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DOE OSTI2022

Ultrafast infrared plasmon switching in aligned carbon-nanotube optical resonators

Reconfigurable plasmonic materials are crucial components in active photonic devices for optical communication, signal processing, and sensing applications. Certain candidates including transparent conducting oxides, small-bandgap semiconductors (i.e. Ge, InSb), and conducting polymers can exhibit switchable free carrier concentrations triggered by optical, electrical or thermal excitations. Here, we show that aligned films of single-walled carbon nanotubes (SWCNTs) can serve as all-optically tunable plasmonic material in the mid-infrared range, thereby adding them to the library of switchable plasmonic materials. Interband optical pumping with femtosecond laser pulses results in the photoexcitation of free charge carriers, which transiently blueshifts the plasmon resonances of patterned, periodic SWCNT nano-resonators spanning the mid-infrared spectral range from 1700 to 2700 cm -1 . Furthermore. the ultrafast plasmon modulation exhibits a nearly single-picosecond decay time, attributed to interband carrier relaxation and inter-tube charge transfer. Given that aligned films of SWCNTs have high thermal stability, excellent photostability, epsilon-near-zero property, and extremely large optical anisotropy, their dynamic tunability represents a promising pathway towards active optical devices in the technologically important mid-infrared range.

single-walled carbon nanotubes↗

DOE OSTI2025

Mesoporous optically clear heat insulators for sustainable building envelopes

Mesoporous materials exhibit highly controlled nanoscale structures, often templated by liquid crystalline assemblies of surfactants, with emergent and often designable physical properties. However, scaling their fabrication to be suitable for uses like envelopes of buildings is challenging. Here we describe fabrication of flexible square-meter-sized films and multi-centimeter-thick slabs made of three-dimensional spatial graphs of mesopore tubes having all structural features under 50 nanometers. Solution-based kinetic fabrication process templates growing networks of cylindrical surfactant micelles with thin tubes of polysiloxane forming gel networks and, upon replacing surfactants and solvents with air, yields lightweight materials with >99% visible-range optical transparency and ~10 mW K-1m-1 thermal conductivity. Such predesigned metamaterials enable transparent thermal barriers for wall-grade insulated glass units, square-meter window retrofits and unconcentrated solar thermal energy harnessing.

14 SOLAR ENERGY↗

DOE OSTI2025

Enabling ITO-free perovskite solar cells through n-doped poly(benzodifurandione) (n-PBDF) electrodes

The burgeoning commercialization of perovskite solar cells (PSCs) is propelled by their exceptional power conversion efficiency (PCE), enhanced stability, and ease of fabrication. However, the rigidity of mainstream transparent conductive oxides (TCOs) limits the adaptability of PSCs to various application scenarios. Although alternative materials such as silver nanowires, carbon nanotubes, graphene, and PEDOT:PSS have been evaluated, the p-type nature confines their device designs to inverted architecture and restricts broader applicability. Here, for the first time, a conducting polymer electrode based on n-doped poly(benzodifurandione) (n-PBDF) was used to replace TCOs in PSCs. The n-PBDF electrodes can be readily fabricated via low-temperature, solution-based processes, indicating substantial potential for reducing manufacturing costs. Furthermore, its integration into PSCs has negligible effect on the phase, morphology, or photophysical properties of the perovskite layer, which is comparable to the typical TCOs. After optimization, the n-PBDF-based device achieves a power conversion efficiency of 12.70 and 11.23%, for rigid and flexible devices, respectively. Our study provides a promising alternative to the widely used TCOs in PSCs, highlighting the advantages of using n-doped conducting polymers in terms of processability and flexibility.

Kumar, Prashant [Purdue University, West Lafayette↗

DOE OSTI2024

Computational Insights into Phase Equilibria Between Wide-Gap Semiconductors and Contact Materials

