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At least 19 records

Chemical Interface Damping Revealed by Single-Particle Absorption Spectroscopy

Plasmon-induced interfacial charge separation is a promising way to efficiently extract energetic carriers through direct plasmon decay. This mechanism of charge transfer has been investigated by single-particle scattering spectroscopy, which measures the homogeneous plasmon line width. The line width is broadened by charge transfer, generally known as chemical interface damping. However, conflicting reports exist regarding the effect of chemical interface damping on the corresponding single-particle absorption spectrum, which is needed to accurately determine absolute light conversion efficiencies. This work aims to resolve this question by directly correlating absorption and scattering spectra of individual gold nanorods in the presence and absence of a charge-accepting interface. We find that for TiO 2 coated nanorods, the absorption line width is indeed broadened due to chemical interface damping but is overall narrower than the scattering line width. Here, chemical interface damping is furthermore found to increase with larger resonance energies. The observed differences in line widths between absorption and scattering are elucidated within the context of an analytically tractable model describing the lowest energy optically bright and higher-order optically dark plasmon modes of the nanorod, including bulk, radiative, and chemical interface damping effects. Taken together, these results establish that single-particle absorption spectroscopy is capable of revealing interfacial charge injection by direct plasmon decay.

absorption

Studies of localized mix and asymmetry caused by the stalk in inertial fusion experiments at OMEGA

In an inertially confined fusion experiment, a capsule of fusion fuel is compressed to high temperatures and densities using lasers, creating a hot plasma in which thermonuclear fusion reactions take place. To achieve efficient conversion of laser energy to fuel heating, the implosion must be as spherically symmetric as possible. One common source of asymmetry that degrades performance is the stalk and glue spot that hold the capsule in place before the experiment. The exact nature and magnitude of this perturbation had not been previously quantified. In this work, inertially confined fusion experiments were executed with an additional stalk on the capsule to measure and quantify the effect of the stalk and glue spot on the symmetry and performance. It is found that the stalk drives low-mode asymmetry by shadowing the laser drive on the part of the shell near the glue spot, enhancing the hot-spot velocity toward the stalk by 40–80 km/s and elongating the hot-spot along the stalk axis. It is also found that localized mix due to the additional stalk has a negligible effect on implosion performance. Two-dimensional radiation-hydrodynamic simulations using the xRAGE code reproduce the direction of the experimentally observed change to hot-spot velocity and implosion performance metrics, but not the observed elongation, suggesting that this feature results from an interaction between stalk perturbations and other preexisting asymmetry seeds, such as laser drive asymmetry.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY

Measurement of Local Electric Field Turbulence in Magnetically Confined Plasmas (Final Report)

This final report describes the development of high-bandwidth plasma fluctuation diagnostics, encompassing the design and implementation of Beam Emission Spectroscopy systems on several fusion experiments such as TFTR, DIII-D and NSTX, the advancement of Alpha particle and Ultrafast Charge-Exchange Recombination Spectroscopy, and the creation of advanced spectrometers for localized studies of electric and magnetic field fluctuations based on the Motional Stark Effect.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY

Energy resolution and gain measurements in Argon-based gas mixtures: Exploring Ar:CF 4 for low energy measurements with TPCs

Time Projection Chambers (TPCs) are among the most advanced charged-particle detectors. Gas-filled TPCs have tracking capabilities that provide 3D-imaging of charged particles with a good energy resolution for spectroscopy. Different gas mixtures have different properties that determine the energy resolution as well as the spatial resolution. Therefore, optimization of operating conditions is required to simultaneously obtain adequate gain, energy resolution, spatial/track resolution, as well as higher drift velocities for high counting rates applications. Ar:CF 4 gas mixture has higher electron drift velocities and lower electron diffusion, which makes it an attractive candidate for TPC filling gas for low energy nuclear physics applications as compared to commonly used Ar:CH 4 and Ar:CO 2 gas mixtures, namely when tracking information is needed. However, other properties, including energy resolution and gain, remain largely unexplored in Ar:CF 4 especially at pressures and other operating conditions relevant for low-energy nuclear physics applications. Here, in this paper we report on gain and energy resolution measurements, using Gas Electron Multipliers (GEMs), in the less explored Ar:CF 4 mixture (Alfonsi et al., 2006), as well as in the more commonly used gas mixtures Ar:CH 4 and Ar:CO 2 . In addition to obtaining energy resolution and gain, we provide results from Garfield++ simulations for gain fluctuations, and their impact on energy resolution is discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

