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At least 1,117 records · Page 62

Spectrally reconfigurable quantum emitters enabled by optimized fast modulation

The ability to shape photon emission facilitates strong photon-mediated interactions between disparate physical systems, thereby enabling applications in quantum information processing, simulation and communication. Spectral control in solid state platforms such as color centers, rare earth ions, and quantum dots is particularly attractive for realizing such applications on-chip. Here we propose the use of frequency-modulated optical transitions for spectral engineering of single photon emission. Using a scattering-matrix formalism, we find that a two-level system, when modulated faster than its optical lifetime, can be treated as a single-photon source with a widely reconfigurable photon spectrum that is amenable to standard numerical optimization techniques. To enable the experimental demonstration of this spectral control scheme, we investigate the Stark tuning properties of the silicon vacancy in silicon carbide, a color center with promise for optical quantum information processing technologies. We find that the silicon vacancy possesses excellent spectral stability and tuning characteristics, allowing us to probe its fast modulation regime, observe the theoretically-predicted two-photon correlations, and demonstrate spectral engineering. Our results suggest that frequency modulation is a powerful technique for the generation of new light states with unprecedented control over the spectral and temporal properties of single photons.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

New High-Energy & Safe Battery Technology with Extreme Fast Charging Capability for Automotive Applications (Final Technical Report)

Being able to refill a cars gas tank when low on fuel is incredibly convenient and is a lacking feature for battery elective vehicles. New High-Energy & Safe Battery Technology with Extreme Fast Charging Capability for Automotive Applications was a research project designed to help correct this lacking feature by developing automotive sized Li-ion battery cells and demonstrating their ability to charge in under 10-minutes. To address the technical challenges Microvast, a cell manufacturer, was joined by Argonne National Labs, battery technology innovator, and BMW, a renown OEM, worked together to define and validate materials and cells for this project. By projects end, Microvast had successfully built and demonstrated a 240 Wh/kg, 35 Ah pouch cell that was capable of over 800 10-minute charge, full discharge cycles. From the outset of the project the plan was to use large amp-hour cells (ie automotive relevant sizes) to ensure the project findings and outcomes were most relevant for electric vehicle applications. The manufacture of cells was done using test manufacturing lines at Microvast and BMW that closely resemble the procedures of a Li-ion battery cell factory.

25 ENERGY STORAGE↗

Nuclear electric propulsion stage requirements and description

The application of a nuclear electric propulsion (NEP) stage in the exploration of near-earth, cometary, and planetary space was discussed. The NEP stage is powered by a liquid-metal-cooled, fast spectrum thermionic reactor capable of providing 120 kWe for 20,000 hours. This power is used to drive a number of mercury ion bombardment thrusters with specific impulse in the range of 4000-5000 seconds. The NEP description, characteristics, and functional requirements are discussed. These requirements are based on a set of five coordinate missions, which are described in detail. These five missions are a representative part of a larger set of missions used as a basic for an advanced propulsion comparison study. Additionally, the NEP stage development plan and test program is outlined and a schedule presented.

Mondt, J. F.↗

Direct nuclear-pumped lasers using the He-3/n,p/H-3 reaction

A description is presented of experimental results concerning a specific class of direct nuclear-pumped lasers classified as 'volumetric nuclear lasers'. In the considered laser system a fissioning gas, He-3, is mixed with the lasing gas to form a homogeneous mixture, resulting in uniform volume excitation. In typical volumetric nuclear lasers a fast-burst reactor is used as a source of neutrons which penetrate a polyethylene moderator. Here the fast neutrons are thermalized. After thermalization, neutrons scatter into the laser cell. Nuclear reactions produce a proton of 0.56 MeV and a tritium ion of 0.19. These ions produce secondary electrons which pump the laser medium creating a population inversion. The results reported demonstrate direct nuclear pumping of He-3-Ar, Xe, Kr, and Cl with the considered system.

Deyoung, R. J.↗

Suprathermal plasma observed on STS-3 Mission by plasma diagnostics package

Artificially produced electron beams were used extensively during the past decade as a means of probing the magnetosphere, and more recently as a means of actively controlling spacecraft potential. Experimentation in these areas has proven valuable, yet at times confusing, due to the interaction of the electron beam with the ambient plasma. The OSS-1/STS-3 Mission in March 1982 provided a unique opportunity to study beam-plasma interactions at an altitude of 240 km. On board for this mission was a Fast Pulse Electron Generator (FPEG). Measurements made by the Plasma Diagnostics Package (PDP) while extended on the Orbiter RMS show modifications of the ion and electron energy distributions during electron beam injection. Observations made by charged particle detectors are discussed and related to measurements of Orbiter potential. Several of the PDP instruments, the joint PDP/FPEG experiment, and observations made during electron beam injection are described.

