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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

The many-body expansion for aqueous systems revisited: II. Alkali metal and halide ion – water interactions

We present a detailed study of the Many-Body Expansion (MBE) for alkali metal and halide ion-water interactions and quantify the effect of these ions on the strength of the surrounding aqueous hydrogen bonding environment. Building on our previous work on neutral water clusters [J. P. Heindel and S. S. Xantheas, J. Chem. Theor. Comput. 16 (11), 6843–6855 (2020)], we carry out the complete MBE for ion-water clusters, Z+/-(H2O)9, where Z = Li+, K+, Cs+, Cl-, Br-, I- and compare with the results for (H2O)10. The 2-B ion-water (I-W) interaction represents a larger percentage of the total cluster binding energy compared to a pure water cluster of the same size with the total 3-B term being smaller and of opposite sign (repulsive) whereas higher order terms are essentially negligible. The same oscillating behavior around zero for MBE terms higher than the 5-B with basis set that was reported for water clusters is also observed for the ion-water clusters considered with Basis Set Superposition Error (BSSE) corrections amending this like in the water cluster case. A remarkable, linear anti-correlation between the total 2-B ion-water and the total 2-B and 3-B water-water interactions is found, quantifying the effect of the different ions in disrupting and altering (weakening) the neighboring hydrogen bonded water network. Our results suggest a universal behavior of the two different families of ions (alkali metals and halides) for both the correlations of the various components of the total binding energies as well as the estimate of the 2-B BSSE correction which is reported to follow a common profile for ion-water and water-water interactions when cast in terms of reduced distances and energies. We expect our insights into the nature of BSSE will be important for future ab initio based, many-body molecular dynamics studies.

ion-water interactions, water-water interaction, m↗
DOE OSTI2024

Hybrid Molecular Beam Epitaxy for Single-Crystalline Oxide Membranes with Binary Oxide Sacrificial Layers

The advancement in thin-film exfoliation for synthesizing oxide membranes has led to possibilities for creating artificially assembled heterostructures with structurally and chemically incompatible materials. The sacrificial layer method is a promising approach to exfoliate as-grown films from a compatible material system, allowing for their integration with dissimilar materials. Nonetheless, the conventional sacrificial layers often possess an intricate stoichiometry, thereby constraining their practicality and adaptability, particularly when considering techniques such as molecular beam epitaxy (MBE). This is where easy-to-grow binary alkaline-earth-metal oxides with a rock salt crystal structure are useful. These oxides, which include (Mg, Ca, Sr, Ba)O, can be used as a sacrificial layer covering a much broader range of lattice parameters compared to conventional sacrificial layers and are easily dissolvable in deionized water. In this study, we show the epitaxial growth of the single-crystalline perovskite SrTiO 3 (STO) on sacrificial layers consisting of crystalline SrO, BaO, and Ba 1–x Ca x O films, employing a hybrid MBE method. Our results highlight the rapid (≤5 min) dissolution of the sacrificial layer when immersed in deionized water, facilitating the fabrication of millimeter-sized STO membranes. Using high-resolution X-ray diffraction, atomic-force microscopy, scanning transmission electron microscopy, impedance spectroscopy, and scattering-type near-field optical microscopy (SNOM), we demonstrate single-crystalline STO membranes with bulk-like intrinsic dielectric properties. The employment of alkaline earth metal oxides as sacrificial layers is likely to simplify membrane synthesis, particularly with MBE, thus expanding the research and application possibilities.

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

Recent progress of MnBi 2 Te 4 epitaxial thin films as a platform for realising the quantum anomalous Hall effect

