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All sources NASA NTRS DOE OSTI

DOE OSTI2022

Synergistic Porosity and Charge Effects in a Supramolecular Porphyrin Cage Promote Efficient Photocatalytic CO 2 Reduction**

Abstract We present a supramolecular approach to catalyzing photochemical CO 2 reduction through second‐sphere porosity and charge effects. An iron porphyrin box ( PB ) bearing 24 cationic groups, FePB‐2(P) , was made via post‐synthetic modification of an alkyne‐functionalized supramolecular synthon. FePB‐2(P) promotes the photochemical CO 2 reduction reaction (CO 2 RR) with 97 % selectivity for CO product, achieving turnover numbers (TON) exceeding 7000 and initial turnover frequencies (TOF max ) reaching 1400 min −1 . The cooperativity between porosity and charge results in a 41‐fold increase in activity relative to the parent Fe tetraphenylporphyrin ( FeTPP ) catalyst, which is far greater than analogs that augment catalysis through porosity ( FePB‐3(N ), 4‐fold increase) or charge (Fe p ‐tetramethylanilinium porphyrin ( Fe‐ p ‐TMA ), 6‐fold increase) alone. This work establishes that synergistic pendants in the secondary coordination sphere can be leveraged as a design element to augment catalysis at primary active sites within confined spaces.

An, Lun↗

DOE OSTI2020

Correlation of Spatiotemporal Dynamics of Polarization and Charge Transport in Blended Hybrid Organic–Inorganic Perovskites on Macro- and Nanoscales

Progress in flexible organic electronics necessitates a full understanding of how local inhomogeneities impact electronic and ionic conduction pathways and underlie macroscopic device characteristics. In this work, we used frequency- and time-resolved macro- and nanoprobe measurements to study spatiotemporal characteristics of multiscale charge transport dynamics in a series of ternary-blended hybrid organic inorganic perovskites (HOIPs) (MA 0.95– x FA x Cs 0.05 PbI 3 ). We show that A-site cation composition defines charge transport mechanisms across broad temporal (10 2 –10 –6 s) and spatial (millimeters–picometers) scales. Ab initio molecular dynamic simulations suggest that insertion of FA results in a dynamic lattice, improved ion transport, and dipole screening. We demonstrate that correlations between macro- and nanoscale measurements provide a pathway for accessing distribution of relaxation in nanoscale polarization and charge transport dynamics of ionically conductive functional perovskites.

36 MATERIALS SCIENCE↗

DOE OSTI2021

The great escape: tunneling out of microstate geometries

We compute the quasi-normal frequencies of scalars in asymptotically-flat microstate geometries that have the same charge as a D1-D5-P black hole, but whose long BTZ-like throat ends in a smooth cap. In general the wave equation is not separable, but we find a class of geometries in which the non-separable term is negligible and we can compute the quasi-normal frequencies using WKB methods. We argue that our results are a universal property of all microstate geometries with deeply-capped BTZ throats. These throats generate large redshifts, which lead to exceptionally-low-energy states with extremely long decay times, set by the central charge of the dual CFT to the power of twice the dimension of the operator dual to the mode. While these decay times are extremely long, we also argue that the energy decay is bounded, at large t , by (log( t )) – 2 and is comparable with the behavior of ultracompact stars, as one should expect for microstate geometries.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Synergistic Porosity and Charge Effects in a Supramolecular Porphyrin Cage Promote Efficient Photocatalytic CO 2 Reduction**

We present a supramolecular approach to catalyzing photochemical CO 2 reduction through second-sphere porosity and charge effects. An iron porphyrin box (PB) bearing 24 cationic groups, FePB-2(P), was made via post-synthetic modification of an alkyne-functionalized supramolecular synthon. FePB-2(P) promotes the photochemical CO 2 reduction reaction (CO 2 RR) with 97 % selectivity for CO product, achieving turnover numbers (TON) exceeding 7000 and initial turnover frequencies (TOF max ) reaching 1400 min -1 . The cooperativity between porosity and charge results in a 41-fold increase in activity relative to the parent Fe tetraphenylporphyrin (FeTPP) catalyst, which is far greater than analogs that augment catalysis through porosity (FePB-3(N), 4-fold increase) or charge (Fe p-tetramethylanilinium porphyrin (Fe-p-TMA), 6-fold increase) alone. In conclusion, this work establishes that synergistic pendants in the secondary coordination sphere can be leveraged as a design element to augment catalysis at primary active sites within confined spaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

