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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Determination of Thermal Damage Threshold in THz Photomixers Using Raman Spectroscopy

The increase of device lifetime and reliability of THz photomixers will play an essential role in their possible future application. Therefore, their optimal work conditions/operation range, i.e., the maximal incident optical power should be experimentally estimated. We fabricated and tested THz photomixer devices based on nitrogen-implanted GaAs integrated with a Bragg reflector. Raman spectroscopy was applied to investigate the material properties and to disclose any reversible or irreversible material changes. The results indicate that degradation effects in the photomixer structures/material could be avoided if the total optical power density does not exceed levels of about 0.7 mW/µm 2 for 100 min of operation. Furthermore, the investigations performed during 1000 min of optical exposure on the photomixer devices’ central region comprising interdigitated metal-semiconductor-metal (MSM) structures suggest a reversible “curing” mechanism if the power density level of ~0.58 mW/µm 2 is not exceeded. Long-term operation (up to 1000 h) reveals that the photomixer structures can withstand an average optical power density of up to ~0.4 mW/µm 2 without degradation when biased at 10 V. Besides the decrease of the position of the A1g (LO) Raman mode from ~291 cm -1 down to ~288 cm -1 with increasing optical power density and operation time, broad Raman modes evolve at about 210 cm -1 , which can be attributed to degradation effects in the active photomixer/MSM area. In addition, the performed carrier lifetime and photomixer experiments demonstrated that these structures generated continuous wave sub-THz radiation efficiently as long as their optimal work conditions/operation range were within the limits established by our Raman studies.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Controllable Thin‐Film Approaches for Doping and Alloying Transition Metal Dichalcogenides Monolayers

Abstract Two‐dimensional (2D) transition metal dichalcogenides (TMDs) exhibit exciting properties and versatile material chemistry that are promising for device miniaturization, energy, quantum information science, and optoelectronics. Their outstanding structural stability permits the introduction of various foreign dopants that can modulate their optical and electronic properties and induce phase transitions, thereby adding new functionalities such as magnetism, ferroelectricity, and quantum states. To accelerate their technological readiness, it is essential to develop controllable synthesis and processing techniques to precisely engineer the compositions and phases of 2D TMDs. While most reviews emphasize properties and applications of doped TMDs, here, recent progress on thin‐film synthesis and processing techniques that show excellent controllability for substitutional doping of 2D TMDs are reported. These techniques are categorized into bottom–up methods that grow doped samples on substrates directly and top–down methods that use energetic sources to implant dopants into existing 2D crystals. The doped and alloyed variants from Group VI TMDs will be at the center of technical discussions, as they are expected to play essential roles in next‐generation optoelectronic applications. Theoretical backgrounds based on first principles calculations will precede the technical discussions to help the reader understand each element's likelihood of substitutional doping and the expected impact on the material properties.

36 MATERIALS SCIENCE↗
DOE OSTI2022

A multi-chord, two-color interferometer using Hilbert transform phase detection for measuring electron density in spheromak plasmas

A new, four-chord, CO 2 /He–Ne heterodyne interferometer has been designed and built for measuring line-averaged plasma density in the HIT-SI3 and subsequent HIT-SIU sustained spheromak devices. The two-color system successfully eliminates vibration-induced errors caused by mirrors that are secured to the vacuum chamber and is able to resolve electron densities ne in the full operating range of 10 18 –10 20 m –3 in both experiments with an integrated error of 4.7 × 10 17 m –2 . Here, data are presented from high toroidal current plasma discharges, showing the time evolution of electron densities n e and j Φ /n e along multiple chords.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Broadband Liquid Crystal Tunable Metasurfaces in the Visible: Liquid Crystal Inhomogeneities Across the Metasurface Parameter Space

