Hall, Alex T. | Search NASA

DOE OSTI2026

Self-driving thin film laboratory: autonomous epitaxial atomic-layer synthesis via real-time computer vision analysis of electron diffraction

Emerging materials science platforms with the ability to make autonomous decisions on the fly are fundamentally changing the outlook and protocols for materials optimization and discovery. Because AI-driven self-navigating schemes can effectively reduce the total number of iterations needed to arrive at the "answer" (i.e. the best stochiometric composition for a desired physical property, optimum materials processing parameters, etc.) by significant margins, they have the potential to revolutionize materials and chemical manufacturing processes at large in research laboratory settings as well as in industrial plants. Here, we demonstrate a successful implementation of real-time closed-loop autonomous navigation of a multi-dimensional materials synthesis parameter space for fabricating phase-pure epitaxial films of a metastable phase of a functional oxide in a combinatorial pulsed laser deposition chamber. Sequential epitaxial growth iterations in search of the optimized recipe to stabilize the desired crystal phase were performed using frame-by-frame quantitative computer vision analysis of reflection high-energy electron diffraction (RHEED) images of the unit-cell level film being deposited. The autonomous scheme regularly resulted in > 30-fold reduction in the number of required experiments compared to a comprehensive mapping of the parameter space. The real-time workflow developed here can be readily extended to a variety of thin film synthesis platforms opening the door for self-driving atomic-level materials design as well as autonomous optimization of semiconductor manufacturing.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Resistance of Boron Nitride Nanotubes to Radiation-Induced Oxidation

We present unprecedented results on the damage thresholds and pathways for boron nitride nanotubes (BNNT) under the influence of energetic electrons in an oxidative gas environment, using an environmental aberration-corrected electron microscope over a range of oxygen pressures. We observe a damage cascade process that resists damage until a higher electron dose, compared with carbon nanotubes, initiating at defect-free BNNT sidewalls and proceeding through the conversion from crystalline nanotubes to amorphous boron nitride (BN), resisting oxidation throughout. We compare with prior results on the oxidation of carbon nanotubes and present a model that attributes the onset of damage in both cases to a physisorbed oxygen layer that reduces the threshold for damage onset. Surprisingly, increased temperatures offer protection against damage, as do electron dose rates that significantly exceed the oxygen dose rates, and our model attributes both effects to a physisorbed oxygen population.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Dataset for "Resistance of Boron Nitride Nanotubes to Radiation-Induced Oxidation" as published in The Journal of Physical Chemistry C

We present unprecedented results on the damage thresholds and pathways for boron nitride nanotubes (BNNT) under the influence of energetic electrons in an oxidative gas environment, using an environmental aberration-corrected electron microscope over a range of oxygen pressures. We observe a damage cascade process that resists damage until a higher electron dose, compared with carbon nanotubes, initiating at defect-free BNNT sidewalls and proceeding through the conversion from crystalline nanotubes to amorphous boron nitride (BN), resisting oxidation throughout. We compare with prior results on the oxidation of carbon nanotubes and present a model that attributes the onset of damage in both cases to a physisorbed oxygen layer that reduces the threshold for damage onset. Surprisingly, increased temperatures offer protection against damage, as do electron dose rates that significantly exceed the oxygen dose rates, and our model attributes both effects to a physisorbed oxygen population.

Adsorption↗

DOE OSTI2024

Ion transport and ultra-efficient osmotic power generation in boron nitride nanotube porins

Nanotube porins form transmembrane nanomaterial-derived scaffolds that mimic the geometry and functionality of biological membrane channels. We report synthesis, transport properties, and osmotic energy harvesting performance of another member of the nanotube porin family: boron nitride nanotube porins (BNNTPs). Cryo–transmission electron microscopy imaging, liposome transport assays, and DNA translocation experiments show that BNNTPs reconstitute into lipid membranes to form functional channels of ~2-nm diameter. Ion transport studies reveal ion conductance characteristics of individual BNNTPs, which show an unusual C 1/4 scaling with ion concentration and pronounced pH sensitivity. Reversal potential measurements indicate that BNNTPs have strong cation selectivity at neutral pH, attributable to the high negative charge on the channel. BNNTPs also deliver very large power density up to 12 kW/m 2 in the osmotic gradient transport experiments at neutral pH, surpassing that of other BNNT-based devices by two orders of magnitude under similar conditions. Our results suggest that BNNTPs are a promising platform for mass transport and osmotic power generation.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Paradigms of frustration in superionic solid electrolytes

Superionic solid electrolytes have widespread use in energy devices, but the fundamental motivations for fast ion conduction are often elusive. In this Perspective, we draw upon atomistic simulations of a wide range of superionic conductors to illustrate some ways frustration can lower diffusion cation barriers in solids. Based on our studies of halides, oxides, sulfides and hydroborates and a survey of published reports, we classify three types of frustration that create competition between different local atomic preferences, thereby flattening the diffusive energy landscape. These include chemical frustration, which derives from competing factors in the anion–cation interaction; structural frustration, which arises from lattice arrangements that induce site distortion or prevent cation ordering; and dynamical frustration, which is associated with temporary fluctuations in the energy landscape due to anion reorientation or cation reconfiguration. For each class of frustration, we provide detailed simulation analyses of various materials to show how ion mobility is facilitated, resulting in stabilizing factors that are both entropic and enthalpic in origin. We propose the use of these categories as a general construct for classifying frustration in superionic conductors and discuss implications for future development of suitable descriptors and improvement strategies.

25 ENERGY STORAGE↗