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At least 595 records · Page 33

Effect of Intermediate Semiconducting TiOx Thin Films on Nanoparticle-Mediated Electron Transfer: Electrooxidation of CO

The concept of nanoparticle-mediated electron transfer (eT) across insulating thin films was elucidated theoretically by Allongue and Chazalviel in 2011. In their model, metal nanoparticles (NPs) are immobilized atop passivating, self-assembled monolayers (SAMs). They found that under certain conditions, related to the thickness of the SAM and the size of the NPs, efficient faradaic oxidation and reduction reactions could proceed at the NP surface. In the absence of NPs, however, eT was suppressed by the insulating SAM thin films. Allongue and Chazalviel concluded that, within certain bounds, eT is mediated by fast tunneling between the conductive electrode and the metal NPs, while the kinetics of the redox reaction are controlled by the NPs. This understanding has been confirmed using a variety of experimental models. The theory is based on electron tunneling; therefore, the nature of the intervening medium (the insulator in prior studies) should not affect the eT rate. In the present manuscript, however, we show that the theory breaks down under certain electrochemical conditions when the medium between conductors is an n-type semiconductor. Specifically, we find that in the presence of either Au or Pt NPs immobilized on a thin film of TiOx, CO electrooxidation does not proceed. In contrast, the exact same systems lead to the efficient reduction of oxygen. At present, we are unable to explain this finding within the context of the model of Allongue and Chazalviel.

Galyamova, Aigerim↗

Dual-Input AND Gate From Single-Channel Thin-Film FET

A regio-regular poly(3-hexylthiophene) (RRP3HT) thin-film transistor having a split-gate architecture has been fabricated on a doped silicon/silicon nitride substrate and characterized. RRP3HT is a semiconducting polymer that has a carrier mobility and on/off ratio when used in a field effect transistor (FET) configuration. This commercially available polymer is very soluble in common organic solvents and is easily processed to form uniform thin films. The most important polymer-based device fabricated and studied is the FET, since it forms the building block in logic circuits and switches for active matrix (light-emitting-diode) (LED) displays, smart cards, and radio frequency identification (RFID) cards.

Miranda, F. A.↗

Thin-Film Paradigm to Probe Interfacial Diffusion during Solid-State Metathesis Reactions

We highlight a paradigm for studying complex reaction mechanisms that guide the synthesis of materials. Thin films of FeCl 2 and Na 2 S 2 were deposited to study the metathesis reaction to form FeS 2 and NaCl. In situ X-ray reflectivity was used to monitor the interface between materials, which revealed a slow, impeded reaction at high temperatures as compared to previous studies using powder samples. AC impedance and X-ray photoelectron spectroscopy provided insight into distribution of elements and conductivity of the phases present during the reaction, and phase-field modeling was used to elucidate the diffusion of ions throughout the thin-film bilayers. Here, the use of thin-film bilayers provides a simplified system to study solid-state metathesis reactions and highlights the complexity of diffusion at solid-state interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Superconductivity and normal-state transport in compressively strained La 2 PrNi 2 O 7 thin films

The discovery of superconductivity under high pressure in Ruddlesden-Popper phases of bulk nickelates has sparked great interest in stabilizing ambient pressure superconductivity in thin-film form using epitaxial strain. Recently, signs of superconductivity have been observed in compressively strained bilayer nickelate thin films with an onset temperature exceeding 40 K, albeit with broad and two-step-like transitions. Here, in this study, we report intrinsic superconductivity and normal-state transport properties in compressively strained La 2 PrNi 2 O 7 thin films, achieved through a combination of isovalent Pr substitution, growth optimization, and precision ozone annealing. The superconducting onset occurs above 48 K, with zero resistance reached above 30 K, and the critical current density at 1.4 K is 100-fold larger than previous reports. The normal-state resistivity exhibits quadratic temperature dependence indicative of Fermi liquid behaviour, and other phenomenological similarities to transport in overdoped cuprates suggest parallels in their emergent properties.

Liu, Yidi [SLAC National Accelerator Laboratory (S↗

Thin film thermal detector

Abnormally large variation of capacitance with temperature is obtained in thin film capacitors when a fixed ionic space charge is present in sufficient density in a dielectric film. This effect is the basis for a new kind of thin film thermal detector, whose performance at room temperature equals or exceeds that of comparable devices at much lower temperatures.