Novel wide-band-gap semiconductors are needed for next-generation power electronics, but there is a gap between a promising material and a functional device. Finding stable (metal) contacts is one of the major challenges that is currently dealt with mainly via trial and error. Herein, we computationally investigate the thermochemistry and phase coexistence at the junction between three wide-gap semiconductors, ..beta..-Ga2O3, GeO2, and GaN, and possible contact materials. The pool of possible contacts includes 47 elemental metals and a set of 4 common, n-type transparent conducting oxides (ZnO, TiO2, SnO2, and In2O3). We use first-principles thermodynamics to model the Gibbs free energies of chemical reactions as a function of gas pressure (pO2/pN2) and equilibrium temperature. We deduce whether a semiconductor/contact interface will be stable at relevant conditions or a chemical reaction between them is to be expected, possibly influencing the long-term reliability and performance of devices. We generally find that most elemental metals tend to oxidize or nitridize and form various interface oxide/nitride layers. Exceptions include select late- and post-transition metals and, in the case of GaN, also the alkali metals, which are predicted to exhibit stable coexistence, although in many cases at relatively low gas partial pressures. Similar is true for the transparent conducting oxides, for which, in most cases, we predict a preference toward forming ternary oxides when in contact with ..beta..-Ga2O3 and GeO2. The only exception is SnO2, which we find to form stable contacts with both oxides. Finally, we show how the same approach can be used to predict gas partial pressure vs temperature phase diagrams to help direct synthesis of ternary compounds. We believe these results provide a valuable guidance in selecting contact materials to wide-gap semiconductors and suitable growth conditions.

contact materials↗

NASA NTRS1988

An investigation of the optical constants and band gap of chromium disilicide

Optical properties of polycrystalline thin films of CrSi2 grown by the diffusion couple method on silicon substrates were investigated. An analysis of the energy dependence of the absorption coefficient indicates that the material is an indirect forbidden gap semiconductor with a band-gap value of slightly less than 0.35 eV. This result was confirmed by measurements of the temperature dependence of the intrinsic conductivity. The value of the bandgap corresponds well to an important window of transparency in the earth's atmosphere (3-5 microns), which makes the material of potential interest for IR detector applications.

Bost, M. C.↗

DOE OSTI2022

Clean quantum point contacts in an InAs quantum well grown on a lattice-mismatched InP substrate

Strong spin-orbit coupling, the resulting large g factor, and small effective mass make InAs an attractive material platform for inducing topological superconductivity. The surface Fermi level pinning in the conduction band enables highly transparent ohmic contact without excessive doping. In this study, we investigate electrostatically defined quantum point contacts (QPCs) in a deep-well InAs two-dimensional electron gas. Despite the 3.3% lattice mismatch between the InAs quantum well and the InP substrate, we report clean QPCs with up to eight pronounced quantized conductance plateaus at zero magnetic field. Source-drain dc bias spectroscopy reveals a harmonic confinement potential with a nearly 5 meV subband spacing. We find a many-body exchange interaction enhancement for the out-of-plane g factor |$g^{*}_{⊥}$|=27±1 , whereas the in-plane g factor is isotropic |$g^{*}_{x}$|=|$g^{*}_{y}$|=12±2 , close to the bulk value for InAs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Summary Report on Ion Irradiation Study of Ceramic Coating on Suppressing FCCI

Advanced cladding is critical for advanced nuclear reactors with an enhanced performance in radiation tolerance and neutron transparency. Using advanced cladding will ensure the adequate thermal conductivity and mechanical stability of the cladding base material, corrosion resistance, high-temperature coolant compatibility of the cladding surface, and chemical stability in the cladding inner wall against fuel cladding chemical interaction (FCCI). An innovative cladding with a three-layer structure (i.e., a modified surface, a clad base material, and a modified inner wall) promises to meet all these requirements. Initial research and development (R&D) regarding this innovative cladding seek to demonstrate the effectiveness of a thin ceramic coating in suppressing FCCI under ion irradiation to high dose. This United States (U.S.) Department of Energy (DOE)–Office of Nuclear Energy (NE) project report summarizes the results of recent ion irradiation studies of diffusion-couple samples with details of an ion irradiation experiment, the characterization of the interface microstructure of cerium (Ce)/titanium nitride (TiN)/oxide-dispersion strengthened (ODS), Ce/TiN/iron (Fe), Ce/ODS, and Ce/Fe samples irradiated with 80 million electron-volts (MeV) of xenon (Xe) ions to 100 displacements per atom (dpa) at 500?C using the Argonne Tandem Linac Accelerator System (ATLAS) facility at Argonne National Laboratory (ANL). The results of the ODS-substrate sample are encouraging and demonstrate the effectiveness of a thin ceramic coating on FCCI mitigation under irradiation. The results from an Fe-substrate sample revealed a complex microstructure, and the root cause is discussed.

