic-field sensors for technical and biomedical applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Fabrication and characterization of large arrays of mesoscopic gold rings on large-aspect-ratio cantilevers

We have fabricated large arrays of mesoscopic metal rings on ultrasensitive cantilevers. The arrays are defined by electron beam lithography and contain up to 10{sup 5} rings. The rings have a circumference of 1 μm, and are made of ultrapure (6N) Au that is deposited onto a silicon-on-insulator wafer without an adhesion layer. Subsequent processing of the SOI wafer results in each array being supported at the end of a free-standing cantilever. To accommodate the large arrays while maintaining a low spring constant, the cantilevers are nearly 1 mm in both lateral dimensions and 100 nm thick. The extreme aspect ratio of the cantilevers, the large array size, and the absence of a sticking layer are intended to enable measurements of the rings' average persistent current in the presence of relatively small magnetic fields. We describe the motivation for these measurements, the fabrication of the devices, and the characterization of the cantilevers' mechanical properties. We also discuss the devices' expected performance in measurements of .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Conducting polymer functionalized single-walled carbon nanotube based chemiresistive biosensor for the detection of human cardiac myoglobin

We report the fabrication of a single-walled carbon nanotube (SWNT) based ultrasensitive label-free chemiresistive biosensor for the detection of human cardiac biomarker, myoglobin (Ag-cMb). Poly(pyrrole-co-pyrrolepropylic acid) with pendant carboxyl groups was electrochemically deposited on electrophoretically aligned SWNT channel, as a conducting linker, for biomolecular immobilization of highly specific cardiac myoglobin antibody. The device was characterized by scanning electron microscopy, source-drain current-voltage (I-V), and charge-transfer characteristic studies. The device exhibited a linear response with a change in conductance in SWNT channel towards the target, Ag-cMb, over the concentration range of 1.0 to 1000 ng ml{sup −1} with a sensitivity of ∼118% per decade with high specificity.

77 NANOSCIENCE AND NANOTECHNOLOGY↗