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At least 1,117 records · Page 62

Disentangling interlayer confinement and pore surface adsorption in functionalized smectites for tunable ethylene gas capture

Smectite-based adsorbents are increasingly being studied as sustainable packaging materials for scavenging ethylene, a plant hormone that accelerates fruit ripening. However, the mechanisms governing their uptake and retention remain poorly understood. Here, to tackle this question we systematically investigate ethylene gas-solid interactions in pristine, acid-activated, and choline-functionalized montmorillonites using a complementary combination of structural, gravimetric, and spectroscopic techniques, including inelastic neutron scattering. We experimentally distinguish ethylene populations associated with interlayer confinement, mesopore, and external surface adsorption. We show that chemical functionalization distinctly controls adsorption pathways: acid activation enhances total uptake by generating mesoporous adsorption sites and promoting partial interlayer intercalation, yielding capacities comparable to those of leading smectite-based adsorbents, while choline functionalization promotes preferential confinement and stabilization of guest molecules within the interlayer galleries. Advanced spectroscopic analysis provides molecular-level insight into confinement environments and interaction strengths. We also establish clear structure-property relationships by correlating uptake values derived from independent techniques, linking chemical modification, accessible adsorption domains, and retention behavior. These findings provide general design principles for tuning gas-solid interactions in functionalized layered silicates and highlight their potential as adaptable platforms for sustainable ethylene gas capture and selective adsorption technologies.

Ethylene adsorption mechanism↗

Two-well injector direct-phonon terahertz quantum cascade lasers

We present an experimental study on a terahertz quantum cascade laser (THz QCL) design that combines both two-well injector and direct-phonon scattering schemes, i.e., a so-called two-well injector direct-phonon design. As a result of the two-well injector direct-phonon scheme presented here, the lasers benefit from both a direct phonon scattering scheme for the lower laser level depopulation and a setback for the doping profile that reduces the overlap of the doped region with active laser states. Additionally, our design also has efficient isolation of the active laser levels from excited and continuum states as indicated by negative differential resistance behavior all the way up to room temperature. This scheme serves as a good platform for improving the temperature performance of THz QCLs as indicated by the encouraging temperature performance results of the device with a relatively high doping level of 7.56 × 10 10 cm −2 and T max ∼ 167 K. With the right optimization of the molecular beam epitaxy growth and interface quality, the injection coupling strength, and the doping density and its profile, the device could potentially reach higher temperatures than the latest records reached for the maximum operating temperature (T max ) of THz QCLs.

47 OTHER INSTRUMENTATION↗

Exploring strongly correlated quantum spin systems with quantum computers

At inception, quantum annealing leveraged quantum mechanics for classical optimization tasks. However, as machine coherence increases, the realization of quantum spin systems has emerged as an even more fruitful application of this computational model. Alternatives to the standard gate model deserve exploration, to achieve useful quantum advantage via analog quantum computing. The recent demonstration of so-called coherent quantum annealing with 1,000s of qubits, further expands the potential for this hardware to explore quantum system dynamics where the effects of quantum fluctuations can be carefully controlled and observed directly. Implementing existing celebrated spin models—or in fact new and dedicated ones—into quantum annealers will lead to observation and detection of quantum phenomena not yet observed, or not visualized directly, in experimental physics laboratories. Rather than computing or simulating quantum systems, these quantum computers allow one to simply build quantum systems, and experiment on them in an uniquely controlled way, with characterization down to the constitutive degree of freedom. This provides an unprecedented opportunity for understanding the physics of quantum spin systems. Keywords: Theoretical physics currently abounds of interesting theoretical spin models to explore frustration, strongly correlated spins, spin liquids, fractionalized excitations, and topological matter. However enticing, such models are generally only weak proxies for the properties of actual materials. In quantum annealers these models could be realized and experimented upon. Moreover, many more realistic models of such materials could be realized in quantum annealers. Employed in this way, quantum annealers provide an extraordinary versatile platform to explore quantum effects that are hard to find, detect, and characterize in natural materials.

36 MATERIALS SCIENCE↗

Fast and High-Fidelity SNAP Gate Enabled by Optimal Control on Floquet-Engineered Systems

Superconducting cavities with high quality factors, coupled to nonlinear ancilla, provide a promising platform for quantum information storage and manipulation. However, the commonly used selective number-dependent arbitrary phase (SNAP) gate faces significant challenges in ultra-high-coherence cavities, where weak dispersive shifts result in prolonged gate times. Here, we propose a protocol to achieve high-fidelity SNAP gates that are orders of magnitude faster than the standard implementation, breaking the speed limit set by the bare dispersive shift. This enhancement is achieved by dynamically amplifying dispersive coupling via sideband interactions, followed by quantum optimal control on Floquet-engineered systems. Additionally, we present a unified perturbation theory that explains both the gate acceleration and associated benign drive-induced decoherence, corroborated by Floquet\textendash Markov simulations. These results pave the way for the experimental realization of high-fidelity control of weakly coupled, high-coherence cavities, and expanding the scope of optimal control techniques in Floquet quantum systems.

You, Xinyuan [Fermilab]↗

Recent developments in 3D-printed membranes for water desalination

The recognition of membrane separations as a vital technology platform for enhancing the efficiency of separation processes has been steadily increasing. Concurrently, 3D printing has emerged as an innovative approach to fabricating reverse osmosis membranes for water desalination and treatment purposes. This method provides a high degree of control over membrane chemistry and structural properties. In particular, when compared to traditional manufacturing techniques, 3D printing holds the potential to expedite customization, a feat that is typically achieved through conventional manufacturing methods but often involves numerous processes and significant costs. This review aims to present the current advancements in membrane manufacturing technology specifically tailored for water desalination purposes, with a particular focus on the development of 3D-printed membranes. A comprehensive analysis of recent progress in 3D-printed membranes is provided. However, conducting experimental work to investigate various influential factors while ensuring consistent results poses a significant challenge. To address this, we explore how membrane manufacturing processes and performance can be effectively pre-designed and guided through the use of molecular dynamics simulations. Finally, this review outlines the challenges faced and presents future perspectives to shed light on research directions for optimizing membrane manufacturing processes and achieving optimal membrane performance.

3D printing membranes↗

FluxRETAP: a REaction TArget Prioritization genome-scale modeling technique for selecting genetic targets

MOTIVATION: Metabolic engineering is rapidly evolving as a result of new advances in synthetic biology tools and automation platforms that enable high throughput strain construction, as well as the development of machine learning tools (ML) for biology. However, selecting genetic engineering targets that effectively guide the metabolic engineering process is still challenging. ML can provide predictive power for synthetic biology, but current technical limitations prevent the independent use of ML approaches without previous biological knowledge. RESULTS: Here, we present FluxRETAP, a simple and computationally inexpensive method that leverages the prior mechanistic knowledge embedded in genome-scale models for suggesting targets for genetic overexpression, downregulation or deletion, with the final goal of increasing the production of a desired metabolite. This method can provide a list of desirable engineering targets that can be combined with current ML pipelines. FluxRETAP captured 100% of reaction targets experimentally verified to improve Escherichia coli isoprenol production, 50% of targets that experimentally improved taxadiene production in E. coli and ∼60% of genetic targets from a verified minimal constrained cut-set in Pseudomonas putida, while providing additional high priority targets that could be tested. Overall, FluxRETAP is an efficient algorithm for identifying a prioritized list of testable genetic and reaction targets. AVAILABILITY AND IMPLEMENTATION: FluxRETAP is implemented in python and released under the creative commons license. The implementation and code are freely available at: https://github.com/JBEI/FluxRETAP.

Czajka, Jeffrey J↗

Validation of time-dependent shift using the pulsed sphere benchmarks

The detailed behavior of neutrons in a rapidly changing time-dependent physical system is a challenging computational physics problem, particularly when using Monte Carlo methods on heterogeneous high-performance computing architectures. A small number of algorithms and code implementations have been shown to be performant for time-independent (fixed source and k-eigenvalue) Monte Carlo, and there are existing simulation tools that successfully solve the time-dependent Monte Carlo problem on smaller computing platforms. To bridge this gap, a time-dependent version of ORNL’s Shift code has been recently developed. Shift’s history-based algorithm on CPUs, and its event-based algorithm on GPUs, have both been observed to scale well to very large numbers of processors, which motivated the extension of this code to solve time-dependent problems. The validation of this new capability requires a comparison with time-dependent neutron experiments. Lawrence Livermore National Laboratory’s (LLNL) pulsed sphere benchmark experiments were simulated in Shift to validate both the time-independent as well as new time-dependent features recently incorporated into Shift. A suite of pulsed-sphere models was simulated using Shift and compared to the available experimental data and simulations with MCNP. Overall results indicate that Shift accurately simulates the pulsed sphere benchmarks, and that the new time-dependent modifications of Shift are working as intended. Validated exascale neutron transport codes are essential for a wide variety of future multiphysics applications.

Palmer, Camille J.↗

A temperature profile diagnostic for radiation waves on OMEGA-60

Predicting and matching radiation wave propagation with computational models has proven difficult. Information provided by experiments studying radiation flow has been limited when only radiation breakout is measured. We have developed the COAX (co-axial) diagnostic platform to provide spatial temperature profiles of a radiation wave through low density foams as a more detailed constraint for simulations. COAX uses a standard, laser-driven OMEGA-60 halfraum to drive radiation down a titanium-laden silicon oxide foam. Point-projection X-ray absorption spectroscopy perpendicular to the radiation flow measures the spatial profile of titanium ionization. The spectroscopic measurement utilizes a broadband capsule backlighter. Imaging and streak spectroscopy are used to characterize the size and spectrum of this source. Radiography provides an additional constraint by capturing the developing shock as the radiation flow becomes subsonic. The DANTE diagnostic is used to measure the halfraum temperature. Here, we provide a spectroscopic analysis of COAX data to determine temperature, and we describe experimental sources of uncertainty. The temperature is obtained by comparison to multi-temperature synthetic spectra post-processed from radiation-hydrodynamics simulations. Quantitative comparison between data and synthetic spectra generated from temperature profiles at relevant simulation times enable determination of a peak temperature of 114 ± 8 eV at 265 ± 22.4 μm from the halfraum. This represents an improvement over the temperature uncertainties of previous radiation flow experiments. Further refinements to the spectroscopic analysis could achieve ±4 eV. The combination between space-resolved spectroscopy and radiography enables us to determine the distance from the halfraum of both the radiation front and the shock front at the time of measurement. For the example shown in this paper the radiation front position is 600–630 μm at 3.43 ± 0.16 ns and the shock front position is 633 μm at 3.3 ± 0.24 ns.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Multiplexed Knockouts in the Model Diatom Phaeodactylum by Episomal Delivery of a Selectable Cas9

Marine diatoms are eukaryotic microalgae that play significant ecological and biogeochemical roles in oceans. They also have significant potential as organismal platforms for exploitation to address biotechnological and industrial goals. In order to address both modes of research, sophisticated molecular and genetic tools are required. We presented here new and improved methodologies for introducing CRISPRCas9 to the model diatom Phaeodactylum tricornutum cells and a streamlined protocol for genotyping mutant cell lines with previously unknown phenotypes. First, bacterialconjugation was optimized for the delivery of Cas9 by transcriptionally fusing Cas9 to a selectable marker by the 2A peptide. An episome cloning strategy using both negative and positive selection was developed to streamline CRISPR-episome assembly. Next, cell line picking and genotyping strategies, that utilize manual sequencing curation, TIDE sequencing analysis, and a T7 endonuclease assay, were developed to shorten the time required to generate mutants. Following this new experimental pipeline, both singlegene and two-gene knockout cell lines were generated at mutagenesis efficiencies of 48% and 25%, respectively. Lastly, a protocol for precise gene insertions via CRISPRCas9 targeting was developed using particle-bombardment transformation methods. Overall, the novel Cas9 episome design and improved genotyping methods presented here allow for quick and easy genotyping and isolation of Phaeodactylum mutant cell lines (less than 3 weeks) without relying on a known phenotype to screen for mutants.

59 BASIC BIOLOGICAL SCIENCES↗

Experimental observation of drumhead surface states in SrAs 3

The topological nodal-line semimetal (TNS) is a unique class of material with a one dimensional line node accompanied by a nearly dispersionless two-dimensional sur- face state. However, a direct observation of the so called drumhead surface state within current nodal-line materials is still elusive. Here, using high-resolution angle- resolved photoemission spectroscopy (ARPES) along with first-principles calculations, we report the observation of a topological nodal-loop (TNL) in SrAs 3 , whereas CaAs 3 exhibits topologically trivial state. Our data reveal that surface projections of the bulk nodal-points are connected by clear drumhead surface states in SrAs 3 . Furthermore, our magneto-transport and magnetization data clearly suggest the presence (absence) of surface state in SrAs 3 (CaAs 3 ). Notably, the observed topological states in RAs 3 (R = Ca, Sr) are well separated from other bands in the vicinity of the Fermi level. RAs 3 , thus, offers a unique opportunity to realize an archetype nodal-loop semimetal and establish a platform for gaining a deeper understanding of the quantum phase transitions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Influences of shock imprinting on mix in a 3D-printed porous media

Mixing of materials in porous media can cause a significant impact on fusion yield as previously demonstrated by the National Ignition Facility (NIF) MARBLE Campaign. Initially, the reactants are separated, with deuterium in the lattice struts and a tritium gas fill in the voids. Lattice parameters such as the strut thickness and relative pitch, provide a control for the mix parameters in the experiment. Los Alamos National Laboratory’s (LANL) BOSQUE project looks to better understand how the mix of the reactants and shell materials impact the fusion burn and resultant yield on various laser platforms. xRAGE’s Eulerian hydrodynamics and adaptive mesh refinement (AMR) provide the unique ability to study the impacts of multiscale features of complex lattice structures. This modeling provides the ability to measure shock front variations as the wave progress’ through a given media. Initial conditions of the lattice are essential to accurately model mix and burn measured by experiment. By varying the initial orientation and densities of these lattice regions the early time dynamics of how the shock is launched into the system is changed and advocates for the study of resulting effects. In this work, we will study the sensitivities of shock effects in varying 3D printed geometric systems and how these shocks alter the structure and mix in the lattice. We will discuss both preliminary experimental results and simulations to help plan and constrain future experiments where we will study the impact of different lattice geometries and lattice bulk densities. This work concludes with the relative impacts of lattice geometries on shock speeds at different bulk densities and the resultant mix widths due to those shock interactions. We see agreement with theory at the higher end of our bulk density study, however, as we approach lower bulk density systems the dynamics of these interactions begin to change.

2 Photon Polymerization↗

From Femtoseconds to Gigaseconds: The SolDeg Platform for the Performance Degradation Analysis of Silicon Heterojunction Solar Cells

Heterojunction Si solar cells exhibit notable performance degradation. Here, we modeled this degradation by electronic defects getting generated by thermal activation across energy barriers over time. To analyze the physics of this degradation, we developed the SolDeg platform to simulate the dynamics of electronic defect generation. First, femtosecond molecular dynamics simulations were performed to create a-Si/c-Si stacks, using the machine learning-based Gaussian approximation potential. Second, we created shocked clusters by a cluster blaster method. Third, the shocked clusters were analyzed to identify which of them supported electronic defects. Fourth, the distribution of energy barriers that control the generation of these electronic defects was determined. Fifth, an accelerated Monte Carlo method was developed to simulate the thermally activated time-dependent defect generation across the barriers. Our main conclusions are as follows. (1) The degradation of a-Si/c-Si heterojunction solar cells via defect generation is controlled by a broad distribution of energy barriers. (2) We developed the SolDeg platform to track the microscopic dynamics of defect generation across this wide barrier distribution and determined the time-dependent defect density N(t) from femtoseconds to gigaseconds, over 24 orders of magnitude in time. (3) We have shown that a stretched exponential analytical form can successfully describe the defect generation N(t) over at least 10 orders of magnitude in time. (4) We found that in relative terms, Voc degrades at a rate of 0.2%/year over the first year, slowing with advancing time. (5) We developed the time correspondence curve to calibrate and validate the accelerated testing of solar cells. We found a compellingly simple scaling relationship between accelerated and normal times t normal ∝ t accel T(accel)/T(normal) . (6) We also carried out experimental studies of defect generation in a-Si:H/c-Si stacks. We found a relatively high degradation rate at early times that slowed considerably at longer time scales.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Giant optical nonlinearity of Fermi polarons in atomically thin semiconductors

