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At least 451 records · Page 25

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DOE OSTI2025

High-Throughput Discovery Illuminates Design Principles and Limits for Long-Lived Charged Species in Organic Electrolytes

The chemical stability of charged molecules in all-organic redox flow batteries (RFBs) is required for the prolonged operation of these devices. Molecular engineering and electrolyte optimization are used to mitigate parasitic reactions and extend the lifetimes of the charge carriers. However, how much can structural variation extend the lifetime? To probe this query, we designed a high-throughput kinetic study of the radical cation of N-methylphenothiazinium, guided by statistical sampling and learning algorithms. Using Argonne’s autonomous discovery facility, we conducted over 6,000 kinetic experiments with robotic sample preparation, parallel kinetic measurements, and machine learning inputs, testing 188 solvent molecules selected from a space of over 540 candidates from 11 chemical classes. Algorithmic selections guided us to stable solvent candidates, which were further tested in high concentration with and without supporting electrolyte. Our findings reveal the inherent difficulty of exceeding the current state of the art through solvent variation. The desired stability is statistically rare and poorly predictable. Among the many tested, only three solvents significantly outperformed our baseline, acetonitrile─and none by more than a factor of 3─suggesting a general challenge in achieving the necessary techno-economic targets. Furthermore, we suggest that self-discharge through solvent homolysis is the cause of the observed limitations. Several structural motifs contribute to >1,000 h half-life stability including molecular simplicity, symmetry, oxidation complement, and strategic fluorination. Importantly, this workflow establishes effective assays for diagnosing and predicting oxidative stress for highly stable liquid electrolytes in all batteries.

Batteries↗

DOE OSTI2020

Theoretical insights into the surface physics and chemistry of redox-active oxides

Redox active oxides are ubiquitous in materials applications, including catalysis, photovoltaics, self-cleaning glasses, chemical sensors, and electronic components. Their utility derives from their unique ability to access multiple metal charge states within a finite energy window. However, this property also confounds our ability to study reducible oxides, because it leads to structural, compositional, and electronic complexities that elude simplistic models of materials structure and function. Oxygen vacancies play a critical role in shaping the functional properties of such oxides; most notably, they lead to mobile charge imbalances that impact surface processes at significant distances from the originating defect. Atomistic simulations are inherently equipped to illuminate these phenomena at a fundamental level; however, reducible oxides pose great challenges due to the high level of electron correlation needed to correctly describe them. Knowing how defects form, couple, propagate, agglomerate, or repel each other and influence the surface properties of reducible oxides is only now coming into the grasp of modern theory and simulation capabilities. This knowledge is also key to discovering and controlling emergent materials processes at nanometer scale and beyond. The manuscript was written with support of all three authors from U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. Work by RR and VG was performed at Pacific Northwest National Laboratory (PNNL), which is a multi-program laboratory operated by Battelle for DOE under Contract DE AC05 76RL01830. AS was supported under Award DE-SC0007347.

Rousseau, Roger J.↗

DOE OSTI2026

Solid-state NMR and theoretical studies illuminate lanthanum borohydride C–H borylation catalysts confined within a zeolite

Zeolite-supported single-site lanthanum borohydride catalyzes C–H borylation of hydrocarbons, while the related silica-supported complex is inactive under comparable conditions. The identical composition of support-La(BH 4 ) 2 (THF) 2 sites in the two materials implies that the support bestows underlying structural features onto La that are required for bond activation catalysis, yet the nature of these effects, which could include confinement effects and/or electronic modulation of the site itself, remains to be identified. We used solid-state nuclear magnetic resonance (SSNMR) spectroscopy and molecular dynamics simulations with machine-learning potentials (ML-MD) to analyze the electronic and steric effects imparted by the faujasite support on the precatalyst structure to correlate with catalytic activity. ML-MD simulations show that THF dissociates from La under the influence of confinement, leading to coordinatively unsaturated sites in the zeolite pores. Then, the La complex grafts on Brønsted acid sites (La BAS ) or isolated silanols (La SiO ) or remains physisorbed in the zeolite pores. Catalytic studies comparing compounds supported on faujasite zeolites containing or lacking BAS and/or silanols show that only the former complexes lead to active sites, ruling out confinement as the sole requirement for catalysis. The DFT calculations and ML-MD simulations also reveal that the surface-lanthanum coordination number is two (bidentate) for La BAS , with the metal center forming long, flexible bonds to two oxygen atoms bridging Si and Al, but only one oxygen atom (monodentate) for La SiO . The structure–activity relationship identifies confined, BAS-grafted species as active sites and provides important guidance for the design of enhanced atom-efficient catalysts.

