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At least 793 records · Page 44

Quantum-parallel vectorized data encodings and computations on trapped-ion and transmon QPUs

Compact data representations in quantum systems are crucial for the development of quantum algorithms for data analysis. In this study, we present two innovative data encoding techniques, known as QCrank and QBArt, which exhibit significant quantum parallelism via uniformly controlled rotation gates. The QCrank method encodes a series of real-valued data as rotations on data qubits, resulting in increased storage capacity. On the other hand, QBArt directly incorporates a binary representation of the data within the computational basis, requiring fewer quantum measurements and enabling well-established arithmetic operations on binary data. We showcase various applications of the proposed encoding methods for various data types. Notably, we demonstrate quantum algorithms for tasks such as DNA pattern matching, Hamming weight computation, complex value conjugation, and the retrieval of a binary image with 384 pixels, all executed on the Quantinuum trapped-ion QPU. Furthermore, we employ several cloud-accessible QPUs, including those from IBMQ and IonQ, to conduct supplementary benchmarking experiments.

97 MATHEMATICS AND COMPUTING↗

A Multiport DC Transformer to Enable Flexible Scalable DC as a Service

The rapid adoption of new DC loads and sources, including photovoltaic arrays, DC fast charging of electric vehicle, battery energy storage and data centers, requires a large amount of DC power conversion. A majority of new deployments also necessitate the integration of multiple DC loads and sources at one site. The traditional approach to serve these new applications relies on multiple standard power converters, each dedicated to a source or load, and results in highly customized systems, with challenging control coordination, complex protection strategies, and poor scalability. Instead, this paper proposes the concept of a multiport DC transformer (MDCT) as a modular building block for realizing a flexible, scalable DC as a Service system and address this rapidly growing need. The MDCT uses the S4T to achieve very tight control of cycle-by-cycle energy exchange between multiple ports, with high efficiency. A single multiport converter replaces 4-6 distinct converters, integrates all energy flows and manages protection. As a result, a new layered control architecture is introduced to ensure stability and scalability of the MDCT, with multiple S4T power converter building blocks connected in parallel to realize a fully modular system and reach the target power levels.

30 DIRECT ENERGY CONVERSION↗

Decovalex-2019 (Executive Summary)

The DECOVALEX Project is an on-going international research collaboration, established in 1992, to advance the understanding and modeling of coupled Thermal (T), Hydrological (H), Mechanical (M) and Chemical (C) processes in geological in geological systems. DECOVALEX was initially motivated by the recognition that prediction of these coupled effects is an essential part of the performance and safety assessment of geologic disposal systems for radioactive waste and spent nuclear fuel. Later it was realized that these processes also play a critical role in other subsurface engineering activities, such as subsurface CO 2 storage, enhanced geothermal systems, and unconventional oil and gas production through hydraulic fracturing. Research teams from many countries (e.g., Canada, China, Czech Republic, Finland, France, Germany, Japan, Republic of Korea, Spain, Sweden, Switzerland, Taiwan, United Kingdom, and the United States) various institutions have participated in the DECOVALEX Project over the years, providing a wide range of perspectives and solutions to these complex problems. These institutions represent radioactive waste management organizations, national research institutes, regulatory agencies, universities, as well as industry and consulting groups. The overall aim of DECOVALEX-2019 was to increase the understanding of various thermo-hydro-mechanical-chemical processes of importance for radionuclide release and transport from a repository to the biosphere and how they can be described and modelled using mathematical models. The scientific and technical objectives are: to increase the basic understanding of T-H-M-C coupled processes in fractured rocks (crystalline, sedimentary, argillaceous) and buffer materials; to investigate the predictive capabilities of different codes to field experiments and to perform verification of codes; to exchange experimental data, and improve the understanding of the constitutive behavior of crystalline and argillaceous rock masses and buffer materials; and to perform THMC calculations in a performance/safety assessment context.

58 GEOSCIENCES↗

DECOVALEX-2019 (Task E Final Report)

The DECOVALEX Project is an on-going international research collaboration, established in 1992, to advance the understanding and modeling of coupled Thermal (T), Hydrological (H), Mechanical (M) and Chemical (C) processes in geological in geological systems. DECOVALEX was initially motivated by the recognition that prediction of these coupled effects is an essential part of the performance and safety assessment of geologic disposal systems for radioactive waste and spent nuclear fuel. Later it was realized that these processes also play a critical role in other subsurface engineering activities, such as subsurface CO 2 storage, enhanced geothermal systems, and unconventional oil and gas production through hydraulic fracturing. Research teams from many countries (e.g., Canada, China, Czech Republic, Finland, France, Germany, Japan, Republic of Korea, Spain, Sweden, Switzerland, Taiwan, United Kingdom, and the United States) various institutions have participated in the DECOVALEX Project over the years, providing a wide range of perspectives and solutions to these complex problems. These institutions represent radioactive waste management organizations, national research institutes, regulatory agencies, universities, as well as industry and consulting groups. This document is the final report of Task E which was proposed and coordinated by Andra, the National Radioactive Waste Management Agency in France, presenting the technical definitions of the problems studied, approaches applied, achievements made and outstanding issues for future research. The purpose of Task E of the DECOVALEX-2019 project is to investigate upscaling THM modelling from small-scale experiments (some cubic meters) to full-scale experiments (some ten cubic meters) and finally to the scale of the waste repository (cubic kilometers). To achieve this aim, the data of two in-situ heating experiments performed by Andra (the French National Radioactive Waste Management Agency) in the Meuse/Haute-Marne Underground Research Laboratory (MHM URL) have formed the basis for the understanding of the THM behavior of the COx at different scales. The first experiment provided the reference values of the THM parameters by means of a calibration exercise and they were used for a blind prediction and an interpretative analysis of the second one.

58 GEOSCIENCES↗

A Decade of Innovative Approaches to Treating and Dispositioning Radioactive Waste at the Savannah River Site - 20620

This year marks the 70. anniversary of the U.S. Department of Energy's (DOE) Savannah River Site (SRS), located near Aiken, South Carolina. SRS is a key industrial complex responsible for environmental stewardship, environmental cleanup, waste management, and disposition of nuclear materials. SRS also continues to have a role in critical defense-related activities and the reprocessing of used reactor fuel. The SRS encompasses 803 square kilometers (310 square miles) in parts of Aiken, Barnwell, and Allendale counties. The Liquid Waste Mission starts with the safe receipt and storage of radioactive liquid waste in the waste tanks, which principally includes Cold War legacy waste, but also waste from support of National Aeronautics Space Administration missions, medical isotope production, and research activities. This 133,000 cubic meters (m{sup 3}) (35 million gallons [Mgal]) of high-level radioactive waste (HLW) is currently held in 43 large underground waste tanks. The capacity of each of these tanks range from 2,800 m{sup 3} to 5,000 m{sup 3} (0.75 to 1.33 Mgal) and were placed in operation between 1954 and 1986. In July 2009, the DOE awarded a stand-alone contract to execute the Liquid Waste Mission at SRS. The Liquid Waste Contractor selected was Savannah River Remediation LLC1 (SRR), which is responsible for receipt, storage, retrieval and treatment of all HLW, disposal of the decontaminated low-activity waste fraction, as well as operationally closing cleaned HLW tanks. Since July 2009, SRR has successfully grouted and operationally closed six large underground tanks, poured 1,476 canisters of vitrified HLW (a stable glass waste form), treated approximately 34,200 m{sup 3} (9.0 Mgal) of HLW, and dispositioned over 41,200 m{sup 3} (10.9 Mgal) of decontaminated salt solution as low-level waste (LLW) into the Saltstone Disposal Units (SDUs) being constructed by SRR on site. The innovative work performed by SRR in the LLW portion of its mission has earned it the Richard S. Hodes Award. The work conducted by SRR is the same work championed by the late Richard S. Hodes, a respected physician, statesmen, and Chairman of the Southeast Compact Commission for Low-Level Radioactive Waste Management. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A Tri-Port Current-Source Soft-Switching Medium-Voltage String Inverter for Large-Scale Solar-Plus-Storage Farms

This article presents a tri-port current-source soft-switching medium-voltage string inverter (TMVSI) to reduce the Levelized cost of energy (LCOE) of large-scale solar-plus-storage (SPS) farms. Throughout this work, the topology, operating principle, circuit simulation, control, and hardware design of the TMVSI are introduced. In addition, three key challenges compromising the performance of the TMVSI are addressed in this article. First, a new feed-forward compensation for model predictive control of the TMVSI is proposed to compensate for sampling and computational delay and high dc-link ripple with low computational cost and high scalability. Second, the use of laminated permanent magnets is proposed to reduce the losses of the MV medium-frequency transformer (MFT) in the TMVSI while increasing its saturation current. Finally, an improved U-shape winding pattern is proposed to decrease the leakage inductance of the MV MFT and reduce the voltage stress across semiconductor switches without adding cost or complexity. Here, the effectiveness of the TMVSI is validated by experiments at up to 20kW/500V in different test cases with custom-built prototypes. The contributions of this work make the TMVSI a viable solution to SPS farms and unleash its potential for LCOE reduction.

14 SOLAR ENERGY↗

Energetics of Base–Acid Pairs for the Design of High-Temperature Fuel Cell Polymer Electrolytes

The interaction energy of base–acid plays a key role in acid retention of phosphoric acid (PA)-doped polymer electrolytes under fuel cell operating conditions. Here, we investigate the energetics of proton-accepting and hydroxide-donating organic bases using density functional theory calculations. Because of their weak basicity, proton-accepting organic bases such as benzimidazole have relatively low interaction energy with the acid in the absence of water (15.3–28.0 kcal mol –1 ). Energetics of the proton-accepting base–PA complex increases by adding water, indicating that the interactions in the base–acid complex strengthen in the presence of water. On the other hand, hydroxide-donating organic bases, such as tetramethylammonium hydroxide, have high interaction energy with PA (~110 kcal mol –1 ), which remains high in the presence of water. The chemical shifts of 31P NMR support the energetics of the base–acid complexes. Overall, this study further discusses the benefit of incorporating hydroxide-donating organic bases into the polymeric structure over proton-accepting bases as a way to increase acid retention.

25 ENERGY STORAGE↗

Fracture Shearing in the Eau Claire Formation

This data set consists of Computed Tomographic (CT) data for five sheared Eau Claire Formation core samples with complex and heterogeneous lithology. Each sample was prefractured, housed in a specially adapted core holder, and sheared in incremental fashion. CT scans were taken before and after each shearing event.

Computed Tomography↗

Leveraging a Neural Network-Enhanced Reproducing Kernel Particle Method for Multiphysics Degradation Modeling of Energy Storage Materials

Energy storage materials exhibit strong electro-chemo-mechanical coupling and highly anisotropic material properties, contributing to the formation and propagation of micro-cracking during charge/discharge cycling and resulting in reduced performance and service life. A coupled electro-chemo-mechanical reproducing kernel particle method (RKPM) formulation has been developed to analyze this system. With microstructural images supplied by the National Renewable Energy Laboratory (NREL), pixel-based model construction by RKPM is used to represent the complex material microstructures that dictate the coupled physics of these systems. Traditional electro-chemo-mechanical models rely on mesh-based finite element methods, which can lead to difficulties in meshing such complex geometries and capturing crack propagation due to mesh dependency. Here, a neural network-enhanced reproducing kernel particle method (NN-RKPM) [1, 2] is introduced to effectively model damage and crack propagation in the material microstructures; the location, orientation, and solution transition near a localization are automatically captured by superimposed block-level NN optimizations. This NN enrichment approach allows for effective modeling of localizations via a fixed background discretization, relieving tedious efforts for adaptive refinement in traditional mesh-based methods. Applications to the heterogeneous microstructures of Li-ion battery cathodes will be presented to demonstrate the effectiveness of the proposed methods. NN-RKPM is additionally used to inform how crack opening and closure in turn affect the coupled chemical equations and material microstructure. Reference: [1] Baek, J., Chen, J. S., Susuki, K., "Neural Network enhanced Reproducing Kernel Particle Method for Modeling Localizations," International Journal for Numerical Methods in Engineering, Vol. 123, pp 4422-4454, https://doi.org/10.1002/nme.7040, 2022. [2] Baek, J., Chen, J. S., "A Neural Network-Based Enrichment of Reproducing Kernel Approximation for Modeling Brittle Fracture", Computer Methods in Applied Mechanics and Engineering Vol. 410, 116590, 2024.

degradation↗

Oxidation of Ammonia with Molecular Complexes

Oxidation of ammonia by molecular complexes is a burgeoning area of research. Several scientific challenges underpin these efforts, requiring a fundamental understanding of individual reactions steps, particularly for cleavage of N-H bonds and formation of N-N bonds. Overall, this perspective evaluates the challenges of designing molecular catalysts for oxidation of ammonia, and highlights recent key contributions to realizing the goals of viable energy storage and retrieval based on the N-H bonds of ammonia in a carbon-free energy cycle.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

In-situ experiment reveals CO2 enriched fluid migration in faulted caprock

Abstract The sealing characteristics of the geological formation located above a CO 2 storage reservoir, the so-called caprock, are essential to ensure efficient geological carbon storage. If CO 2 were to leak through the caprock, temporal changes in fluid geochemistry can reveal fundamental information on migration mechanisms and induced fluid–rock interactions. Here, we present the results from a unique in-situ injection experiment, where CO 2 -enriched fluid was continuously injected in a faulted caprock analogue. Our results show that the CO 2 migration follows complex pathways within the fault structure. The joint analysis of noble gases, ion concentrations and carbon isotopes allow us to quantify mixing between injected CO 2 -enriched fluid and resident formation water and to describe the temporal evolution of water–rock interaction processes. The results presented here are a crucial complement to the geophysical monitoring at the fracture scale highlighting a unique migration of CO 2 in fault zones.

Science & Technology - Other Topics↗

Hydrogen in disordered titania: connecting local chemistry, structure, and stoichiometry through accelerated exploration

Hydrogen incorporation in native surface oxides of metal alloys often controls the onset of metal hydriding, with implications for materials corrosion and hydrogen storage. A key representative example is titania, which forms as a passivating layer on a variety of titanium alloys for structural and functional applications. These oxides tend to be structurally diverse, featuring polymorphic phases, grain boundaries, and amorphous regions that generate a disparate set of unique local environments for hydrogen. Here, we introduce a workflow that can efficiently and accurately navigate this complexity. First, a machine learning force field, trained on ab initio molecular dynamics simulations, was used to generate amorphous configurations. Density functional theory calculations were then performed on these structures to identify local oxygen environments, which were compared against experimental observations. Second, to classify subtle differences across the disordered configuration space, we employ a graph-based sampling procedure. Finally, local hydrogen binding energies and hopping kinetics are computed using exhaustive density functional theory calculations on representative configurations. Here, we leverage this methodology to show that hydrogen binding energetics are described by local oxygen coordination, which in turn is affected by stoichiometry, and form the basis of hopping kinetics and diffusion. Together these results imply that hydrogen incorporation and transport in TiO x can be tailored through compositional engineering, with implications for improving the performance and durability of titanium-derived alloys in hydrogen environments.

36 MATERIALS SCIENCE↗

Influence of crossover on capacity fade of symmetric redox flow cells

Volumetrically unbalanced compositionally symmetric cell cycling with potentiostatic (CV) or galvanostatic-with-potential-hold (CCCV) protocols is a rigorous technique for evaluating the calendar lifetime of reactants for redox flow batteries. Here, we evaluate the influence of reactant crossover through the membrane on symmetric cell cycling behavior. We tested symmetric cells of anthraquinone disulfonic acid (AQDS) with Nafion membranes of varied thickness and manufacture (NR211, NR212, N115, and N117, ranging 25–183 μm). Membranes were tested both as-received and pretreated with a common procedure of soaking in water at elevated temperature and then in dilute hydrogen peroxide. We found no significant difference in capacity fade rates of symmetric cells with any of the membranes as-received, indicating a negligible influence of crossover. However, we observed increased capacity fade with increased permeability through pretreated membranes. Supported by zero-dimensional modeling and operando UV-vis spectrophotometry, we propose a mechanism for net crossover in AQDS symmetric cells based on a higher time-averaged concentration of quinhydrone dimers in the non-capacity limiting side (NCLS) compared to the capacity limiting side (CLS), driving net crossover of AQDS reactants out of the CLS. Further, we illustrate other hypothetical scenarios of net crossover using the zero-dimensional model. Overall, many membrane–electrolyte systems used in symmetric cell studies have sufficiently low crossover flux as to avoid the influence of crossover on capacity fade, but under conditions of higher crossover flux, complex interactions of crossover and chemical reactions may result in diverse capacity fade trajectories, the mechanisms of which may be untangled with operando characterization and modeling.

25 ENERGY STORAGE↗

Evaluation of Electron Tomography Capabilities for Shale Imaging

Despite the advantageous resolution of electron tomography (ET), reconstruction of three-dimensional (3D) images from multiple two-dimensional (2D) projections presents several challenges, including small signal-to-noise ratios, and a limited projection range. This study evaluates the capabilities of ET for thin sections of shale, a complex nanoporous medium. A numerical phantom with 1.24 nm pixel size is constructed based on the tomographic reconstruction of a Barnett shale. A dataset of 2D projection images is numerically generated from the 3D phantom and studied over a range of conditions. First, common reconstruction techniques are used to reconstruct the shale structure. The reconstruction uncertainty is quantified by comparing overall values of storage and transport metrics, as well as the misclassification of pore voxels compared to the phantom. We then select the most robust reconstruction technique and we vary the acquisition conditions to quantify the effect of artifacts. We find a strong agreement for large pores over the different acquisition workflows, while a wider variability exists for nanometer-scale features. Furthermore, the limited projection range and reconstruction are identified as the main experimental bottlenecks, thereby suggesting that sample thinning, advanced holders, and advanced reconstruction algorithms offer opportunities for improvement.

3D scanning transmission electron microscopy↗

Elucidating the Role of CO in the NO Storage Mechanism on Pd/SSZ-13 with in Situ DRIFTS

Pd ion exchanged zeolites emerged as promising materials for the adsorption and oxidation of air pollutants. For low-temperature vehicle exhaust, dispersed Pd ions are able to adsorb NO x even in H 2 O-rich exhaust in the presence of carbon monoxide. In order to understand this phenomenon, changes in Pd ligand environment have to be monitored in-situ. Herein, we directly observe the activation of hydrated Pd ion shielded by H 2 O into a carbonyl-nitrosyl complex Pd 2+ (NO)(CO) in SSZ-13 zeolite. The subsequent thermal desorption of ligands on Pd 2+ (NO)(CO) complex proceeds to nitrosyl Pd 2+ rather than to carbonyl Pd 2+ under various conditions. Thus, CO molecules act as additional ligands to provide alternative pathway through Pd 2+ (NO)(CO) complex with lower energy barrier for accelerating NO adsorption on hydrated Pd 2+ ion, which is kinetically limited in the absence of CO. We further demonstrate that hydration of Pd ions in the zeolite is a prerequisite for CO-induced reduction of Pd ions to metallic Pd. The reduction of Pd ions by CO is limited under dry conditions even at a high temperature of 500°C, while water makes it possible at near RT. However, the primary NO adsorption sites are Pd 2+ ions even in gases containing CO and water. These findings clarify additional mechanistic aspects of the passive NO x adsorption (PNA) process and will help extend the NOx adsorption chemistry in zeolite-based adsorbers to practical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effect of Charged Block Length Mismatch on Double Diblock Polyelectrolyte Complex Micelle Cores

Polyelectrolyte complex micelles are hydrophilic nanoparticles that self-assemble in aqueous environments due to associative microphase separation between oppositely charged blocky polyelectrolytes. In this work, we employ a suite of physical characterization tools to examine the effect of charged block length mismatch on the equilibrium structure of double diblock polyelectrolyte complex micelles (D-PCMs) by mixing a diverse library of peptide and synthetic charged-neutral block polyelectrolytes with a wide range of charged block lengths (25–200 units) and chemistries. Early work on D-PCMs suggested that this class of micelles can only be formed from blocky polyelectrolytes with identical charged block lengths, a phenomenon referred to as chain length recognition. Here, we use salt annealing to create PCMs at equilibrium, which shows that chain length recognition, a longstanding hurdle to repeatable self-assembly from mismatched polyelectrolytes, can be overcome. Interestingly, D-PCM structure–property relationships display a range of values that vary systematically with the charged block lengths and chemical identity of constituent polyelectrolyte pairings and cannot be described by generalizable scaling laws. We discuss the interdependent growth behavior of the radius, ionic pair aggregation number, and density in the micelle core for three chemically distinct diblock pairings and suggest a potential physical mechanism that leads to this unique behavior. By comparing the results of these D-PCMs to the scaling laws recently developed for single diblock polyelectrolyte complex micelles (S-PCMs: diblock + homopolymer), we observe that D-PCM design schemes reduce the size and aggregation number and restrict their growth to a function of charged block length relative to S-PCMs. Understanding these favorable attributes enables more predictive use of a wider array of charged molecular building blocks to anticipate and control macroscopic properties of micelles spanning countless storage and delivery applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Adsorption and reaction of methanol on Fe 3 O 4 (001)

The interaction of methanol with iron oxide surfaces is of interest due to its potential in hydrogen storage, and from a fundamental perspective as a chemical probe of the reactivity. We present here a study examining the adsorption and reaction of methanol on magnetite Fe 3 O 4 (001) at cryogenic temperatures using a combination of temperature programmed desorption, x-ray photoelectron spectroscopy, and scanning tunneling microscopy. We report the methanol desorption profile from Fe 3 O 4 (001) is complex, exhibiting peaks at 145, 175, 238, and 273 K, corresponding to the desorption of intact methanol, as well as peaks at 350 and 500 K due to the reaction of methoxy intermediates. The saturation of a monolayer of methanol corresponds to ~5 molecules/unit cell (u.c.), which is slightly higher than the number of surface octahedral iron atoms of 4/u.c. We probe the kinetics and thermodynamics of the desorption of molecular methanol using inversion analysis. The deconvolution of the complex desorption profile into individual peaks allows for calculations of both the desorption energy and the prefactor of each feature. The initial 0.7 methanol/u.c. reacts to form a methoxy and hydroxy intermediates by 180 K, which remains on the surface above room temperature after intact methanol has desorbed. The methoxy species react via one of two channels, a recombination reaction with surface hydroxyls to form additional methanol at ~350 K, and a disproportionation reaction to form methanol and formaldehyde at ~500 K. Only 20% of the methoxy species undergo the disproportionation reaction, with most of them reacting via the 350 K pathway.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Efficient ptychographic phase retrieval via a matrix-free Levenberg-Marquardt algorithm

The phase retrieval problem, where one aims to recover a complex-valued image from far-field intensity measurements, is a classic problem encountered in a range of imaging applications. Modern phase retrieval approaches usually rely on gradient descent methods in a nonlinear minimization framework. Calculating closed-form gradients for use in these methods is tedious work, and formulating second order derivatives is even more laborious. Additionally, second order techniques often require the storage and inversion of large matrices of partial derivatives, with memory requirements that can be prohibitive for data-rich imaging modalities. We use a reverse-mode automatic differentiation (AD) framework to implement an efficient matrix-free version of the Levenberg-Marquardt (LM) algorithm, a longstanding method that finds popular use in nonlinear least-square minimization problems but which has seen little use in phase retrieval. Furthermore, we extend the basic LM algorithm so that it can be applied for more general constrained optimization problems (including phase retrieval problems) beyond just the least-square applications. Since we use AD, we only need to specify the physics-based forward model for a specific imaging application; the first and second-order derivative terms are calculated automatically through matrix-vector products, without explicitly forming the large Jacobian or Gauss-Newton matrices typically required for the LM method. We demonstrate that this algorithm can be used to solve both the unconstrained ptychographic object retrieval problem and the constrained “blind” ptychographic object and probe retrieval problems, under the popular Gaussian noise model as well as the Poisson noise model. We compare this algorithm to state-of-the-art first order ptychographic reconstruction methods to demonstrate empirically that this method outperforms best-in-class first-order methods: it provides excellent convergence guarantees with (in many cases) a superlinear rate of convergence, all with a computational cost comparable to, or lower than, the tested first-order algorithms.

36 MATERIALS SCIENCE↗