Optical metasurfaces—planar nanostructured devices that can arbitrarily tailor the wavefront of light—may be reconfigured by changing their dielectric environment. The application of external stimuli to liquid crystals is a particularly promising means of tuning the optical properties of embedded metasurfaces because of liquid crystals' large and broadband optical anisotropy. However, the detailed behavior of liquid crystals immediately adjacent to the nanostructured meta-atoms elements is often overlooked, despite the optics of the device depending sensitively on this behavior (e.g., the spectral position of the meta-atom resonances). This is of increasing concern as the wavelength of operation further approaches the short-wavelength end of the visible spectrum and, therefore, the length scale of the inhomogeneities in the liquid crystal director field. In this manuscript, we undertake a fully comprehensive study, across the metasurface geometrical parameter space, of broadband (450-700 nm) all-dielectric liquid crystal tunable metasurfaces operating in the visible. Here, through combined experimental characterization, liquid crystal modeling, and optical simulations, we reveal and quantify the improved accuracy with which the optical properties of the liquid crystal tunable metasurfaces may be described, and identify the underlying physical mechanism: the three-dimensional spatial overlap of the liquid crystal director field and metasurface optical near fields in the vicinity of the meta-atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Temporal and spatial tuning of optical constants in praseodymium doped ceria by electrochemical means

Abstract Temporal and spatial tuning of the refractive index of optical thin films is desired for flat optics applications. The redistribution of mobile ions in mixed ionic-electronic conductors (MIEC) has been demonstrated to serve as a viable means for achieving optical tuning down to the nanoscale. Here we studied the dynamic range of the optical tuning achievable in the refractive index, in the MIEC oxide – Pr x Ce 1− x O 2− δ (PCO), for x = 0.1, 0.2 and 0.4, at 500 °C, by in-situ spectrophotometry. Significant increases in the modulation of both the imaginary and real optical constants in the visible and the adjacent spectra were obtained for increased doping levels. Device employing an electrochemical titration method was implemented to modulate the oxygen concentration, and thereby the optical transmission of PCO. Incorporation of a patterned top electrode allowed for the demonstration of spatial control of PCO thin film properties by in-situ video imaging of the optical switching process. The electrochemically induced optical state is shown to remain non-volatile upon quenching the device to room temperature under applied bias.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Second Harmonic Generation from a Single Plasmonic Nanorod Strongly Coupled to a WSe 2 Monolayer

Monolayer transition metal dichalcogenides, coupled to metal plasmonic nanocavities, have recently emerged as new platforms for strong light–matter interactions. These systems are expected to have nonlinear-optical properties that will enable them to be used as entangled photon sources, compact wave-mixing devices, and other elements for classical and quantum photonic technologies. Here, we report the first experimental investigation of the nonlinear properties of these strongly coupled systems, by observing second harmonic generation from a WSe 2 monolayer strongly coupled to a single gold nanorod. In this work, the pump-frequency dependence of the second-harmonic signal displays a pronounced splitting that can be explained by a coupled-oscillator model with second-order nonlinearities. Rigorous numerical simulations utilizing a nonperturbative nonlinear hydrodynamic model of conduction electrons support this interpretation and reproduce experimental results. Our study thus lays the groundwork for understanding the nonlinear properties of strongly coupled nanoscale systems.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Charge transfer in transition metal dichalcogenide alloy heterostructures

Two-dimensional (2D) transition metal dichalcogenides and their alloys provide a unique platform for exploring interlayer charge transfer in van der Waals heterostructures. These structures are crucial for advancing the next-generation electronic, optoelectronic, and quantum devices. In this study, interlayer charge transfer in heterostructures composed of MoSe 2 , MoS 2 , and their alloy, MoSSe, is investigated using transient absorption, Raman, and photoluminescence spectroscopy. The experimental results reveal that electron transfer in the alloy heterostructures, MoSSe/MoS 2 and MoSe 2 /MoSSe, is faster than in the pure MoSe 2 /MoS 2 heterostructure, despite the smaller conduction band offsets of the alloy systems. Raman spectroscopy confirms that alloy layers support phonon modes matching those of the pure layers, aligning with theoretical models of phonon-assisted interlayer charge transfer. Additionally, efficient hole transfer is observed in both alloy heterostructures. The findings suggest transition metal dichalcogenides alloys can be used for engineering heterostructures with desired charge transfer properties. By leveraging compositionally tunable band gaps and optical properties, alloy-based heterostructures offer opportunities for designing tailored materials suitable for diverse applications such as photodetectors, light-emitting devices, and flexible electronics. Furthermore, the ultrafast charge transfer observed in these systems provides insights into the fundamental mechanisms governing interlayer interactions in 2D materials.