Cui, Jinlei [Ames Laboratory, and Iowa State Univ.↗

DOE OSTI2023

Metal-semiconductor-metal structured p-i-n GaN/AlGaN ultrafast detectors for deep-UV photodetection

We report the productive outcome of the design, fabrication, and testing of a new class of GaN/AlGaN-based ultrafast, sensitive photodiodes for deep-UV solar blind photodetection. Pt was employed as the interdigitated metal electrode to establish that while a Schottky contact was formed at the metal/semiconductor heterojunction, it was the quantum wells in the p-i-n vertical structure that produced the diode characteristics of the detectors. The metal–semiconductor–metal design retained its ultrafast property as expected in the p-i-n structure because the spacing between the interdigitated fingers was asymmetrically implemented to optimize the photogenerated carriers’ transit time from the quantum well to the external circuitry. Also, the vertical p-i-n structure provided its renowned efficient photocarrier generation, which was significantly enhanced by the delta quantum well architecture of the vertical epitaxial structure. The active area of the device was 300 μm × 300 μm with 5-μm finger width, and asymmetric electrode spacing of 2 μm, 3 μm, and 5 μm. Here, the best device had peak responsivity of 3.5 A/W under 262-nm illumination with full width half maximum of 337.2-ps and 37.5-ps rise times when biased with 20 V.

efficient↗

NASA NTRS1993

Earth global mosaic observations with NIMS-Galileo

During the Earth-1 Galileo flyby (December 1990), the Near-Infrared Mapping Spectrometer (NIMS) experiment investigated the illuminated side of the Earth in the spectral range 0.7-5.2 micrometers. Mosaics of the entire terrestrial globe were recorded with a spatial resolution ranging from 100 to 500 km. From these spectra, information is retrieved upon the large-scale temperature structure in the stratosphere and in the mesosphere (0-70 km altitude range) from the inversion of the CO2 bands at 4.3 and 4.8 micrometers. These data also permit monitoring of the cloud temperatures, and derivation of the abundances of several minor atmospheric constituents (H2O, CO, N2O, CH4 and O3). These observations constitute a continuation of the study of the atmospheres of the three planets (i.e. Venus, the Earth and Jupiter) targeted by the Galileo spacecraft during its mission. Observing these atmospheres with the NIMS instrument in the near-infrared will provide a unique data set, useful for comparative planetary studies.

Drossart, P.↗

DOE OSTI2021

Ionizing-radiation beamline monitoring system

Embodiments are directed generally to an ionizing-radiation beamline monitoring system that includes a vacuum chamber structure with vacuum compatible flanges through which an incident ionizing-radiation beam enters the monitoring system. Embodiments further include at least one scintillator within the vacuum chamber structure that can be at least partially translated in the ionizing-radiation beam while oriented at an angle greater than 10 degrees to a normal of the incident ionizing-radiation beam, a machine vision camera coupled to a light-tight structure at atmospheric/ambient pressure that is attached to the vacuum chamber structure by a flange attached to a vacuum-tight viewport window with the camera and lens optical axis oriented at an angle of less than 80 degrees with respect to a normal of the scintillator, and at least one ultraviolet (“UV”) illumination source facing the scintillator in the ionizing-radiation beam for monitoring a scintillator stability comprising scintillator radiation damage.

