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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 55 records · Page 3

P-Type Transparent Cu-Alloyed ZnS Deposited at Room Temperature

All transparent conducting materials (TCMs) of technological practicality are n-type; the inferior conductivity of p-type TCMs has limited their adoption. Additionally, many relatively high-performing p-type TCMs require synthesis temperatures > 400 °C. Here, room-temperature pulsed laser deposition of copper-alloyed zinc sulfide (Cu x Zn 1- x S) thin films (0 ≤ x ≤ 0.75) is reported. For 0.09 ≤ x ≤ 0.35, Cu x Zn 1- x S has high p-type conductivity, up to 42 S cm -1 at x = 0.30, with an optical band gap tunable from ≈3.0–3.3 eV and transparency, averaged over the visible, of 50%–71% for 200–250 nm thick films. In this range, synchrotron X-ray and electron diffraction reveal a nanocrystalline ZnS structure. Secondary crystalline Cu y S phases are not observed, and at higher Cu concentrations, x > 0.45, films are amorphous and poorly conducting. Furthermore, within the TCM regime, the conductivity is temperature independent, indicating degenerate hole conduction. A decrease in lattice parameter with Cu content suggests that the hole conduction is due to substitutional incorporation of Cu onto Zn sites. This hole-conducting phase is embedded in a less conducting amorphous Cu y S, which dominates at higher Cu concentrations. Finally, the combination of high hole conductivity and optical transparency for the peak conductivity Cu x Zn 1- x S films is among the best reported to date for a room temperature deposited p-type TCM.

36 MATERIALS SCIENCE↗

Cellulosic gels, films and composites including the gels, and methods of forming same

Disclosed are cellulose-based 5 flexible aerogels and xerogels containing bacterial cellulose nanorods, ribbons, fibers, and the like, wherein the gels have tunable optical, heat transfer, and stiffness properties. Further disclosed are highly transparent and flexible cellulose nanofiber-polysiloxane composite aerogels featuring enhanced mechanical robustness, tunable optical anisotropy, and low thermal conductivity.

Smalyukh, Ivan I.↗

First-Principles Investigation of Borophene as a Monolayer Transparent Conductor

Two-dimensional boron is promising as a tunable monolayer metal for nano-optoelectronics. We study the optoelectronic properties of two likely allotropes of two-dimensional boron, β12 and δ6, using first-principles density functional theory and many-body perturbation theory. We find that both systems are anisotropic metals, with strong energy- and thickness-dependent optical transparency and a weak (<1%) absorbance in the visible range. Additionally, using state-of-the-art methods for the description of the electron–phonon and electron–electron interactions, we show that the electrical conductivity is limited by electron–phonon interactions. Furthermore, our results indicate that both structures are suitable as a transparent electrode.

36 MATERIALS SCIENCE↗

Tunability of indium tin oxide materials for mid-infrared plasmonics applications

Transparent conductive oxides (TCOs) have emerged as alternative plasmonic materials in recent years to replace noble metals. The advantages of TCOs include CMOS compatibility, tunability of optical and structural properties, and reduced losses. In this work, we demonstrate how post-deposition annealing of indium tin oxide (ITO) films in oxygen atmosphere allows for tuning their optical dispersion properties to the mid-infrared spectral range while simultaneously reducing their absorption losses. In particular, we show a materials strategy that extends the epsilon-near-zero (ENZ) point of ITO from the near-infrared to the mid-infrared range. This is demonstrated by fabricating periodic arrays of ITO discs of varying diameters and characterizing their plasmonic resonances in the mid-infrared range from λ = 5 to 10 µm. The developed ITO plasmonic structures pave the way to the development of novel infrared active devices for sensing and spectroscopy on a silicon-compatible platform.