Maserjian, J.↗

Temperature and processing effects on lithium ion conductivity of solution‐deposited lithium zirconium phosphate (LiZr 2 P 3 O 12 ) thin films

Abstract Lithium zirconium phosphate (LiZr 2 P 3 O 12 ) thin films have been prepared on platinized silicon substrates via a chemical solution deposition approach with processing temperatures between 700°C and 775°C. Films that were subject to a single high‐temperature anneal were found to crystallize at temperatures above 725°C. Crystallization was observed in films annealed after each deposited layer at 700°C and above. In both cases, grain size was found to increase with annealing temperature. Ion conductivity was found to increase with annealing temperature in singly annealed films. In per‐layer annealed films ion conductivity was found to initially increase then decrease with increasing annealing temperature. A maximum ion conductivity of 1.6 × 10 −6 S/cm was observed for the singly annealed 775°C condition, while a maximum ion conductivity of 5.8 × 10 −7 S/cm was observed for the 725°C per‐layer annealed condition. These results are consistent with an increasing influence of cross‐plane, internal interface resistance and vapor phase carrier loss in the per‐layer annealed samples. This work demonstrates that post‐deposition processing methods can strongly affect the ion conducting properties of LiZr 2 P 3 O 12 thin films.

Brummel, Ian A.↗

Coexisting Phases in NaNbO 3 Thin Films Influenced by Epitaxial Strain and Size Effects

Coherently strained NaNbO 3 thin films are synthesized across a range of thicknesses, enabling the study of size effects under epitaxial strain in antiferroelectric thin films without relaxation. Competing antiferroelectric‐ferroelectric phases are observed, leading to the stabilization of phase coexistence, multistate switching with strong retention and fatigue performance, and potential avenues to boost energy storage properties.

antiferroelectrics↗

Stress-induced structural changes in superconducting Nb thin films

Here we report on the analysis of stress-induced structural changes and the formation of an omega (ω) phase in polycrystalline Nb thin films deposited on Si by high-power impulse magnetron sputtering (HiPIMS) for superconducting qubits using x-ray diffraction (XRD), transmission electron microscopy (TEM), and density-functional theory (DFT). XRD analysis indicates that internal stresses in the Nb thin films lead to the formation of {112}$\langle$111$\rangle$ deformation twins and TEM analysis shows that ω phases nucleate at some of the twin boundaries in the Nb thin films. The size of ω phases ranges from 10 to 100 nm, which is comparable to the coherence length of Nb (≈40 nm), and ≈1% volume fraction of Nb grains exhibit this ω phase. The details of the formation mechanism and superconducting properties of the ω phases are investigated by DFT and potential roles of the ω phase in Nb as a source of decoherence in superconducting qubits are also discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Epitaxial growth and characterization of magnesium gallate (MgGa 2 O 4 ) thin films by pulsed laser deposition

To advance high power device application of MgGa 2 O 4 , it is imperative to achieve crystalline epitaxial thin films and to observe its materials’ characteristics within a wide range of growth conditions. However, there is no published work on the growth of this promising ultrawide bandgap material till this day. In this study, we report the crystalline growth of MgGa 2 O 4 thin films on c-plane (006) sapphire substrates using the pulsed laser deposition (PLD) technique in a broad range of temperature and oxygen pressure. The temperature range for this crystalline growth was within the temperature range of 300°C to 700°C and a pressure range of 1x10 -1 to 1x10 -3 Torr. Within this parameter range, the structural, chemical, optical, and surface property of MgGa 2 O 4 thin films have been investigated. Specifically, the acquired XRD patterns confirmed the film growth along the [111] preferential crystal orientation in the lattice. Here, the rocking curve measurement of the prominent (222) plane showed an increasing trend of the crystallinity with growth temperature and pressure. Furthermore, the XRD phi (φ) scan demonstrated the six-fold rotational symmetry of the MgGa 2 O 4 films and the epitaxial relationship of 30° between the film and the sapphire substrate. The XPS spectra confirmed the presence of +2 and +3 oxidation state for Mg and Ga respectively, in the films. The direct bandgap of MgGa 2 O 4 films was obtained ~5.27±0.03 eV by analyzing the UV-Vis absorbance spectra using the Tauc equation. The SEM images exhibited a granular surface morphology of the MgGa 2 O 4 films with an increasing trend in the grain size from low to high temperature and pressure. The refractive index and thickness of these films were in the range of ~1.90±0.02 and ~70±2.0 nm, respectively determined by fitting the spectroscopic ellipsometry data.