2D material↗
DOE OSTI2025

Efficient Measurement of Length Distribution of 1D Nanoparticles in Solution via Optical Polarimetry

The efficient measurement of the length distribution of nanotubes, nanowires, and other one-dimensional (1D) nanoparticles in solution is important to enable their incorporation into materials and devices and to optimize their processing for properties of interest, such as thermal/electrical conductivity or mechanical strength, in suspensions and composites. We report an electric-field (E-field)-assisted optical-polarimetry technique to measure the length distribution of ensembles of high-aspect-ratio particles in dilute suspension. The degree of alignment of polarizable 1D particles suspended in a fluid under Brownian motion explicitly depends on the E-field strength and the particle length. We show that it is possible to extract the length distribution of 1D nanoparticles suspended in an insulating fluid by applying a range of E-fields and using optical polarimetry to measure the corresponding alignment order parameter. Notably, the method is relatively insensitive to the diameter of the 1D particles, which can be poorly known or vary within a sample. The technique is validated with silver nanowires and carbon nanotubes of known lengths, as well as polymer-depletion-length-separated single-wall carbon nanotube samples with length distributions independently measured with analytical ultracentrifugation. Finally, we demonstrate the ability of the optical-polarimetry technique to quantify changes in the length distribution of ultranarrow, sub-nanometer-diameter single-wall carbon nanotubes under different types and durations of ultrasonication. Within its range of applicability (polarizable 1D nanoparticles in the 0.5 to 15 μm length range, constrained by the voltage stability of the media and the suspended particles), the E-field-assisted optical-polarimetry method is a particularly efficient and accurate method to measure the length distribution of nanowires and nanotubes in suspension.

1D nanoparticles↗
DOE OSTI2025

Effect of growth dynamics on the structural, photophysical and pseudocapacitance properties of famatinite copper antimony sulphide colloidal nanostructures (including nanosheets)

Facile phase selective synthesis of copper antimony sulphide (CAS) nanostructures is important because of their tunable photoconductive and electrochemical properties. In this study, off-stoichiometric famatinite phase CAS (fCAS) quasi-spherical and quasi-hexagonal colloidal nanostructures (including nanosheets) of sizes, 2.4–18.0 nm were grown under variable conditions of temperature (60–200 °C), time and oleylamine capping ligand concentration using copper(II) acetylacetonate and antimony(III) diethyldithiocarbamate precursors. Data from powder X-ray diffraction, Raman spectroscopy and high-resolution scanning/transmission electron microscopy confirm the tetragonal structure of the famatinite phase. X-ray photoelectron spectroscopy, transmission electron microscopy and scanning electron microscopy-energy dispersive X-ray spectroscopy data suggest a correlation of particle size, morphology and composition of the off-stoichiometric fCAS nanostructures with growth temperature and time, and oleylamine concentration. The off-stoichiometric Cu 3-a Sb 1+b S 4±c (a, b, c – mole fractions) nanostructures being severely copper-deficient and antimony-rich, exhibit shallow-lying acceptor copper vacancy states, deep-lying donor states of antimony interstitials, sulphur vacancies and antimony-copper antisites and shallow-lying acceptor surface trapping states. Further, these electronic states are likely implicated in tunable UV-visible absorption and bandgaps between 2.3 and 2.8 eV, and broad visible-NIR photoluminescence with fast recombination of radiative lifetimes between 0.2 and 6.2 ns, confirmed from absorption, steady-state and time-resolved photoluminescence spectroscopies. Additionally, cyclic voltammetry and electrochemical impedance spectroscopy confirm that electrodes of the fCAS nanostructures display slightly variable pseudocapacitance of charge-storage primarily via possible sodium ion intercalation with a high specific capacitance of ~84 F g -1 obtained at a scan rate of 5 mV s -1 . Overall, these results show the influence of composition, in particular point defects, phase quality and morphology on the optical and pseudocapacitance properties of fCAS nanostructures, suitable as solar absorbers or electrodes for energy storage devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