36 MATERIALS SCIENCE↗

Transparent conducting oxides: A -doped superlattice approach

Two-dimensional electron gases (2DEGs) at the interface of oxide heterostructures have been the subject of recent experiment and theory, due to the intriguing phenomena that occur in confined electronic states. However, while much has been done to understand the origin of 2DEGs and related phenomena, very little has been explored with regards to the control of conduction pathways and the distribution of charge carriers. Using first principles simulations and experimental thin film synthesis methods, we examine the effect of dimensionality on carrier transport in La delta-doped SrTiO3 (STO) superlattices, as a function of the thickness of the insulating STO spacer. Our computed Fermi surfaces and layer-resolved carrier density proles demonstrate that there is a critical thickness of the STO spacer, below which carrier transport is dominated by three-dimensional conduction of interface charges arising from appreciable overlap of the quantum mechanical wavefunctions between neighboring delta-doped layers. We observe that, experimentally, these superlattices remain highly transparent to visible light. Band structure calculations indicate that this is a result of the appropriately large gap between the O 2p and Ti d states. The tunability of the quantum mechanical wavefunctions and the optical transparency highlight the potential for using oxide heterostructures in novel opto-electronic devices; thus providing a route to the creation of novel transparent conducting oxides.

Cooper, Valentino R↗

Thermally Responsive Hydrogels for Passive Temperature Regulation under Direct Sunlight

By spontaneously emitting midinfrared radiation to outer space through the atmospheric window and reflecting sunlight, daytime radiative coolers achieve notable passive cooling performance. However, existing daytime radiative cooling systems generally lack the ability to adaptively switch between heating and cooling states based on ambient conditions. Herein a passive thermal regulation system that features a temperature‐dependent switchable solar reflectance from 0.05 (low temperature) to 0.8 (high temperature) is presented. This, along with a ≈0.95 midinfrared emittance, it enables automatic switching between radiative cooling and solar heating. Switchablity is enabled using a poly( N ‐isopropylacrylamide) (PNIPAM) hydrogel which exhibits high solar scattering above its tunable lower critical solution temperature (LCST) and transparency below its LCST. The lower part of the hydrogel is loaded with graphite to absorb solar energy in the heating state. In testing under sunny and partly cloudy outside conditions, this system maintains a temperature close to the set LCST.

Xie, Dajie↗

Effect of Interface Structure on the Hydrophobicity, Mechanical and Optical Properties of HfO2/Mo/HfO2 Multilayer Films

We report on the super-hydrophobicity and tunable and optical and mechanical properties of transparent HfO2(50 nm)/Mo(20 nm)/HfO2(50 nm) multilayer films facilitated by engineering the ceramic-metal interface microstructure. A comparative study of nano-columnar and glassy (dense) structured HfO2/Mo/HfO2 multilayer films demonstrate the remarkable effect of interface structure on their hydrophobicity and mechanical properties. The nano-columnar structured multilayer films exhibit the dominance over the glassy structured stack in terms of their enhanced characteristics, namely the mechanical characteristics, anti-reflection behavior, visible transmittance, and hydrophobicity. While hydrophobicity is derived from the combined effect of hierarchical surface roughness and nano-columnar structure of the top and bottom Hf-oxide ceramic layers, the enhanced mechanical response is derived from the columnar structure of Mo metallic interlayer vertically aligned with overall multilayer stack. The combination of super-hydrophobicity and enhanced mechanical properties of optically transparent HfO2/Mo/HfO2 multilayer films through HfO2-Mo interface structure control as demonstrated in this work may provide a pathway to further tune the efficiency and in the optimization of architectures for energy-saving applications.

EFFICIENT GLASS WINDOWS, ELECTRICAL-PROPERTIES, TH↗

Large-area borophene sheets on sacrificial Cu(111) films promoted by recrystallization from subsurface boron

Borophene, an atomically thin covalently bonded boron sheet, has attracted great attention as a novel quantum material because of its structural tunability and potential utilization in flexible and transparent electronics. So far, borophene has been synthesized on silver or copper single crystals, but these substrates are small, very expensive, and unsuitable for study of transport properties or electronics applications. Here, we report synthesis of borophene on nanometer-scale thick Cu(111) films grown on sapphire. We have developed a process of enlarging faceted borophene islands, by repeated submersion of boron into copper at high temperature and resurfacing and re-crystallization at lower temperature. This discovery was enabled by real-time feedback from low-energy electron microscopy and diffraction. We demonstrate synthesis of borophene as faceted micrometer-size monocrystal islands or as full-monolayer sheets. The process is scalable to wafer size; moreover, Cu films could be sacrificed and sapphire reused. Our work opens the door for new experiments and brings applications one step closer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Simple thermal vapor deposition process for and characterization of n-type indium oxysulfide thin films