Since the first realisation of the quantum anomalous Hall effect (QAHE) in a dilute magnetic-doped topological insulator thin film in 2013, the quantisation temperature has been limited to less than 1 K due to magnetic disorder in dilute magnetic systems. With magnetic moments ordered into the crystal lattice, the intrinsic magnetic topological insulator MnBi 2 Te 4 has the potential to eliminate or significantly reduce magnetic disorder and improve the quantisation temperature. Surprisingly, to date, the QAHE has yet to be observed in molecular beam epitaxy (MBE)-grown MnBi 2 Te 4 thin films at zero magnetic field, and what leads to the difficulty in quantisation is still an active research area. Although bulk MnBi 2 Te 4 and exfoliated flakes have been well studied, revealing both the QAHE and axion insulator phases, experimental progress on MBE thin films has been slower. Furthermore, understanding how the breakdown of the QAHE occurs in MnBi 2 Te 4 thin films and finding solutions that will enable mass-produced millimetre-size QAHE devices operating at elevated temperatures are required. In this mini-review, we will summarise recent studies on the electronic and magnetic properties of MBE MnBi 2 Te 4 thin films and discuss mechanisms that could explain the failure of the QAHE from the aspects of defects, electronic structure, magnetic order, and consequences of their delicate interplay. Finally, we propose several strategies for realising the QAHE at elevated temperatures in MnBi 2 Te 4 thin films.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Synthesis of La 2–x Sr x CuO 4 films via atomic layer-by-layer molecular beam epitaxy

Atomic layer-by-layer molecular beam epitaxy (ALL-MBE) is a sophisticated technique to synthesize high-temperature superconductor (HTS) materials. ALL-MBE produces single-crystal HTS films with atomically smooth surfaces and interfaces, as well as precise multilayer heterostructures engineered down to a single atomic layer level. This enables the fabrication of tunnel junctions, nanowires, nanorings, and other HTS devices of interest. Our group has focused on ALL-MBE synthesis and materials science of La 2–x Sr x CuO 4 (LSCO), a representative HTS cuprate. In the past two decades, we have synthesized over three thousand LSCO thin films and characterized them by a range of analytical techniques. Here, we present in full detail a systematic process for the synthesis and engineering of atomically perfect LSCO films. The procedure includes the preparation of substrates, calibration of the elemental sources, the recipe for ALL growth of LSCO films without any secondary-phase precipitates, post-growth annealing of the films, and ex situ film characterization. This report should aid replication and dissemination of this technique of synthesizing single-crystal LSCO films for basic research as well as for HTS electronic applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Incorporation of Ti in epitaxial Fe2TiO4 thin films

The titanomagnetites (Fe2-xTixO4, x = 1) are a family of reducible spinel-structure oxides of interest for their favorable magnetic, catalytic, and electrical transport properties. To understand the stability of the system during low temperature deposition, epitaxial thin films of Fe2TiO4 were deposited by molecular beam epitaxy on MgO(001) at 250 – 375°C. The homogeneous incorporation of Ti, Fe valence, and film morphology were all found to be strongly dependent on the oxidation conditions at the low substrate temperatures employed. More oxidizing conditions led to phase separation into epitaxial, faceted Fe3O4 and rutile TiO2. Less oxidizing conditions resulted in polycrystalline films that exhibited Ti segregation to the film surface, as well as mixed Fe valence (Fe3+, Fe2+, Fe0). A narrow window of intermediate oxygen partial pressure during deposition yielded nearly homogeneous Ti incorporation and a large fraction of Fe2+. However, these films were poorly crystallized, and no occupation of tetrahedral sites in the spinel lattice by Fe2+ was detected by x-ray magnetic circular dichroism at the Fe L-edge. After vacuum annealing, a small fraction of Fe2+ was found to occupy tetrahedral sites. Comparison of these results with previous work suggests that the restriction of the deposition conditions to low temperature by the MgO substrate limits the incorporation of Ti into the spinel lattice. This work suggests a path towards obtaining stoichiometric, well-crystallized Fe2TiO4 by MBE by utilizing high substrate temperature and low oxygen partial pressure during deposition on temperature-stable substrates.