A laserball calibration device for the SNO+ scintillator phase

Located 2 km underground in SNOLAB, Sudbury, Canada, SNO+ is a large scale liquid scintillator experiment that primarily aims to search for neutrinoless double beta decay. Whilst SNO+ has light and radioactive calibration sources external to the inner volume, an internally deployed optical source is necessary for the full characterization of the detector model. A laser diffuser ball developed for SNO has previously demonstrated to be an effective optical calibration device for both SNO and SNO+ water phase. Since the introduction of liquid scintillator for SNO+, the material compatibility, cleanliness, and radiopurity requirements of any materials in contact with the internal medium have increased. Improving on the original SNO laserball design, a new laserball calibration device has been developed for the SNO+ scintillator phase with the goal of measuring the optical properties of the detector and performing routine PMT gain and timing calibrations. Simulations have been written to model the diffusion properties to optimise optical and temporal performance for calibration. Prototype laserballs have been built and characterised, demonstrating sub-ns timing resolution and a quasi-isotropic light distribution.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Continuously tunable uniaxial strain control of van der Waals heterostructure devices

Uniaxial strain has been widely used as a powerful tool for investigating and controlling the properties of quantum materials. However, existing strain techniques have so far mostly been limited to use with bulk crystals. Although recent progress has been made in extending the application of strain to two-dimensional van der Waals (vdW) heterostructures, these techniques have been limited to optical characterization and extremely simple electrical device geometries. Here, we report a piezoelectric-based in situ uniaxial strain technique enabling simultaneous electrical transport and optical spectroscopy characterization of dual-gated vdW heterostructure devices. Critically, our technique remains compatible with vdW heterostructure devices of arbitrary complexity fabricated on conventional silicon/silicon dioxide wafer substrates. We demonstrate a large and continuously tunable strain of up to –0.15% at millikelvin temperatures, with larger strain values also likely achievable. We quantify the strain transmission from the silicon wafer to the vdW heterostructure, and further demonstrate the ability of strain to modify the electronic properties of twisted bilayer graphene. Our technique provides a highly versatile new method for exploring the effect of uniaxial strain on both the electrical and optical properties of vdW heterostructures and can be easily extended to include additional characterization techniques.

Electrical properties and parameters↗
DOE OSTI2024

Quantitative modeling of gate-tunable cavity exciton-polaritons in transition-metal dichalcogenides

We performed a comprehensive real-space simulation study of propagative exciton-polaritons (EPs) of tungsten disulfide (WS 2 ) inside a Fabry–Pérot cavity. Through our simulations, we were able to construct the dispersion relation and determine the propagation length (L p ) of EPs, both of which show sensitive dependence on the applied gate voltage. We found that L p increases at higher gate voltages when excited at the exciton energy but shows opposite gate dependence at the trion energy. These observations are direct evidence of the coupling between the cavity mode with excitons and trions of WS 2 . Furthermore, we demonstrate a proof-of-concept device based on the tunable cavity EPs of WS 2 , which is promising for application as photonic transistors, modulators, or electrical-to-optical converters. Furthermore, our work unveils the real-space transport properties of gate-tunable cavity EPs and paves the way for future applications of EPs in nanophotonic devices and circuits.