The search continues for alternative nontoxic n-type electron transport layers in optoelectronic thin-film devices. Indium oxysulfide, In 2 (O,S) 3 , represents one promising material for this application, especially when paired with chalcogenide absorber layers. The ternary nature of the composition allows for electrical conductivity and optical bandgap tuning by tailoring the sulfur to oxygen ratio in the oxysulfide alloy. However, thin films of In 2 (O,S) 3 are typically deposited only by chemical bath deposition or plasma-enhanced atomic layer deposition. Here we report deposition of thin films of In 2 (O,S) 3 in a custom-built thermal reactor using only water vapor and hydrogen sulfide as the coreactants. This advance is enabled by the use of a recently reported, highly reactive indium formamidinate precursor. As shown by x-ray photoelectron spectroscopy, the composition can be tuned from pure In 2 (O,S) 3 to pure In 2 S 3 by varying the ratio of cycles employing water or hydrogen sulfide. The oxygen to the sulfur ratio in the film can be controlled by altering the dose sequence, although films typically contain more sulfur than would be expected naively from the percentage of hydrogen sulfide doses in the deposition recipe. Rutherford backscattering spectrometry confirms the composition is sulfur-rich relative to the dosing ratio. Structural characterization indicates films are relatively amorphous in nature. Electrically, these films offer reasonably constant electron mobility at different O:S ratios, with an electron concentration tunable over 4 orders of magnitude. These oxysulfide films possess a higher indirect bandgap than their oxygen-free indium sulfide counterparts, indicating higher transmittance to blue light. These indium oxysulfide films may be suitable candidates for electron transport layers in thin-film solar cells where their wider bandgap might result in higher optical transparency and thus short circuit current density, while the tunability of their conduction band offset with an absorber layer may result in higher open circuit voltage.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

MgSiP 2 : An Infrared Nonlinear Optical Crystal with a Large Non‐Resonant Phase‐Matchable Second Harmonic Coefficient and High Laser Damage Threshold

Superior infrared nonlinear optical (NLO) crystals are in urgent demand in the development of lasers and optical technologies for communications and computing. The critical challenge is to find a crystal with large non‐resonant phase‐matchable NLO coefficients and high laser damage threshold (LDTs) simultaneously, which however scale inversely. This work reports such a material, MgSiP 2, that exhibits a large second harmonic generation (SHG) coefficient of d 14 ≈ d 36 = 89 ± 5 pm V −1 at 1550 nm fundamental wavelength, surpassing the commercial NLO crystals AgGaS 2 , AgGaSe 2 , and ZnGeP 2 . First principles theory reveals the polarizability and geometric arrangement of the [SiP 4 ] tetrahedral units as the origin of this large nonlinear response. Remarkably, it also exhibits a high LDT value of 684 GW cm −2 , which is six times larger than ZnGeP 2 and three times larger than CdSiP 2 . It has a wide transparency window of 0.53–10.35 µm, allowing broadband tunability. Further, it is Type I and Type II phase‐matchable with large effective SHG coefficients of d eff,I ≈80.2 pm V −1 and d eff,II ≈73.4 pm V −1 . The outstanding properties of MgSiP 2 make it a highly attractive candidate for optical frequency conversion in the infrared.

36 MATERIALS SCIENCE↗

Tunable Three-Body Loss in a Nonlinear Rydberg Medium

Long-range Rydberg interactions, in combination with electromagnetically induced transparency (EIT), give rise to strongly interacting photons where the strength, sign, and form of the interactions are widely tunable and controllable. Such control can be applied to both coherent and dissipative interactions, which provides the potential for generating novel few-photon states. Recently it has been shown that Rydberg-EIT is a rare system in which three-body interactions can be as strong or stronger than two-body interactions. In this work, we study three-body scattering loss for Rydberg-EIT in a wide regime of single and two-photon detunings. We report our numerical simulations of the full three-body wave function and analytical estimates based on Fermi’s golden rule strongly suggest that the observed features in the outgoing photonic correlations are caused by the resonant enhancement of the three-body losses.