36 MATERIALS SCIENCE↗

NASA NTRS1984

Design, analysis and test verification of advanced encapsulation systems

Investigations into transparent conductive polymers were begun. Polypyrrole was electrochemically deposited, but the film characteristics were poor. A proprietary polymer material supplied by Polaroid was evaluated and showed promise as a readily processable material. A method was developed for calculating the magnitude and location of the maximum electric field for the family of solar-cell-like shapes. A method for calculating the lines of force for three dimensional electric fields was developed and applied to a geometry of interest to the photovoltaic program.

Garcia, A., III↗

DOE OSTI2022

Pressure Engineering Promising Transparent Oxides with Large Conductivity Enhancement and Strong Thermal Stability

Abstract Transparent conducting oxides (TCO) with high electrical conductivity and high visible light transparency are desired for a wide range of high‐impact engineering. Yet, usually, a compromise must be made between conductivity and transparency, limiting the practical application of a TCO to the next level. Furthermore, TCO performance is highly sensitive to composition, so conventional synthesis methods, such as chemical doping, cannot unravel the mysteries of the quantitative structure–performance relationship. Thus, improving the fundamental understanding or creating materials‐by‐design has limited success. Here, a strategy is proposed to modulate the lattice and electronic and optical properties precisely by applying pressure on a TCO. Strikingly, after compression–decompression treatment on the indium titanium oxides (ITiO), a highly transparent and metastable phase with two orders of magnitude enhancement in conductivity is synthesized from an irreversible phase transition. Moreover, this phase possesses previously unattainable filter efficiency on hazardous blue light up to 600 °C, providing potential for healthcare‐related applications with strong thermal stability up to 200 °C. These results demonstrate that pressure engineering is a clean and effective tool for tailoring functional materials that are not achievable by other means, providing an exciting alternative property‐tuning dimension in materials science.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Status Report on the Development of Cladding Inner-wall and Outer-wall Coatings

Advanced cladding is critical for nuclear reactors with enhanced performance in radiation tolerance, neutron transparency and reactor safety. Using advanced cladding will ensure the adequate thermal conductivity and mechanical stability of the cladding base material, corrosion resistance and high-temperature coolant compatibility of the cladding surface, and chemical stability in the cladding inner wall against fuel cladding chemical interaction (FCCI). An innovative cladding with a three-layer structure (i.e., a modified outer surface, a robust clad base material, and a modified inner wall) promises to meet all these requirements. In this status report, the initial efforts on the development of cladding inner-wall and outer-wall coatings are summarized. The activities covered in this report are (1) High-resolution TEM studies of TiN/HT-9 interface atomic structure and chemistry after ion irradiation, (2) High-resolution TEM studies of TiN/14YWT ODS interface atomic structure after thermal cycling, (3) Inner-wall TiN coating for an experimental 14YWT ODS cladding, and (4) Corrosion test of TiN coated Ziracloy-4 bar samples.

36 - MATERIALS SCIENCE↗

NASA NTRS1993

Transparent conductive coatings in the far ultraviolet

In certain cases a space-borne optical instrument with a dielectric window requires a transparent conductive coating deposited on the window to remove the electrostatic charge collected due to the bombardment of ionized particles. Semiconductor and metal films are studied for use as transparent conductive coatings for the front window of far ultraviolet camera. Cr is found to be the best coating material. The theoretical search for the semiconductor and metal coating materials and experimental results for ITO and Cr films are reported.

Kim, Jongmin↗

NASA NTRS1995

Silicon Satellites: Picosats, Nanosats, and Microsats

Silicon, the most abundant solid element in the Earth's lithosphere, is a useful material for spacecraft construction. Silicon is stronger than stainless steel, has a thermal conductivity about half that of aluminum, is transparent to much of the infrared radiation spectrum, and can form a stable oxide. These unique properties enable silicon to become most of the mass of a satellite, it can simultaneously function as structure, heat transfer system, radiation shield, optics, and semiconductor substrate. Semiconductor batch-fabrication techniques can produce low-power digital circuits, low-power analog circuits, silicon-based radio frequency circuits, and micro-electromechanical systems (MEMS) such as thrusters and acceleration sensors on silicon substrates. By exploiting these fabrication techniques, it is possible to produce highly-integrated satellites for a number of applications. This paper analyzes the limitations of silicon satellites due to size. Picosatellites (approximately 1 gram mass), nanosatellites (about 1 kg mass), and highly capable microsatellites (about 10 kg mass) can perform various missions with lifetimes of a few days to greater than a decade.