Unravelling fast-charging degradation in NMC/Gr pouch cells: Lithium plating and SEI properties

As fast-charging technology expands across the electric vehicle and emerging energy-storage applications, understanding its impact on battery performance and longevity is critical. In this study, 1.8 Ah LiNi 0.6 Mn 0.2 Co 0.2 O 2 /graphite pouch cells were charged at various charging rates (0.5C, 2C, 4C, and 6C) to investigate the degradation mechanisms. Our results showed that well-designed NMC/Gr pouch cells could reach over 1000 cycles with a 2C charging rate, while only reaching around 500 cycles with 4C and 6C charging rates. Fast-charging effects on NMC and graphite electrodes were obtained through a series of post-mortem characterizations, including electrochemical impedance spectroscopy (EIS), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM) with energy-dispersive X-ray spectroscopy (EDS). Although higher charging rates cause pulverization of NMC secondary particles, the dominant degradation mechanism driving the fading of fast-charging-related performance lies in the graphite anode, where lithium plating and LiF-rich solid electrolyte interphase (SEI) formation result in Li inventory loss and impedance growth. The postmortem results suggest that the formation of a LiF-rich SEI, which exacerbates anode impedance and some irreversible Li + ion loss, is likely driven by the substantial decomposition of PF 6 − during fast charging, an effect often overlooked in smaller laboratory-scale studies.

Luo, Mei [Argonne National Laboratory (ANL), Argon

CHICOX, a heavy-ion detection system for GRETA

The CHICOX detection system is an array of position sensitive parallel plate avalanche counters used for heavy ion detection in in-beam particle-gamma coincidence experiments. CHICOX, an upgrade of the CHICO2 array, is geometrically compatible with the GRETINA and GRETA gamma-ray arrays and provides an angular resolution sufficient to utilize the excellent position resolution of GRETINA/GRETA. CHICOX was successfully commissioned and fielded as an auxiliary detector to GRETINA in a campaign of stable-beam Coulomb excitation experiments at the ATLAS facility of Argonne National Laboratory. We report here on the design and in-beam performance of the CHICOX array.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

Assessment of errors in analytic modeling of permanent magnet electron spectrometers for laser-plasma accelerators

Here, we assess the error in three treatments of a critical electron beam diagnostic for laser-plasma acceleration (LPA) experiments: a permanent magnet electron spectrometer. Since LPA electron spectrometers are often difficult to calibrate due to the scarcity of well-characterized, tunable electron beam sources in the appropriate energy range and the mechanical complexity of electron spectrometers, the standard of calibration is Hall probe measurements. We first compare the electron spectrometer performance between SIMION calculations and the Hall probe measurements. We find up to a 60% (<8%) error in determining the absolute energy for electrons below (above) 80 MeV when using the SIMION-modeled magnetic field vs the measured magnetic field due to SIMION overpredicting fringe field strength. The difference in spectrometer energy resolution is within ∼10% between the modeled and measured fields. We then assess a simple block model, which is commonly used. We find that the simple block model presented here sufficiently captures the predicted as-built spectrometer performance for any application provided that the user can tolerate uncertainties on absolute energy determination up to 5% and errors on energy resolution up to 1%.

Electromagnetic optics

Antenna arrays for neutrino mass measurements with cyclotron radiation emission spectroscopy

Cyclotron Radiation Emission Spectroscopy (CRES) is a technique for precision measurements of kinetic energies of charged particles, pioneered by the Project 8 experiment to measure the neutrino mass using the tritium end-point method. It was recently employed for the first time to measure the molecular tritium spectrum and place a limit on the neutrino mass using a cubic-centimeter-scale detector. Future direct neutrino mass experiments are developing the technique to overcome the systematic and statistical limitations of current detectors. Here, this paper describes one such approach, namely the use of antenna arrays for CRES in free space. Phenomenology, detector design, simulation, and performance estimates are discussed, culminating with an example design with a projected sensitivity of 𝑚 𝛽 < ⁢0.04 eV/𝑐 2 . Prototype antenna array measurements are also shown for a demonstrator-scale setup as a benchmark for the simulation. By consolidating these results, this paper serves as a comprehensive reference for the development and performance of antenna arrays for CRES.