42 ENGINEERING↗
DOE OSTI2025

Efficient on-chip terahertz generation and detection with GaN photoconductive emitters

Photoconductive emitters for terahertz generation hold promise for highly efficient down-conversion of optical photons because it is not constrained by the Manley-Rowe relation. Existing terahertz photoconductive devices, however, faces limits in efficiency due to the semiconductor properties of commonly used GaAs materials. Here, we demonstrate that large bandgap semiconductor GaN, characterized by its high breakdown electric field, facilitates the highly efficient generation of terahertz waves in a coplanar stripline waveguide. Towards this goal, we investigated the excitonic contribution to the electro-optic response of GaN under static electric field both through experiments and first-principles calculations, revealing a robust excitonic Stark shift. Using this electro-optic effect, we developed a novel ultraviolet pump-probe spectroscopy for in-situ characterization of the terahertz electric field strength generated by the GaN photoconductive emitter. Our findings show that terahertz power scales quadratically with optical excitation power and applied electric field over a broad parameter range. We achieved an optical-to-terahertz conversion efficiency approaching 100% within the 0.03–1 THz bandwidth at the highest bias field (116 kV/cm) in our experiment. Further optimization of GaN-based terahertz generation devices could achieve even greater optical-to-terahertz conversion efficiencies.

Uzundal, Can B↗
DOE OSTI2023

Millimeter-Thick Liquid Crystalline Elastomer Actuators Prepared by-Surface-Enforced Alignment

Here, liquid crystalline elastomers (LCE) are thermally cyclable, compliant actuators with compelling mechanical properties. The large and programmable deformation of LCE has led to numerous functional examinations spanning optics, medical devices, and robotics. A well-established method to prepare complex LCE actuators is to utilize surface-enforced photoalignment. Herein, a facile and scalable approach is reported to circumvent the physical limits of surface-enforced alignment (e.g., samples that are 50 µm or less) to amplify the achievable force output in LCE. Applying an approach termed direct layering, the thermomechanical response of LCE elements prepared with +1 disclination patterns in a range of compositions and thicknesses is contrasted. The design and preparation of +1 disclination patterns and arrays is explored to assess the contribution of sample geometry and overlap to deformation and force output. The methodology detailed in this contribution allows for the preparation of elements ≈1 mm in thickness that are capable of actuating large objects. Furthermore, the fabrication of these elements uniquely enables the realization of mechanical instabilities to hasten the actuation rate in response to thermal change and to enable leaping.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Design of 3D Oxide–Metal Hybrid Metamaterial for Tailorable Light–Matter Interactions in Visible and Near-Infrared Region

Dielectric–metallic hybrid metamaterials exhibit extraordinary optical properties due to the light–matter interactions at the dielectric–metallic interfaces. The ability in precision control of the light–matter interactions in nanoscale is key to tailor the optical properties of hybrid metamaterials. In this work, a complex 3D framework of multilayered self-assembled BaTiO 3 (BTO)-Au hybrid thin films is demonstrated with such precision control of the light–matter interaction in nanoscale. Here, unique “bamboo-like” Au nanostructures are formed via the bilayer and trilayer stacking of BTO-Au hybrid layers with interlayers of SrTiO 3 , CeO 2 , or MgO. Different film strain states introduced by the three interlayers result in variable diameter and density of Au nanopillars. Both simulated and experimental optical data demonstrate the localized surface plasmon resonance change and hyperbolic dispersion wavelength shift in visible to near-infrared because of the effective tuning of the Au nanopillar aspect ratio and free electron density. The highly tunable optical properties along with the ferroelectric behavior and thermal robustness of the 3D hybrid film enable it to be a great candidate for multifunctional applications. This study demonstrates a unique 3D approach for precision optical property tuning and combined functionalities in oxide–metal metamaterial systems toward future integrated photonic and electronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Time-resolved magneto-optical effects in the altermagnet candidate MnTe

α -MnTe is an antiferromagnetic semiconductor with above room temperature T N = 310 K, which is promising for spintronic applications. Recently, it was reported to be an altermagnet, containing bands with momentum-dependent spin splitting; time-resolved experimental probes of MnTe are, therefore, important both for understanding novel magnetic properties and potential device applications. Here, we investigate ultrafast spin dynamics in epitaxial MnTe(001)/InP(111) thin films using pump-probe magneto-optical measurements in the Kerr configuration. At room temperature, we observe an oscillation mode at 55 GHz that does not appear at zero magnetic field. Combining field and polarization dependence, we identify this mode as a magnon, likely originating from inverse stimulated Raman scattering. Magnetic field-dependent oscillations persist up to at least 335 K, which could reflect coupling to known short-range magnetic order in MnTe above T N . Additionally, we observe two optical phonons at 3.6 and 4.2 THz, which broaden and redshift with increasing temperature.

