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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Graphene-polyelectrolyte multilayer membranes with tunable structure and internal charge

One great advantage of graphene-polyelectrolyte multilayer (GPM) membranes is their tunable structure and internal charge for improved separation performance. In this study, we synthesized GO-dominant GPM membrane with internal negatively-charged domains, polyethyleneimine (PEI)-dominant GPM membrane with internal positively-charged domains and charge-balanced dense/loose GPM membranes by simply adjusting the ionic strength and pH of the GO and PEI solutions used in layer-by-layer membrane synthesis. A combined system of quartz crystal microbalance with dissipation (QCM-D) and ellipsometry was used to analyze the mass deposition, film thickness, and layer density of the GPM membranes. The performance of the GPM membranes were compared in terms of both permeability and selectivity to determine the optimal membrane structure and synthesis strategy. One effective strategy to improve the GPM membrane permeability-selectivity tradeoff is to assemble charge-balanced dense membranes under weak electrostatic interactions. This balanced membrane exhibits the highest MgCl 2 selectivity (~86%). Another effective strategy for improved cation removal is to create PEI-dominant membranes that provide internal positively-charged barrier to enhance cation selectivity without sacrificing water permeability. Finally, these findings shine lights on the development of a systematic approach to push the boundary of permeability-selectivity tradeoff for GPM membranes.

42 ENGINEERING↗
DOE OSTI2023

Observation of time-dependent internal charge amplification in a planar germanium detector at cryogenic temperature

For the first time, time-dependent internal charge amplification through impact ionization has been observed in a planar germanium (Ge) detector operated at cryogenic temperature. In a time period of 30 and 45 min after applying a bias voltage, the charge energy corresponding to a baseline of the 59.54 keVγ rays from a 241 Am source is amplified for a short period of time and then decreases back to the baseline. The amplification of charge energy depends strongly on the applied positive bias voltage with drifting holes across the detector. No such phenomenon is visible with drifting electrons across the detector. We find that the observed charge amplification is dictated by the impact ionization of charged states, which has a strong correlation with impurity level and applied electric field. We analyze the dominant physics mechanisms that are responsible for the creation and the impact ionization of charged states. Our analysis suggests that the appropriate level of impurity in a Ge detector can enhance charge yield through the impact ionization of charged states to achieve extremely low-energy detection threshold (< 10 meV) for MeV-scale dark matter searches if the charge amplification can be stabilized.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Self-organizing layers from complex molecular anions

Ions are promising building blocks for tunable self-organizing materials with advanced technological applications. However, because of strong Coulomb attraction with counterions, the intrinsic properties of ions are difficult to exploit for preparation of bulk materials. Here, we report the precisely-controlled preparation of macroscopic surface layers by soft landing of mass selected complex anions which determine the self organization of the layers with their molecular properties. The family of halogenated dodecaborates [B12X12]2- (X = F, Cl, Br, I), in which the internal charge distribution between core and shell regions of the molecular ions systematically vary, was deposited on different self assembled monolayer surfaces (SAMs) on gold at high coverage. Layers of anions were found to be stabilized by accumulation of neutral molecules. Different phases, self-organization mechanisms and optical properties were observed to depend upon the internal charge distribution of the deposited anions, the underlying surface and the coadsorbed molecules. This demonstrates rational control of the properties of anion based layers.

Warneke, Jonas (ORCID:0000000232337412)↗
DOE OSTI2023

Low-energy solar neutrino detection utilizing advanced germanium detectors

We explore the possibility to use advanced germanium (Ge) detectors as a low-energy solar neutrino observatory by means of neutrino-nucleus elastic scattering. A Ge detector utilizing internal charge amplification for the charge carriers created by the ionization of impurities is a novel technology with experimental sensitivity for detecting low-energy solar neutrinos. Ge internal charge amplification (GeICA) detectors will amplify the charge carriers induced by neutrino interacting with Ge atoms through the emission of phonons. It is those phonons that will create charge carriers through the ionization of impurities to achieve an extremely low energy threshold of ~0.01 eV. We demonstrate the phonon absorption, excitation, and ionization probability of impurities in a Ge detector with impurity levels of 3 × 10 10 cm -3 , 9 × 10 10 cm -3 , and 2 × 10 11 cm -3 . We present the sensitivity of such a Ge experiment for detecting solar neutrinos in the low-energy region. We show that, if GeICA technology becomes available, then a new opportunity arises to observe pp and 7 Be solar neutrinos. Such a novel detector with only 1 kg of high-purity Ge will give ~10 events per year for pp neutrinos and ~5 events per year for 7 Be neutrinos with a detection energy threshold of 0.01 eV.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2018

Direct detection of MeV-scale dark matter utilizing germanium internal amplification for the charge created by the ionization of impurities

Light, MeV-scale dark matter (DM) is an exciting DM candidate that is undetectable by current experiments. A germanium (Ge) detector utilizing internal charge amplification for the charge carriers created by the ionization of impurities is a promising new technology with experimental sensitivity for detecting MeV-scale DM. We analyze the physics mechanisms of the signal formation, charge creation, charge internal amplification, and the projected sensitivity for directly detecting MeV-scale DM particles. We present a design for a novel Ge detector at helium temperature (~4 K) enabling ionization of impurities from DM impacts. With large localized E-fields, the ionized excitations can be accelerated to kinetic energies larger than the Ge bandgap at which point they can create additional electron–hole pairs, producing intrinsic amplification to achieve an ultra-low energy threshold of ~0.1 eV for detecting low-mass DM particles in the MeV scale. Correspondingly, such a Ge detector with 1 kg-year exposure will have high sensitivity to a DM-nucleon cross section of ~5 × 10 -45 cm 2 at a DM mass of ~10 MeV/c 2 and a DM-electron cross section of ~ 5 × 10 -46 cm 2 at a DM mass of 1 MeV/c 2 .

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Core–Shell Covalently Linked Graphitic Carbon Nitride–Melamine–Resorcinol–Formaldehyde Microsphere Polymers for Efficient Photocatalytic CO 2 Reduction to Methanol

Photocatalytic reduction of CO 2 with light and H 2 O to form CH 3 OH is a promising route to mitigate carbon emissions and climate changes. Although semiconducting metal oxides are potential photocatalysts for this reaction, low photon efficiency and leaching of environmental unfriendly, toxic metals limit their applicability. Here, we report a metal-free, core-shell photocatalysts consisting of graphitic carbon nitride (g-C 3 N 4 , CN) covalently linked to melamine-resorcinol-formaldehyde (MRF) microsphere polymers for this reaction. Cova-lent linkage enabled efficient separation of photo-generated carriers and photocatalysis. Using 100 mg of a photocatalyst containing 15 wt.% CN, a CH 3 OH yield of 0.99 μmol·h -1 was achieved at a reaction temperature of 80 °C and 0.5 MPa with external quantum efficiencies ranging from 5.5% at 380 nm to 1.7% at 550 nm. The yield was about 20 and 10 times higher than that of its components CN and MRF, respectively. Characterization with XPS, TEM, and bulk and surface elemental analyses supported a core-shell structure and charge transfer at C-N bond at the CN-MRF interface between the methoxy group in the 2,4-trishydroxylmethyl-1,3-diphenol part of MRF and the terminal amino groups in the CN. This enhanced ligand-to-ligand charge transfer resulted in 67% of photo-excited internal charge transferred from CN to hy-droxymethylamino group in MRF, whose amino group was the catalytic site for CO 2 photocatalytic reduction to CH 3 OH. Furthermore, this study provides a series of new metal-free photocatalyst designs and insights into the molecular-level structure-mediated photocatalytic response

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Insights into the Oxidation Mechanism of Vivianite to Metavivianite from First-Principles Calculations

Vivianite, a hydrous ferrous iron-phosphate mineral (Fe 3 (PO 4 ) 2 ·8H 2 O), readily oxidizes in contact with air yielding the less hydrous mixed-valent iron-phosphate mineral metavivianite. This topotactic transformation nominally occurs by oxidative dehydrogenation in which outgoing electrons from the iron sublattice are charge compensated by hydrolysis of structural water. However, the details of this internal charge balancing mechanism that allows the structure to remain electrostatically stable remain unknown. Here, in this study, we use density functional theory (DFT) calculations and ab initio thermodynamics (AIT) to evaluate the energetics of this process in terms of hydrogen release as a function of environmental variables such as partial pressure and temperature. The results show a thermodynamic driving force for vivianite phase transformation as oxidation progresses that is triggered by its rigid structure that has a limited accommodation for hydrogen vacancies. In contrast, metavivianite has a more flexible lattice and hydrogen bond network that stabilizes these hydrogen defects. Metavivianite is shown to be a stable intermediate for 66% residual Fe 2+ down to 33% Fe 2+ , below which other phases/structures such as santabarbarite should be more thermodynamically favorable. Our study provides a basis for experimental tests of our mechanistic findings and helps fill a basic knowledge gap about the solid-state process that defines how vivianite interacts with its surrounding environment.

Sassi, Michel [Pacific Northwest National Laborato↗
DOE OSTI2023

Electrochemical Characterization of Biomolecular Electron Transfer at Conductive Polymer Interfaces

Bio-electrochemical systems (BESs) are promising for renewable energy generation but remain hindered by inefficient electron transfer at electrode surfaces. As the toolbox of bio-anode materials increases, rigorous electrochemical characterization of emerging materials is needed. Here, we holistically characterize the electrochemical interaction of flavin mononucleotide (FMN), an electron shuttle in biological systems and a cofactor for oxidoreductase enzymes, with the bio-inspired mixed conducting polymer poly{3-[6'-(N-methylimidazolium)hexyl]thiophene} (P3HT-Im + ). The behavior of this polymer is compared to the equivalent polymer without the histidine-like imidazolium. We find improved conductivity and charge storage in imidazolium-containing polymers beyond what is explained by differences in the electroactive area. The P3HT-Im + further shows internal charge storage but with negligible faradaic contribution, indicating that charge storage capacity may translate to improved biocatalysis non-intuitive ways. Finally, one-electron transfer is observed between FMN and glassy carbon, while a bio-similar two-electron transfer is observed for the P3HT-Im + . To our knowledge, this is the first example of a concerted two-electron transfer between FMN and an electrode interface, which we attribute to the bio-inspired, histidine-like imidazolium functional groups in the polymer. These studies demonstrate the importance of bio-relevant materials characterization when such materials are deployed in BESs.

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

Mapping hidden space-charge distributions across crystalline metal oxide/group IV semiconductor interfaces

The electronic structures of semiconducting heterojunctions are critically dependent on composition including the presence and concentrations of dopants, both intended and unintended. Dopant profiles in the interfacial region can have major effects on band energies which in turn drive transport properties. Here, in this study, we use core-level photoelectron line shapes excited with hard x rays to extract information about electric fields resulting from internal charge transfer in epitaxial La 0.03 Sr 0.97 Zr x Ti 1–x O 3 /Ge(001) (0.1≤x≤0.7) heterostructures. Experiments were carried out for heterojunctions involving both n- and p-type Ge substrates. These heterojunctions were not amenable to electronic characterization of all regions by transport measurements because the doped substrates act as electrical shunts, precluding probing the more resistive films and masking interface conductivity. However, the core-level line shapes were found to be a rich source of information on built-in potentials that exist throughout the heterostructure, and yielded valuable insight into the impact of band bending on band alignment at the buried interfaces. The electronic effects expected for Ge with uniform n- and p-type doping are eclipsed by those of unintended oxygen dopants in the Ge near the interface. This study illustrates the power of hard x-ray photoemission spectroscopy and related modeling to determine electronic structure in material systems for which insight from traditional transport measurements is limited.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Exploring the Potential of Residual Impurities in Germanium Detectors for MeV-Scale Dark Matter Detection

Abstract The direct detection of MeV-scale dark matter (DM) particles hinges on achieving an exceptionally low-energy detection threshold. Germanium (Ge) detectors, meticulously tailored with precise impurity compositions, hold the potential to enhance sensitivity to energy levels below the sub-electronvolt (sub-eV) range. This study explores the behavior of residual impurities inherent to Ge detectors at helium temperatures, unveiling a captivating freeze-out phenomenon leading to the formation of excited localized states known as dipole states. Using compelling evidence from relative capacitance measurements obtained from two detectors, we elucidate the transition of impurity atoms from free charge states to these dipole states as the temperature drops from 11 to 6.5 K. Our investigation comprehensively covers the intricate formation of these dipole states in bothn-type andp-type impurities. Furthermore, we shed light on the electric field generated by these dipole states, revealing their ability to trap charges and facilitate the creation of cluster dipole states. Confirming findings from previous measurements, we establish that these excited dipole states exhibit a binding energy of less than 10 meV, offering an exceptionally low detection threshold for MeV-scale DM. Building upon this concept, we propose the development of a 1-kg Ge detector with internal charge amplification—an innovative approach poised to surpass electrical noise and enable the detection of MeV-scale DM with unprecedented sensitivity.

Physics↗
DOE OSTI2023

Design and performance of the Fermilab Constant Fraction Discriminator ASIC

Here, we present the design and performance characterization results of the novel Fermilab Constant Fraction Discriminator ASIC (FCFD) developed to readout low gain avalanche detector (LGAD) signals by directly using a constant fraction discriminator (CFD) to measure signal arrival time. Silicon detectors with time resolutions less than 30ps will play a critical role in future collider experiments, and LGADs have been demonstrated to provide the required time resolution and radiation tolerance for many such applications. The FCFD has a specially designed discriminator that is robust against amplitude variations of the signal from the LGAD that normally requires an additional correction step when using a traditional leading edge discriminator. The application of the CFD directly in the ASIC promises to be more reliable and reduces the complication of evolving time-walk corrections throughout the operational lifetime of the detector system. We will present a summary of the measured performance of the FCFD for input signals generated by internal charge injection, LGAD signals from an infrared laser, and LGAD signals from minimum-ionizing particles. The mean time response for LGAD signals with charge ranging between 5 and 26 fC has been measured to vary no more than 10ps, orders of magnitude more stable than an uncorrected leading edge discriminator based measurement, and effectively removes the need for any additional time-walk correction. The measured contribution to the time resolution from the FCFD ASIC is found to be 10ps for signals with charge above 20fC.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

A sub-5 ps jitter time-to-digital converter ASIC with back-gate delay tuning in 22 nm CMOS

We present the design of a Time-to-Digital Converter (TDC) ASIC together with performance characterization results at cryogenic temperature (6-8 K), and at room temperature using emulated Low-Gain Avalanche Detector (LGAD) signals. The TDC design uses a two-step architecture with a ring-oscillator based counter and a Vernier delay line fine TDC. The TDC is implemented in an FD-SOI process, and back-gate tuning is used not only to correct threshold variation due to cryogenic operation, but also as a novel way to tune TDC delay elements with very little overhead. Using this technique, we demonstrate a design with very low power (0.5 mW) and area (0.003 mm 2 ). We present test results using the Fermilab Constant Fraction Discriminator (FCFD) ASIC to produce discriminated signals from an internal charge injection mechanism that mimics the waveform and signal amplitude of minimum ionizing particles impinging on LGAD sensors. We characterize the time precision of the full system and verify that the TDC ASIC contributes a negligible amount to the total system time precision, fully consistent with the expected jitter contribution of less than 5 ps. In conclusion, the results presented here demonstrate the utility of our TDC for applications in physics and quantum communications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Evaluating the efficacy of aluminide coatings to improve oxidation resistance of high performance engine valve alloys

Increasing peak cylinder pressures and operating temperatures of turbo-charged internal combustion engines (ICEs) engines present new challenges for existing materials employed in engine exhaust valves. Oxidation induced degradation of current Ni based alloys for these components will be a life-limiting mechanism while strict cost margins in the automotive transportation industry further limit the choice of suitable candidate materials. Metallic diffusion aluminide coatings can provide a cost-effective way to improve the oxidation resistance of underlying materials. In this study, the high temperature oxidation behavior of diffusion nickel aluminide coatings on two Ni based alloys (commercially available alloy 31V and a developmental alloy) during cyclic oxidation behavior in air+10% H 2 O at 900 °C was investigated. A complete depletion of the beneficial Al-rich β-(NiFe)Al phase was observed in the coating on alloy 31V while a significant fraction of this phase was retained in the coating on the second alloy. A coupled thermodynamic-kinetic model showed that the disappearance of the Al-rich phase in the coating on 31V was mainly due to the combined effect of steeper chemical potential gradients of Al and Ti between the coating and the substrate and their faster diffusivities compared to the coated developmental alloy. Finally, a higher content of Fe was shown to support the retention of β-(NiFe)Al phase in the coating on the developmental alloy while the presence of Ti in the alloy was shown to be detrimental for long-term coating performance.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Modeling surface spin polarization on ceria-supported Pt nanoparticles

In this work, we employ density functional theory simulations to investigate possible spin polarization of CeO 2 -(111) surface and its impact on the interactions between a ceria support and Pt nanoparticles. With a Gaussian type orbital basis, our simulations suggest that the CeO 2 -(111) surface exhibits a robust surface spin polarization due to the internal charge transfer between atomic Ce and O layers. In turn, it can lower the surface oxygen vacancy formation energy and enhance the oxide reducibility. We show that the inclusion of spin polarization can significantly reduce the major activation barrier in the proposed reaction pathway of CO oxidation on ceria-supported Pt nanoparticles. For metal-support interactions, surface spin polarization enhances the bonding between Pt nanoparticles and ceria surface oxygen, while CO adsorption on Pt nanoparticles weakens the interfacial interaction regardless of spin polarization. However, the stable surface spin polarization can only be found in the simulations based on the Gaussian type orbital basis. Furthermore, given the potential importance in the design of future high-performance catalysts, our present study suggests a pressing need to examine the surface ferromagnetism of transition metal oxides in both experiment and theory.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Machine learning for precise hit position reconstruction in Resistive Silicon Detectors

RSDs are LGAD silicon sensors with 100% fill factor, based on the principle of AC-coupled resistive read-out. Signal sharing and internal charge multiplication are the RSD key features to achieve picosecond-level time resolution and micron-level spatial resolution, thus making these sensors promising candidates as 4D-trackers for future experiments. This paper describes the use of a neural network to reconstruct the hit position of ionizing particles, an approach that can boost the performance of the RSD with respect to analytical models. The neural network has been trained in the laboratory and then validated on test beam data. The device-under-test in this work is a 450 μm-pitch matrix from the FBK RSD2 production, which achieved a resolution of about 65 μm at the DESY Test Beam Facility, a 50% improvement compared to a simple analytical reconstruction method, and a factor two better than the resolution of a standard pixel sensor of equal pitch size with binary read-out. The test beam result is compatible with the laboratory ones obtained during the neural network training, confirming the ability of the machine learning model to provide accurate predictions even in environments very different from the training one. Prospects for future improvements are also discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