Physics - Nuclear physics and radiation physics

Polaron Delocalization and Transport in Doped Graphene Nanoribbon Thin Films

Graphene nanoribbons (GNRs) are quantum-confined π-conjugated monolayer semiconductors with attractive properties for optoelectronic applications. However, the ground- and excited-state properties of charge carriers in GNRs are still poorly understood, particularly with regards to the coupling between charges and the GNR lattice and the degree to which this coupling impacts local and macroscopic charge transport. To address this issue, we systematically correlate carrier density-dependent charge transport with spectroscopic modulations in chemically doped thin films of armchair graphene nanoribbons (9-aGNRs). This study combines Fourier transform infrared (FTIR) and ultraviolet−visible−near-infrared (UV−vis−NIR) spectroscopy with both local and macroscopic conductivity measurements to arrive at a full and self-consistent picture of transport in doped GNR thin films. Using three different molecular p-type dopants (i.e., oxidants), we demonstrate that hole polarons are the dominant quasi-particle determining charge transport in GNRs and that the degree of polaron delocalization depends sensitively on the dopant and the hole density. For all three dopants, the local conductivity probed by microwave spectroscopy substantially exceeds the long-range conductivity obtained by four-point probe measurements. Interestingly, the dopant size substantially influences charge transport at high hole densities. We ascribe this effect to different propensities for forming bipolarons with lower mobilities than polarons. Comparison of GNR transport and spectral properties to other prototypical π-conjugated semiconductors (e.g., semiconducting polymers or carbon nanotubes) benchmark the charge transport properties of GNR thin films for optoelectronic devices and applications.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Rapid spatial analysis of surrogate TRISO fuel particles using laser-induced breakdown spectroscopy image analysis

Laser-induced breakdown spectroscopy (LIBS) mapping enables rapid elemental and spatial analysis of solid samples. In this work, surrogate TRi-structural ISOtropic (TRISO) particles with various layers consisting of Zr, W, C, and Si were used to demonstrate the use of a new thickness measurement tool developed to analyze elemental images generated from LIBS maps. Zr particles with varying outer-layer thicknesses ranging from 16 to 32 μm were measured with scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS) and LIBS with both a complementary metal-oxide-semiconductor (CMOS) detector and an intensified charged coupled device (ICCD) detector. LIBS maps of particles were completed using CMOS and ICCD spectrometers with effective spatial resolutions of 4 and 2 μm, respectively. The novel thickness measurement tool identified layer regions within a LIBS map and then identified the locations of the boundaries between these layers. The tool then generated up to 1000 random profiles stemming radially from the center region, which were used to measure the layer thickness/radius. This image analysis tool demonstrated LIBS's ability to provide values comparable with SEM-EDS (3.7% relative difference) along with a 95% reduction in measurement time. Furthermore, the precision of these measurements was on par with the SEM-EDS measurements at <15% relative standard deviation. Following the analysis of the Zr particles, W particles with increased complexity (e.g., five versus three layers) were analyzed using both the CMOS and ICCD spectrometers simultaneously. The spatial dimensions were extracted with an average relative difference of 2.7% and an average relative standard deviation of 9%.

Andrews, Hunter B. [Oak Ridge National Laboratory

Characterization of core neutrals using passive measurements of the D α spectrum near the X -point in the DIII-D tokamak

New spectroscopic measurements of deuterium Balmer-α emission are used to infer the spatial distribution of neutral particles near the X-point in a diverted high confinement mode plasma. The charge exchange neutral spectroscopy (CENS) diagnostic—recently installed on the DIII-D tokamak—uses 15 lines of sight extending from the edge of the confined region (ρ ≈ 0.7) to the X-point in lower single-null plasmas. Each CENS line of sight is spectrally resolved around the deuterium Balmer-α wavelength (6561 Å) to measure the Doppler shift, line broadening, and intensity of Dα emission. Thermal line broadening is used to identify emission from neutrals undergoing charge-exchange (CX) with high temperature ions in the confined plasma. This spectral information allows a more accurate determination of the neutral density deeper inside the confined plasma compared to traditional filter-based diagnostics. We present two methods of analyzing CENS measurements: (1) fitting the spectrum from each view-chord separately, and (2) a tomographic method for inverting the neutral density over a 2D region of space using all CENS views collectively. The neutral density profile is found to decay exponentially in the radial direction with two scale-lengths. In the pedestal region the neutral density decays at a rate approximately equal to the local mean-free-path for CX collisions, $L_{n_\mathrm{D0}}\approx \lambda_\text{CX}$. Further inside the plasma the neutral density decays at a rate equal to the mean-free-path for ionization, $L_{n_\mathrm{D0}}\approx \lambda_\text{inz.}$. The separatrix $n_\mathrm{D0}$ value is found to be approximately $2\times10^{15}$ m−3. Based on results from the 2D inversion, the density of neutrals is found to increase along the separatrix approaching the X-point by a factor of $\approx 5\times$ over the region covered by the CENS diagnostic.

