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At least 1,279 records · Page 71
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Tuning transport across MoS2/graphene interfaces via as-grown lateral heterostructures

An unexploited property of graphene-based heterojunctions is the tunable doping of the junction via electrostatic gating. This unique property may be key in advancing electronic transport across interfaces with semiconductors. Here, we engineer transport in semiconducting TMDs by constructing a lateral heterostructure with epitaxial graphene and tuning its intrinsic doping to form a p–n junction between the graphene and the semiconducting TMDs. Graphene grown on SiC (epitaxial graphene) is intrinsically doped via substrate polarization without the introduction of an external dopant, thus enabling a platform for pristine heterostructures with a target band alignment. We demonstrate an electrostatically tunable graphene/MoS 2 p–n junction with >20× reduction and >10× increased tunability in contact resistance (R c ) compared with metal/TMD junctions, attributed to band alignment engineering and the tunable density of states in graphene. This unique concept provides improved control over transport across 2D p–n junctions.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Guiding the design of oxidation-resistant Fe-based single atom alloy catalysts with insights from configurational space

The high activity and selectivity of Fe-based heterogeneous catalysts toward a variety of reactions that require the breaking of strong bonds are offset in large part by their considerable instability with respect to oxidative deactivation. While it has been shown that the stability of Fe catalysts is considerably enhanced by alloying them with precious metals (even at the single-atom limit), rational design criteria for choosing such secondary metals are still missing. Since oxidative deactivation occurs due to the strong binding of oxygen to Fe and reduction by adsorbed hydrogen mitigates the deactivation, we propose here to use the binding affinity of oxygen and hydrogen adatoms as the basis for rational design. As it would also be beneficial to use cheaper secondary metals, we have scanned over a large subset of 3d–5d mid-to late transition metal single atoms and computationally determined their effect on the oxygen and hydrogen adlayer binding as a function of chemical potential and adsorbate coverage. We further determine the underlying chemical origins that are responsible for these effects and connect them to experimentally tunable quantities. Our results reveal a reliable periodic trend wherein oxygen binding is weakened greatest as one moves right and down the periodic table. Hydrogen binding shows the same trend only at high (but relevant) coverages and otherwise tends to have its binding slightly increased in all systems. Trends with secondary metal coverage are also uncovered and connected to experimentally tunable parameters.

Hensley, Alyssa↗
DOE OSTI2024

Probing electronic and dielectric properties of ultrathin Ga 2 O 3 /Al 2 O 3 atomic layer stacks made with in vacuo atomic layer deposition

Ultrathin (1–4 nm) films of wide-bandgap semiconductors are important to many applications in microelectronics, and the film properties can be sensitively affected by defects especially at the substrate/film interface. Motivated by this, an in vacuo atomic layer deposition (ALD) was developed for the synthesis of ultrathin films of Ga 2 O 3 /Al 2 O 3 atomic layer stacks (ALSs) on Al electrodes. It is found that the Ga 2 O 3 /Al 2 O 3 ALS can form an interface with the Al electrode with negligible interfacial defects under the optimal ALD condition whether the starting atomic layer is Ga 2 O 3 or Al 2 O 3 . Such an interface is the key to achieving an optimal and tunable electronic structure and dielectric properties in Ga 2 O 3 /Al 2 O 3 ALS ultrathin films. In situ scanning tunneling spectroscopy confirms that the electronic structure of Ga 2 O 3 /Al 2 O 3 ALS can have tunable bandgaps (E g ) between ~2.0 eV for 100% Ga 2 O 3 and ~3.4 eV for 100% Al 2 O 3 . With variable ratios of Ga:Al, the measured E g exhibits significant non-linearity, agreeing with the density functional theory simulation, and tunable carrier concentration. Furthermore, the dielectric constant of ultrathin Ga 2 O 3 /Al 2 O 3 ALS capacitors is tunable through the variation in the ratio of the constituent Ga 2 O 3 and Al 2 O 3 atomic layer numbers from 9.83 for 100% Ga 2 O 3 to 8.28 for 100% Al 2 O 3 . The high ε leads to excellent effective oxide thickness ~1.7–2.1 nm for the ultrathin Ga 2 O 3 /Al 2 O 3 ALS, which is comparable to that of high-K dielectric materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Strain-switchable field-induced superconductivity