Janson, Siegfried W.↗

DOE OSTI2020

On-device lead sequestration for perovskite solar cells

Perovskite solar cells, as an emerging high-efficiency and low-cost photovoltaic technology face challenges on their way towards commercialization. Substantial improvements have been made to device stability but potential issues with lead toxicity and leaching from devices remain relatively unexplored. The potential for lead leakage could be perceived as an environmental and public health risk when using perovskite solar cells in building-integrated photovoltaics. Here we present a chemical approach for on-device sequestration of more than 96 per cent of lead leakage caused by severe device damage. A coating of lead-absorbing material is applied to the front and back sides of the device stack. On the glass side of the front transparent conducting electrode, we use a transparent lead-absorbing molecular film containing phosphonic acid groups that bind strongly to lead. On the back (metal) electrode side, we place a polymer film blended with lead-chelating agents between the metal electrode and a standard photovoltaic packing film. The lead-absorbing films on both sides swell to absorb the lead, rather than dissolve, when subjected to water soaking, thus retaining structural integrity for easy collection of lead after damage.

14 SOLAR ENERGY↗

DOE OSTI2025

Indium Tin-Doped Oxide Interactions with Solvent Radiolysis Products

Transparent conductive oxides (TCOs), such as indium tin-doped oxide (ITO), are ubiquitous as components of electronics and are ideal electrode substrates for catalysis, energy transformation reactions, and energy storage applications. Recently, researchers have recognized their effectiveness as electrode materials for manipulating actinide oxidation states in solution. Despite their popularity as electrode materials, prior studies focused extensively on the direct radiolysis of TCO materials in air and rarely examined these effects within a solution, limiting our fundamental understanding of the interactions between solvent radiolysis products and these substrates in high radiation environments. Here, in this study, we characterize the effects of solvent radiolysis products—arising from the gamma irradiation of water, aqueous nitric acid solutions, and n-dodecane—on the composition, surface speciation, and band structure of ITO thin films on a glass substrate as a function of absorbed dose using UV-visible spectroscopy, scanning electron microscopy, photoelectrochemistry, and X-ray photoelectron spectroscopy. Our work demonstrates that mesoporous thin film electrodes of ITO exposed to gamma radiation in each solvent accumulate defects and exhibit solvent and dose dependent changes to their surface and interfacial properties. These electrodes maintain their electrochemical function and improve their photoelectrochemical performance up to at least 100 kGy of accumulated gamma dose, confirming their utility in solvents exposed to ionizing radiation fields.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

On the Equilibrium Electrostatic Potential and Light-Induced Charge Redistribution in Halide Perovskite Structures

Lead halide perovskites are semiconductor materials which are employed as nonintentionally doped absorbers inserted between two selective carrier transport layers (SCTL), realizing a p-i-n or n-i-p heterojunction. In our study, we have developed and investigated a lateral device, based on methylammonium lead iodide (MAPbI3) in which the p-i-n heterojunction develops in the horizontal direction. Our research suggests that the effective doping level in the MAPbI3 film should be very low, below 1012 cm-3. Along the vertical direction, this doping level is not enough to screen the electric field of the buried heterojunction with the SCTL. The perovskite work function is therefore affected by the work function of the SCTL underneath. From drift-diffusion simulations, we show that intrinsic perovskite-SCTL structures develop mV range surface photovoltages (SPVs) under continuous illumination. However, perovskite-SCTL structures can develop SPVs of hundreds of mV, as confirmed by our measurements. We therefore analyzed the compatibility between low doping and low defect densities in the perovskite layer and such high SPV values using numerical modeling. It is shown that these high SPV values could originate from electronic processes due to large band offsets in the buried perovskite-SCTL heterojunctions, or at the SCTL-transparent conductive oxide (TCO) buried heterojunction. However, such electronic processes can hardly explain the long SPV persistence after switching off the illumination.