Paterson, W.↗

Forcing of the Coupled Ionosphere-Thermosphere (IT) System During Magnetic Storms

Poynting flux shows peaks around auroral zone AND inside polar cap. Energy enters IT system at all local times in polar cap. Track-integrated flux at DMSP often peaks at polar latitudes- probably due to increased area of polar cap during storm main phases. center dot lon temperatures at DMSP show large increases in polar region at all local times; cusp and auroral zones do not show distinctively high Ti. center dot I on temperatures in the polar cap are higher than in the auroral zones during quiet times. center dot Neutral densities at GRACE and GOCE show maxima at polar latitudes without clear auroral signatures. Response is fast, minutes from onset to density peaks. center dot GUVI observations of O/N2 ratio during storms show similar response as direct measurements of ion and neutral densities, i.e. high temperatures in polar cap during prestorm quiet period, heating proceeding from polar cap to lower latitudes during storm main phase. center dot Discrepancy between maps of Poynting flux and of ion temperatures/neutral densities suggests that connection between Poynting flux and Joule heating is not simple.

Magnetic Storms↗

Multivariate prognosis of battery advanced state of health via transformers

De-risking energy storage investments necessary to meet CO 2 reduction targets requires a deep understanding of the connections between battery health, design, and use. The historical definition of the battery state of health (SOH) as the percentage of current versus initial capacity is inadequate for this purpose, motivating an expanded SOH consisting of an interrelated set of descriptors including capacity, energy, ionic and electronic impedances, open-circuit voltages, and microstructure metrics. In this work, we introduce deep transformer networks for the simultaneous prognosis of 28 battery SOH descriptors using two cycling datasets representing six lithium-ion cathode chemistries, multiple electrolyte/anode compositions, and different charge-discharge scenarios. The accuracy of these predictions for battery life (with an unprecedented mean absolute error of 19 cycles in predicting end of life for a lithium-iron-phosphate fast-charging dataset) illustrates the promise of deep learning toward providing enhanced understanding and control of battery health.

25 ENERGY STORAGE↗

Structural effects of composition tuning in A-site disordered perovskite La0.5Li0.5−xMxTiO3 (M = Na, K) nanorods for fast interfacial transport for solid composite electrolyte design

Polymer-ceramic composite electrolytes (CPE) have emerged as promising replacements for currently used liquid organic electrolytes, which pose as safety hazards, in Li-ion batteries. Limits in conductivity enhancement in CPEs is often attributed to a high resistance for Li-ion transport along the interface due to the incompatibility of the polymer and ceramic phases. A clear understanding of the interfacial structure and how this impacts interfacial Li-ion transport is needed in order to efficiently design a CPE with optimal ionic conductivity. In this study, density functional theory (DFT) calculations, in conjunction with scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS), are used to unveil the bulk and surface structure of La0.5Li0.5−xMxTiO3 (M = Na, K) (LMTO) nanorods, a newly-reported ceramic system with promising applications in CPEs, and the LMTO interactions with the poly(lithium sulfonyl (trifluoromethane sulfonyl)imide methacrylate) (p(MTFSILi)) polymerized ionic liquid. Substitution of lithium for sodium and potassium onto the A-site perovskite lattice is shown to increase the stability of the preferred pseudocubic perovskite phase because of their increased cation size which allows them to reduce the TiO6 octahedral rotations in the bulk and at the surface. STEM and EELS results show that LMTO nanorods with differing compositions have Ti-enriched (110)-oriented surfaces. Increased sodium and potassium compositions in LMTO is also shown using the DFT calculations to weaken the binding of the lithium atom to the MTFSI unit when LiMTFSI is adsorbed to the LMTO surface. This weakening of lithium binding to the polymer at the LMTO interface indicates that the lithium mobility is increased, correlating to an increase in interfacial Li-ion transport. Overall, this work provides insights into how to tune the interfacial interactions between the polymer (p(MTFSI)) and ceramic (LMTO) for optimal CPE design.

Shepard, Lauren B [Pennsylvania State University, ↗

Compact high repetition rate Thomson parabola ion spectrometer

Here, we present the development of a compact Thomson parabola ion spectrometer capable of characterizing the energy spectra of various ion species of multi-MeV ion beams from >10 20 W/cm 2 laser produced plasmas at rates commensurate with the highest available from any of the current and near-future PW-class laser facilities. This diagnostic makes use of a polyvinyl toluene based fast plastic scintillator (EJ-260), and the emitted light is collected using an optical imaging system coupled to a thermoelectrically cooled scientific complementary metal–oxide–semiconductor camera. This offers a robust solution for data acquisition at a high repetition rate, while avoiding the added complications and nonlinearities of micro-channel plate based systems. Different ion energy ranges can be probed using a modular magnet setup, a variable electric field, and a varying drift-distance. We have demonstrated operation and data collection with this system at up to 0.2 Hz from plasmas created by irradiating a solid target, limited only by the targeting system. With the appropriate software, on-the-fly ion spectral analysis will be possible, enabling real-time experimental control at multi-Hz repetition rates.

47 OTHER INSTRUMENTATION↗

Observation of shock-front separation in multi-ion-species collisional plasma shocks

We observe shock-front separation and species-dependent shock widths in multi-ion-species collisional plasma shocks, which are produced by obliquely merging plasma jets of a He/Ar mixture (97% He and 3% Ar by initial number density) on the plasma liner experiment. Visible plasma emission near the He-I 587.6-nm and Ar-II 476.5–514.5-nm lines is simultaneously recorded by splitting a single visible image of the shock into two different fast-framing cameras with different narrow bandpass filters (589 ± 5 nm for observing the He-I line and 500 ± 25 nm for the Ar-II lines). For conditions in these experiments (pre-shock ion and electron densities ≈5×10 14 cm –3 , ion and electron temperatures of ≈2.2 eV, and relative plasma-merging speed of 22 km/s), the observationally inferred magnitude of He/Ar shock-front separation and the shock widths themselves are <1 cm, which correspond to ~50 post-shock thermal ion–ion mean free paths. These experimental length scales are in reasonable qualitative and quantitative agreement with results from 1D multi-fluid simulations using the CHICAGO code. However, we note there are differences between the experimentally inferred and simulation-predicted ionization states and line emission intensities, particularly in the post-shock region. Overall, the experimental and simulation results are consistent with theoretical predictions that the lighter He ions diffuse farther ahead within the overall shock front than the heavier Ar ions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Ion temperature profiles in the horns of the plasma sheet

The plasma sheet horns are the low-altitude extensions of the plasma sheet that lie poleward of the plasmasphere and equatorward of the tail lobes. Within the horns, magnetic field lines of increasing geomagnetic latitudes map to increasing distances into the downtail plasma sheet. Plasma data from the fast plasma experiment on ISEE 2 have been analyzed for 11 outbound crossings of the horns in the premidnight sector of the magnetosphere at typical altitudes of 2-4 R(E). These crossings typically occurred on time scales of less than 1 hour, providing almost instantaneous snapshots of plasma gradients within the horns. Ion temperatures observed during these crossings generally decreased by a factor of four to eight as magnetic field lines of increasing geomagnetic latitude were traversed. If we make the reasonable assumption that the ion temperatures are constant along the field lines within the plasma sheet, then this result implies that the ion temperatures in the downtail plasma sheet also commonly decrease by this same factor over the radial range extending from the inner edge of the plasma sheet at the plasmapause boundary to the outer edge at a neutral line in the distant tail.

Suszcynsky, D. M.↗

On the injection and scattering of protons in Jupiter's magnetosphere

The interaction, scattering, and acceleration of Jovian ions through magnetohydrodynamic waves are investigated. A model of the Alfven speed in the plasma sheet for both inbound and outbound legs of the Voyager 1 encounter is presented, and underlying assumptions are discussed. Theoretical ingredients of a rotationally driven Jovian substorm are defined, and the convective growth rate of the fast wave for both a warm and a cold beam is derived. The mean-free path for scattering based on in situ measurements of magnetic fluctuations in the plasma sheet is estimated, and the results indicate that scattering of super-Alfvenic ions occurs on a regular basis throughout the plasma sheet, and the observed level of magnetic fluctuations is sufficiently high to stop ionospheric protons.

Barbosa, D. D.↗

Mechanically and Thermally Robust Gel Electrolytes Built from A Charged Double Helical Polymer

Polymer electrolytes have received tremendous interest in the development of solid-state batteries, but often fall short in one or more key properties required for practical applications. Herein, a rigid gel polymer electrolyte prepared by immobilizing a liquid mixture of a lithium salt and poly(ethylene glycol) dimethyl ether with only 8 wt% poly(2,2′-disulfonyl-4,4′-benzidine terephthalamide) (PBDT) is reported. The high charge density and rigid double helical structure of PBDT lead to formation of a nanofibrillar structure that endows this electrolyte with stronger mechanical properties, wider temperature window, and higher battery rate capability compared to all other poly(ethylene oxide) (PEO)-based electrolytes. The ion transport mechanism in this rigid polymer electrolyte is systematically studied using multiple complementary techniques. Li/LiFePO 4 cells show excellent capacity retention over long-term cycling, with thermal cycling reversibility between ambient temperature and elevated temperatures, demonstrating compelling potential for solid-state batteries targeting fast charging at high temperatures and slower discharging at ambient temperature.

36 MATERIALS SCIENCE↗

Accelerated Degradation in a Quasi-Single-Crystalline Layered Oxide Cathode for Lithium-Ion Batteries Caused by Residual Grain Boundaries

The rapidly growing demand of electrical vehicle (EV) requires high-energy-density lithium-ion batteries (LIBs) with excellent cycling stability and safety performance. However, conventional polycrystalline high-Ni cathodes severely suffer from intrinsic chemo-mechanical degradation and fast capacity fade. The emerging single-crystallization strategy offers a promising pathway to improve the chemo-mechanical stability, however, the single-crystallinity of the cathode is not always guaranteed and residual grain boundaries (GBs) could persist in nonideal synthesis conditions, leading to the formation of ‘quasi’ single-crystalline (QSC) cathodes. So far, there is a lack of understanding of the influence of these residual GBs on the electrochemical performance and structural stability. Herein, we investigate the degradation pathway of a QSC high-Ni cathode through transmission electron microscopy and X-ray techniques. The residual GBs caused by insufficient calcination time, dramatically exacerbate the cathode’s chemo-mechanical instability and cycling performance. Our work offers important guidance for the next-generation cathodes for long-life LIBs.

25 ENERGY STORAGE↗

Cost Analysis and Projections for U.S.-Manufactured Automotive Lithium-ion Batteries

This document reports on a study conducted to estimate the cost of U.S-produced automotive battery packs for model years (MY) 2023 to 2035, using Argonne National Laboratory’s BatPaC tool. The costs were estimated by designing batteries for several classes of vehicles for four discrete model years (2023, 2026, 2030, and 2035), where a representative battery technology and material prices are selected based on information available today. Correlations were developed from the four discrete years to enable annual pack cost estimates as a function of pack size (kWh) and model year. A consolidated cost curve was then developed that includes battery size, technology by model year, and the anticipated sales volumes of each class of vehicles over the years. This cost curve estimates the volume-averaged, U.S.-manufactured battery pack cost of PHEVs and BEVs in the United States to be $\$140$/kWh for the model year 2023, which will reduce to $\$86$/kWh in MY2035. Applying tax credits from section 45X of the Inflation Reduction Act can further reduce the average pack cost to as low as $\$56$/kWh in MY2029. The report also includes several sensitivity studies that investigate the effect of pack production volume, material prices, fast charge requirements, and labor rates.

25 ENERGY STORAGE↗

Model ion abundances for Comet Halley

A computer model for comet comae was applied to predict ion abundances for comet Halley, assuming that the volatile component of the nucleus is 85% water and that the remaining volatile molecules are composed of carbon, nitrogen, oxygen, and sulfur. Model parameters such as heliocentric distance, size, and albedo are chosen to be consistent with the 13 to 14 March 1986 encounter of Giotto with the comet. Photoprocesses, gas-phase chemical kinetics, coma energy balance including a separate electron temperature, multifluid hydrodynamics with a transition to free molecular flow, fast streaming atomic and molecular hydrogen, and counter and cross streaming of species in the coma-solar wind interaction are taken into consideration. A comparison of the model results with data from the ion mass spectrometer at 6000 and 1500 km from the nucleus shows good agreement. Implications of the coma physics and chemistry are discussed.

Huebner, W. F.↗

Spin-exchange carrier multiplication in manganese-doped colloidal quantum dots

Abstract Carrier multiplication is a process whereby a kinetic energy of a carrier relaxes via generation of additional electron–hole pairs (excitons). This effect has been extensively studied in the context of advanced photoconversion as it could boost the yield of generated excitons. Carrier multiplication is driven by carrier–carrier interactions that lead to excitation of a valence-band electron to the conduction band. Normally, the rate of phonon-assisted relaxation exceeds that of Coulombic collisions, which limits the carrier multiplication yield. Here we show that this limitation can be overcome by exploiting not ‘direct’ but ‘spin-exchange’ Coulomb interactions in manganese-doped core/shell PbSe/CdSe quantum dots. In these structures, carrier multiplication occurs via two spin-exchange steps. First, an exciton generated in the CdSe shell is rapidly transferred to a Mn dopant. Then, the excited Mn ion undergoes spin-flip relaxation via a spin-conserving pathway, which creates two excitons in the PbSe core. Due to the extremely fast, subpicosecond timescales of spin-exchange interactions, the Mn-doped quantum dots exhibit an up-to-threefold enhancement of the multiexciton yield versus the undoped samples, which points towards the considerable potential of spin-exchange carrier multiplication in advanced photoconversion.

36 MATERIALS SCIENCE↗