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At least 865 records · Page 48

Towards Generalizable and Efficient Circuit Topology Design: A Graph-Transformer-based Surrogate Model with Curriculum Learning

Unlike circuit parameter and sizing optimizations, the automated design of analog circuit topologies poses significant challenges for learning-based approaches. One challenge arises from the combinatorial growth of the topology space with circuit size, which limits the topology optimization efficiency. Moreover, traditional circuit evaluation methods are time-consuming, while the presence of data discontinuity in the topology space makes the accurate prediction of circuit performance exceptionally difficult for unseen topologies. To tackle these challenges, we design a novel Graph-Transformer-based Network (GTN) as the surrogate model for circuit evaluation, offering a substantial acceleration in the speed of circuit topology optimization without sacrificing performance. Our GTN model architecture is designed to embed voltage changes in circuit loops and current flows in connected devices, enabling accurate performance predictions for circuits with unseen topologies. To address the cold start problem when scaling GTN to large-scale circuits, we further introduce a curriculum learning strategy that progressively trains GTN from small-scale to large-scale circuits. This approach enables the model to first learn fundamental physical principles from simpler topologies and gradually adapt to complex configurations, effectively bridging the circuit complexity gap and improving prediction accuracy. Taking the power converter circuit design as an experimental task, our GTN model significantly outperforms an analytical approach and baseline methods directly utilizing graph neural networks. Furthermore, GTN achieves less than 5% relative error and 196× speed-up compared with high-fidelity simulation. Notably, our GTN surrogate model empowers an automatic circuit design framework to discover circuits of comparable quality to those identified through high-fidelity simulation while reducing the time required by up to 98.2%. With curriculum learning, the enhanced GTN achieves a 51% improvement for performance prediction of large-scale circuits compared to the GTN model without this strategy. These advancements establish GTN as a scalable framework for automated analog circuit design across varying circuit complexity levels.

Lu, Haoshu [New Jersey Institute of Technology (NJ↗

Low- and intermediate-temperature oxidation of dimethyl ether up to 100 atm in a supercritical pressure jet-stirred reactor

Understanding the low- and intermediate-temperature oxidation chemistry of oxygenated fuels like dimethyl ether (DME) at high pressure is paramount to the development of advanced engines with low carbon emissions. The supercritical pressure jet-stirred reactor (SP-JSR) recently developed at Princeton provides a new platform for conducting kinetic studies at low and intermediate temperatures at extremely high pressures with a uniform temperature distribution and a short flow residence time. This paper uses the SP-JSR to investigate DME oxidation at equivalence ratios of 0.175, 1.0, and 1.72, for pressures of 10 and 100 atm, and temperatures ranging from 400 to 900 K. The results demonstrate weakened NTC behavior at 100 atm relative to 10 atm due to increased flux through QOOH + O 2 = O 2 QOOH relative to QOOH = 2 CH 2 O + OH at 100 atm. Furthermore, the intermediate-temperature oxidation window is shifted to lower temperatures at 100 atm. The experimental data are compared with several chemical kinetic models from the literature. The existing models are seen to agree quite well with the experimental data at 10 atm. However, the models fail to properly capture the NTC behavior at 100 atm. Reaction pathway analyses indicate that both the low- and intermediate-temperature chemistries are controlled by RO 2 consumption pathways. The reaction rates for several of the important reactions, such as DME + OH = CH 3 OCH 2 + H 2 O, H 2 O 2 (+M) = 2 OH (+M), and 2 HO 2 = 2 OH + O 2 are updated in this work. Furthermore, the updated model improves the predictability for all key species compared to the original model.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Flexible machine-learning interatomic potential for simulating structural disordering behavior of Li 7 La 3 Zr 2 O 12 solid electrolytes

Batteries based on solid-state electrolytes, including Li 7 La 3 Zr 2 O 12 (LLZO), promise improved safety and increased energy density; however, atomic disorder at grain boundaries and phase boundaries can severely deteriorate their performance. Machine-learning (ML) interatomic potentials offer a uniquely compelling solution for simulating chemical processes, rare events, and phase transitions associated with these complex interfaces by mixing high scalability with quantum-level accuracy, provided that they can be trained to properly address atomic disorder. To this end, we report the construction and validation of an ML potential that is specifically designed to simulate crystalline, disordered, and amorphous LLZO systems across a wide range of conditions. The ML model is based on a neural network algorithm and is trained using ab initio data. Performance tests prove that the developed ML potential can predict accurate structural and vibrational characteristics, elastic properties, and Li diffusivity of LLZO comparable to ab initio simulations. As a demonstration of its applicability to larger systems, we show that the potential can correctly capture grain boundary effects on diffusivity, as well as the thermal transition behavior of LLZO. Here these examples show that the ML potential enables simulations of transitions between well-defined and disordered structures with quantum-level accuracy at speeds thousands of times faster than ab initio methods.

25 ENERGY STORAGE↗

Automated identification and calculation of prompt effects in kinetic mechanisms using statistical models

The kinetics of prompt dissociation involves rovibrationally excited species (generally formed by exothermic reactions) which may dissociate or isomerize prior to thermalization via collisions with the bath gas. Treating such rovibrationally excited species (so-called "hot" species) with standard kinetic phenomenology may result in incorrect macroscopic representation of their reactivity. Here this work presents the first fully automated methodology for the calculation of prompt effects of a chosen species in a kinetic mechanism, including (i) reaction selection; (ii) theoretical calculation of rate constants and prompt branching fractions; and (iii) final rate constant fitting. The energy partition between hot fragments is estimated using a variety of statistical models, including a new physically sound microcanonical statistical model based on the rovibrational density of states of the fragments. The methodology is validated against literature data for the prompt dissociations of HCO and C 3 H 7 radicals. The microcanonical statistical model is in better agreement with trajectory simulations for larger species and is thus applicable for practical systems that typically involve large molecules, for which direct dynamics calculations are impractical. The automated workflow is applied to the evaluation of the effects of prompt dissociation for two isomeric radicals C 4 H 7 1-3 (1-methylallyl) and C 4 H 7 1-4 (3-buten-1-yl). Twelve H-atom abstraction reactions are selected and the corresponding rate constants are computed with first principles theory. The microcanonical statistical model predicts that prompt dissociations of C 4 H 7 1-3 and C 4 H 7 1-4 are already significant at 1000K, resulting in differences of up to an order of magnitude at 2000K with respect to the phenomenological thermal rate constants. To illustrate the effects of prompt dissociation on simulations of experimental data, the calculated prompt rate constants are implemented in both CRECK and C3MechV3.3 kinetic mechanisms. Simulations of experimental flame data illustrate the noticeable impact of prompt dissociation kinetics on the high-temperature combustion reactivity of C 4 H 8 -1 and C 4 H 8 -2.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

An experimental and modeling study on autoignition of 2-phenylethanol and its blends with n-heptane

2-Phenylethanol (2-PE) is an aromatic alcohol with high research octane number, high octane sensitivity, and a potential to be produced using biomass. Considering that 2-PE can be used as a fuel additive for boosting the anti-knocking quality of gasoline in spark-ignition engines and as the low reactivity fuel or fuel component in dual-fuel reactivity controlled compression ignition (RCCI) engines, it is of fundamental and practical interest to understand the autoignition chemistry of 2-PE, especially at low-to-intermediate temperatures (<1000 K). Based upon the experimental ignition delay time (IDT) results of neat 2-PE obtained from our previous rapid compression machine (RCM) investigation and the literature shock tube study, a detailed chemical kinetic model of 2-PE is developed herein, covering low-to-high temperature regimes. Besides, RCM experiments using binary fuel blends of 2-PE and n-heptane (nC7) are conducted in this work to investigate the nC7/2-PE blending effects, as they represent a dual-fuel system for RCCI operations. Furthermore, the newly developed 2-PE model is merged with a well-validated nC7 kinetic model to generate the current nC7/2-PE binary blend model. Overall, the consolidated model reasonably predicts the experimental IDT data of neat 2-PE and nC7/2-PE blends, as well as captures the experimental effects of pressure, equivalence ratio, and blending ratio on autoignition. Finally, model-based chemical kinetic analyses are carried out to understand and identify the controlling chemistry accounting for the observed blending effects in RCM experiments. In conclusion, the analyses reveal that nC7 enhances 2-PE autoignition via providing extra $\dot{O}$H radicals to the shared radical pool, while the diminished nC7 promoting effect on 2-PE autoignition with increasing temperature is due to the negative temperature coefficient characteristics of nC7.

2-phenlyethanol↗

MBX V1.2: Accelerating Data-Driven Many-Body Molecular Dynamics Simulations

The MBX software provides an advanced platform for molecular dynamics simulations, leveraging state-of-the-art MB-pol and MB-nrg data-driven many-body potential energy functions. Developed over the past decade, these potential energy functions integrate physics-based and machine-learned many-body terms trained on electronic structure data calculated at the "gold standard" coupled-cluster level of theory. Recent advancements in MBX have focused on optimizing its performance, resulting in the release of MBX v1.2. While the inherently many-body nature of MB-pol and MB-nrg ensures high accuracy, it poses computational challenges. MBX v1.2 addresses these challenges with significant performance improvements, including enhanced parallelism that fully harnesses the power of modern multicore CPUs. In conclusion, these advancements enable simulations on nanosecond time scales for condensed-phase systems, significantly expanding the scope of high-accuracy, predictive simulations of complex molecular systems powered by data-driven many-body potential energy functions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A quantitative model for a nanoscale switch accurately predicts thermal actuation behavior

Manipulation of temperature can be used to actuate DNA origami nano-hinges containing gold nanoparticles. We develop a physical model of this system that uses partition function analysis of the interaction between the nano-hinge and nanoparticle to predict the probability that the nano-hinge is open at a given temperature. The model agrees well with experimental data and predicts experimental conditions that allow the actuation temperature of the nano-hinge to be tuned over a range of temperatures from 30 °C to 45 °C. Additionally, the model identifies microscopic interactions that are important to the macroscopic behavior of the system, revealing surprising features of the system. This combination of physical insight and predictive potential is likely to inform future designs that integrate nanoparticles into dynamic DNA origami structures or use strand binding interactions to control dynamic DNA origami behavior. Furthermore, our modeling approach could be expanded to consider the incorporation, stability, and actuation of other types of functional elements or actuation mechanisms integrated into nucleic acid devices.

36 MATERIALS SCIENCE↗

Comparative and Cost Analysis of a Novel Predictive Power Ramp Rate Control Method: A Case Study in a PV Power Plant in Puerto Rico

One of the most important aspects that need to be addressed to increase solar energy penetration is the power ramp-rate control. In weak grids such as the one found in Puerto Rico, it is important to smooth power fluctuations caused by the intermittence of passing clouds. In this work, a novel power ramp-rate control strategy is proposed. Additionally, a comparison with some of the most common power ramp-rate control methods is performed using a proposed model and real solar radiation data from the Coto Laurel photovoltaic power plant located in Ponce, Puerto Rico. The proposed model was validated using one-year real data from Coto Laurel. The power ramp-rate control methods were compared in real-time simulations using the OP5700 from Opal-RT Technologies considering power ramp rate fluctuations, power ramp-rate violations, fluctuations in the state-of-charge, among other indicators. Moreover, the proposed power ramp-rate control strategy, called predictive dynamic smoothing was explained and compared. Results indicate that the predictive dynamic smoothing produced a considerably reduced Levelized Cost of Storage compared to other power ramp-rate control methods and provided a higher lifetime expectancy for lithium batteries.

36 MATERIALS SCIENCE↗

Assessment of Cloud-based Applications for Enabling a Scalable Riskinformed Predictive Maintenance Strategy

The current light-water reactor fleet uses time-based maintenance strategies to achieve high-capacity factors. But to make nuclear more competitive in the energy market, these reactors could utilize emerging artificial intelligence (AI) and cloud computing technologies to achieve a cost-effective, predictive-maintenance strategy. This paper presents discussion and results on the application of cloud computing in the nuclear industry. The technical viability of cloud computing was analyzed using data from a boiling-water reactor’s safety relief valve. The models were hosted on three different systems: a local personal computer, Idaho National Laboratory’s high-performance computer system, and Microsoft Azure. The data were loaded and processed, and two types of models were trained in an A/B fashion. Based on the speed at which these actions were completed, it was determined that cloud computing affords adequate computing resources. Additionally, the computing power can scale with the demanded load. To enable cloud computing in the existing fleet, additional sensors, networks, and other requirements must be implemented to ensure a smooth transition from current maintenance strategies. However, the benefit is that the plants no longer need to manage their own servers, software, cybersecurity, and information technology support staff for in-house data analytics purpose. Many of these features can be offloaded to the cloud provider for a potential cost savings. Demonstrating how AI can improve the maintenance and operation of non-safety-related systems seems the likely path forward for implementing AI and cloud computing resources inside nuclear power plants.

azure↗

COCOMO2: A Coarse-Grained Model for Interacting Folded and Disordered Proteins

Biomolecular interactions are essential in many biological processes, including complex formation and phase separation processes. Coarse-grained computational models are especially valuable for studying such processes via simulation. Here, we present COCOMO2, an updated residue-based coarse-grained model that extends its applicability from intrinsically disordered peptides to folded proteins. This is accomplished with the introduction of a surface exposure scaling factor, which adjusts interaction strengths based on solvent accessibility, to enable the more realistic modeling of interactions involving folded domains without additional computational costs. COCOMO2 was parametrized directly with solubility and phase separation data to improve its performance on predicting concentration-dependent phase separation for a broader range of biomolecular systems compared to the original version. COCOMO2 enables new applications including the study of condensates that involve IDPs together with folded domains and the study of complex assembly processes. COCOMO2 also provides an expanded foundation for the development of multiscale approaches for modeling biomolecular interactions that span from residue-level to atomistic resolution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermochemical Data Fusion Using Graph Representation Learning