Field-induced superconductivity is a rare phenomenon where an applied magnetic field enhances or induces superconductivity. Here, we use applied stress as a control switch between a field-tunable superconducting state and a robust non–field-tunable state. This marks the first demonstration of a strain-tunable superconducting spin valve with infinite magnetoresistance. We combine tunable uniaxial stress and applied magnetic field on the ferromagnetic superconductor Eu(Fe 0.88 Co 0.12 ) 2 As 2 to shift the field-induced zero-resistance temperature between 4 K and a record-high value of 10 K. We use x-ray diffraction and spectroscopy measurements under stress and field to reveal that strain tuning of the nematic order and field tuning of the ferromagnetism act as independent control parameters of the superconductivity. Combining comprehensive measurements with DFT calculations, we propose that field-induced superconductivity arises from a novel mechanism, namely, the uniquely dominant effect of the Eu dipolar field when the exchange field splitting is nearly zero.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1975

Waveguide CO2 laser gain: Dependence on gas kinetic and discharge properties

Using a simple rate equation approach the gas kinetic and discharge properties of waveguide CO2 lasers were examined. The dependence was calculated of the population inversion and laser small signal gain on gas pressure, gas mixture, pumping rate (discharge current), tube bore diameter, and wall temperature. At higher pressures the gain is optimized by using more helium rich mixtures and smaller bore diameters. The dependence of laser tunability on the gas kinetic properties and cavity losses was determined, it was found that for loss cavities the laser tunability may substantially exceed the molecular fullwidth at half maximum. The more helium rich gas mixtures give greater tunability when cavity losses are small and less tunability when cavity losses are large. The role of the various gases in the waveguide CO2 laser is the same as that in conventional devices, by contrast with conventional lasers, the waveguide laser transition is homogeneously broadened. The dependence of gain on gas pressure and other kinetic and discharge properties differs substantially from that predicted by scaling results from conventional low pressure lasers.

Cohen, S. C.↗
NASA NTRS1976

Waveguide CO2 laser gain - Dependence on gas kinetic and discharge properties

A simple rate-equation approach is used to examine the gas-kinetic and discharge properties of waveguide CO2 lasers. The dependence of the population inversion and laser small-signal gain on gas pressure, gas mixture, pumping rate (discharge current), tube bore diameter, and wall temperature is calculated along with the dependence of laser tunability on the gas-kinetic properties and cavity losses. It is found that for low-loss cavities, the laser tunability may substantially exceed the molecular full width at half-maximum. Furthermore, the more helium-rich gas mixtures give greater tunability when cavity losses are small, and less tunability when cavity losses are large. By contrast with conventional lasers, the waveguide-laser transition is homogeneously broadened. Thus, the dependence of gain on gas pressure and other kinetic properties differs substantially from that predicted by scaling results from conventional low-pressure lasers.

Cohen, S. C.↗
NASA NTRS2006

Water Vapor Sensors Go Sky-High to Assure Aircraft Safety

JPL used a special tunable diode laser, which NASA scientists could tune to different wavelengths, like a radio being tuned to different frequencies, to accurately target specific molecules and detect small traces of gas. This tunable diode laser was designed to emit near-infrared light at wavelengths absorbed by the gas or gases being detected. The light energy being absorbed by the target gas is related to the molecules present. This is usually measured in parts per million or parts per billion. Multiple measurements are made every second, making the system quick to respond to variations in the target gas. NASA scientists developed this technology as part of the 1999 Mars Polar Lander mission to explore the possibility of life-giving elements on Mars. NASA has since used the tunable diode laser-based gas sensor on aircraft and on balloons to successfully study weather and climate, global warming, emissions from aircraft, and numerous other areas where chemical gas analysis is needed. SpectraSensors, Inc., was formed in 1999 as a spinoff company of JPL, to commercialize tunable diode laser-based analyzers for industrial gas-sensing applications (Spinoff 2000). Now, the San Dimas, California-based firm has come back to the market with a new product featuring the NASA-developed instrument for atmospheric monitoring. This instrument is now helping aircraft avoid hazardous weather conditions and enabling the National Weather Service to provide more accurate weather forecasts.