Friedman, Peter S.↗

DOE OSTI2023

Ionizing-radiation beamline monitoring system

Friedman, Peter S.↗

NASA NTRS2017

Active Electrostatic flight for airless bodies

The environment near the surface of asteroids, comets, and the Moon is electrically charged due to the Sun’s photoelectric bombardment and lofting dust, which follows the Sun illumination as the body spins. Charged dust is ever present, in the form of dusty plasma, even at high altitudes, following the solar illumination. If a body with high surface resistivity is exposed to the solar wind and solar radiation, sunexposed areas and shadowed areas become differentially charged. The E-Glider (Electrostatic Glider) is an enabling capability for operation at airless bodies, a solution applicable to many types of in-situ missions, which leverages the natural environment. This platform directly addresses the "All Access Mobility" Challenge, one of the NASA’s Space Technology Grand Challenges. Exploration of comets, asteroids, moons and planetary bodies is limited by mobility on those bodies. The lack of an atmosphere, the low gravity levels, and the unknown surface soil properties pose a very difficult challenge for all forms of know locomotion at airless bodies. This EGlider levitates by extending thin, charged, appendages, which are also articulated to direct the levitation force in the most convenient direction for propulsion and maneuvering. The charging is maintained through continuous charge emission. It lands, wherever it is most convenient, by retracting the appendages or by firing a cold-gas thruster, or by deploying an anchor. Preliminary calculations indicate that a 1 kg mass can be electrostatically levitated in a microgravity field with a 2 m diameter electrostatically inflated ribbon structure at 19kV, hence the need for a “balloon-like” system. The wings could be made of very thin Au-coated Mylar film, which are electrostatically inflated, and would provide the lift due to electrostatic repulsion with the naturally charged asteroid surface. Since the E-glider would follow the Sun’s illumination, the solar panels on the vehicle would constantly charge a battery. Further articulation at the root of the lateral strands or inflated membrane wings, would generate a component of lift depending on the articulation angle, hence a selective maneuvering capability which, to all effects, would lead to electrostatic (rather than aerodynamic) flight.

Schaub, Hanspeter↗

DOE OSTI2020

Atomic force microscopy: Emerging illuminated and operando techniques for solar fuel research

Integrated photoelectrochemical devices rely on the synergy between components to efficiently generate sustainable fuels from sunlight. The micro- and/or nanoscale characteristics of the components and their interfaces often control critical processes of the device, such as charge-carrier generation, electron and ion transport, surface potentials, and electrocatalysis. Understanding the spatial properties and structure–property relationships of these components can provide insight into designing scalable and efficient solar fuel components and systems. These processes can be probed ex situ or in situ with nanometer-scale spatial resolution using emerging scanning-probe techniques based on atomic force microscopy (AFM). In this Perspective, we summarize recent developments of AFM-based techniques relevant to solar fuel research. We review recent progress in AFM for (1) steady-state and dynamic light-induced surface photovoltage measurements; (2) nanoelectrical conductive measurements to resolve charge-carrier heterogeneity and junction energetics; (3) operando investigations of morphological changes, as well as surface electrochemical potentials, currents, and photovoltages in liquids. Opportunities for research covered here include: (1) control of ambient conditions for performing AFM measurements; (2) in situ visualization of corrosion and morphological evolution of electrodes; (3) operando AFM techniques to allow nanoscale mapping of local catalytic activities and photo-induced currents and potentials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1987

Information retrieval from holographic interferograms: Fundamentals and problems

Holographic interferograms can contain large amounts of information about flow and temperature fields. Their information content can be very high because they can be viewed from many different directions. This multidirectionality, and fringe localization add to the information contained in the fringe pattern if diffuse illumination is used. Additional information, and increased accuracy can be obtained through the use of dual reference wave holography to add reference fringes or to effect discrete phase shift or hetrodyne interferometry. Automated analysis of fringes is possible if interferograms are of simple structure and good quality. However, in practice a large number of practical problems can arise, so that a difficult image processing task results.

Vest, Charles M.↗

NASA NTRS1989

Observations of molecular and atomic gas in photodissociation regions

Dense gas at the ionized/neutral boundaries of molecular clouds illuminated by far-UV photons plays an important role in the appearance of the neutral interstellar medium. It also is a laboratory for the study of UV-photochemistry and of a number of heating and cooling phenomena not seen elsewhere. Fine structure lines of neutral and low ionization potential species dominate the cooling in the outer part of the photodissociation regions. Observations of these lines show that the regions are dense and highly clumped. Observations of H2 and CO show that heating by UV photons plays a significant role in the excitation of molecular lines near the H II/neutral boundary. Warm CO is more abundant in these regions than predicted by the standard theoretical models. Optical reflection nebulas provide an ideal laboratory for the study of photodissocciation region phenomena.