X-point neutrals

Depth-Dependent Emission from Silver Dopants in Single CdSe Nanoplatelets

Dopants in semiconductor nanostructures offer tremendous control over electronic, optical, and magnetic properties beyond what is achievable in bulk materials. We demonstrate that the broad dopant emission in semiconductor nanoplatelets effectively maps the electron wave function across the nanoplatelet thickness. Both the emission energy and lifetime of the dopant transition depend strongly on the depth of the dopant within the nanoplatelet. This dependence arises from the electrostatic self-interaction of the charged dopant, which varies with proximity to the dielectric discontinuity at the nanoplatelet surface. Through comprehensive single-particle spectroscopy of silver-doped CdSe nanoplatelets, we verify that acceptors near the center emit at higher energies with shorter lifetimes, while those near the surface emit at lower energies with longer lifetimes. This spatial mapping also reveals unusual two-color emission from individual nanoplatelets, with enhanced Auger recombination yielding exceptional photon antibunching (>90% purity) at room temperature, suggesting potential applications in quantum information technologies.

cadmium selenide

Coupling of TIGRESS and EMMA with Auxiliary Array TIP at TRIUMF

The combination of a germanium detector array and recoil mass spectrometer allows for high-sensitivity experiments in nuclear structure and astrophysics by enabling high-energy-resolution -ray spectroscopy and reaction measurements of weak fusion-evaporation, transfer or radiative-capture reactions in the presence of dominant background reaction channels. The TIGRESS -ray spectrometer with an upgraded data acquisition system has been coupled with the EMMA mass spectrometer alongside a suite of auxiliary detectors housed within TIGRESS such as TIP. This paper reviews the unique combination of radioactive beams at TRIUMF with the capabilities of TIGRESS and EMMA in the context of fusion-evaporation with TIP and radiative-capture reactions without an auxiliary array.

A/Q identification

Signatures of fractional charges via anyon–trions in twisted MoTe 2

Fractionalization of the electron charge e is one of the most striking phenomena arising from strong electron–electron interactions. A celebrated example is the emergence of anyons with fractional charges in fractional quantum Hall effect (FQHE) states. Recently, zero-field fractional Chern insulators (FCIs), lattice analogues of the FQHE states that form without Landau levels, have been realized. FCIs provide a unique platform to investigate anyons, yet their detection remains a challenge. Here we report the observation of anyon–trions, a new type of excitonic complex formed by binding a trion with a fractional charge in twisted MoTe 2 bilayers. Photoluminescence spectroscopy of quantum-confined excitons reveals emergent peaks that appear only within slightly doped FCI states. The new spectral features are red-shifted relative to the trions in undoped FCIs, but share the same electric field, temperature and magnetic field dependence. These observations suggest their origin as trions binding with elementary quasi-particles, that is, anyon–trions. Crucially, the ratio of binding energies between the anyon–trions in the −2/3 and −3/5 FCI states matches the expected fractional charge ratio of e/3 to e/5. This provides strong evidence for fractional charges in FCI—an essential property of anyons. Our results address a fundamental question in FCI physics and establish trion spectroscopy as a powerful probe of fractionally charged excitations, complementary to transport- and tunnelling-based approaches.

Quantum Hall

Identification of Prompt Proton Emission in $N = Z - 1$ 61 Ga: Isospin Symmetry at the Limit of Nuclear Binding

Excited states in the proton drip line nucleus 61 Ga were populated via the fusion-evaporation reaction 24 Mg ⁢( 40 Ca, 𝑝⁢2⁢𝑛)⁢ 61 Ga. The experimental setup at Argonne National Laboratory comprised a novel combination of the Gammasphere array with two CD-shaped double-sided Si-strip detectors inside the Microball CsI(Tl) charged-particle detection array, as well as the Neutron-Shell liquid scintillators and the Fragment Mass Analyzer. Owing to the setup’s unprecedented in-beam proton spectroscopy and tracking capabilities, a coincidence between a 957.6(5)-keV 𝛾 ray and a 1.876(24)-MeV proton line was observed, which identifies the quasibound proton 𝜋⁢𝑔 9/2 single-particle state in 61 Ga at 𝐸 𝑥 = 2150⁢(34) keV. This probes isospin symmetry at the limit of nuclear binding by providing a unique challenge for the shell-model interpretation of mirror nuclei beyond doubly magic 56 Ni .