Source record↗
NASA NTRS2008

Frequency-Tuneable Pre-Stabilized Lasers for LISA via Sideband Locking

Laser frequency noise mitigation is one of the most challenging aspects of the LISA interferometric measurement system. The unstabilized frequency fluctuations must be suppressed by roughly twelve orders of magnitude in order to achieve a stability sufficient for gravitational wave detection. This enormous suppression will be achieved through a combination of stabilization and common-mode rejection. The stabilization component will itself be achieved in two stages: pre-stabilization to a local optical cavity followed by arm-locking to some combination of the inter-spacecraft distances. In order for these two stabilization stages to work simultaneously, the lock-point of the pre-stabilization loop must be frequency tunable. The current baseline stabilization technique, locking to an optical cavity, does not provide tunability between cavity resonance, which are typically spaced by 100s of MHz. Here we present a modification to the traditional Pound-Drever-Hall cavity locking technique that allows the laser to be locked to a cavity resonance with an adjustable frequency offset. This technique requires no modifications to the optical cavity itself, thus preserving the stability of the frequency reference. We present measurements of the system stability, demonstrating that the pre-stabilization level satisfies LISA requirements. We also present a demonstration of a phase-lock loop which utilizes the tunable sideband locking technique as a pre-stabilizations tage. The performance of the pre-stabilized phase-lock-loop indicates that the tunable sideband technique will meet the requirements as an actuator for arm-locking in LISA.

Thorpe, James Ira↗
DOE OSTI2021

Imaging Reconfigurable Molecular Concentration on a Graphene Field-Effect Transistor

The spatial arrangement of adsorbates deposited onto a clean surface under vacuum typically cannot be reversibly tuned. Here we use scanning tunneling microscopy to demonstrate that molecules deposited onto graphene field-effect transistors (FETs) exhibit reversible, electrically tunable surface concentration. Continuous gate-tunable control over the surface concentration of charged F 4 TCNQ molecules was achieved on a graphene FET at T = 4.5K. This capability enables the precisely controlled impurity doping of graphene devices and also provides a new method for determining molecular energy level alignment based on the gate-dependence of molecular concentration. Gate-tunable molecular concentration is explained by a dynamical molecular rearrangement process that reduces total electronic energy by maintaining Fermi level pinning in the device substrate. Finally, the molecular surface concentration is fully determined by the device back-gate voltage, its geometric capacitance, and the energy difference between the graphene Dirac point and the molecular LUMO level.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Dopamine-Mediated Polymer Coating Facilitates Area-Selective Atomic Layer Deposition

Area-selective atomic layer deposition (ALD) has the potential to significantly improve current fabrication approaches by introducing a bottom-up process in which robust and conformal thin films are selectively deposited onto patterned substrates. This bottom-up approach requires selective areas of the substrates to be masked to inhibit deposition. Spontaneous self-assembly and organization of a mask, incorporating adhesion and other functions, are particularly attractive for this role as they do not require a separate patterning step. In this work, we make use of the pH/light tunability of catechol adhesion to develop a catechol-functionalized polymer that exhibits tunable adhesion strengths on different materials based on their specific chemistry. Tunable selective deposition was shown between metal/metal oxide substrates by controlling the local pH. Moreover, by controlling the adhesion strength through UV light, the deposition of hafnium oxide (HfO 2 ) during ALD was successfully inhibited.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Solid-State Lighting Using Side-by-Side White Phosphorescent Organic Light-Emitting Diodes

White organic light-emitting diodes (WOLEDs) have become increasingly popular for use in solid-state illumination, where diffuse, large area light sources that achieve a high color rendering index and luminous power efficiency are desirable. Color-tunable emission, where the light source combines emission from multiple, separately addressed color elements, is conveniently provided by WOLEDs for the purpose of adapting the lighting source to a particular illumination requirement. In this work, we demonstrate a method for side-by-side positioning of monochromatic blue and yellow phosphorescent OLED stripes that are combined to create tunable white light, using a high resolution mechanical peel-off patterning method. We achieve a peak luminous power efficiency of 17.1 ± 0.3 lm W –1 and an external quantum efficiency of 11.8 ± 0.2% and demonstrate color tunability of the 1960 Commission Internationale d’Eclairage chromaticity coordinates from (u,v) = (0.33,0.36) to (0.12,0.32). This corresponds to a tuning rnge of the color rendering index from 74 ± 1 to 86 ± 1 and the correlated color temperature from 2000 to 8000 ± 500 K. Here, due to the nondestructive nature of the peel-off technique, patterned devices exhibit a lifetime comparable to conventional, shadow mask-patterned devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Tuning the Spin Transition and Carrier Type in Rare-Earth Cobaltates via Compositional Complexity