74 ATOMIC AND MOLECULAR PHYSICS↗

Electrochromic Properties of Perovskite NdNiO 3 Thin Films for Smart Windows

Semiconductors with electrically tunable band gaps are of great interest in controlling transparency to electromagnetic radiation. Thin films of perovskite nickelate NdNiO 3 (NNO), a class of correlated oxides, were deposited on single-crystal (LaAlO 3 (LAO)) and polycrystalline (fluorine-doped tin oxide-coated glass (FTO)) substrates by magnetron sputtering, chemical solution deposition (CSD), and atomic layer deposition (ALD). Their electrochromic behaviors were investigated using a three-electrode setup in basic (KOH solution, pH = 12) electrolyte. During bleaching/coloration process, the proton intercalation/deintercalation and simultaneous electron compensation in the NNO lattice under electrical bias led to crossover of the material between the pristine-conducting phase (Ni 3+ ) and the strongly correlated insulating phase (Ni 2+ ), which serves as the working principle for electrochromic (tunable opacity in the visible range) behavior. Cyclic voltammetry (CV) scans demonstrate that NNO films are electrochemically stable in basic solutions for all three film deposition methods explored here. CV scans at varying rates enabled the extraction of diffusion coefficient of protons in thin film NNO, which is similar to 10 –7 cm 2 s –1 among all films studied. Large light transmittance modulation by bleaching and coloration was observed on films grown on both LAO and FTO substrates, suggesting its potential as an electrochromic material candidate for smart windows and optical shutter applications. Here, porous NNO films obtained by chemical solution deposition tend to demonstrate stronger electrochromic activity than dense films grown by sputtering or ALD.

36 MATERIALS SCIENCE↗

Microscopically crumpled indium-tin-oxide thin films as compliant electrodes with tunable transmittance

Indium-tin-oxide (ITO) thin films are perceived to be stiff and brittle. This letter reports that crumpled ITO thin films on adhesive poly-acrylate dielectric elastomer can make compliant electrodes, sustaining compression of up to 25% × 25% equi-biaxial strain and unfolding. Its optical transmittance reduces with crumpling, but restored with unfolding. A dielectric elastomer actuator (DEA) using the 14.2% × 14.2% initially crumpled ITO thin-film electrodes is electrically activated to produce a 37% areal strain. Such electric unfolding turns the translucent DEA to be transparent, with transmittance increased from 39.14% to 52.08%. This transmittance tunability promises to make a low-cost smart privacy window.

36 MATERIALS SCIENCE↗

Self‐Standing Chiral Covalent Organic Framework Thin Films with Full‐Color Tunable Guest‐Induced Circularly Polarized Luminescence

Abstract Exploring self‐standing chiral covalent organic framework (COF) thin films with controllable circularly polarized luminescence (CPL) is of paramount significance but remains a challenging task. Herein, we demonstrate the first example of self‐standing chiral COF films employing a polymerization‐dispersion‐filtration strategy. Pristine, low‐quality chiral COF films were produced by interfacial polymerization and then re‐dispersed into COF colloidal solutions. Via vacuum assisted assembly, these COF colloids were densely stacked and assembled into self‐standing, pure chiral COF films ( L‐ / D‐ CCOF‐F) that were transparent, smooth, crack‐free and highly crystalline. These films were tunable in thicknesses, areas, and roughness, along with strong diffuse reflectance circular dichroism (DRCD) and cyan CPL signals, showing an intrinsic luminescence asymmetric factor ( g lum ) of ~4.3×10 −3 . Furthermore, these COF films served as host adsorbents to load various achiral organic dye guests through adsorption. The effective chiral transfer and energy transfer between CCOF‐F and achiral fluorescent dyes endowed the dyes with strong chirality and tunable DRCD, resulting in intense, full‐color‐tunable solid‐state CPL. Notably, the ordered arrangement of dye guest molecules within the preferentially oriented chiral pores of CCOF‐F contributed to an amplified | g lum | factor of up to 7.2×10 −2 , which is state‐of‐the‐art for COF‐based CPL materials. This work provides new insights into the design and fabrication of self‐standing chiral COF films, demonstrating their great potential for chiroptical applications.

