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At least 1,099 records · Page 61

Optical contrast analysis of α -RuCl 3 nanoflakes on oxidized silicon wafers

α-RuCl 3 , a narrow-band Mott insulator with a large work function, offers intriguing potential as a quantum material or as a charge acceptor for electrical contacts in van der Waals devices. In this work, we perform a systematic study of the optical reflection contrast of α-RuCl 3 nanoflakes on oxidized silicon wafers and estimate the accuracy of this imaging technique to assess the crystal thickness. Via spectroscopic micro-ellipsometry measurements, we characterize the wavelength-dependent complex refractive index of α-RuCl 3 nanoflakes of varying thickness in the visible and near-infrared. Building on these results, we simulate the optical contrast of α-RuCl 3 nanoflakes with thicknesses below 100 nm on SiO 2 /Si substrates under different illumination conditions. We compare the simulated optical contrast with experimental values extracted from optical microscopy images and obtain good agreement. Finally, we show that optical contrast imaging allows us to retrieve the thickness of the RuCl 3 nanoflakes exfoliated on an oxidized silicon substrate with a mean deviation of –0.2 nm for thicknesses below 100 nm with a standard deviation of only 1 nm. Our results demonstrate that optical contrast can be used as a non-invasive, fast, and reliable technique to estimate the α-RuCl 3 thickness.

2D materials↗

Gain characterization of LGAD sensors with beta particles and 28-MeV protons

Low Gain Avalanche Diodes, also known as LGADs, are widely considered for fast-timing applications in high energy physics, nuclear physics, space science, medical imaging, and precision measurements of rare processes. Such devices are silicon-based and feature an intrinsic gain due to a p + -doped layer that allows the production of a controlled avalanche of carriers, with multiplication on the order of 10–100. This technology can provide time resolution on the order of 20–30 ps, and variants of this technology can provide precision tracking too. The characterization of LGAD performance has so far primarily been focused on the interaction of minimum ionizing particles for high energy and nuclear physics applications. This article expands the study of LGAD performance to highly-ionizing particles, such as 28-MeV protons, which are relevant for several future scientific applications, e.g. in biology and medical physics, among others. These studies were performed with a beam of 28-MeV protons from a tandem Van de Graaff accelerator at Brookhaven National Laboratory and beta particles from a ^90Sr source; these were used to characterize the response and the gain of an LGAD as a function of bias voltage and collected charge. Here, the experimental results are also compared to TCAD simulations.

47 OTHER INSTRUMENTATION↗

Dual functionality of over-lithiated NMC for high energy silicon-based lithium-ion batteries

Owing to their high specific capacity and suitably low operating potential, silicon-based anodes are an attractive alternative to graphite in next-generation lithium-ion batteries. However, silicon anodes suffer from low initial coulombic efficiency and fast capacity decay, limiting their widespread application. Pre-lithiation strategies are highly appealing to compensate for irreversible active lithium loss and to boost the cell energy density. In this work, we maximize the cell energy density by direct pre-lithiation of the NMC (LiNi 0.5 Mn 0.3 Co 0.2 O 2 ) cathode to Li 1+x NMCO 2 without introducing inactive deadweight to either electrode. First, we demonstrate that Li 1+x NMCO 2 can be synthesized chemically, via reaction between NMC and lithium napthalide, and electrochemically. The NMC cathode is tolerant of a one-time over-lithiation up to 60 mA h g NMC -1 , giving capacity retention on par with untreated NMC in half cell electrochemical cycling. Using synchrotron X-ray absorption spectroscopy (ex situ) and diffraction (in situ), we demonstrate that higher amounts of over-lithiation lead to local structure distortion – driven by transition metal reduction to Jahn–Teller active Mn 3+ and Co 2+ – as well as bulk structural hysteresis during over-lithiation and layer “buckling” that increases the amount of lithium extracted from the structure in the charged state. The Li 1+x NMCO 2 with low-to-moderate over-lithiation capacity (23, 46, and 70 mA h g NMC -1 ) is proven to be a highly effective dual-purpose lithium source and cathode material in full cell tests with a commercially relevant Si–graphite anode. These cells show higher capacity, superior cycle life, and improved coulombic efficiencies when compared to those with stoichiometric NMC cathodes. Finally, this study introduces a new and simple method to pre-lithiate layered transition metal oxide cathodes, opening up new possibilities for the development of high energy density lithium-ion batteries with next-generation anodes.