There is growing interest in material candidates with properties that can be engineered beyond traditional design limits. Compositionally complex oxides (CCO), often called high entropy oxides, are excellent candidates, wherein a lattice site shares more than four cations, forming single-phase solid solutions with unique properties. However, the nature of compositional complexity in dictating properties remains unclear, with characteristics that are difficult to calculate from first principles. Here, in this study, compositional complexity is demonstrated as a tunable parameter in a spin-transition oxide semiconductor La 1- x (Nd, Sm, Gd, Y) x/4 CoO 3 , by varying the population x of rare earth cations over 0.00≤ x≤ 0.80. Across the series, increasing complexity is revealed to systematically improve crystallinity, increase the amount of electron versus hole carriers, and tune the spin transition temperature and on-off ratio. At high a population (x = 0.8), Seebeck measurements indicate a crossover from hole-majority to electron-majority conduction without the introduction of conventional electron donors, and tunable complexity is proposed as new method to dope semiconductors. First principles calculations combined with angle resolved photoemission reveal an unconventional doping mechanism of lattice distortions leading to asymmetric hole localization over electrons. Thus, tunable complexity is demonstrated as a facile knob to improve crystallinity, tune electronic transitions, and to dope semiconductors beyond traditional means.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Long‐Range Non‐Coulombic Coupling at the LaAlO 3 /SrTiO 3 Interface

The LaAlO 3 /SrTiO 3 interface hosts a plethora of gate‐tunable electronic phases. Gating of LaAlO 3 /SrTiO 3 interfaces is usually assumed to occur electrostatically. However, increasing evidence suggests that non‐local interactions can influence and, in some cases, dominate the coupling between applied gate voltages and electronic properties. Here, quasi‐1D ballistic electron waveguides are sketched at the LaAlO 3 /SrTiO 3 interface as a probe to understand how gate tunability varies as a function of spatial separation. Gate tunability measurements reveal the scaling law to be at odds with the pure electrostatic coupling observed in traditional semiconductor systems. The non‐Coulombic gating at the interface is attributed to a long‐range nanoelectromechanical coupling between the gate and electron waveguide, possibly mediated by the ferroelastic domains in SrTiO 3 . The long‐range interactions at the LaAlO 3 /SrTiO 3 interface add unexpected richness and complexity to this correlated electron system.

36 MATERIALS SCIENCE↗
DOE OSTI2023

2D Exotic Optical Lattice via a Digital‐Coding Circular Airy Beam

Optical lattices have been widely used from classical to quantum physics. The tunable and scalable fabrication of lattices would be of great significance in lattice‐based multipartite applications. This work demonstrates first that a circular Airy beam (CAB), which has the peculiar properties of self‐healing and abrupt autofocusing, can be used to generate two‐dimensional (2D) optical lattices in propagation when encoded by a programmable spatial mask, resulting in the formation of large‐scale and tunable optical lattices with both axis and axial symmetry, and even high‐orbital kaleidoscope shapes. The efficient diffraction of CAB during the spatial crosstalk with the mask enables the realization of tunable lattices with rich periodicity and complexity. The study shows a flexible method to manipulate lattices with large‐scale and versatile structures for potential applications in integrated and scalable optical and photonic devices.

Sun, Peisheng↗
DOE OSTI2024

Microstructural Underpinnings of Giant Intrinsic Exchange Bias in Epitaxial NiCo 2 O 4 Thin Films

Understanding intrinsic exchange bias in nominally single-component ferromagnetic or ferrimagnetic materials is crucial for simplifying related device architectures. However, the mechanisms behind this phenomenon and its tunability remain elusive, which hinders the efforts to achieve unidirectional magnetization for widespread applications. Inspired by the high tunability of ferrimagnetic inverse spinel NiCo 2 O 4 , the origin of intrinsic exchange bias in NiCo 2 O 4 (111) films deposited on Al 2 O 3 (0001) substrates are investigated. The comprehensive characterizations, including electron diffraction, X-ray reflectometry and spectroscopy, and polarized neutron reflectometry, reveal that intrinsic exchange bias in NiCo 2 O 4 (111)/Al 2 O 3 (0001) arises from a reconstructed antiferromagnetic rock-salt Ni x Co 1-x O layer at the interface between the film and the substrate due to a significant structural mismatch. Remarkably, by engineering the interfacial structure under optimal growth conditions, it can achieve exchange bias larger than coercivity, leading to unidirectional magnetization. Such giant intrinsic exchange bias can be utilized for realistic device applications. This work establishes a new material platform based on NiCo 2 O 4 , an emergent spintronics material, to study tunable interfacial magnetic and spintronic properties.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Multicolored microwave absorbers with dynamic frequency modulation