Hrabar, Yuliia [Lund Univ. (Sweden)] (ORCID:000000

Passivation‐Induced Species Dynamics and Microstructural Evolution in Solid‐State Lithium–Sulfur Cathodes

Solid-state lithium–sulfur (SSLS) batteries offer high theoretical energy density, yet their practical viability is hindered by poor sulfur utilization and limited rechargeability. At the core of this challenge lies the passivating nature of Li 2 S, which restricts ionic and electronic transport, suppresses interfacial activity, and severely impedes the reversibility of electrochemical reactions. In this study, we elucidate the mechanistic origins of these limitations by resolving how charge and discharge species form, grow, and spatially evolve within the cathode microstructure under varied current densities and electrode compositions. By resolving the species distribution at the particle scale and coupling it with Raman spectroscopy and X-ray diffraction, we demonstrate how Li 2 S formation induces localized surface passivation that progressively limits electrochemical accessibility within the cathode microstructure. Sulfur utilization is found to be strongly governed by the interplay between sulfur loading, residual porosity, and interfacial architecture. High sulfur contents result in buried, electrochemically isolated domains due to poor solid electrolyte (SE) percolation, while low sulfur contents trigger SE degradation via parasitic reactions. The resulting sulfur-porosity maps delineate the mechanistic boundaries between reversible and transport-limited regimes, offering actionable design guidance for SSLS cathodes with enhanced sulfur utilization.

electrode microstructure

Exploring Atomic-Scale Interactions at the Interface of Reducible Oxide and Ruthenium Nanocatalyst for Ammonia Decomposition

Restructuring atomic-scale interfaces between noble metal nanoparticles and metal oxides provides a promising approach to enhancing catalytic properties. In this study, Ru nanoparticles were supported on CeO 2 , ZrO 2 , and HfO 2 via pyrolysis of MOFs under oxygen-suppressed high-temperature conditions. Despite its nearly ideal particle size (∼2.3 nm), the Ru–CeO 2 /C catalyst exhibited the lowest ammonia decomposition activity. X-ray absorption spectroscopy and DFT calculations revealed that electron transfer from Ru to CeO 2 formed positively charged Ru and partially reduced Ce 4+ , weakening the catalytic performance. In contrast, oxygen-deficient ZrO 2 and HfO 2 support donated electrons to Ru, preserving its metallic state. These findings demonstrate that the reducibility of oxide supports governs the direction and magnitude of interfacial charge transfer, directly tuning catalytic behavior. This study provides insights into the design of oxide-supported Ru catalysts for ammonia decomposition.

Catalysts

Single-Particle Insights Into the Electronic Structure and Enhanced Stability of CsPbBr 3 /FAPbBr 3 Core/Crown Nanoplatelets at the Nanometer Scale

Colloidal perovskite nanoplatelets (NPLs), despite their exceptional optoelectronic properties, face significant challenges due to their intrinsic instability and trap-assisted non-radiative recombination. Although many studies employing surface engineering, such as selecting ligands or coating to passivate defects, have demonstrated improved optoelectronic properties, these enhancements are typically inferred from bulk-ensemble measurements; the effects at the single-particle level remain elusive. Here, we conduct single-particle-level studies using scanning tunneling spectroscopy (STS) on a unique core–crown system, CsPbBr 3 @FAPbBr 3 NPLs, where the lateral surfaces of the CsPbBr 3 core are coated with an FAPbBr 3 crown. Experimental density-of-states (DOS) analysis reveals a 47% reduction in deep-trap states in core-crown NPLs compared to core-only NPLs, consistent with nearly two-fold enhancements in photoluminescence quantum yields. Progressive I–V sweep measurements demonstrate superior electrical stability in core-crown NPLs, preserving band structure with minimal degradation, while core-only NPLs exhibit rapid bandgap shrinkage and trap formation. Density functional theory (DFT) calculations indicate that FA incorporation distorts Pb octahedral lattice, widening the bandgap. This study elucidates how surface engineering modulates charge localization, passivates defects, and enhances stability at the single-particle level. Moreover, by uncovering bias-induced trap states in single unpassivated NPLs, this study establishes a precise, robust approach for characterizing emerging perovskite nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY