Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “LaS”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 73 records · Page 4

Novel usage of deep learning and high-performance computing in long-baseline neutrino oscillation experiments

Mención Internacional en el título de doctorDeep-learning methods are playing a crucial role in numerous scientific and industrialapplications. Over the past two decades, these techniques have helped in the collection,reconstruction, and analysis of large data samples in particle physics experiments. Themain topic of this PhD research is the study of deep-learning techniques in long-baselineneutrino oscillation experiments. Neutrinos are mysterious light elementary particles,and their investigation is essential to shed light on some of the remaining open questionsin physics. The work presented here describes an algorithm based on a convolutionalneural network developed to provide highly accurate and efficient selections of electronneutrino and muon neutrino interactions in the Deep Underground Neutrino Experiment(DUNE). With this algorithm, the electron neutrino (antineutrino) selection efficiencypeaks at 90% (94%) and exceeds 85% (90%) for reconstructed neutrino energies between2-5 GeV. The selection efficiency for muon neutrino (antineutrino) interactions is foundto have a maximum of 96% (97%) and exceeds 90% (95%) efficiency for reconstructedneutrino energies above 2 GeV. When considering all electron neutrino and antineutrinointeractions as signal (both those appearing from oscillations and those intrinsic tothe beam), a selection purity of 90% is achieved. These event selections are criticalto maximise the sensitivity of the experiment to CP-violating effects, key to furtherunderstand the matter-antimatter asymmetry of the Universe.In high-energy physics experiments, deep learning has also been explored for producingfast simulations and physically-motivated manipulations of simulated images. Some ofthose simulations, such as the light production and detection, are very computationallyexpensive and require novel methods to produce the necessary samples while controllingthe varied underlying physics model parameters. To do so, we invented the model-assistedgenerative adversarial network (MAGAN), first validated on simple generic case studiesand then successfully applied to the DUNE photon-detector simulation.Moreover, we also developed graph neural networks for 3D-voxel classification ofambiguities and optical crosstalk for a different particle physics experiment, most preciselyfor the proposed SuperFGD. This novel 3D-granular plastic-scintillator neutrino detectorwill be used to upgrade the near detector of the T2K neutrino oscillation experiment, and our method reports efficiencies and purities of 94-96% per event in the classificationof particle track voxels.Due to the growth and complexity of deep neural networks, researchers have beeninvestigating techniques to train those networks in a more computationally-efficient way.Many efforts have been made by the community to optimise deep-learning models byparallelising or distributing their training computation across multiple devices. In thisthesis, we study an approach based on data locality for those neural networks that cannotbenefit from scaling their computation due to a significant bottleneck in the data I/O.The research also includes a detailed study on the performance of deep neural networkson hardware accelerator boards.Los métodos de aprendizaje profundo son cada vez más utilizados en numerosas aplicacionescientíficas e industriales hoy en día. Durante las dos últimas décadas, estastécnicas se han empleado en la recolección, reconstrucción y análisis de la gran cantidadde datos generados por experimentos de física de partículas. El tema principal de estatesis doctoral es el uso de estos modelos de aprendizaje profundo en experimentos defísica de neutrinos, en concreto en los experimentos de larga distancia DUNE y T2K. Losneutrinos, partículas fundamentales neutras, de las más ligeras del Universo, pueden serclave para explicar algunas de las cuestiones todavía sin resolver en física fundamental.Entre las diferentes contribuciones que esta tesis ha hecho a su estudio, cabe destacar eldesarrollo de un algoritmo basado en una red de neuronas convolucional para seleccionarcon gran eficiencia y precisión las interacciones de neutrinos electrónicos y muónicos enel Deep Underground Neutrino Experiment (DUNE). La eficiencia de selección obtenidapara neutrinos (antineutrinos) electrónicos alcanza un máximo del 90% (94%) y supera el85% (90%) para neutrinos con energías reconstruidas en el rango 2-5 GeV. La selección deneutrinos (antineutrinos) muónicos tiene una eficiencia máxima del 96% (97%) y excedeel 90% (95%) para neutrinos con energías reconstruidas de más de 2 GeV. Considerandocomo señal todas las interacciones de neutrinos y antineutrinos electrónicos (procedentestanto de oscilaciones como intrínsecos en el haz inicial), se logra una pureza en la seleccióndel 90%. Dichas selecciones de eventos son fundamentales para maximizar la sensibilidaddel experimento a los efectos de violació...

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Resumen del Informe de Progreso del PR100: Resultados Preliminares del Modelo y Conjuntos de Datos Solares y Eólica de Alta Resolución

El estudio de Resiliencia y Transiciones a 100% Energia Renovable de Puerto Rico (PR100) es un estudio de 2 anos de la Oficina de Movilizacion de la Red del Departamento de Energia y seis laboratorios nacionales para analizar exhaustivamente las rutas dirigidas por las personas interesadas hacia un futuro de energia limpia en Puerto Rico. En el Ano 1 del estudio, el equipo PR100, creo y analizo los modelos que alcanzan las metas de energia renovable para Puerto Rico y los objetivos de resiliencia energetica a corto y largo plazo. Este informe, que resume el progreso en el Ano 1, proporciona las consideraciones que pueden informar posibles decisiones de fondos e implementacion potenciales por parte de las agencias federales y locales clave y partes interesadas. El resumen de este informe sigue a la publicacion en julio 2022 de un Informe de Seis Meses de Progreso de PR100. (en ingles y espanol), asi como webinarios publicos en febrero 2022 para lanzar el estudio y julio 2022 para presentar la actualizacion a 6 meses. Un informe final por escrito y visuales por la web seran publicados a finales del 2023. Todas las publicaciones y eventos publicos asociados con el estudio estaran disponibles en ingles y espanol. This report is also available in English https://www.nrel.gov/docs/fy23osti/85018.pdf.

14 SOLAR ENERGY↗

Advanced composite combustor structural concepts program

An analytical study was conducted to assess the feasibility of and benefits derived from the use of high temperature composite materials in aircraft turbine engine combustor liners. The study included a survey and screening of the properties of three candidate composite materials including tungsten reinforced superalloys, carbon-carbon and silicon carbide (SiC) fibers reinforcing a ceramic matrix of lithium aluminosilicate (LAS). The SiC-LAS material was selected as offering the greatest near term potential primarily on the basis of high temperature capability. A limited experimental investigation was conducted to quantify some of the more critical mechanical properties of the SiC-LAS composite having a multidirection 0/45/-45/90 deg fiber orientation favored for the combustor linear application. Rigorous cyclic thermal tests demonstrated that SiC-LAS was extremely resistant to the thermal fatigue mechanisms that usually limit the life of metallic combustor liners. A thermal design study led to the definition of a composite liner concept that incorporated film cooled SiC-LAS shingles mounted on a Hastelloy X shell. With coolant fluxes consistent with the most advanced metallic liner technology, the calculated hot surface temperatures of the shingles were within the apparent near term capability of the material. Structural analyses indicated that the stresses in the composite panels were low, primarily because of the low coefficient of expansion of the material and it was concluded that the dominant failure mode of the liner would be an as yet unidentified deterioration of the composite from prolonged exposure to high temperature. An economic study, based on a medium thrust size commercial aircraft engine, indicated that the SiC-LAS combustor liner would weigh 22.8N (11.27 lb) less and cost less to manufacture than advanced metallic liner concepts intended for use in the late 1980's.

Sattar, M. A.↗

Design, Development and Test Challenges: Separation Mechanisms for the Orion Pad Abort-1 Flight Test

On May 6, 2010, NASA launched the first successful integrated flight test, Pad Abort-1, of the Orion Project from the White Sands Missile Range in Las Cruces, New Mexico. This test demonstrated the ability to perform an emergency pad abort of a full-scale 4.8 m diameter, 8200 kg crew capsule. During development of the critical separation mechanisms for this flight test, various challenges were overcome related to environments definition, installation complications, separation joint retraction speed, thruster ordnance development issues, load path validation and significant design loads increases. The Launch Abort System retention and release (LAS R&R) mechanism consisted of 6 discrete structural connections between the LAS and the crew module (CM) simulator, each of which had a preloaded tension tie, Superbolt torque-nut and frangible nut. During the flight test, the frangible nuts were pyrotechnically split, permitting the CM to separate from the LAS. The LAS separation event was the driving case in the shock environment for many co-located hardware items. During development testing, it was necessary to measure the source shock during the separation event so the predicted shock environment could be validated and used for certification testing of multiple hardware items. The Lockheed Martin test team measured the source separation shock due to the LAS R&R function, which dramatically decreased the predicted environment by 90% at 100 Hz. During development testing a hydraulic tensioner was used to preload the joint; however, the joint relaxation with the tensioner proved unsatisfactory so the design was modified to include a Superbolt torque-nut. The observed preload creep during lab testing was 4% after 30 days, with 2.5% occurring in the first 24 hours. The conversion of strain energy (preload) to kinetic energy (retraction) was measured to be 50-75%. Design features and careful monitoring of multiple strain gauges on each tension tie allowed a pure tensile load to be applied after stacking at the launch pad. Following installation, preload in each joint was monitored for 24 hours. Due to unforeseen complications and the influence of temperature on the portable data acquisition system, the team encountered difficulty in tracking the joint relaxation. In some cases, bond-line failure of the strain gauges occurred.

Dinsel, Alison↗

Overview of C/C-SiC Composite Development for the Orion Launch Abort System

Past and present efforts by the authors to further understanding of the ceramic matrix composite (CMC) material used in the valve components of the Orion Launch Abort System (LAS) Attitude Control Motor (ACM) will be presented. The LAS is designed to quickly lift the Orion Crew Exploration Vehicle (CEV) away from its launch vehicle in emergency abort scenarios. The ACM is a solid rocket motor which utilizes eight throttleable nozzles to maintain proper orientation of the CEV during abort operations. Launch abort systems have not been available for use by NASA on manned launches since the last Apollo ]Saturn launch in 1975. The CMC material, carbon-carbon/silicon-carbide (C/C-SiC), is manufactured by Fiber Materials, Inc. and consists of a rigid 4-directional carbon-fiber tow weave reinforced with a mixed carbon plus SiC matrix. Several valve and full system (8-valve) static motor tests have been conducted by the motor vendor. The culmination of these tests was the successful flight test of the Orion LAS Pad Abort One (PA ]1) vehicle on May 6, 2010. Due to the fast pace of the LAS development program, NASA Marshall Space Flight Center assisted the LAS community by performing a series of material and component evaluations using fired hardware from valve and full ]system development motor tests, and from the PA-1 flight ACM motor. Information will be presented on the structure of the C/C-SiC material, as well as the efficacy of various non ]destructive evaluation (NDE) techniques, including but not limited to: radiography, computed tomography, nanofocus computed tomography, and X-ray transmission microscopy. Examinations of the microstructure of the material via scanning electron microscopy and energy dispersive spectroscopy will also be discussed. The findings resulting from the subject effort are assisting the LAS Project in risk assessments and in possible modifications to the final ACM operational design.

Allen, Lee R.↗

Spatial distributions of Tribrachidium, Rugoconites, and Obamus from the Ediacara Member (Rawnsley Quartzite), South Australia

The spatial distribution of in situ sessile organisms, including those from the fossil record, provides information about life histories, such as possible dispersal and/or settlement mechanisms, and how taxa interact with one another and their local environments. At Nilpena Ediacara National Park (NENP), South Australia, the exquisite preservation and excavation of 33 fossiliferous bedding planes from the Ediacara Member of the Rawnsley Quartzite reveals in situ communities of the Ediacara Biota. Here, the spatial distributions of three relatively common taxa, Tribrachidium, Rugoconites, and Obamus, occurring on excavated surfaces were analyzed using spatial point pattern analysis. Tribrachidium have a variable spatial distribution, implying that settlement or post-settlement conditions/preferences had an effect on populations. Rugoconites display aggregation, possibly related to their reproductive methods in combination with settlement location availability at the time of dispersal and/or settlement. Additionally, post-settlement environmental controls could have affected Rugoconites on other surfaces, resulting in lower populations and densities. Both Tribrachidium and Rugoconites also commonly occur as individuals or in low numbers on a number of beds, thus constraining possible reproductive strategies and environmental/substrate preferences. The distribution of Obamus is consistent with selective settlement, aggregating near conspecifics and on substrates of mature microbial mat. This dispersal process is the first example of substrate-selective dispersal among the Ediacara Biota, thus making Obamus similar to numerous modern sessile invertebrates with similar dispersal and settlement strategies. Resumen La distribución espacial de los organismos sésiles in situ, incluyendo los del registro fósil, brinda información sobre las historias de vida, tal como los posibles mecanismos de dispersión y/o asentamiento, y sobre cómo los taxones interactúan entre sí y entre sus entornos locales. En el Parque Nacional Nilpena Ediacara (NENP), Australia Meridional, la excelente preservación y excavación de 33 planos de lecho fosilífero del Miembro Ediacara de la Cuarcita Rawnsley revela comunidades in situ de la biota ediacárica. En este estudio analizamos las distribuciones espaciales de tres taxones relativamente comunes, Tribrachidium, Rugoconites y Obamus, que se encuentran en superficies excavadas mediante el análisis de patrones de puntos espaciales. Tribrachidium tiene una distribución espacial variable, lo que implica que las condiciones/preferencias durante o después del asentamiento tuvieron un efecto en las poblaciones. Rugoconites muestran agregación, posiblemente relacionado con sus métodos reproductivos en combinación con la disponibilidad de lugares de asentamiento en el momento de la dispersión y/o asentamiento. Además, los controles ambientales posteriormente al asentamiento podrían estar afectando a Rugoconites en otras superficies, lo que resultaría en poblaciones y densidades más bajas. Tanto Tribrachidium como Rugoconites ocurren como individuos en varios lechos, restringiendo las posibles estrategias reproductivas y las preferencias ambientales/de sustrato. La distribución de Obamus es consistente con un asentamiento selectivo, agregando cerca de sus congéneres y sobre sustratos de tapete microbiano maduro. Este proceso de dispersión es el primer ejemplo de dispersión selectiva de sustrato entre la biota ediacárica, lo que hace que Obamus sea similar a numerosos invertebrados sésiles modernos con estrategias similares de dispersión y asentamiento.

Phillip C. Boan↗

Avances a un ano del PR100: Resultados Preliminares del Modelzacion y Conjuntos de Datos Solares y Eolicos de Alta Resolucion

El estudio de Resiliencia y Transiciones a 100% Energia Renovable de Puerto Rico (PR100) es un estudio de 2 ano de la Oficina de Movilizacion de la Red del Departamento de Energia y seis laboratorios nacionales para analizar exhaustivamente las rutas dirigidas por las personas interesadas hacia un futuro de energia limpia en Puerto Rico. En el Ano 1 del estudio, el equipo PR100, creo y analizo los modelos que alcanzan las metas de energia renovable para Puerto Rico y los objetivos de resiliencia energetica a corto y largo plazo. Esta presentacion, que resume el progreso en el Ano 1, proporciona las consideraciones que pueden informar posibles decisiones de fondos e implementacion potenciales por parte de las agencias federales y locales clave y partes interesadas. Esta presentacion sigue a la publicacion en julio 2022 de un Informe de Seis Meses de Progreso de PR100 (en ingles y espanol), asi como webinarios publicos en febrero 2022 para lanzar el estudio y julio 2022 para presentar la actualizacion a 6 meses. Un informe final por escrito y visuales por la web seran publicados a finales del 2023. Todas las publicaciones y eventos publicos asociados con el estudio estaran disponibles en ingles y espanol. This report is also available in English https://www.nrel.gov/docs/fy23osti/85126.pdf.

datos de recursos eolicos↗

Polynomial Scaling Localized Active Space Unitary Selective Coupled Cluster Singles and Doubles

We present a polynomial-scaling algorithm for the localized active space unitary selective coupled cluster singles and doubles (LAS-USCCSD) method. In this approach, cluster excitations are selected based on a threshold ϵ determined by the absolute gradients of the LAS-UCCSD energy with respect to cluster amplitudes. Using the generalized Wick’s theorem for multireference wave functions, we derive the gradient expression as a polynomial function of one-, two-, and three-body reduced density matrices and 1- and 2-electron integrals, valid for any multireference wave function. The resulting gradient implementation exhibits a memory scaling of 𝒪(N 6 ), with N spin orbitals in the combined active space of all fragments. The variational quantum eigensolver is used to optimize the selected cluster excitations on a quantum simulator. Furthermore, by plotting the energy error, defined as the difference between the LAS-USCCSD and corresponding CASCI energies, against the inverse cluster amplitude selection threshold (ϵ –1 ) for polyene chains containing 2 to 5 π-bond units, we establish a relationship between the energy error and the threshold. To further validate the accuracy of LAS-USCCSD, we computed the cis–trans isomerization energy of stilbene (a 20-qubit system) and the magnetic coupling constant of the tris-hydroxo-bridged chromium dimer [Cr 2 (OH) 3 (NH 3 ) 6 ] 3+ (evaluated as both 12- and 20-qubit systems) using the Qiskit-Qulacs simulator. Assessing such examples is important to determine the practical feasibility of quantum simulations for chemically realistic systems. Toward this goal, with the LAS-USCCSD algorithm we estimated the quantum resources required for simulating an active space of (30e,22o) in [Cr 2 (OH) 3 (NH 3 ) 6 ] 3+ , a size that remains beyond the reach of current quantum simulators for accurate treatment.

Algorithms↗

Fragment-based initialization for quantum subspace methods

Here, we present a novel quantum-classical algorithm called LAS-QKSD for multireference systems, by combining a classical localized active space (LAS) fragment-based multireference algorithm with the quantum Krylov subspace diagonalization (QKSD) method for quantum computers. The algorithm uses wave function information from a LAS self-consistent field (LASSCF) calculation to prepare an initial state with better overlap with the target ground state than the Hartree-Fock state. This is coupled with the use of QKSD to ultimately converge to the exact energy, providing faster convergence than starting from the Hartree-Fock state. Fragmentation has the two-fold benefit of fewer configurations on the classical side of the algorithm as well as fewer state preparation gates on the quantum side. First, we compare the LAS-QKSD method to the classical LASSCF method and to QKSD with a Hartree-Fock initial state. We then examine ways to load the LASSCF wave function using direct initialization and a QKSD-motivated spectral filtering approach. Finally, using a bimetallic complex, we show that the LAS-QKSD method is an efficient alternative to highly expensive complete active space SCF (CASSCF) calculations on strongly correlated systems.

D'Cunha, Ruhee↗

Lanthanum sulfides as high temperature thermoelectric materials

Thermoelectric property measurements have been made for the nonstoichiometric lanthanum sulfides, LaS(R) with R in the range 1.33-1.50. The Seebeck coefficients and electrical resistivities increase with temperature from 200 to 1100 C. Power factors (defined as Seebeck coefficient squared divided by electrical resistivity) generally increase both as the temperature is increased and as the compound composition is varied from LaS(1.48) to LaS(1.35). The power factor values combined with estimates of thermal conductivities for LaS(1.38) and LaS(1.4) yield figures of merit greater than 0.0005 at 1000 C.

Danielson, L. R.↗

Orion Crew Exploration Vehicle Launch Abort System Guidance and Control Analysis Overview

Aborts during the critical ascent flight phase require the design and operation of Orion Crew Exploration Vehicle (CEV) systems to escape from the Crew Launch Vehicle (CLV) and return the crew safely to the Earth. To accomplish this requirement of continuous abort coverage, CEV ascent abort modes are being designed and analyzed to accommodate the velocity, altitude, atmospheric, and vehicle configuration changes that occur during ascent. Aborts from the launch pad to early in the flight of the CLV second stage are performed using the Launch Abort System (LAS). During this type of abort, the LAS Abort Motor is used to pull the Crew Module (CM) safely away from the CLV and Service Module (SM). LAS abort guidance and control studies and design trades are being conducted so that more informed decisions can be made regarding the vehicle abort requirements, design, and operation. This paper presents an overview of the Orion CEV, an overview of the LAS ascent abort mode, and a summary of key LAS abort analysis methods and results.

Davidson, John B.↗

The Ejectable Data Recorder: A Lean, Risk-Informed Approach for Hardware Development

NASA is developing the Orion spacecraft to transport crew from the Earth to the Moon as part of the Artemis series of missions. To provide a crew escape capability from pre-launch through ascent, the Orion vehicle is equipped with a Launch Abort System (LAS), built by Lockheed Martin, which pulls the capsule away from the launch vehicle in the event of an abort scenario. The Ascent Abort 2 (AA-2) test flight occurred on July 2, 2019,and tested a production version of the LAS to ensure that it can operate as intended, and to collect a large data set from hundreds of sensors on the vehicle to support Orion flight certification. In the original AA-2 architecture, a single-string set of communications antennas on the LAS would downlink all of the in-flight test data to ground stations. However, that communications architecture was predicted to have data dropouts during abort and jettison of the LAS, and would not support data transmission at all after LAS jettison. As a result, a comprehensive trade study was completed, yielding the addition of antennas on the crew module (CM), a buffer/rebroadcast capability for key portions of the flight, and an ejectable data recorder (EDR) subsystem. This EDR subsystem would serve as a backup to the radio frequency (RF) communications system, and would be non-flight critical, providing a unique capability that enabled management to take a different approach with the hardware and software development. The Crew Module and Separation Ring were developed as “Class 1”Flight Hardware, albeit with some tailoring approaches to enable efficiencies. The Class 1 designation requires full rigor for flight hardware and software, documenting everything that happens to a piece of hardware from procurement through disposal, requiring a full spectrum of acceptance tests, and the highest rigor of quality assurance processes. At the other end of the spectrum, Class 3hardware is controlled, but not intended for flight, and leaves the level of rigor up to the project manager. This classification is often used for research and development projects. Similarly,Class-1E has been recently defined at NASA for ISS payloads and technology development projects that are not flight critical and do not need the full rigor of Class 1 to be successful. The EDR subsystem was challenged at commencement to adopt a skunkworks and agile-like approach to hardware development, allowing for a different risk posture than the rest of the AA-2 hardware. After initially pursuing Class 1 processes, the EDR subsystem design evolved to incorporating numerous commercial components, leading to re-designation as a Class-1E subsystem. The resulting EDR subsystem was fully successful in meeting all flight system requirements, and achieved 100% retrieval of flight test data. This paper will discuss the risk posture of the EDR subsystem and the subsequent tailoring that was enacted as part of its Class-1E status.

EDR↗

The Orion Pad Abort 1 (PA-1) Flight Test: A Propulsion Success

This poster provides a concise overview of the highly successful Orion Pad Abort 1 (PA-1) flight test, and the three rocket motors that contributed to this success. The primary purpose of the Orion PA-1 flight was to help certify the Orion Launch Abort System (LAS), which can be utilized in the unlikely event of an emergency on the launchpad or during mission vehicle ascent. The PA-1 test was the first fully integrated flight test of the Orion LAS, one of the primary systems within the Orion Multi-Purpose Crew Vehicle (MPCV). The Orion MPCV is part of the architecture within the Space Launch System (SLS), which is being designed to transport astronauts beyond low-Earth orbit for future exploration missions. Had the Orion PA-1 flight abort occurred during launch preparations for a real human spaceflight mission, the PA-1 LAS would have saved the lives of the crew. The PA-1 flight test was largely successful due to the three solid rocket motors of the LAS: the Attitude Control Motor (ACM); the Jettison Motor (JM); and the Abort Motor (AM). All three rocket motors successfully performed their required functions during the Orion PA-1 flight test, flown on May 6, 2010 at the White Sands Missile Range in New Mexico, culminating in a successful demonstration of an abort capability from the launchpad.

JM↗

Investigating the Role of Acid Sites in the Hydrocracking of Polyethylene-EVOH Multilayer Film Waste over Pt/BEA Catalyst

Multilayer polymer films (MFs) containing poly(ethylene-co-vinyl alcohol) (EVOH) and polyolefins are ubiquitous in single-use food and medical packaging. MFs are currently landfilled or incinerated rather than mechanically recycled because of the processing difficulties associated with their form factor and complex multicomponent structures. Advanced chemical recycling is a promising solution. Prior reports have explored hydrogenolysis and hydrodeoxygenation to convert EVOH, but these technologies are limited by catalyst deactivation and slow apparent kinetics, respectively. Alternatively, in this work, we demonstrate the efficient hydrocracking of commercial MFs into naphtha range (C5-C12) alkanes over platinum (Pt) supported on acidic zeolites. Mixtures of low-density polyethylene (LDPE) and EVOH are utilized as MF surrogates to gain fundamental insights. Pt deposited on BEA supports with varying Lewis acid site (LAS) concentrations are synthesized and tested for hydrocracking. Surprisingly, Pt/BEA with high LAS concentrations demonstrate improved activity for LPDE/EVOH blends over LDPE alone. In contrast, LAS concentrations are shown to have no influence on LDPE hydrocracking. LAS and Brønsted acid sites (BAS) catalyze the dehydration of EVOH to form water, which improves LDPE hydrocracking. Polyaromatics formed primarily via EVOH thermal degradation lead to detrimental coke formation, which hinders hydrocracking activity. Reaction conditions and feed ratios of LDPE and EVOH are tuned to balance these competing effects. Reusability tests demonstrate that Pt/BEA maintains high activity (81% conversion in 2 h) and high selectivity towards naphtha (78%) over multiple reuse cycles. Furthermore, these findings position hydrocracking as a promising technology for the circularity of complex MF plastic waste.

36 MATERIALS SCIENCE↗

Impact of Site Identity, Location, and Accessibility on Polyethylene Conversion Rates and Product Selectivities over Metal-Free MFI Zeolites

Brønsted (BAS), Lewis (LAS), and surface Brønsted (SBAS) acid sites have been investigated for polyethylene (PE) upcycling by zeolite catalysts, but there is no clear consensus regarding their catalytic roles, partly due to the complexity of the catalysts used and varying reaction conditions across studies. This work systematically determined how these sites impact PE conversion rates and product distributions by utilizing a suite of microporous MFI catalysts with varying Si/Al ratios, acid site densities, and inherent mesoporosities. PE conversion rates did not trend with total BAS or LAS densities due to a combination of internal mass transfer limitation and the apparent inability of LAS alone to cleave C–C bonds, but a strong, statistically significant correlation was present with respect to SBAS density and mesopore surface area, jointly, owing to accelerated polymer activation on external surfaces to smaller diffusion-limited chains. However, ingress of these SBAS-derived fragments ultimately remained rate limiting, as demonstrated by solid conversion rates that increased with mesopore surface area at similar SBAS density and likewise increased with SBAS density at similar mesopore surface area. In batch PE cracking reactions, light gaseous product selectivities were most sensitive to total BAS, with higher densities generally exhibiting higher selectivity to C 3 and linear C 4 –C 7 products and higher alkane/alkene product ratios, consistent with increased β-scission turnovers. Insights from this work help systematically clarify the roles of BAS, LAS, SBAS, and mesopores in PE cracking reactions and inform the development of tailored zeolite catalysts for efficient polyolefin upcycling.

accessibility↗

Bridging the gap between molecules and materials in quantum chemistry with localized active spaces

The number of materials that “bridge the gap” between single molecules and extended solids, such as metal-organic frameworks and organic semiconductors, has been increasing. Consequently, there is a growing need for modeling approaches that effectively integrate the real-space molecular perspective employed by computational chemists and the reciprocal-space dispersive perspective employed by computational physicists. Here, we propose the localized active space (LAS) approach as a promising method to successfully bridge this gap. The LAS approach extends the active space concept from multiconfigurational methods such as complete active space self-consistent field theory to multiple molecular fragments via a product-form wave function ansatz. Here, we apply this method to solid state phenomena by treating each unit cell as a fragment with different sets of local quantum numbers (e.g., charge and excitation number). State interaction between these LAS states (LASSI) thus provides a comprehensive basis for the study of charge and energy transfer, meeting and surpassing the capabilities of single-reference fragmentation approaches such as constrained density functional theory (cDFT). Most centrally, we show how combining this LASSI approach with multiconfigurational pair-density functional theory (MC-PDFT) provides an elegant and efficient method to compute band structures that capture multiconfigurational character. We apply the LASSI band structure approach to the computation of band gaps in stretched hydrogen chain, polyacetylene, and bulk nickel oxide (NiO), finding good or excellent quantitative agreement with reference values in all cases. Additionally, we use the LAS basis in one-dimensional model systems to demonstrate its ability to treat difficult solid-state phenomena such as exciton transfer and excitation at p-n junctions.

method development↗

Terrestrial laser scanning data (Levels 0 and 1) for Pasoh, Malaysia, Sep 2024

This data package contains data from terrestrial laser scanning (TLS) at the Pasoh Forest Reserve, Malaysia. The Pasoh Forest Reserve is a facility of the Forest Research Institute Malaysia, and contains evergreen lowland dipterocarp forest. The Next-Generation Ecosystem Experiments Tropics (NGEE-Tropics) study areas at Pasoh were established to study how different species respond to climatic variation and soil water availability. Two study areas were chosen representing different topography and species. The TLS data archived here were collected to provide detailed, three-dimensional information about forest structure. Specifically, data were collected to allow tree-level characterization of woody structure and leaf area for 12 focal trees with FloraPulse and sap flux sensors, facilitating estimation of woody biomass and leaf area to allow upscaling of water content and transpiration data to the tree-level. Scan positions were not selected to provide consistent data for non-focal trees with the study areas. This data package contains the following data: - High-level files document further details of the campaign and data package: 1_CampaignSummary.csv provides details about the campaign and study site, 2_ScanAreasDetail.csv provides details about each separate scan area (groups of scans post-processed into a single point cloud), 3_TerrestrialLidarSensor.csv provides further technical details about the Riegl VZ-400i TLS sensor, TLS_CSV_dd.csv is a CSV Data Dictionary providing information about the fields in CSV files following the ESS-DIVE CSV File Formatting Guidelines Reporting Format, TLS_flmd.csv is a File Level Metadata file providing information about each file in the data package following the ESS-DIVE File Level Metadata Reporting Format, and README.txt is a text file describing the overall project and file structure. - Level 0 data are the raw data (.PROJ folders) as recorded by the Riegl VZ-400i TLS instrument before scan co-registration and post-processing with the Riegl's proprietary RiSCAN PRO software, which requires a license. - Level 1 data contain post-processed, co-registered data from each scan area. The "PointClouds" folder for each scan area contains a .las file with 1 cm resolution point cloud data exported from RiSCAN PRO. These are the main files likely to be of interest to most users and can be further processed with any software capable of manipulating .las files (e.g. Python, R CloudCompare). The "Project Information" folder contains log files from post-processing in RiSCAN PRO that may be of interest to users who want to see detailed records of post-processing, including all PDF reports generated by RiSCAN PRO. The "ScanPositions" folder contains information about the final position of all TLS scans, after post-processing, in multiple formats. The file ScanPositions_*.csv provides final geo-referenced scan positions, and the file SOP_backup_*.csv can be used in RiSCAN PRO to restore the co-registered scan positions if users wish to re-process raw data (Level 0 .PROJ folders) with RiSCAN PRO software (e.g., subsample to a different resolution, exclude a certain scan position, or apply different filters on reflectance or deviation values) without redoing time-consuming co-registration steps.

54 ENVIRONMENTAL SCIENCES↗

Terrestrial laser scanning data (Levels 0 and 1) from Urban Biogeochemistry Pilot Project sites, Knoxville, Tennessee, Jul 2024 - Jul 2025

This data package contains data from terrestrial laser scanning (TLS) at five urban park sites in Knoxville, Tennessee, USA. All parks include open-grown and/or closed-canopy trees and mixed nearby land use. These study sites were established as part of the Urban Biogeochemistry Pilot Project, which has an overall goal of better understanding how hydrobiogeochemical cycling is altered within the human environment. These five sites represent a gradient of urbanization, and were instrumented to understand hydrological and biogeochemical cycling (e.g., soil moisture, soil physical properties and biogeochemistry, tree transpiration, species type). The TLS data archived here were collected to provide detailed, three-dimensional information about forest structure. Specifically, data were collected to allow tree- and stand-level characterization of woody structure and leaf area. TLS scans were placed to capture the area around trees with sap flow sensors, and as much of a 50 m radius area around the meteorological station as possible given site property limits. Derived products will allow upscaling of water content and transpiration data. This data package contains the following data: - High-level files document further details of the campaign and data package: 1_CampaignSummary.csv provides details about the campaign and study site, 2_ScanAreasDetail.csv provides details about each separate scan area (groups of scans post-processed into a single point cloud), 3_TerrestrialLidarSensor.csv provides further technical details about the Riegl VZ-400i TLS sensor, TLS_CSV_dd.csv is a CSV Data Dictionary providing information about the fields in CSV files following the ESS-DIVE CSV File Formatting Guidelines Reporting Format, TLS_flmd.csv is a File Level Metadata file providing information about each file in the data package following the ESS-DIVE File Level Metadata Reporting Format, and README.txt is a text file describing the overall project and file structure. - Level 0 data are the raw data (.PROJ folders) as recorded by the Riegl VZ-400i TLS instrument before scan co-registration and post-processing with the Riegl's proprietary RiSCAN PRO software, which requires a license. - Level 1 data contain post-processed, co-registered data from each scan area. The "PointClouds" folder for each scan area contains a .las file with 1 cm resolution point cloud data exported from RiSCAN PRO. These are the main files likely to be of interest to most users and can be further processed with any software capable of manipulating .las files (e.g. Python, R CloudCompare). The "Project Information" folder contains log files from post-processing in RiSCAN PRO that may be of interest to users who want to see detailed records of post-processing, including all PDF reports generated by RiSCAN PRO. The "ScanPositions" folder contains information about the final position of all TLS scans, after post-processing, in multiple formats. The file ScanPositions_*.csv provides final geo-referenced scan positions, and the file SOP_backup_*.csv can be used in RiSCAN PRO to restore the co-registered scan positions if users wish to re-process raw data (Level 0 .PROJ folders) with RiSCAN PRO software (e.g., subsample to a different resolution, exclude a certain scan position, or apply different filters on reflectance or deviation values) without redoing time-consuming co-registration steps.

54 ENVIRONMENTAL SCIENCES↗