Tang, Xihao↗

Tunable electrochromic behavior of titanium-based MXenes

Two-dimensional transition metal carbides, nitrides and carbonitrides, popular by the name MXenes, are a promising class of materials as they exhibit intriguing optical, optoelectronic and electrochemical properties. Taking advantage of their metallic conductivity and hydrophilicity, titanium carbide MXenes (Ti 3 C 2 T x and others) are used to fabricate solution processable transparent conducting electrodes (TCEs) for the design of three-electrode electrochromic cells. However, the tunable electrochromic behavior of various titanium-based MXene compositions across the entire visible spectrum has not yet been demonstrated. Here, we investigate the intrinsic electrochromic properties of titanium-based MXenes, Ti 3 C 2 T x , Ti 3 CNT x , Ti 2 CT x , and Ti 1.6 Nb 0.4 CT x , where individual MXenes serve as a transparent conducting, electrochromic, and plasmonic material layer. Plasmonic extinction bands for Ti 3 C 2 T x , Ti 2 CT x and Ti 1.6 Nb 0.4 CT x are centered at 800, 550 and 480 nm, which are electrochemically tunable to 630, 470 and 410 nm, respectively, whereas Ti 3 CNT x shows a reversible change in transmittance in the wide visible range. Additionally, the switching rates of MXene electrodes with no additional transparent conductor electrodes are estimated and correlated with the respective electrical figure of merit values. This work demonstrates that MXene-based electrochromic cells are tunable in the entire visible spectrum and suggests the potential of the MXene family of materials in optoelectronic, plasmonic, and photonic applications, such as tunable visible optical filters and modulators, to name a few.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Silicon-Phosphorene Nanocavity-Enhanced Optical Emission at Telecommunications Wavelengths

Generating and amplifying light in silicon (Si) continues to attract significant attention due to the possibility of integrating optical and electronic components in a single material platform. Unfortunately, silicon is an indirect band gap material and therefore an inefficient emitter of light. With the rise of integrated photonics, the search for silicon-based light sources has evolved from a scientific quest to a major technological bottleneck for scalable, CMOS-compatible, light sources. Recently, emerging two-dimensional materials have opened the prospect of tailoring material properties based on atomic layers. Few-layer phosphorene, which is isolated through exfoliation from black phosphorus (BP), is a great candidate to partner with silicon due to its layer-tunable direct band gap in the near-infrared where silicon is transparent. Here we demonstrate a hybrid silicon optical emitter composed of few-layer phosphorene nanomaterial flakes coupled to silicon photonic crystal resonators. We show single-mode emission in the telecommunications band of 1.55 μm ($E_g$ = 0.8 eV) under continuous wave optical excitation at room temperature. The solution-processed few-layer BP flakes enable tunable emission across a broad range of wavelengths and the simultaneous creation of multiple devices. Our work highlights the versatility of the Si-BP material platform for creating optically active devices in integrated silicon chips.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Active Control of Nitride Plasmonic Dispersion in the Far Infrared.

We investigate plasmonic structures in nitride-based materials for far-infrared (IR) applications. The two dimensional electron gas (2DEG) in the GaN/AlGaN material system, much like metal- dielectric structures, is a patternable plasmonic medium. However, it also permits for direct tunability via an applied voltage. While there have been proof-of-principle demonstrations of plasma excitations in nitride 2DEGs, exploration of the potential of this material system has thus far been limited. We recently demonstrated coherent phenomena such as the formation of plasmonic crystals, strong coupling of tunable crystal defects to a plasmonic crystal, and electromagnetically induced transparency in GaAs/AlGaAs 2DEGs at sub-THz frequencies. In this project, we explore whether these effects can be realized in nitride 2DEG materials above 1 THz and at temperatures exceeding 77 K.

Shaner, Eric A.↗