36 MATERIALS SCIENCE↗

Electrolysis on a Chip with Tunable Thin Film Nanostructured PGM Electrocatalysts Generated from Self-Assembled Block Copolymer Templates

Self-assembled block copolymers are promising templates for fabricating thin film materials with tuned periodic feature sizes and geometry at the nanoscale. Here, a series of nanostructured platinum and iridium oxide electrocatalysts templated from poly(styrene)-block-poly(vinyl pyridine) (PSbPVP) block copolymers via an incipient wetness impregnation (IWI) pathway is reported. Both nanowire and nanocylinder electrocatalysts of varying feature sizes are assessed and higher catalyst loadings are achieved by the alkylation of the pyridine moieties in the PVP block prior to IWI. Electrocatalyst evaluations featuring hydrogen pump and water electrolysis demonstrations are carried out on interdigitated electrode (IDE) chips flexible with liquid supporting electrolytes and thin film polymer electrolytes. Notably, the mass activities of the nanostructured electrocatalysts from alkylated block copolymer templates are 35%–94% higher than electrocatalysts from non-alkylated block copolymer templates. Standing cylinder nanostructures lead to higher mass activities than lamellar variants despite their not having the largest surface area per unit catalyst loading demonstrating that mesostructure architectures have a profound impact on reactivity. Overall, IDE chips with model thin film electrocatalysts prepared from self-assembled block copolymers offer a high-throughput experimental method for correlating electrocatalyst nanostructure and composition to electrochemical reactivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Strongly temperature dependent ferroelectric switching in AlN, Al 1-x Sc x N, and Al 1-x B x N thin films

This manuscript reports the temperature dependence of ferroelectric switching in Al 0.84 Sc 0.16 N, Al 0.93 B 0.07 N, and AlN thin films. Polarization reversal is demonstrated in all compositions and is strongly temperature dependent. Between room temperature and 300 °C, the coercive field drops by almost 50% in all samples, while there was very small temperature dependence of the remanent polarization value. Furthermore, over this same temperature range, the relative permittivity increased between 5% and 10%. Polarization reversal was confirmed by piezoelectric coefficient analysis and chemical etching. Applying intrinsic/homogeneous switching models produces nonphysical fits, while models based on thermal activation suggest that switching is regulated by a distribution of pinning sites or nucleation barriers with an average activation energy near 28 meV.

36 MATERIALS SCIENCE↗

Performance Enhancement of Tunable Bandpass Filters Using Selective Etched Ferroelectric Thin Films

The inclusion of voltage-tunable barium strontium titanate (BSTO) thin films into planar band pass filters offers tremendous potential to increase their versatility. The ability to tune the passband so as to correct for minor deviations in manufacturing tolerances, or to completely reconfigure the operating frequencies of a microwave communication system, are highly sought-after goals. However, use of ferroelectric films in these devices results in higher dielectric losses, which in turn increase the insertion loss and decrease the quality factors of the filters. This study explores the use of patterned ferroelectric layers to minimize dielectric losses without degrading tunability. Patterning the ferroelectric layers enables us to constrict the width of the ferroelectric layers between the coupled microstrip lines, and minimize losses due to ferroelectric layers. Coupled one-pole microstrip bandpass filters with fundamental resonances at approx. 7.2 GHz and well defined harmonic resonances at approx. 14.4 and approx. 21.6 GHz, were designed, simulated and tested. For one of the filters, experimental results verified that its center frequency was tunable by 528 MHz at a center frequency of 21.957 GHz, with insertion losses varying from 4.3 to 2.5 dB, at 0 and 3.5 V/micron, respectively. These data demonstrate that the tuning-to-loss figure of merit of tunable microstrip filters can be greatly improved using patterned ferroelectric thin films as the tuning element, and tuning can be controlled by engineering the ferroelectric constriction in the coupled sections.

Miranda, Felix A.↗

A K-band Frequency Agile Microstrip Bandpass Filter using a Thin Film HTS/Ferroelectric/dielectric Multilayer Configuration

We report on YBa2Cu3O(7-delta) (YBCO) thin film/SrTiO3 (STO) thin film K-band tunable bandpass filters on LaAlO3 (LAO) dielectric substrates. The 2 pole filter has a center frequency of 19 GHz and a 4% bandwidth. Tunability is achieved through the non-linear dc electric field dependence of the relative dielectric constant of STO(epsilon(sub rSTO). A large tunability ((Delta)f/f(sub 0) = (f(sub Vmax) - f(sub 0)/f(sub 0), where f(sub 0) is the center frequency of the filter at no bias and f(sub Vmax) is the center frequency of the filter at the maximum applied bias) of greater than 10% was obtained in YBCO/STO/LAO microstrip bandpass filters operating below 77 K. A center frequency shift of 2.3 GHz (i.e., a tunability factor of approximately 15%) was obtained at a 400 V bipolar dc bias, and 30 K, with minimal degradation in the insertion loss of the filter. This paper addresses design, fabrication and testing of tunable filters based on STO ferroelectric thin films. The performance of the YBCO/STO/LAO filters is compared to that of gold/STO/LAO counterparts.

Subramanyam, Guru↗

Steady-State and Frequency Response of a Thin-Film Heat Flux Gauge

A new and simpler design of thin-film heat flux gauge has been developed for use In high-heat-flux environments. Heat flux gauges of the same design were fabricated on three different substrates and tested. The heat flux gauge comprises a thermopile and a thermocouple junction, which measures the surface temperature. The thermopile has 40 pairs of S-type thermocouples and is covered by two thermal resistance layers. Calibration and testing of these gauges were first carried out in an arc-lamp calibration facility. Sensitivity of the gauge was discussed in terms of the relative conductivity and surface temperature. The heat flux calculated from the gauge output was In good agreement with the precalibrated standard sensor. The steady-state and the transient response characteristics of the heat flux gauge were also investigated using a carbon dioxide pulse laser as a heat source. The dynamic frequency response was evaluated in terms of the nondimensional amplitude ratio with respect to the frequency spectrum of a chopped laser bcam. The frequency response of the gauge was determined to be about 3 kHz. The temperature profiles in the thin-film heat flux gauge were obtained numerically in steady-state conditions using FLUENT and compared with the experimental results.

Fralick, Gustave C.↗

Strain‐Driven Mixed‐Phase Domain Architectures and Topological Transitions in Pb 1− x Sr x TiO 3 Thin Films

Abstract The potential for creating hierarchical domain structures, or mixtures of energetically degenerate phases with distinct patterns that can be modified continually, in ferroelectric thin films offers a pathway to control their mesoscale structure beyond lattice‐mismatch strain with a substrate. Here, it is demonstrated that varying the strontium content provides deterministic strain‐driven control of hierarchical domain structures in Pb 1− x Sr x TiO 3 solid‐solution thin films wherein two types, c / a and a 1 / a 2 , of nanodomains can coexist. Combining phase‐field simulations, epitaxial thin‐film growth, detailed structural, domain, and physical‐property characterization, it is observed that the system undergoes a gradual transformation (with increasing strontium content) from droplet‐like a 1 / a 2 domains in a c / a domain matrix, to a connected‐labyrinth geometry of c / a domains, to a disconnected labyrinth structure of the same, and, finally, to droplet‐like c / a domains in an a 1 / a 2 domain matrix. A relationship between the different mixed‐phase modulation patterns and its topological nature is established. Annealing the connected‐labyrinth structure leads to domain coarsening forming distinctive regions of parallel c / a and a 1 / a 2 domain stripes, offering additional design flexibility. Finally, it is found that the connected‐labyrinth domain patterns exhibit the highest dielectric permittivity.

Kavle, Pravin↗

Future Directions for Thin Films in Space Workshop at SPRAT XVIII

For approximately ten years, the SPRAT conference series at NASA Glenn (formerly Lewis) Research Center has devoted a workshop to the topic of thin-film solar cell technology and its potential for space applications. While thin-film materials have been investigated for a number of years, including copper sulfide research at NASA in the 1960 s, there has been a re-birth of interest in this class of materials for space applications in the past dozen years or so. There are several reasons for this renaissance. An important contributor is efficiency improvements beyond ten percent. Another contributor is the increase in interest represented by funding opportunities by NASA and several agencies in the U.S. Department of Defense (Missile Defense Agency, Air Force, and DARPA). Finally, there have been several intriguing missions identified through various means, these include: station-keeping for high-altitude airships, space solar power, planetary surface power, and solar electric propulsion. To aid in leading the discussion for this workshop, a series of seven questions were posed. These are reproduced below as well as a summary of key points and conclusions from the workshop as well as an attendees list and results of an informal poll related to long-term potential of thin films for space.

Hepp, Aloysius F.↗