High-throughput injection-acceleration of electron bunches from a linear accelerator to a laser wakefield accelerator

Plasma-based accelerators (PBAs) driven by either intense lasers (laser wakefield accelerators, LWFAs) or particle beams (plasma wakefield accelerators, PWFAs), can accelerate charged particles at extremely high gradients compared to conventional radio-frequency (RF) accelerators. In the past two decades, great strides have been made in this field, making PBA a candidate for next-generation light sources and colliders. However, these challenging applications necessarily require beams with good stability, high quality, controllable polarization and excellent reproducibility. To date, such beams are generated only by conventional RF accelerators. As such, it is important to demonstrate the injection and acceleration of beams first produced using a conventional RF accelerator, by a PBA. In some recent studies on LWFA staging and external injection-acceleration in PWFA only a very small fraction (from below 0.1% to few percent) of the injected charge (the coupling efficiency) was accelerated. For future colliders where beam energy will need to be boosted using multiple stages, the coupling efficiency per stage must approach 100%. Here we report the first demonstration of external injection from a photocathode-RF-gun-based conventional linear accelerator (LINAC) into a LWFA and subsequent acceleration without any significant loss of charge or degradation of quality, which is achieved by properly shaping and matching the beam into the plasma structure. Furthermore, this is an important step towards realizing a high-throughput, multi-stage, high-energy, hybrid conventional-plasma accelerator.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Charge-Density-Wave Thin-Film Devices Printed with Chemically Exfoliated 1T-TaS 2 Ink

In this work, we report on the preparation of inks containing fillers derived from quasi-two-dimensional charge-density-wave materials, their application for inkjet printing, and the evaluation of their electronic properties in printed thin-film form. The inks were prepared by liquid-phase exfoliation of CVT-grown 1T-TaS 2 crystals to produce fillers with nm-scale thickness and μm-scale lateral dimensions. Exfoliated 1T-TaS 2 was dispersed in a mixture of isopropyl alcohol and ethylene glycol to allow fine-tuning of filler particles thermophysical properties for inkjet printing. The temperature-dependent electrical and current fluctuation measurements of printed thin films demonstrated that the charge-density-wave properties of 1T-TaS 2 are preserved after processing. The functionality of the printed thin-film devices can be defined by the nearly commensurate to the commensurate charge-density-wave phase transition of individual exfoliated 1T-TaS 2 filler particles rather than by electron-hopping transport between them. The obtained results are important for the development of printed electronics with diverse functionality achieved by the incorporation of quasi-two-dimensional van der Waals quantum materials.

1T-TaS2↗

DOE OSTI2023

Sensitivity Analysis of a Polyphase Wireless Power Transfer System under Off-Nominal Conditions

Misaligned and/or variable coil airgaps cause coupling coefficient variation in wireless power transfer (WPT) systems, resulting in a decrease in the system’s transmitted power and efficiency. This paper presents sensitivity analyses of a three-phase, Y-Y connected, series-tuned WPT system in the frequency domain in terms of several different electric vehicle wireless charging off-nominal conditions (misalignments in Δ x and Δ y directions, change of airgap Δ z , and the roll Δψ, pitch Δθ, and yaw ΔΦ angles) as specified in Society of Automotive Engineers (SAE) J2954 Standard. Coil inductance matrices were obtained by measuring the self- and mutual inductances of the primary and secondary coil phase windings at variable airgap classes (from 5 cm to 30 cm) for five different charging positions as identified in SAE J2954. These 6 × 6 inductance matrices were used in sensitivity and Plexim/PLECS simulation analyses. The sensitivity of the WPT system was analyzed analytically using the input impedance and phase angle, voltage gain, current gain, quality factor, and coupling coefficient parameters of the series-tuned WPT system. The results were confirmed experimentally on a 50 kW WPT system.