defects↗

DOE OSTI2022

Fabrication of ultrathin suspended membranes from atomic layer deposition films

In this report, ultrathin films suspended as freestanding membranes are critical to many microelectronic and materials science applications. However, fabrication methods are currently limited in either their flexibility, due to material selectivity issues during the final membrane release, or their scalability. Here, we demonstrate a novel fabrication process for suspending ultrathin films with thicknesses as low as 4 nm and lateral dimensions up to 20 x 1000 μm from a variety of materials grown by atomic layer deposition. A silicon nitride membrane serves as the support for a sacrificial polymer layer and an ultrathin atomic layer deposition film which, after plasma etching, will form the membrane. The high chemical selectivity between atomic layer deposition-grown transition metal nitrides and oxides and the sacrificial polymer means that ultrathin films of a variety of materials can be released without damage using a single process. Electrically conductive titanium nitride membranes can be produced by this method and are of significant interest for electron microscopy applications. Electron transparency of titanium nitride membranes was found to be ~14% higher than silicon nitride of the same thickness, and of similar conductivity to graphite, meaning that ultrathin, conductive, and electron transparent membranes can be fabricated at scale. These membranes are ideal supports for electron and photon characterization techniques, as well as microelectromechanical system applications that require a conductive membrane.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Effects of pillar design on the thermal performance of vacuum-insulated glazing

Vacuum-insulated glazing (VIG) with a low-emittance coating has a great market potential as an effective transparent insulator. The thermal insulating performance of VIG is determined by its design, including material selection and configuration of different components. Thermal conductance of the vacuum gap as a transport bottleneck is one of the primary factors controlling the thermal transport across VIG. In particular, because support pillars provide the main thermal transport channels across the vacuum gap, increasing the pillar thermal resistance is a key strategy for creating effective thermal insulation while maintaining the vacuum space. Here, the effects of various pillar design parameters, such as thermal conductivity, geometry, and arrangement, on the VIG thermal performance were comprehensively investigated via the finite element method. In addition, analytical models for thermal transport were examined and thermal conductance across the VIG unit was experimentally measured for validation. The pillar design parameters, especially the height, shape, spacing, and arrangement of the pillars, showed significant effects on the thermal performance of VIG. This research also shows that the smaller contact area for horizontal pillars can effectively decrease the heat loss by more than 30%. Because current VIG analytical equations of thermal performance are only applicable to cylindrical pillars, an analytical equation that can better describe the thermal performance of rectangular parallelepiped pillars is presented, along with a discussion about the mechanism of thermal transfer for different pillar shapes. Thermo-mechanical analyses based on 3D FEM simulations can provide valuable insights into the effect of various design parameters on the overall performance the VIG, allowing for the development of an optimal VIG design.

36 MATERIALS SCIENCE↗

NASA NTRS2003

Basic and Applied Materials Science Research Efforts at MSFC Germane to NASA Goals

Presently, a number of investigations are ongoing that blend basic research with engineering applications in support of NASA goals. These include (1) "Pore Formation and Mobility (PFMI) " An ISS Glovebox Investigation" NASA Selected Project - 400-34-3D; (2) "Interactions Between Rotating Bodies" Center Director's Discretionary Fund (CDDF) Project - 279-62-00-16; (3) "Molybdenum - Rhenium (Mo-Re) Alloys for Nuclear Fuel Containment" TD Collaboration - 800-11-02; (4) "Fabrication of Alumina - Metal Composites for Propulsion Components" ED Collaboration - 090-50-10; (5) "Radiation Shielding for Deep-Space Missions" SD Effort; (6) "Other Research". In brief, "Pore Formation and Mobility" is an experiment to be conducted in the ISS Microgravity Science Glovebox that will systematically investigate the development, movement, and interactions of bubbles (porosity) during the controlled directional solidification of a transparent material. In addition to promoting our general knowledge of porosity physics, this work will serve as a guide to future ISS experiments utilizing metal alloys. "Interactions Between Rotating Bodies" is a CDDF sponsored project that is critically examining, through theory and experiment, claims of "new" physics relating to gravity modification and electric field effects. "Molybdenum - Rhenium Alloys for Nuclear Fuel Containment" is a TD collaboration in support of nuclear propulsion. Mo-Re alloys are being evaluated and developed for nuclear fuel containment. "Fabrication of Alumina - Metal Composites for Propulsion Components" is an ED collaboration with the intent of increasing strength and decreasing weight of metal engine components through the incorporation of nanometer-sized alumina fibers. "Radiation Shielding for Deep-Space Missions" is an SD effort aimed at minimizing the health risk from radiation to human space voyagers; work to date has been primarily programmatic but experiments to develop hydrogen-rich materials for shielding are planned. "Other Research" includes: BUNDLE (Bridgman Unidirectional Dendrite in a Liquid Experiment) activities (primarily crucible development), vibrational float-zone processing (with Vanderbilt University), use of ultrasonics in materials processing (with UAH), rotational effects on microstructural development, and application of magnetic fields for mixing.

Source record↗