25 ENERGY STORAGE↗

Gas Stopper Developments for Improved Purity and Intensity of Low-Energy, Rare Isotope Ion Beams (Final Technical Report)

This final technical report summarizes the work of the Michigan State University (MSU) team supported by grant # DE-SC0021423 awarded by the Office of Nuclear Physics, Department of Energy. Objectives: The successful fulfillment of the FRIB science mission hinges on ensuring the availability of fast, stopped, and reaccelerated beams consisting of rare isotopes. This project's research and development focus was dedicated to supporting the advancement and creation of a cutting-edge linear gas stopper. The primary aim is to efficiently convert the high-intensity fast beams of rare isotopes provided by FRIB into high-quality, low-energy beams. These beams are essential for conducting stopped beam experiments or for subsequent reacceleration. The overarching goal is to advance technology, aiming to increase the beam rate capability of the linear gas stopper for medium-to-heavy-mass rare isotopes by more than tenfold compared to the currently most effective gas stopper in operation, and to improve the purity of the delivered beams. Project Description: The existing technology employed in gas stopping devices designed for low-energy, rare-isotope beams presents limitations in both the purity of extracted beams and the intensities of injected beams. These limitations are incompatible with the requirements of the recently commissioned rare isotope beam facility, FRIB. Our research and development efforts, aligned with the previously outlined objectives, focused on addressing the most critical aspects for enhancing beam-rate capability and purity. Specifically, advanced particle-in-cell simulations were developed and integrated into a simulation pipeline to explore the efficacy of multi-layer RF carpets on increasing ion transport efficiency with high incoming beam rates that generate space charge fields which can limit it. We also explored the possibility of using a collision-induced-dissociation (CID) gas cell to break up molecular contaminant ions that are generated during the stopping process. A prototype CID gas cell was constructed and tested with beams from an offline ion source, validating the concept with the successful demonstration of breaking of molecular ions. The outcome of this research enabled the formulation a conceptual design for a next-generation linear gas stopping device specifically tailored for FRIB. This device is envisioned to deliver rare-isotope-ion beams at a rate of 10 8 particles per second or higher, accompanied by advancements in purity. Methods employed: This project leverages advancements in technologies initially designed for the Advanced Cryogenic Gas Stopper (ACGS), the current state-of-the-art linear gas stopper, through the use of new simulations and beam purification via collision-induced-dissociation. The methods include: 1. Development of a prototype low-energy, low-pressure CID gas stopper. This prototype features a thin, approximately 20 nm, Si 3 N 4 entrance window designed for dissociating stable and rare-isotope molecular ions. The goal is to enhance beam purification and overall efficiency. 2. Creation of Particle-in-cell (PIC) simulations to assess the advantages of multi-layer RF carpets and multi-point extraction for ion transport efficiency. These simulations rely on the 3DCylPIC package, specifically designed for studying devices of this nature. The goal is to quantify and mitigate ion transport losses due to space charge generated in the stopping process of large numbers of ions. 3. Perform ion transport simulations across an RF carpet using an 8-phase travelling wave and evaluate its performance. Compared to the 4-phase RF carpets used in ACGS, the 8-phase carpets will double the wavelength of the generated traveling wave allowing for larger maximum RF amplitudes that could result in improved ion transport efficiency for high-intensity incoming beams when large space charge fields are present. Impact: Tackling the primary challenges associated with transforming high-energy projectile fragment beams into low-energy beams—specifically, addressing efficiency and purity—holds significant promise for advancing FRIB science. This advancement will particularly impact precision mass measurements, laser spectroscopy of short-lived nuclei, and studies in astrophysics and nuclear reactions using reaccelerated beams. These domains play a crucial role in addressing key questions outlined in the 2023 NSAC long-range plan, spanning nuclear structure, nuclear astrophysics, and fundamental symmetries. Additionally, they contribute to addressing 10 out of the 17 benchmarks identified by the NRC RISAC. The development of a next-generation gas stopping device capable of delivering low-energy, rare-isotope beams at a rate of 10 8 particles per second, or more, with high purity holds the potential to unlock experiments that would otherwise be unfeasible. Furthermore, it is expected to reduce the time required for experiments at FRIB, thereby maximizing scientific output. The research and development activities performed as part of this project bolstered essential competencies at FRIB in beam physics and ion source technologies, provided valuable training opportunities for junior scientists.