42 ENGINEERING↗

DOE OSTI2020

Large-area low-noise flexible organic photodiodes for detecting faint visible light

Silicon photodiodes are the foundation of light-detection technology; yet their rigid structure and limited area scaling at low cost hamper their use in several emerging applications. A detailed methodology for the characterization of organic photodiodes based on polymeric bulk heterojunctions reveals the influence that charge-collecting electrodes have on the electronic noise at low frequency. The performance of optimized organic photodiodes is found to rival that of low-noise silicon photodiodes in all metrics within the visible spectral range, except response time, which is still video-rate compatible. Solution-processed organic photodiodes offer several design opportunities exemplified in a biometric monitoring application that uses ring-shaped, large-area, flexible, organic photodiodes with silicon-level performance.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Charge carrier coupling to the soft phonon mode in a ferroelectric semiconductor

Many crystalline solids possess strongly anharmonic “soft” phonon modes characterized by diminishing frequency as temperature approaches a critical point associated with a symmetry breaking phase transition. While electron–soft phonon coupling can introduce unique scattering channels for charge carriers in ferroelectrics, recent studies on the nonferroelectric lead halide perovskites have also suggested the central role of anharmonic phonons bearing resemblance to soft modes in charge carrier screening. Here we apply coherent phonon spectroscopy to directly study electron coupling to the soft transverse optical phonon mode in a ferroelectric semiconductor SbSI. Photogenerated charge carriers in SbSI are found to be exceptionally long lived and are associated with a transient electro-optical effect that can be explained by interactions between charge carriers and thermally stimulated soft phonon excitations. Furthermore, these results provide strong evidence for the role of electron–soft phonon coupling in the efficient screening of charge carriers and in reducing charge recombination rates, both desirable properties for optoelectronics.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Experimental demonstration of optical stochastic cooling

Particle accelerators and storage rings have been transformative instruments of discovery, and, for many applications, innovations in particle-beam cooling have been a principal driver of that success. Stochastic cooling (SC), one of the most important conceptual and technological advances in this area cools a beam through granular sampling and correction of its phase-space structure, thus bearing resemblance to a ‘Maxwell’s demon’. The extension of SC from the microwave regime up to optical frequencies and bandwidths has long been pursued, as it could increase the achievable cooling rates by three to four orders of magnitude and provide a powerful tool for future accelerators. First proposed nearly 30 years ago, optical stochastic cooling (OSC) replaces the conventional microwave elements of SC with optical-frequency analogues and is, in principle, compatible with any species of charged-particle beam. Here we describe a demonstration of OSC in a proof-of-principle experiment at the Fermi National Accelerator Laboratory’s Integrable Optics Test Accelerator. The experiment used 100-MeV electrons and a non-amplified configuration of OSC with a radiation wavelength of 950 nm, and achieved strong, simultaneous cooling of the beam in all degrees of freedom. This realization of SC at optical frequencies serves as a foundation for more advanced experiments with high-gain optical amplification, and advances opportunities for future operational OSC systems with potential benefit to a broad user community in the accelerator-based sciences.

43 PARTICLE ACCELERATORS↗

NASA NTRS1978

Frequency analysis of 4- to 6-keV electrons associated with an auroral arc

The high time resolution (HTR) experiment considered consists of four sections, including electrostatic deflection plates, electron multiplier, preamplifier-integrator, and frequency analyzer. Electrons in the energy range from 4 to 6 keV electrons are selected by the deflection system, after which they are detected, multiplied, and passed to the charge sensitive preamplifier. The charge pulses are amplified and integrated, and the resulting voltage pulse series is fed to the frequency analyzer. The experiment is essentially a flux detector, so that estimates of the input flux can be made from the mean value of the output spectrum. The results obtained with the HTR in a rocket flight on March 14, 1974, are discussed. The lack of modulation noticed in the high-frequency range indicates that there is insufficient wave energy available in the vicinity of the rocket to produce a wave-particle interaction which the HTR is able to observe. This finding is consistent with the stabilization of the plasma by the low flux of energetic electrons.

Murphree, J. S.↗

DOE OSTI2025

Ultrabroadband THz conductivity of gated graphene in- and out-of-equilibrium

We employ ultrabroadband terahertz (THz) spectroscopy to expose the high-frequency transport properties of Dirac fermions in monolayer graphene. By controlling the carrier concentration via tunable electrical gating, both equilibrium and transient optical conductivities are obtained for a range of Fermi levels. The frequency-dependent equilibrium response is determined through a combination of time-domain THz and Fourier-transform infrared spectroscopy for energies up to the near-infrared, which also provides a measure of the gate-voltage dependent Fermi level. Transient changes in the real and imaginary parts of the graphene conductivity are electro-optically resolved for frequencies up to 15 THz after near-infrared femtosecond excitation, both at the charge-neutral point and for higher electrostatic-doping levels. Modeling of the THz response provides insight into changes of the carrier spectral weights and scattering rates, and reveals an additional broad-frequency ($$\approx$$ 8 THz) component to the photo-induced response, which we attribute to the zero-momentum mode of quantum-critical transport observed here in large-area CVD graphene.

Coslovich, G↗

DOE OSTI2025

Electrical Control of the Nuclear Spin States of Rare-Earth Adatoms

Rare-earth adatoms on surfaces have been studied for potential atomic-scale magnetic storage, quantum sensing, and quantum computing applications. Despite accumulating experimental efforts, a comprehensive description of the electronic configurations of the adatoms remains elusive. Here, we investigate two charge states and several electronic configurations, including 5d and 6s valence shells, for a Sm adatom on a MgO substrate using multiconfigurational ab initio methods, for the possibility of using the Sm nuclear spin levels as qubits. For the configurations in a neutral charge state, we find that the electronic ground state is a singlet, and thus the hyperfine interaction associated with the 147 Sm nucleus is absent, which may greatly enhance nuclear spin coherence time. The degeneracy of the nuclear levels is lifted by the nuclear quadrupole interaction. We show that the splitting of the nuclear levels can be controlled by a static electric field, and that Rabi oscillations between the nuclear levels can be induced by a time-dependent electric field. For the configurations in a singly charged state, electronic Kramers doublets are formed. The electronic configurations including an unpaired 6s orbital exhibit a strong hyperfine Stark effect due to a large Fermi contact contribution to the hyperfine interaction. In these configurations, electric-field-induced Rabi oscillations between the electronic-nuclear levels can occur at frequencies up to 3 orders of magnitude higher than those for the neutral charge state. The proposed system may be experimentally observed within scanning tunneling microscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2016

Hall2De Simulations with a First-Principles Electron Transport Model Based on the Electron Cyclotron Drift Instability

Several years of work have combined plasma measurements in a laboratory Hall thruster and r-z numerical simulations with Hall2De to isolate the spatial variation of the anomalous collision frequency needed in Ohm’s law to produce the observed thruster behavior. This numerical solution is used here to test the validity of a first-principles model of the anomalous transport in these devices before such model is implemented self-consistently in r-z fluid codes like Hall2De. The first-principles model employs quasi-linear theory and is based on the hypothesis that the Electron Cyclotron Drift Instability (ECDI) excites ion acoustic turbulence that, in turn, enhances the effective collision frequency in these devices. We find that a model of the ECDI that assumes Maxwellian velocity distributions for electrons and singly-charged, main-beam, cold ions (Ti=0.07 eV) is insufficient to explain the expected variation of the anomalous collision frequency both in the interior and exterior of the acceleration channel. When warm ions (~0.5-3 eV) are accounted for, the ECDI model in the channel interior appears more promising but fails by orders of magnitude in the near plume region due to the much higher Landau damping of the ion acoustic waves there. This implies that either (a) some process allows the ECDI instability to remain uninhibited by classical Landau damping or, (b) that a different instability (or instabilities) altogether, also insusceptible to Landau damping, is/are active in this region. A previous hypothesis, that convection of wave energy generated by the ECDI in the channel plays a significant role in the near plume, is not supported by the results of the simulations.

Mikellides, Ioannis G.↗

DOE OSTI2022

Supergravity black holes, Love numbers, and harmonic coordinates

A problem which has now come to a head in general relativity, primarily as a result of the many recent detections of gravitational waves from the coalescence of compact binaries, is that there are very few viable theories against which to “test” it. To perform realistic tests of theories of gravity, we need to be able to look beyond general relativity and evaluate the consistency of a parametrized, physically acceptable, family of black hole metric alternatives with observational data from, especially, gravitational wave detections using, for example, an agnostic Bayesian approach. In this paper we further examine properties of one class of such metrics, which in fact arise as solutions of ungauged supergravity. In particular, we examine the massless, neutral, minimally coupled scalar wave equation in a general stationary, axisymmetric background metric such as that of a charged rotating black hole, when the scalar field is either time independent or in the low-frequency, near-zone limit, with a view to calculating the Love numbers of tidal perturbations, and of obtaining harmonic coordinates for the background metric. For a four-parameter family of charged asymptotically flat rotating black hole solutions of ungauged supergravity theory known as STU black holes, which includes Kaluza-Klein black holes and the Kerr-Sen black hole as special cases, we find that all time-independent solutions, and hence the harmonic coordinates of the metrics, are identical to those of the Kerr solution. In the low-frequency limit we find the scalar fields exhibit the same SL(2,R) symmetry as holds in the case of the Kerr solution. We point out extensions of our results to a wider class of metrics, which includes solutions of Einstein-Maxwell-dilaton theory.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