Kaspar, Tiffany C.↗
DOE OSTI2025

Many-body expansion based machine learning models for octahedral transition metal complexes

Abstract Graph-based machine learning (ML) models for material properties show great potential to accelerate virtual high-throughput screening of large chemical spaces. However, in their simplest forms, graph-based models do not include any 3D information and are unable to distinguish stereoisomers such as those arising from different orderings of ligands around a metal center in coordination complexes. In this work we present a modification to revised autocorrelation descriptors, a molecular graph featurization method, for predicting spin state dependent properties of octahedral transition metal complexes (TMCs). Inspired by analytical semi-empirical models for TMCs, the new modeling strategy is based on the many-body expansion (MBE) and allows one to tune the captured stereoisomer information by changing the truncation order of the MBE. We present the necessary modifications to include this approach in two commonly used ML methods, kernel ridge regression and feed-forward neural networks. On a test set composed of all possible isomers of binary TMCs, the best MBE models achieve mean absolute errors (MAEs) of 2.75 kcal mol −1 on spin-splitting energies and 0.26 eV on frontier orbital energy gaps, a 30%–40% reduction in error compared to models based on our previous approach. We also observe improved generalization to previously unseen ligands where the best-performing models exhibit MAEs of 4.00 kcal mol −1 (i.e. a 0.73 kcal mol −1 reduction) on the spin-splitting energies and 0.53 eV (i.e. a 0.10 eV reduction) on the frontier orbital energy gaps. Because the new approach incorporates insights from electronic structure theory, such as ligand additivity relationships, these models exhibit systematic generalization from homoleptic to heteroleptic complexes, allowing for efficient screening of TMC search spaces.

Meyer, Ralf (ORCID:0000000322360261)↗
DOE OSTI2020

Precursor selection in hybrid molecular beam epitaxy of alkaline-earth stannates

One of the challenges of oxide molecular beam epitaxy (MBE) is the synthesis of oxides containing metals with high electronegativity (metals that are hard to oxidize). The use of reactive organometallic precursors can potentially address this issue. To investigate the formation of radicals in MBE, we explored three carefully chosen metal-organic precursors of tin for SnO 2 and BaSnO 3 growth: tetramethyltin (TMT), tetraethyltin (TET), and hexamethylditin (HMDT). All three precursors produced single-crystalline, atomically smooth, and epitaxial SnO 2 (101) films on r-Al 2 O 3 (101¯2) in the presence of oxygen plasma. The study of growth kinetics revealed reaction-limited and flux-limited regimes except for TET, which also exhibited a decrease in the deposition rate with increasing temperature above ~800 °C. Contrary to these similarities, the performance of these precursors was dramatically different for BaSnO 3 growth. TMT and TET were ineffective in supplying adequate tin, whereas HMDT yielded phase-pure, stoichiometric BaSnO 3 films. Significantly, HMDT resulted in phase-pure and stoichiometric BaSnO 3 films even without the use of an oxygen plasma (i.e., with molecular oxygen alone). Furthermore, these results are discussed using the ability of HMDT to form tin radicals and therefore assisting with Sn → Sn 4+ oxidation reaction. Structural and electronic transport properties of films grown using HMDT with and without oxygen plasma are compared. This study provides guideline for the choice of precursors that will enable the synthesis of metal oxides containing hard-to-oxidize metals using reactive radicals in MBE.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Many-Body Effects in Aqueous Systems: Synergies Between Interaction Analysis Techniques and Force Field Development

Interaction analysis techniques, including the many-body expansion (MBE), symmetry-adapted perturbation theory, and energy decomposition analysis, allow for an intuitive understanding of complex molecular interactions. We review these methods by first providing a historical context for the study of many-body interactions and discussing how nonadditivities emerge from Hamiltonians containing strictly pairwise-additive interactions. We then elaborate on the synergy between these interaction analysis techniques and the development of advanced force fields aimed at accurately reproducing the Born–Oppenheimer potential energy surface. In particular, we focus on ab initio–based force fields that aim to explicitly reproduce many-body terms and are fitted to high-level electronic structure results. These force fields generally incorporate many-body effects through ( a) parameterization of distributed multipoles, ( b) explicit fitting of the MBE, ( c) inclusion of many-atom features in a neural network, and ( d) coarse-graining of many-body terms into an effective two-body term. We also discuss the emerging use of the MBE to improve the accuracy and speed of ab initio molecular dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Bifacial PV Module Energy Modeling Validation Study

The cost delta between monofacial and bifacial photovoltaic (PV) modules was decreasing in 2018 when this study was initially proposed, making bifacial modules an attractive offering. However, there were limited field studies available that could be considered utility-scale representative, and PV module manufacturers were stating large ranges for the expected energy yield improvements of bifacial technology. This generated uncertainties regarding bifacial performance gains and the actual LCOE (levelized cost of energy). There was also relatively low confidence in the industry’s energy modeling tools’ ability to accurately predict bifacial energy yield, meaning that early adopters of bifacial modules were not able to fully account for the increased energy yield in their energy and financial models. The intent of this project was to provide the solar industry with greater certainty on the energy yield gains of bifacial modules and provide higher confidence in the ability for different energy modeling software to model bifacial PV site performance. Achieving this would allow for bifacial technology to become bankable (i.e. accepted by Independent Engineers, site financiers and other PV site stakeholders), offering a step change in PV site performance that had not been seen since the widespread adoption of the single-axis tracker. Over the course of this study other economic factors including a significant tariff exemption for bifacial modules resulted in accelerated adoption of bifacial technology throughout the US utility scale solar segment. The number of early adopters increased rapidly, and with many investors accepting this module choice the question of bifacial bankability was seemingly answered faster than expected. However, PVEL’s study has still achieved significant accomplishments in demonstrating the accuracy of bifacial modeling across three different software platforms. The results of this study have shown that the mean biased error (MBE) between the field data and the predicted values from all three software platforms were aligned with a maximum MBE of 1.3% and a minimum MBE of -1.8%.

14 SOLAR ENERGY↗
NASA NTRS1983

Silicon sheet with molecular beam epitaxy for high efficiency solar cells

The capabilities of the new technique of Molecular Beam Epitaxy (MBE) are applied to the growth of high efficiency silicon solar cells. Because MBE can provide well controlled doping profiles of any desired arbitrary design, including doping profiles of such complexity as built-in surface fields or tandem junction cells, it would appear to be the ideal method for development of high efficiency solar cells. It was proposed that UCLA grow and characterize silicon films and p-n junctions of MBE to determine whether the high crystal quality needed for solar cells could be achieved.

Allen, F. G.↗
NASA NTRS1997

Ka-Band GaAs FET Monolithic Power Amplifier Development

Over the course of this program, very extensive progress was made in Ka-band GaAs technology. At the beginning of the program, odd-shaped VPE MESFET wafers were used. A breakthrough in power and efficiency was achieved with highly doped (8 x 10(exp 17) cm(exp -3) MBE grown MESFET material. We obtained power of 112 mW with 16 dB gain and 21.6% efficiency at 34 GHz with a monolithic 50-100-250 micron amplifier. The next breakthrough came with the use of heterostructures grown by MBE (AlGaAs/InGaAs where the InGaAs is highly doped). This allowed us to achieve high power density with high efficiency. A benchmark 40% efficiency was achieved with a single-stage 100 micron MMIC at 32.5 GHz. The corresponding three-stage 50-100-250 micron amplifier achieved 180 mW with 23 dB gain and 30.3% efficiency. The next breakthrough came with 3-inch MBE grown PHEMT wafers incorporating an etch-stop layer for the gate recess (using RIE). Again, state-of-the-art performances were achieved: 40% efficiency with 235 mW output power and 20.7 dB gain. The single-stage 2 x 600 micron chip demonstrated 794 mW output power with 5 dB gain and 38.2% power-added efficiency (PAE). The Ka-band technology developed under this program has promise for extensive use: JPL demonstrated 32 GHz phased arrays with a three-stage amplifier developed under this contract. A variation of the three-stage amplifier was used successfully in a 4 x 4 phased array transmitter developed under another NASA contract.

Saunier, Paul↗
NASA NTRS2002

Development of High Quantum Efficiency UV/Blue Photocathode Epitaxial Semiconductor Heterostructures for Scintillation and Cherenkov Radiation Detection

The primary goal of this research project was to further extend the use of advanced heteroepitaxial-semiconductor crystal growth techniques such as molecular beam epitaxy (MBE) and to demonstrate significant gains in UV/blue photonic detection by designing and fabricating atomically-tailored heteroepitaxial GaAlN/GaInN photocathode device structures. This NASA Explorer technology research program has focused on the development of photocathodes for Cherenkov and scintillation radiation detection. Support from the program allowed us to enhance our MBE system to include a nitrogen plasma source and a magnetic bearing turbomolecular pump for delivery and removal of high purity atomic nitrogen during GaAlN/GaInN film growth. Under this program we have also designed, built and incorporated a cesium activation stage. In addition, a connected UHV chamber with photocathode transfer/positioner components as well as a hybrid phototube stage was designed and built to make in-situ quantum efficiency measurements without ever having to remove the photocathodes from UHV conditions. Thus we have constructed a system with the capability to couple atomically-tailored MBE-grown photocathode heterostructures with real high gain readout devices for single photon detection evaluation.

Leopold, Daniel J.↗
NASA NTRS1994

Growth of delta-doped layers on silicon CCD/S for enhanced ultraviolet response

The backside surface potential well of a backside-illuminated CCD is confined to within about half a nanometer of the surface by using molecular beam epitaxy (MBE) to grow a delta-doped silicon layer on the back surface. Delta-doping in an MBE process is achieved by temporarily interrupting the evaporated silicon source during MBE growth without interrupting the evaporated p+ dopant source (e.g., boron). This produces an extremely sharp dopant profile in which the dopant is confined to only a few atomic layers, creating an electric field high enough to confine the backside surface potential well to within half a nanometer of the surface. Because the probability of UV-generated electrons being trapped by such a narrow potential well is low, the internal quantum efficiency of the CCD is nearly 100% throughout the UV wavelength range. Furthermore, the quantum efficiency is quite stable.

Hoenk, Michael E.↗
NASA NTRS2005

N-Type delta Doping of High-Purity Silicon Imaging Arrays

A process for n-type (electron-donor) delta doping has shown promise as a means of modifying back-illuminated image detectors made from n-doped high-purity silicon to enable them to detect high-energy photons (ultraviolet and x-rays) and low-energy charged particles (electrons and ions). This process is applicable to imaging detectors of several types, including charge-coupled devices, hybrid devices, and complementary metal oxide/semiconductor detector arrays. Delta doping is so named because its density-vs.-depth characteristic is reminiscent of the Dirac delta function (impulse function): the dopant is highly concentrated in a very thin layer. Preferably, the dopant is concentrated in one or at most two atomic layers in a crystal plane and, therefore, delta doping is also known as atomic-plane doping. The use of doping to enable detection of high-energy photons and low-energy particles was reported in several prior NASA Tech Briefs articles. As described in more detail in those articles, the main benefit afforded by delta doping of a back-illuminated silicon detector is to eliminate a "dead" layer at the back surface of the silicon wherein high-energy photons and low-energy particles are absorbed without detection. An additional benefit is that the delta-doped layer can serve as a back-side electrical contact. Delta doping of p-type silicon detectors is well established. The development of the present process addresses concerns specific to the delta doping of high-purity silicon detectors, which are typically n-type. The present process involves relatively low temperatures, is fully compatible with other processes used to fabricate the detectors, and does not entail interruption of those processes. Indeed, this process can be the last stage in the fabrication of an imaging detector that has, in all other respects, already been fully processed, including metallized. This process includes molecular-beam epitaxy (MBE) for deposition of three layers, including metallization. The success of the process depends on accurate temperature control, surface treatment, growth of high-quality crystalline silicon, and precise control of thicknesses of layers. MBE affords the necessary nanometer- scale control of the placement of atoms for delta doping. More specifically, the process consists of MBE deposition of a thin silicon buffer layer, the n-type delta doping layer, and a thin silicon cap layer. The n dopant selected for initial experiments was antimony, but other n dopants as (phosphorus or arsenic) could be used. All n-type dopants in silicon tend to surface-segregate during growth, leading to a broadened dopant-concentration- versus-depth profile. In order to keep the profile as narrow as possible, the substrate temperature is held below 300 C during deposition of the silicon cap layer onto the antimony delta layer. The deposition of silicon includes a silicon- surface-preparation step, involving H-termination, that enables the growth of high-quality crystalline silicon at the relatively low temperature with close to full electrical activation of donors in the surface layer.

Blacksberg, Jordana↗
NASA NTRS2003

Artifacts for Calibration of Submicron Width Measurements

Artifacts that are fabricated with the help of molecular-beam epitaxy (MBE) are undergoing development for use as dimensional calibration standards with submicron widths. Such standards are needed for calibrating instruments (principally, scanning electron microscopes and scanning probe microscopes) for measuring the widths of features in advanced integrated circuits. Dimensional calibration standards fabricated by an older process that involves lithography and etching of trenches in (110) surfaces of single-crystal silicon are generally reproducible to within dimensional tolerances of about 15 nm. It is anticipated that when the artifacts of the present type are fully developed, their critical dimensions will be reproducible to within 1 nm. These artifacts are expected to find increasing use in the semiconductor-device and integrated- circuit industries as the width tolerances on semiconductor devices shrink to a few nanometers during the next few years. Unlike in the older process, one does not rely on lithography and etching to define the critical dimensions. Instead, one relies on the inherent smoothness and flatness of MBE layers deposited under controlled conditions and defines the critical dimensions as the thicknesses of such layers. An artifact of the present type is fabricated in two stages (see figure): In the first stage, a multilayer epitaxial wafer is grown on a very flat substrate. In the second stage, the wafer is cleaved to expose the layers, then the exposed layers are differentially etched (taking advantage of large differences between the etch rates of the different epitaxial layer materials). The resulting structure includes narrow and well-defined trenches and a shelf with thicknesses determined by the thicknesses of the epitaxial layers from which they were etched. Eventually, it should be possible to add a third fabrication stage in which durable, electronically inert artifacts could be replicated in diamondlike carbon from a master made by MBE and etching as described above.

Grunthaner, Frank↗
NASA NTRS2016

Solar Activity Studies using Microwave Imaging Observations

We report on the status of solar cycle 24 based on polar prominence eruptions (PEs) and microwave brightness enhancement (MBE) information obtained by the Nobeyama radioheliograph. The north polar region of the Sun had near-zero field strength for more than three years (2012-2015) and ended only in September 2015 as indicated by the presence of polar PEs and the lack of MBE. The zero-polar-field condition in the south started only around 2013, but it ended by June 2014. Thus the asymmetry in the times of polarity reversal switched between cycle 23 and 24. The polar MBE is a good proxy for the polar magnetic field strength as indicated by the high degree of correlation between the two. The cross-correlation between the high- and low-latitude MBEs is significant for a lag of approximately 5.5 to 7.3 years, suggesting that the polar field of one cycle indicates the sunspot number of the next cycle in agreement with the Babcock-Leighton mechanism of solar cycles. The extended period of near-zero field in the north-polar region should result in a weak and delayed sunspot activity in the northern hemisphere in cycle 25.

microwave radio emission↗
DOE OSTI2025

Atomically precise synthesis of oxides with hybrid molecular beam epitaxy

Advancements in synthesis science are revolutionizing the way we create atomically precise materials. Techniques like molecular beam epitaxy (MBE) have set the benchmark for addressing long-standing questions in materials science by leveraging improved control over the composition and structure of existing materials and enabling materials discovery. In this review, we discuss recent innovations in MBE that are redefining its capabilities, enabling the fabrication of ultra-pure, defect-engineered films and the stabilization of metastable phases that were previously unattainable. These advancements are unlocking new opportunities in electronic, magnetic, and quantum technologies, where the precise tuning of material properties is essential for advancing device functionality and performance.

complex oxides↗
DOE OSTI2025

Molecular beam epitaxy growth of IrO 2 using plasma-only oxidation

Growth of IrO 2 films via molecular beam epitaxy (MBE) using an oxygen plasma as the sole oxidant is demonstrated for the first time. We investigate the oxidizing conditions required for IrO 2 by characterizing the species present in the plasma using optical emission spectroscopy and comparing the thermodynamic equilibrium between Ir/IrO 2 under atomic and molecular oxygen. Across the pressure range accessible, monatomic oxygen was the primary reactive species present in the plasma. IrO 2 films were grown under varying Ir flux, oxygen pressure, and substrate temperature to understand growth thermodynamics and kinetics. Structural characterization assessed film phase and composition, crystallinity, strain, and surface morphology. The optimized films from this study validate plasma-only reactive growth by MBE as a successful method for growing IrO 2 .

36 MATERIALS SCIENCE↗