43 PARTICLE ACCELERATORS↗

Performance Analysis and Radiation Damage Estimation of the Stopping Target Monitor Detectors in Mu2e

The Mu2e experiment aims to search for the charged lepton flavour violating (CLFV) process of a coherent, neutrinoless, conversion of a muon into an electron within the proximity of an aluminium nucleus. Mu2e seeks to measure the ratio (R μe ) of the rate of this conversion process, relative to that of ordinary muon capture. Mu2e will achieve world-leading sensitivity, improving the current limit of Rμe < 7 ×10 -13 (90% C.L.),set by the SINDRUM-II experiment, by an order of 104. This corresponds to a single-event sensitivity of Rμe < 2.87 × 10 -17 (90% C.L.). Many beyond Standard Model (BSM) theories require CLFV to occur at a rate accessible by Mu2e. Any observation of CLFV at Mu2e would have profound implications on particle physics. The Stopping Target Monitor (STM) will be comprised of both a HPGe and a LaBr3 detector which will monitor the signals of photons produced in stopped-muon processes to a required accuracy of 10%. To achieve the desired sensitivity, it is imperative that the detectors perform at their optimal level. The STM detectors are placed within a harsh radiation environment in the form of a high energy ‘flash’ of gamma radiation as well as a flux of fast neutrons. Estimations of radiation damage to HPGe in literature is limited. This thesis reports an approach which utilizes the Kinetic-Energy Released in Matter (KERMA) parameter that considers the energy dependence of the incident flux and the cross-section information for the incident particle. Resampling schemes have been adopted to give a realistic rate over the experiment run time. The results have then been normalized to the radiation damage caused by a 252 Cf source. The estimated time before annealing of the detector is necessary is found to be 75 and 78 months in the case of neutron damage and τ ~ 24 years, 11 months in the case of electron/positron induced damage. This shows significant improvement on the previous estimations.

36 MATERIALS SCIENCE↗

Modeling of flash sintering of ionic ceramics

A fundamental understanding of the influence of defects in ionic ceramics at the atomic, microstructural, and macroscopic levels, before, during, and after the flash sintering event is key to the development of ceramic processing operations that lead to fast, low cost, and environmentally safe fabrication of materials. The observed phenomenology of the flash process encompasses multiple time and length scales and have resulted on a wide variety of what sometimes appears to be contradictory explanations. Here, this article summarizes the latest developments on the modeling and simulation of flash sintering, specifically those related to the understanding of the equilibrium and kinetic properties and the corresponding microstructural evolution of ionic ceramics. Challenges and opportunities in the development of theoretical analyses that include unidentified multiphysical effects are discussed, as they pertain to the processing of technologically relevant ceramic materials for advanced structures and devices.

36 MATERIALS SCIENCE↗

Ultrafast exciton and trion dynamics in highly 𝑛-doped Mo⁢S 2 monolayers: Many-body effects

Understanding many-body interactions of excitons and charge carriers in monolayer semiconductors is crucial for tuning their unique optical properties and optimizing their performance in optoelectronic devices. However, the sensitivity of these atomically thin semiconductors to doping, defects, and strain–arising from synthesis, substrate, and environmental conditions–hinders consistent observation of many-body effects. In this work, we employed linear and ultrafast transient optical absorption spectroscopy to investigate the influence of background doping on exciton many-body interactions in Mo⁢S 2 monolayers. Using reversible molecular physisorption gating, we achieved a high background doping density of 4.9 × 10 13 c⁢m −2 in an argon environment, which is significantly higher than those attainable with conventional electrical gating. Our results reveal a photoinduced 𝐴-exciton resonance redshift, attributed to band-gap renormalization at a low background-doping density of 4.3 × 10 12 c⁢m −2 in an air environment, transitioning to a blueshift at a high background-doping density of 4.9 × 10 13 c⁢m −2 due to dominant Pauli blocking effects and vertical excitation shifts. We further observed transient energy splitting between free-exciton and -trion states up to 57 meV due to exciton-electron interactions. The ultrafast spectroscopy further revealed exciton and trion dynamics, including fast energy splitting of exciton and trion resonances within 1 picosecond (ps) followed by a rapid decay having a lifetime of ∼5.4 ps. Furthermore, our results demonstrate the critical role of background-doping conditions in tuning many-body interactions and quasiparticle dynamics in 2D semiconductors, providing valuable insights for future device design and material engineering.

Doped semiconductors↗

Timing resolution and rate capability of Photonis miniPlanacon XPM85212/A1-S MCP-PMT

In this paper we report on a set of experiments that focus on measuring the timing performance of the Photonis miniPlanacon XPM85212/A1-S microchannel plate photomultiplier tubes along with the detector response at high event rates. The detector has a single photoelectron timing resolution of 30 ps at low rates ( 10 kHz ). We show that both the gain and the timing start to deteriorate around 1 MHz with 20 photoelectrons per channel at 1 0 4 target gain, giving the current per unit of area limits of 1.38 μ A / cm 2 and 2.38 μ A / cm 2 for the two tested devices. Photo-multiplier tubes with lower micro-channel plate resistivity exhibit a better rate capability due to the faster replenishment of the charge inside the microchannels. As we demonstrate, another method to improve the rate capability is to operate the photon detector tubes at a lower gain by reducing the supply voltage and compensating for the loss of amplitude by an additional amplification stage at the expense of the achieved timing resolution. The tube active area over which the beam is spread also plays a role since the same amount of light yields a better rate capability when spread over a larger area. The tubes exposed to high event rates showed an uncharacteristically slow recovery back to its initial gain with 80 % of the initial gain recovered only after several tens of minutes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Charged Wellbore Casing Controlled Source Electromagnetics (CWC-CSEM) for Reservoir Imaging and Monitoring (Final report)

This project addresses the needs of the U.S. Department of Energy (DOE) to develop advanced monitoring technologies and protocols to track the fate of subsurface carbon dioxide (CO2) plumes for carbon storage. Specifically, the project seeks to develop and test a unique and novel system of technologies consisting of electromagnetic data acquisition, coupled multiphysics imaging, and reservoir model enhancement to understand the migration and long-term distribution of CO2 in the subsurface. The overarching objective is to develop an integrated approach for long term monitoring of carbon storage. The two main components of the project include the methodology development and the test of the method at a field site. The methodology component consists of 1) developing the field procedure and protocol for collecting time-lapse controlled-source electromagnetic (CSEM) data with source electric current injected into the subsurface through wellbore casings; 2) building of background 3D electrical conductivity utilizing multiple sources of data such as supplemental surface transient EM (TEM) surveys, well-logs, and seismic structural information, for enhancing CSEM signal from reservoir depths; and 3) coupled multiphysics simulations and inversion of CSEM data constrained by production data and by structural information from seismic imaging of the reservoir and overlying formations. The testing component used the field site of Bell Creek Oil Field, which served both as a field laboratory for the method development as well as a test site to evaluate the CSEM signal strengths and the methodology developed in this research project. We have accomplished all the proposed tasks and developed the methodology as planned. These include the procedure for time-lapse CSEM data acquisition, data processing techniques, integration with 3D conductivity model building, fast reservoir simulation for history matching using machine learning, and interpreting CSEM data with coupling to the reservoir modeling. Collectively, the outcome of these tasks form a coherent workflow that can be applied to monitor dedicated carbon storage in saline reservoirs. The testing component evaluated the applicability and limitations of the method, and concluded that the method would be ideal for monitoring dedicated carbon storage sites utilizing saline reservoirs.

54 ENVIRONMENTAL SCIENCES↗

Marine Hydrogen Demonstration

This report summarizes Phase 1 of a project involving the design of a Floating Hydrogen Production and Dispensing Barge destined for the Port of San Francisco (SF). The H 2 Barge is designed to produce renewable H 2 at the rate of ~ 530 kg/day, storing 512 kg of hydrogen at 517-bar, allowing fast refueling of hydrogen fuel cell vessels and land-side hydrogen delivery trailers for distribution into the nascent SF hydrogen ecosystem. The broader considerations that impacted the H2 Barge design are also described. An account is given of a new review process formulated by the United States Coast Guard (USCG) to review this first-of-its-kind maritime implementation of hydrogen technology. The immediate goals of the H 2 Barge Project are to 1) demonstrate the feasibility, viability and methods of hydrogen production, storage and fueling in a maritime context, 2) help shape (where needed) and navigate the required local, state and federal regulatory gauntlet and 3) catalyze a “green hydrogen ecosystem” (both marine and landside) with locally produced renewable hydrogen at the San Francisco waterfront. A summary is also given of the modeling and experimental activity of Phase 1 directed to the development of science-based refueling protocols for large marine Type IV 250-bar hydrogen tanks. Combined modeling and experimental studies are reported of the filling of large (28 kg) 250-bar Type IV hydrogen tanks of the type being deployed on early hydrogen ferries, such as the MV Sea Change. The primary question was to determine how such tanks can be successfully filled (state of charge greater than 97%) within 45 minutes without exceeding the 82 °C temperature limit historically set for such tanks. The studies show that a gas injector is needed avoid thermal stratification during filling which can result in potential hot spots. Pre-cooling of the hydrogen was found to be essential in most cases, as ambient conditions greatly affect the need for a pre-cooling to achieve the 45-minute fill time. Pre-cooling cannot be supplied by nearby water, such as that found in nature (bays, lakes, rivers, etc.) because pre-cooling cooling below 0 °C was found to be necessary to avoid excessive compression heating. The experimental results afforded a calibration of the engineering model (SOFIL) for these large 250-bar tanks, which now enables using SOFIL to predict volume-averaged hydrogen filling temperatures to an accuracy of +/- 2.7°C for these tanks. The model can therefore be used to evaluate potential scenarios for development of a standardized fueling methodology for ferries utilizing large Type-IV tanks of the type examined here.

08 HYDROGEN↗

Pulse shape measurements for neutron/gamma discrimination using the TOFPET2 ASIC

Many highly pixelated organic scintillator detection systems would benefit from independent readout of each scintillator pixel. Recent advances in Silicon Photomultiplier (SiPM) technology makes this goal feasible, however the data acquisition from potentially hundreds or thousands of channels requires a low-cost and compact solution. For pixelated neutron detection with organic scintillators, the capability to distinguish between neutron and gamma interactions using Pulse Shape Discrimination (PSD) is required along with pulse charge and time of arrival. The TOFPET2 ASIC from PETsys Electronics is a 64-channel readout chip providing pulse time and charge integration measurements from SiPMs, and is specifically designed for time-of-flight positron-emission tomography. Using an 8 × 8 array of 6 mm × 6 mm J-series SiPMs from SensL/OnSemi (ArrayJ-60035-64P-PCB), we have studied the energy and PSD performance of the TOFPET2 ASIC using a 4 × 4 array of 6 mm × 6 mm × 30 mm trans -Stilbene crystals from Inrad Optics and a custom SiPM routing board from PETsys Electronics. In conclusion, using a time-over-threshold method, we measure a maximum PSD figure-of-merit of approximately 1.2 at 478 keV (the Compton edge of 662 keV) for a J-series SiPM operating at an over-voltage of 3V.

47 OTHER INSTRUMENTATION↗

Metrology of Time-Domain Soft X-Ray Attosecond Pulses and Reevaluation of Pulse Durations of Three Recent Experiments

Attosecond pulses in the soft x-ray (SXR) to water-window energy region offer the tools for creating and studying target-specific localized inner-shell electrons or holes in materials, enabling monitoring or controlling charge and energy flows in a dynamic system on attosecond timescales. Recently, a number of laboratories have reported generation of continuum harmonics in the hundred-electron-volt to kilovolt region with few-cycle long-wavelength mid-infrared lasers. These harmonics have the bandwidth to support pulses with durations of a few to a few-ten attoseconds. But harmonics generated in a gas medium have attochirps that cannot be fully compensated by materials over a broad spectral range; thus, realistically what are the typical shortest attosecond pulses that one can generate? To answer this question, it is essential that the temporal attosecond pulses be accurately characterized. By reanalyzing the soft x-ray attosecond metrology reported in three recent experiments using a newly developed broadband phase retrieval algorithm, we demonstrate here that the generated attosecond pulses in the first two papers have durations of about 60 as, longer than what they have reported. Similarly, the duration from the third experiment is retrieved to be about half of the 322-as upper limit cited in that work. We also introduce the autocorrelation (AC) of the streaking spectrogram. By comparing the ACs from the experiments and from the retrieved SXR pulses, the accuracy of the retrieved results can be directly visualized. Our retrieval method is fast and accurate, and it shall provide a powerful tool for the metrology of the emerging few-ten-attosecond pulses.

74 ATOMIC AND MOLECULAR PHYSICS↗

Superionic conducting vacancy-rich β-Li 3 N electrolyte for stable cycling of all-solid-state lithium metal batteries

The advancement of all-solid-state lithium metal batteries requires breakthroughs in solid-state electrolytes (SSEs) for the suppression of lithium dendrite growth at high current densities and high capacities (>3 mAh cm -2 ) and innovation of SSEs in terms of crystal structure, ionic conductivity and rigidness. Here we report a superionic conducting, highly lithium-compatible and air-stable vacancy-rich β-Li 3 N SSE. This vacancy-rich β-Li 3 N SSE shows a high ionic conductivity of 2.14 × 10 -3 S cm -1 at 25 °C and surpasses almost all the reported nitride-based SSEs. A Li- and N-vacancy-mediated fast lithium-ion migration mechanism is unravelled regarding vacancy-triggered reduced activation energy and increased mobile lithium-ion population. All-solid-state lithium symmetric cells using vacancy-rich β-Li 3 N achieve breakthroughs in high critical current densities up to 45 mA cm -2 and high capacities up to 7.5 mAh cm -2 , and ultra-stable lithium stripping and plating processes over 2,000 cycles. The high lithium compatibility mechanism of vacancy-rich β-Li 3 N is unveiled as intrinsic stability to lithium metal. In addition, β-Li 3 N possesses excellent air stability through the formation of protection surfaces. All-solid-state lithium metal batteries using the vacancy-rich β-Li 3 N as SSE interlayers and lithium cobalt oxide (LCO) and Ni-rich LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM83) cathodes exhibit excellent battery performance. Extremely stable cycling performance is demonstrated with high capacity retentions of 82.05% with 95.2 mAh g -1 over 5,000 cycles at 1.0 C for LCO and 92.5% with 153.6 mAh g -1 over 3,500 cycles at 1.0 C for NCM83. Utilizing the vacancy-rich β-Li 3 N SSE and NCM83 cathodes, the all-solid-state lithium metal batteries successfully accomplished mild rapid charge and discharge rates up to 5.0 C, retaining 60.47% of the capacity. Notably, these batteries exhibited a high areal capacity, registering approximately 5.0 mAh cm -2 for the compact pellet-type cells and around 2.2 mAh cm -2 for the all-solid-state lithium metal pouch cells.

25 ENERGY STORAGE↗

Large gyro-orbit model of ion velocity distribution in plasma near a wall in a grazing-angle magnetic field

A model is presented for the ion distribution function in a plasma at a solid target with a magnetic field $\boldsymbol {B}$ inclined at a small angle, $\alpha \ll 1$ (in radians), to the target. Adiabatic electrons are assumed, requiring $\alpha \gg \sqrt {Zm_{e}/m_{i}}$ , where $m_{e}$ and $m_{i}$ are the electron and ion mass, respectively, and $Z$ is the charge state of the ion. An electric field $\boldsymbol {E}$ is present to repel electrons, and so the characteristic size of the electrostatic potential $\phi$ is set by the electron temperature $T_{e}$ , $e\phi \sim T_{e}$ , where $e$ is the proton charge. An asymptotic scale separation between the Debye length $\lambda _{D} = \sqrt {\epsilon _0 T_{{e}} / e^{2} n_{{e}} }$ , the ion sound gyro-radius $\rho _{s} = \sqrt { m_{i} ( ZT_{e} + T_{i} ) } / (ZeB)$ and the size of the collisional region $d_{c} = \alpha \lambda _{\textrm {mfp}}$ is assumed, $\lambda _{D} \ll \rho _{s} \ll d_{c}$ . Here $\epsilon _0$ is the permittivity of free space, $n_{e}$ is the electron density, $T_{i}$ is the ion temperature, $B= |\boldsymbol {B}|$ and $\lambda _{\textrm {mfp}}$ is the collisional mean free path of an ion. The form of the ion distribution function is assumed at distances $x$ from the wall such that $\rho _{s} \ll x \ll d_{c}$ , that is, collisions are not treated. A self-consistent solution of the electrostatic potential for $x \sim \rho _{s}$ is required to solve for the quasi-periodic ion trajectories and for the ion distribution function at the target. The large gyro-orbit model presented here allows to bypass the numerical solution of $\phi (x)$ and results in an analytical expression for the ion distribution function at the target. It assumes that $\tau =T_{i}/(ZT_{e})\gg 1$ , and ignores the electric force on the quasi-periodic ion trajectory until close to the target. For $\tau \gtrsim 1$ , the model provides an extremely fast approximation to energy–angle distributions of ions at the target. These can be used to make sputtering predictions.

Physics↗

Characterization of self-magnetic pinch (SMP) radiographic diode performance on RITS-6 at Sandia National Laboratories. I. Diode dynamics, DC heating to extend radiation pulse

Radiographic diodes focus on an intense electron beam to a small spot size to minimize the source area of energetic photons for radiographic interrogation. The self-magnetic pinch (SMP) diode has been developed as such a source and operated as a load for the six-cavity radiographic integrated test stand (RITS-6) inductive voltage adder driver. While experiments support the generally accepted conclusion that a 1:1 aspect diode (cathode diameter equals anode–cathode gap) delivers optimum SMP performance, such experiments also show that reducing the cathode diameter, while reducing spot size, also results in reduced radiation dose, by as much as 50%, and degraded shot reproducibility. Analysis of the effective electron impingement angle on the anode converter with time made possible by a newly developed dose-rate array diagnostic indicates that fast-developing oscillations of the angle are correlated with early termination of the radiation pulse on many of the smaller-diameter SMP shots. This behavior as a function of relative cathode size persists through experiments with output voltages and currents up to 11.5 MV and 225 kA, respectively, and with spot sizes below approximately few millimeters. Since simulations to date have not predicted such oscillatory behavior, considerable discussion of the angle behavior of SMP shots is made to lend credence to the inference. We report there is clear anecdotal evidence that DC heating of the SMP diode region leads to stabilization of this oscillatory behavior. This is the first of two papers on the performance of the SMP diode on the RITS-6 accelerator.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

High-Performance Electron Sources: Numerical Methods and Beam Dynamics at the Precision Frontier

Electron sources have a wide range of applications and there are many stakeholders that express continuing need for improvements and performance enhancements. Whether we consider ultra-cold, high-brightness, high-charge or high-average current source needs, there are some common themes from the point of view of the beam dynamics involved. These are the following ones: ability to model accurately the emission processes, including the presence of often complicated cathode and other boundary surfaces with a wide range of spatial scales; ability to deal accurately and efficiently with a large number of particles interacting pair-wise, including the stochastic part of these interactions with a wide range of spatial scales; and ability to propagate the particle distributions in time, including collisions with a wide range of temporal scales. These tasks require high precision and accuracy since the goal is usually generation, transport and preservation of very high-quality beams. This grant addressed one of the rem

43 PARTICLE ACCELERATORS↗

Looking at the bigger picture: Identifying the photoproducts of pyruvic acid at 193 nm

Here, photodissociation of pyruvic acid (PA) was studied in the gas-phase at 193 nm using two complementary techniques. The time-sliced velocity map imaging arrangement was used to determine kinetic energy release distributions of fragments and estimate dissociation timescales. The multiplexed photoionization mass spectrometer setup was used to identify and quantify photoproducts, including isomers and free radicals, by their mass-to-charge ratios, photoionization spectra, and kinetic time profiles. Using these two techniques, it is possible to observe the major dissociation products of PA photodissociation: CO 2 , CO, H, OH, HCO, CH 2 CO, CH 3 CO, and CH 3 . Acetaldehyde and vinyl alcohol are minor primary photoproducts at 193 nm, but products that are known to arise from their unimolecular dissociation, such as HCO, H 2 CO, and CH 4 , are identified and quantified. A multivariate analysis that takes into account the yields of the observed products and assumes a set of feasible primary dissociation reactions provides a reasonable description of the photoinitiated chemistry of PA despite the necessary simplifications caused by the complexity of the dissociation. These experiments offer the first comprehensive description of the dissociation pathways of PA initiated on the S 3 excited state. Most of the observed products and yields are rationalized on the basis of three reaction mechanisms: (i) decarboxylation terminating in CO 2 + other primary products (~50%); (ii) Norrish type I dissociation typical of carbonyls (~30%); and (iii) O—H and C—H bond fission reactions generating the H atom (~10%). The analysis shows that most of the dissociation reactions create more than two products. This observation is not surprising considering the high excitation energy (~51 800 cm –1 ) and fairly low energy required for dissociation of PA. We find that two-body fragmentation processes yielding CO 2 are minor, and the expected, unstable primary co-fragment, methylhydroxycarbene, is not observed because it probably undergoes fast secondary dissociation and/or isomerization. Norrish type I dissociation pathways generate OH and only small yields of CH 3 CO and HOCO, which have low dissociation energies and further decompose via three-body fragmentation processes. Experiments with d 1 -PA (CH 3 COCOOD) support the interpretations. The dissociation on S 3 is fast, as indicated by the products’ recoil angular anisotropy, but the roles of internal conversion and intersystem crossing to lower states are yet to be determined.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Collaborative Research: Unravelling the Physics Associated with the Production of Extremely Dense Plasma States of Microscale (Final Report) Nanosecond-pulsed Discharges

The aim of this project is to study and establish the physical mechanisms that contribute to the formation of anomalously dense plasmas in high-pressure nanosecond-pulsed discharges. These discharges have a broad range of applications such as plasma-assisted combustion, plasma flow actuators, biomedical sterilization and exotic materials synthesis. The structure and formation of these discharges, producing high plasma densities of ~10 14 -10 15 cm -3 , are well-studied and understood. Fast-pulsed microscale high-pressure discharges can be driven to even higher densities of > 10 19 cm -3 , approaching warm dense matter conditions. The mechanisms that generate these plasmas have not been understood. Analysis of the warm dense matter state under laboratory conditions is an expensive and non-trivial endeavor. For instance, dense plasmas can be generated by electrical explosions of metal foils and wires. Plasmas generated after the explosion have a short lifetime and often present difficult conditions for diagnostics. Generation of dense plasmas was also achieved during high-voltage nanosecond pulsed discharges when the so-called explosive electron emission is obtained. Unfortunately, this process is very difficult to control for the studies of warm dense matter. In our recent study, we have shown that additional heating of plasma by lasers can further increase the density of plasma and even lead to the fully ionized state. This method, potentially, allows better control of the plasma parameters. In this work, we studied a second stage laser-heated micro-discharge using a self-consistent one-dimensional particle-in-cell Monte Carlo-collision (1D PIC-MCC) model coupled with Maxwell’s equations. We predicted the generation of a fully ionized plasma on the picosecond time scale. However, this model considered the plasma as an ideal gas despite the high pressure and the nearly fully ionized state. The ideal plasma model assumes that the dilute gas approximation is valid, where the inter-particle interactions are negligible. For charged particles this assumption holds as long as the shielded Coulomb potential assumption is valid. For very high plasma densities, this concept breaks down since the Debye sphere surrounding each charged particle no longer contains enough electrons to statistically provide the shielding of the single particle Coulomb interaction potential. At such densities, the plasma can no longer be described as ideal and non-ideal coupling effects need to be considered. In this report, we elucidate our recent work of developing a PIC-MCC model with improvements for non-ideal plasma conditions due to Coulomb coupling at high densities. In particular, we study the interaction of green light radiation and a dense microplasma, and explore the non-ideal plasma effects in this interaction. In this computational model, we implement the two most important non-ideal effects: ionization potential depression (IPD) and enhanced collision cross sections. Our primary goal is to study the physics associated with electromagnetic (EM) wave heating, also called the second-stage wave-heating, and establish the role of plasma non-ideality in this phenomenon. Our secondary goal is to improve the chemistry mechanism of the 1D PIC-MCC model by including a more detailed excited species collision treatment. At high pressures, stepwise ionization from excited species might play an important role in the ionization process. Previously, this ionization mechanism was neglected due to the excitation collision cross section of xenon being smaller than that of ionization. However, a preliminary study showed that the excited species density in the initial microplasma was an order of magnitude higher than the electron density. Therefore, my aim is to determine the significance of this additional ionization pathway to the plasma generation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