Gray, Isaiah↗
DOE OSTI2024

Ultra-High Efficiency and Stable All-Perovskite Tandem Solar Cells

In the project period, the research team has fabricated more than 6,000 single-junction wide-bandgap (wide-E g ) and low-bandgap (low-E g ) perovskite solar cells (PSCs) and more than 2,000 all-perovskite tandem solar cells (APTSCs). The best-performing wide-E g and low-E g PSCs and APTSCs showed PCEs greater than 19%, 23%, and 30%, respectively. The average PCEs for wide-E g and low-E g PSCs and APTSCs fabricated by the benchmark processes are (18.5 ± 0.4)%, (21.9 ± 0.8)%, and (26.8 ± 2.1)%, respectively. We have demonstrated APTSCs with T 80 lifetime of more than 1,000 h, which were measured by maximum power point tracking (MPPT) under one sun operation in the air. The team has also utilized various advanced characterization techniques to study the optical and electrical properties of wide-E g and low-E g perovskite materials and devices, developing a better understanding of the unique working principle and degradation mechanism of APTSCs. The team has met most GNG decision criteria except for the stability goal of APTSCs under 85 °C/85 RH accelerated lifetime test (ALT). The shortfall of the device ALT stability is mainly limited by the intrinsic instability of Sn-Pb perovskites under illumination at elevated temperatures. The team discussed with stakeholders in the PV academic and industry about these durability concerns and concluded that this is the major technical barrier preventing the market entry of APTSCs. Future fundamental study and R&D work are needed to advance this promising technology.

14 SOLAR ENERGY↗
DOE OSTI2024

Mechanisms of Hysteresis and Reversibility across the Voltage-Driven Perovskite–Brownmillerite Transformation in Electrolyte-Gated Ultrathin La 0.5 Sr 0.5 CoO 3−δ

Perovskite cobaltites have emerged as archetypes for electrochemical control of materials properties in electrolyte-gate devices. Voltage-driven redox cycling can be performed between fully oxygenated perovskite and oxygen-vacancy-ordered brownmillerite phases, enabling exceptional modulation of the crystal structure, electronic transport, thermal transport, magnetism, and optical properties. The vast majority of studies, however, have focused heavily on the perovskite and brownmillerite end points. In contrast, here we focus on hysteresis and reversibility across the entire perovskite ↔ brownmillerite topotactic transformation, combining gate-voltage hysteresis loops, minor hysteresis loops, quantitative operando synchrotron X-ray diffraction, and temperature-dependent (magneto)transport, on ion-gel-gated ultrathin (10-unit-cell) epitaxial La 0.5 Sr 0.5 CoO 3-δ films. Further, gate-voltage hysteresis loops combined with operando diffraction reveal a wealth of new mechanistic findings, including asymmetric redox kinetics due to differing oxygen diffusivities in the two phases, nonmonotonic transformation rates due to the first-order nature of the transformation, and limits on reversibility due to first-cycle structural degradation. Minor loops additionally enable the first rational design of an optimal gate-voltage cycle. Combining this knowledge, we demonstrate state-of-the-art nonvolatile cycling of electronic and magnetic properties, encompassing >10 5 transport ON/OFF ratios at room temperature, and reversible metal-insulator-metal and ferromagnet-nonferromagnet-ferromagnet cycling, all at 10-unit-cell thickness with high room-temperature stability. This paves the way for future work to establish the ultimate cycling frequency and endurance of such devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