Microwave-absorbing materials are extensively used in intelligent electronic devices and stealth technologies where the ability to dynamically adjust microwave-absorbing capacity in response to specific requirements is vitally important. Herein, we report a new approach for constructing dynamically tunable microwave absorbers with ultrawide tunable frequency ranges that are simultaneously endowed with vibrant structural colors. Here, the methodology produces structural colors and adjusts absorption properties by constructing ZnO coatings with precisely adjustable thicknesses on a polypyrrole/melamine foam (PPy/MF) surface by atomic layer deposition (ALD) in conjunction with a pressure-driven strategy that regulates the compression ratio. The electrical conductivity, electromagnetic parameters, thickness, and pore size of the ZnO-coated PPy/MF (ZnO/PPy/MF) are effectively adjusted, and simply applying external pressure widens the tunable frequency range and the effective absorption bandwidth. As a result, the effective absorption frequency of ZnO/PPy/MF is dynamically adjustable from the S band to the Ku band, thereby covering 94.3% of the entire microwave spectrum. Moreover, the brilliant and uniform structural colors of ZnO/PPy/MF, which span various color categories, are precisely regulated by tuning the thickness of the ZnO coating by adjusting the number of ALD cycles. ZnO/PPy/MF is strongly hydrophobic, which endows it with remarkable self-cleaning properties. Therefore, ZnO/PPy/MF provides a conceptually novel platform for the development of next-generation smart microwave-absorbing materials due to its integrated dynamic frequency-regulating ability, brilliant structural coloration, and self-cleaning features.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Lattice-Mismatched van der Waals Epitaxy and Photoluminescence of Two-Dimensional GaxIn1-xSe Alloys on Si(111)

GaxIn1-xSe (GIS) alloys are two-dimensional (2D) layered materials with band gaps and lattice parameters of interest for many energy and electronic applications. They can be fabricated using van der Waals epitaxy, which is an emerging technique that offers unprecedented opportunities for 2D optoelectronic devices and epitaxy processes. This work has demonstrated van der Waals epitaxy of GIS alloys for the first time. Films with x compositions of 0, 0.062, 0.164, 0.680, 0.894, and 1 and tunable lattice constants were grown on Si(111) substrates, and characterized by X-ray diffraction pole figure and transmission electron microscope analysis. In spite of the lattice mismatches (InSe is 4.1% too large and GaSe is 2.8% too small), these alloys grow epitaxially, with Si(111) || GIS(001) and Si[1-10] || GIS[100] orientation. Photoluminescence was used to measure tunable band gaps in the absorber-relevant 1.3-2.0 eV range as a function of x composition and showed GIS did not degrade after capping with Se and prolonged storage. Therefore, GIS alloys exhibit a technologically advantageous combination of tunable band gap and photoluminescence with relaxed lattice parameter and rotational registry with the substrate.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Chemically Controllable Porous Polymer–Nanocrystal Composites with Hierarchical Arrangement Show Substrate Transport Selectivity

Functional organic–inorganic hybrid materials with tunable properties are useful across many application areas, ranging from gas storage to electronics, flame retardants, separations, and catalysis. Combining polymers, with a suite of functional groups and conformational flexibility, and inorganic nanoparticles, with tunable surface chemistry and composition, yields hybrids with novel functional properties. Specifically, in catalysis, control of the electronic environment at a metal interface is paramount in determining the catalytic properties. In this contribution, we describe a modular process to prepare porous polymer–nanocrystal (NC) composites in a hierarchical, multilayered synthesis, in which multiple parameters can be accurately tuned: polymer functional groups and the corresponding pore structure, the polymer layer thickness, and the NC size, shape, and composition. This process provides for a variety of controlled materials with high surface area, tunable chemistry, and thermal and chemical stabilities. Furthermore, we demonstrate their utility for shape- and size-selective catalytic conversions both in oxidation and hydrogenation reactions, where they show increased selectivity by orders of magnitude compared to conventional polymer-supported metal catalysts. In light of the high degree of control in the composite structure, this method allows for the design and realization of catalysts for several reactions and reaction environments and for nanomaterials with other applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