In this study, realizing strong nonlinear optical responses is a long-standing goal of both fundamental and technological importance. Recently, substantial efforts have been focused on exploring excitons in solids to achieve nonlinearities even down to few-photon levels. However, a crucial tradeoff arises as strong light–matter interactions require large oscillator strength and short radiative lifetime of excitons, which limits their nonlinearity. Here we experimentally demonstrate strong nonlinear optical responses with large oscillator strength by exploiting the coupling between excitons and carriers in an atomically thin semiconductor. By controlling the electric field and electrostatic doping of trilayer WSe 2 , we observe the hybridization between intralayer and interlayer excitons and the formation of Fermi polarons. Substantial optical nonlinearity is observed under continuous-wave and pulsed laser excitation, where the Fermi polaron resonance blueshifts by as much as ~10 meV. Intriguingly, we observe a remarkable asymmetry in the optical nonlinearity between electron and hole doping, which is tunable by the applied electric field. We attribute these features to the optically induced valley polarization due to the interactions between excitons and free charges. Our results establish atomically thin heterostructures as a highly versatile platform for engineering nonlinear optical response with applications to classical and quantum optoelectronics.

2d materials↗

A Simulated Evaluation of Powder Flowability Through a Partially Obstructed Consumable in Blown Powder Directed Energy Deposition Systems

Abstract In the interest of continued industrialization of metal additive manufacturing in modern production environments, cost is often referenced as a primary deterrent to new adopters. Conventional economic models for additive systems, processes, and supply chains often focus on specific process applications with little generalizability, or they neglect significant costs associated with production such as machine maintenance and consumable part replacement. Compounding the latter issue are substantial knowledge gaps in consumable part wear characterization for additive and other convergent manufacturing systems. In coaxial blown powder directed energy deposition systems, gas atomized metal powder is wasted during material deposition at a rate that is partly dependent on present wear phenomena in a consumable nozzle housed in the cladding head assembly. The price and lead time required to replace the nozzle incentivizes its reuse even when visibly worn. Often this initiates a process quality decline in the form of underbuilt geometry and internal defects due to losses in powder catchment efficiency. While depositing H13 steel using a hybrid manufacturing machine tool equipped with such a deposition system, a unique partial clog with a bridge-like structure formed at the consumable nozzle exit when supporting argon gas flows failed mid-process. To further understand coaxial multi-phase powder flow in the event of support gas failure, a computational fluid dynamics simulation is tailored to relevant process parameters, H13 powder material profile, and machine operator observations collected after the incident. The resulting differences in powder flow compared to control gas flow parameters is presented and discussed. The powder flowability and performance of the clogged nozzle is then assessed by using an optical profilometer to extract the profile of the clog and recreate the clog geometry within the simulation environment. In past work this simulation has been experimentally validated for a 316L steel powder material profile and used specifically for analyzing powder stream geometry and catchment efficiency. After the initial powder flow characterization, the clog is removed, and the nozzle is reprofiled. After removing the obstructing clog, the newly unobstructed nozzle geometry, the original off the shelf nozzle geometry, and additional nozzle profiles exploring different consumable refurbishment strategies are reevaluated in the simulation. Powder catchment efficiency for all variant nozzle geometries and relevant flow variables are compared and discussed, along with potential mitigation strategies for optimizing powder flowability with worn consumables. This work expands on the known morphology of blown powder obstructions and wear defects present in consumable coaxial nozzles while discussing pragmatic simulation driven responses to unanticipated subsystem failure in hybrid manufacturing machining platforms.

DeWitte, Lisa↗

Kinetic mix at gas-shell interface in inverted corona fusion targets

Gas-filled, laser-driven “inverted corona” fusion targets have attracted interest as a low-convergence neutron source and platform for studying kinetic physics. At the fill pressures under investigation, ejected particles from the shell can penetrate deeply into the gas before colliding, leading to significant mixing across the gas–shell interface. Here, we use kinetic-ion, fluid-electron hybrid particle-in-cell simulations to explore the nature of that mix. Simulations of the system demonstrate characteristics of a weakly collisional electrostatic shock, whereby a strong electric field accelerates shell ions into the rarefied gas and reflects upstream gas ions. This interpenetration is mediated by collisional processes: At higher initial gas pressure, fewer shell particles pass into the mix region and reach the hotspot. This effect is detectable through neutron yield scaling vs gas pressure. Predictions of neutron yield scaling show excellent agreement with experimental data recorded at the OMEGA laser facility, suggesting that 1D kinetic mechanisms are sufficient to capture the mix process.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Toward an improved nonlocal thermodynamic equilibrium model for more predictive simulations of ignition scale hohlraums

Recently, nonlocal thermodynamic equilibrium (NLTE) modeling has been identified as the primary reason for discrepant predictions of the peak neutron production time in indirectly driven inertial confinement fusion (ICF) platforms. It has also been observed that predictions of collisional excitation rates differ by as much as 50% from measurements. Theoretical uncertainties in dielectronic recombination rates have also been posited as possibly contributing to errors in NLTE predictions. This work examines the impact of multipliers on collisional excitation and dielectronic recombination rates on simulations of a directly driven gold sphere and an indirect drive ICF implosion. It is found that multipliers on the collisional excitation rates have a strong impact on radiant intensity and electron temperature and a weaker impact on ionization state, whereas multipliers on dielectronic recombinations rates strongly impact ionization state with a smaller impact on radiant intensity and electron temperature. A self-consistent NLTE model which places multipliers on differing transitions, as motivated by experimental measurements and more detailed atomic physics predictions, improves agreement but does not completely eliminate discrepancies with measurements of the radiant intensity within the 2–4 keV spectral range.

Farmer, W. A. [Lawrence Livermore National Laborat↗

Interfacial electroneutrality controls transport of asymmetric salts through charge-patterned mosaic membranes

Membranes that selectively enhance target solute permeation while rejecting competing species are essential for precision separations. This study introduces charge-patterned mosaic membranes (CMMs) that selectively transport divalent asymmetric salts by leveraging a net-neutral membrane–solution interface. This mechanism, dictated by the charge ratio of positive and negative domains on the membrane surface and the balance of cations and anions in the salt, is supported by analytical, numerical, and experimental results. Analytical solutions identified cationic domain coverages (f + ) of 33%, 50%, and 66% as optimal for the selective transport of +2:−1 salts, +1:−1 salts, and +1:−2 salts, respectively, under conditions where the pattern size (L) is significantly larger than the Debye length. Numerical simulations and experiments using CMMs with alternating charged-stripes inkjet-printed onto nanostructure copolymer substrates confirmed these findings. By varying stripe widths to control f + , pressure-driven filtration experiments demonstrated selective enrichment of MgCl 2 and K 2 SO 4 at the predicted f + values, with deviations from these values leading to salt rejection. These results highlight the pivotal role of a net-neutral interface in enabling asymmetric salt enrichment. This study positions CMMs as a versatile platform for tuning ion selectivity, addressing challenges in resource recovery, water treatment, and precision separations.

additive manufacturing↗

Investigating the impact of intermediate-mode perturbations on diagnosing plasma conditions in DT cryogenic implosions via synthetic x-ray Thomson scattering

The pursuit of inertial confinement fusion ignition target designs requires precise experimental validation of the conditions within imploding capsules, in particular the density and temperature of the compressed shell. Previous work has identified x-ray Thomson scattering (XRTS) as a viable diagnostic tool for inferring the in-flight compressed deuterium-tritium shell conditions during capsule implosions (Poole et al 2022 Phys. Plasmas 29 072703). However, this study focused on one-dimensional simulations, which do not account for the growth of hydrodynamic instabilities. In this work, two-dimensional DRACO simulations incorporating intermediate-mode perturbations up to Legendre mode l = 50 were used to generate synthetic XRTS spectra with the SPECT3D code. The analysis employed Markov-Chain Monte Carlo techniques to infer plasma conditions from these spectra. The results demonstrate that the XRTS diagnostic platform can effectively discern the in-flight compressed shell conditions for targets with varying adiabats, even in the presence of intermediate-mode perturbations. This work underscores the potential of XRTS for realistic inertial confinement fusion experiments, providing a robust method for probing the complex dynamics of fusion implosions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