pH-dependent reactivity of water at MgO(100) and MgO(111) surfaces

Facet-dependent surface charging of metal oxides in water dominates the ion transport behavior across the interface, in turn impacting many natural and industrial processes such as adsorption, the formation and stabilization of nanoparticle suspensions, corrosion, and heterogeneous catalysis. Here we investigated the pH-dependent surface chemistry of two low-index MgO single crystal surfaces, namely MgO(100) and MgO(111), using vibrational sum frequency generation (vSFG) spectroscopy. This allowed us to evaluate facet-dependent pH effects on the hydration and hydroxylation at the solid/aqueous interface and point-of-zero charge (PZC) values. The MgO system is complicated by its thermodynamic instability with respect to Mg(OH) 2 in water at ambient conditions. Here, for both hydroxylated MgO(100) and MgO(111) surfaces, the PZC is found to be around pH ∼ 12, which compares well with reported values for MgO single crystal and nanoparticle surfaces. However, structure specific differences in the molecular water hydrogen bonding network near the surface are evident at mildly acidic pH. To our knowledge, this is the first account of the PZC values for the MgO(111) single-crystal surface, an electrostatically unstable MgO termination that is prone to reconstruction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Integrated Multiport Conductive and Wireless Architecture for Electric Vehicle Charging

This paper explores the opportunity of integrating conductive and wireless electric vehicle charging architectures and presents an integrated multiport charging architecture suitable for simultaneous conductive and wireless charging of electric vehicles. The architecture successfully integrates the primary side power electronic high frequency inverter and the high frequency transformer with the wireless transmitter and receiver to achieve independent power flow at each port. Design of the integrated magnetics is discussed, and results are presented that demonstrate the decoupled power flow at each port. The proposed integrated architecture increases the utilization of the same charging infrastructure without a proportionate increase in the cost.

Mukherjee, Subho [ORNL] (ORCID:0009000672297925)↗

DOE OSTI2026

DOE EV Data Collection - Charging Data

Charging data are collected from one of three sources, each with varying levels of additional information. These sources, in approximate order from most to least additional information, are: • The electric vehicle supply equipment (charger) • Onboard the vehicle itself • From a utility submeter. Many chargers provide software that allows for the collection and reporting of charging session data. If unavailable, data may be recorded by the charging vehicle’s onboard systems. If neither of these options is available, data can be acquired from utility submeters that simply track the energy flowing to one or more chargers. Data collected directly from the electric vehicle supply equipment (EVSE) are typically the most accurate and highest frequency. However, it is not always possible to discern which exact vehicle is being charged during any one session. EVSE-side data can be identified where a single charger ID but a range of vehicle IDs are present (e.g., CH001, EV001-EV005). Data collected from the vehicle’s onboard systems usually does not provide information on which exact charger is being used. Vehicle-side data can be identified where a single Vehicle ID but a range of Charger IDs are present (e.g., EV001, CH001-CH005). Data collected from utility submeters provide no information on which specific vehicle is charging or which specific charger is in use. Submeter data can be identified where multiple Vehicle IDs and multiple Charger IDs are present, but only a single Fleet ID is present (e.g., EV001-EV005, CH001-CH005, Fleet01). The **Charge Data Daily/Session Dictionaries** contains definitions for each available parameter collected as part of an individual charging session, aggregated at either a daily or session level. The parameters available will vary between vehicles and chargers. The **Charger Attributes** table contains specific charger characteristics, coded to at least one anonymous Charger ID and linked to either a single or a range of Vehicle IDs. Vehicle ID can be used as a key between charging data and vehicle attribute tables. The **Charger Attributes Data Dictionary** contains definitions for each available parameter collected on the physical and operational characteristics of the charging hardware itself. The **Vehicle Attributes Data Dictionary** contains definitions for each available parameter associated with a vehicle’s physical and functional attributes and fleet context. The **Vehicle Attributes** table contains specific vehicle characteristics, coded to an anonymous Vehicle ID. This Vehicle ID can be used as a key between vehicle data and vehicle attribute tables, and in cases where charging data are supplied, links a vehicle with the charger(s) that supplied it power. The **Charging Data** tables contain the data from each charger’s operations, coded to at least one anonymous Charger ID and linked to either a single or a range of Vehicle IDs. Vehicle ID can be used as a key between charging data and vehicle attribute tables. Data is being uploaded quarterly through 2023 and subject to change until the conclusion of the project.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