Jaffe, D. T.↗

NASA NTRS1972

Silicon solar cell development and radiation effects study for low temperature and low illumination intensity operation, volume 2

The results are presented of a study to determine the effect of in-situ proton irradiation upon low temperature, low intensity performance of several cell types. The cell types were selected in an attempt to distinguish variations in temperature-dependent radiation resistance which could be attributed to the n-p or p-n structure, diffused or implanted junctions, crucible grown or float-zone type base material, and high or low base resistivity. The results indicate that while expected variations of performance occur at room temperature, all cell types degrade more or less similarly at lower temperatures with normalized degradation becoming increasingly rapid as temperature is reduced. Recommendations for an optimized cell for Jupiter probe use are included along with a definition of the testing required on these cells to insure good performance characteristics.

Kirkpatrick, A. R.↗

DOE OSTI2026

Understanding and mitigating degradation in amine-based sorbents for CO 2 direct air capture

The success of direct air capture (DAC) of CO 2 depends on sorbents that combine high capacity, low energy requirements, and long-term durability. Amine-based sorbents-including solid-supported aminopolymers, grafted amines, and amine-functionalized resins-remain the leading candidates, but their limited lifetimes drive up costs and constrain deployment. In this review, we outline the current understanding of amine-based sorbent degradation with an emphasis on clearly identifying what is known about structure-property-performance relationships, as well as important knowledge gaps. More specifically, we discuss how polymer chemistry, sorbent design variables, and environmental and process conditions contribute to performance loss. In parallel, we outline how advances in spectroscopy, modeling, and accelerated testing are beginning to illuminate chemical and physical degradation mechanisms. Looking forward, we identify future research directions that will be critical for gaining a deeper understanding of degradation, as well as opportunities for developing innovative mitigation strategies for improving the lifetime of amine-based sorbents.

organic↗

DOE OSTI2025

The influence of ambient light spectrum (LED, INC, CFL, Xenon…) on the efficiency of perovskite indoor photovoltaic solar cells for Internet of Things (IoT) applications

This record provides a numerical investigation of a MAGeI₃-based perovskite solar cell with the structure FTO/TiO₂/MAGeI₃/Spiro-OMeTAD, evaluated for both outdoor and indoor light-harvesting applications using the SCAPS-1D simulator. Device performance is analyzed under AM 1.5G sunlight and several artificial light sources, including LED, incandescent, compact fluorescent lamp (CFL), flashlight, and xenon illumination. The study reports initial and optimized power conversion efficiencies and examines the influence of absorber layer thickness and bandgap on device performance under different lighting conditions. The results highlight the potential of MAGeI₃-based perovskite solar cells for indoor energy harvesting and low-power Internet of Things (IoT) applications.

14 SOLAR ENERGY↗

DOE OSTI2023

Ferroelectric Polarization in BaTiO 3 Nanocrystals Controls Photoelectrochemical Water Oxidation and Photocatalytic Hydrogen Evolution

Ferroelectric (FE) semiconductors such as BaTiO 3 support a remnant polarization after the application of an electric field that can promote the separation of photogenerated charge carriers. Here, we demonstrate FE-enhanced photocatalytic hydrogen evolution and photoelectrochemical water oxidation with barium titanate nanocrystals for the first time. Nanocrystals of the ferroelectric tetragonal structure type were obtained by a hydrothermal synthesis from TiO 2 and barium hydroxide in 63% yield. BaTiO 3 nanocrystal films on tantalum substrates exhibit water oxidation photocurrents of 0.141 mA cm –2 at 1.23 V RHE under UV light (60 mW cm –2 ) illumination. Electric polarization at 52.8 kV cm –1 normal to the film plane increases the photocurrent by a factor of 2 or decreases it by a factor of 3.5, depending on the field polarity. It also shifts the onset potential by –0.15 or +0.09 V and it modifies the surface photovoltage signal. Lastly, exposure to an electric field increases the H 2 evolution rate of Pt/BaTiO 3 by a factor of ~1.5, and it raises the selectivity of photodeposition of silver onto the (001) facets of the nanocrystal. All FE enhancements can be removed by heating samples above the Curie temperature of BaTiO 3 . Furthermore, these findings can be explained by FE dipole-induced changes to the potential drop across the space charge layer of the material. The ability to use the ferroelectric effect to enhance hydrogen evolution and water oxidation is of potential interest for the development of improved solar energy for fuel conversion systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Extreme elevational migration spurred cryptic speciation in giant hummingbirds

The ecoevolutionary drivers of species niche expansion or contraction are critical for biodiversity but challenging to infer. Niche expansion may be promoted by local adaptation or constrained by physiological performance trade-offs. For birds, evolutionary shifts in migratory behavior permit the broadening of the climatic niche by expansion into varied, seasonal environments. Broader niches can be short-lived if diversifying selection and geography promote speciation and niche subdivision across climatic gradients. To illuminate niche breadth dynamics, we can ask how “outlier” species defy constraints. Of the 363 hummingbird species, the giant hummingbird (Patagona gigas) has the broadest climatic niche by a large margin. To test the roles of migratory behavior, performance trade-offs, and genetic structure in maintaining its exceptional niche breadth, we studied its movements, respiratory traits, and population genomics. Satellite and light-level geolocator tracks revealed an >8,300-km loop migration over the Central Andean Plateau. This migration included a 3-wk, ~4,100-m ascent punctuated by upward bursts and pauses, resembling the acclimatization routines of human mountain climbers, and accompanied by surging blood-hemoglobin concentrations. Extreme migration was accompanied by deep genomic divergence from high-elevation resident populations, with decisive postzygotic barriers to gene flow. The two forms occur side-by-side but differ almost imperceptibly in size, plumage, and respiratory traits. The high-elevation resident taxon is the world’s largest hummingbird, a previously undiscovered species that we describe and name here. The giant hummingbirds demonstrate evolutionary limits on niche breadth: when the ancestral niche expanded due to evolution (or loss) of an extreme migratory behavior, speciation followed.

Science & Technology - Other Topics↗

DOE OSTI2024

High-angular-momentum Rydberg states in a room-temperature vapor cell for dc electric-field sensing

We prepare and analyze Rydberg states with orbital quantum numbers ℓ ≤ 6 using three-optical-photon electromagnetically induced transparency (EIT) and radio frequency (rf) dressing, and employ the high- ℓ states in electric-field sensing. Rubidium-85 atoms in a room-temperature vapor cell are first promoted into the 25 F 5 / 2 state via Rydberg-EIT with three infrared laser beams. Two rf dressing fields then (near-)resonantly couple the 25 F , 25 H ( ℓ = 5 ) , and 25 I ( ℓ = 6 ) Rydberg states. The dependence of the rf-dressed Rydberg-state level structure on rf powers, rf and laser frequencies is characterized using EIT. Furthermore, we discuss the principles of dc-electric-field sensing using high- ℓ Rydberg states and experimentally demonstrate the method using test electric fields of ≲ 50 V/m induced via photo-illumination of the vapor-cell wall. We measure the highly nonlinear dependence of the dc-electric-field strength on the power of the photo-illumination laser. Numerical calculations, which reproduce our experimental observations well, elucidate the underlying physics. Our paper is relevant to high-precision spectroscopy of high- ℓ Rydberg states, Rydberg-atom-based electric-field sensing, and plasma electric-field diagnostics. Published by the American Physical Society 2024

Duspayev, Alisher (ORCID:0000000153225762)↗

DOE OSTI2022

Volumetric additive manufacturing of silica glass with microscale computed axial lithography

Glass is increasingly desired as a material for manufacturing complex microscopic geometries, from the micro-optics in compact consumer products to microfluidic systems for chemical synthesis and biological analyses. As the size, geometric, surface roughness, and mechanical strength requirements of glass evolve, conventional processing methods are challenged. We introduce microscale computed axial lithography (micro-CAL) of fused silica components, by tomographically illuminating a photopolymer-silica nanocomposite that is then sintered. We fabricated three-dimensional microfluidics with internal diameters of 150 micrometers, free-form micro-optical elements with a surface roughness of 6 nanometers, and complex high-strength trusses and lattice structures with minimum feature sizes of 50 micrometers. As a high-speed, layer-free digital light manufacturing process, micro-CAL can process nanocomposites with high solids content and high geometric freedom, enabling new device structures and applications.

36 MATERIALS SCIENCE↗