Large databases are required for “Big Data” applications in catalysis and materials science. Thermochemical databases can be created by combining data from various sources and by correcting low-fidelity datasets to higher accuracy with minimal computation. To achieve this “data fusion”, thermochemical quantities of interest, calculated at various levels of density functional theory (DFT), need to be mapped to the same, high levels of theory. In this work, a graph theoretical, statistical framework is proposed for such tasks. Subgraph frequencies are shown to provide a natural representation for learning these fusion maps. The maps are linear and are learnt with automated descriptor selection. Using a dataset of as few as ~1% from the QM9 database of 133,885 molecules, these models can predict multiple thermochemical quantities at a higher level of theory with an accuracy of 1 kcal/mol. Here, the method is explainable, generalizable, and provides a diagnostic tool for outlier identification

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

MultiTaskDeltaNet: change detection-based image segmentation for operando ETEM with application to carbon gasification kinetics

Transforming in situ transmission electron microscopy (TEM) imaging into a tool for spatially-resolved operando characterization of solid-state reactions requires automated, high-precision semantic segmentation of dynamically evolving features. However, traditional deep learning methods for semantic segmentation often face limitations due to the scarcity of labeled data, visually ambiguous features of interest, and scenarios involving small objects. To tackle these challenges, we introduce MultiTaskDeltaNet (MTDN), a novel deep learning architecture that creatively reconceptualizes the segmentation task as a change detection problem. By implementing a unique Siamese network with a U-Net backbone and using paired images to capture feature changes, MTDN effectively leverages minimal data to produce high-quality segmentations. Furthermore, MTDN utilizes a multi-task learning strategy to exploit correlations between physical features of interest. In an evaluation using data from in situ environmental TEM (ETEM) videos of filamentous carbon gasification, MTDN demonstrated a significant advantage over conventional segmentation models, particularly in accurately delineating fine structural features. Notably, MTDN achieved a 10.22% performance improvement over conventional segmentation models in predicting small and visually ambiguous physical features. This work bridges key gaps between deep learning and practical TEM image analysis, advancing automated characterization of nanomaterials in complex experimental settings.

08 HYDROGEN↗

Spectrophotometric determination of the stability of La hydroxyl complexes at near neutral to alkaline pH from 25 to 75 °C

The hydrolysis of rare earth elements (REE) potentially controls their mobility during fluid-rock interaction in a broad range of pH and temperature conditions. However, there is still a lack of thermodynamic data for modeling accurately the stability of REE hydroxyl complexes in hydrothermal aqueous fluids. Here, in this study, UV–Vis spectrophotometric experiments were conducted from 25 to 75 °C in near-neutral to alkaline NaOH-bearing aqueous solutions with varying lanthanum (La) concentrations (0 to ∼0.23 mmol/kg). The color indicator m-cresol purple was used to determine in situ pH and derive the average OH− ligand number ($\overrightarrow{n}$) and formation constants for the La hydroxyl complexes (LaOH 2+ , La(OH) 2 + , and La(OH) 3 0 ). From 25 to 50 °C, $\overrightarrow{n}$ ranges between ∼1 and 2 at pH from 7.0 to 9.3. At 75 °C, $\overrightarrow{n}$ ranges between ∼1.5 and 3 at pH from 6.3 to 8.8. These results suggest the predominance of LaOH 2+ and La(OH) 2 + complexes from 25 to 50 °C, and an increased predominance of La(OH) 3 0 at 75 °C. The cumulative formation constants (β n °, n = 1 to 3) are derived for the reaction La 3+ + nOH − = La(OH) n 3-n , and fitted between 25 and 250 °C by combining the UV–Vis and literature solubility data. The resulting logβ n ° are expressed as function of temperature (T in Kelvin): logβ 1 ° = −1.786 + 0.0133 T + 1.049·10 3 /T; logβ 2 ° = −5.797 + 0.0267 T + 2.713·10 3 /T; logβ 3 ° = 6.435 + 0.0223 T + 512.7/T. A comparison between these new fits and existing extrapolations using the Helgeson-Kirkham-Flowers equation of state indicates significant differences in the predicted hydrolysis of La. The latter extrapolations should therefore be updated for the hydrolysis of REE.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Kinetic Model for Predicting Trace Gas Uptake and Reaction

A model is developed to describe trace gas uptake and reaction with applications to aerosols and microdroplets. Gas uptake by the liquid is formulated as a coupled equilibria that links gas, surface, and bulk regions of the droplet or solution. Previously, this framework was used in explicit stochastic reaction-diffusion simulations to predict the reactive uptake kinetics of ozone with droplets containing aqueous aconitic acid, maleic acid, and sodium nitrite. With the use of prior data and simulation results, a new equation for the uptake coefficient is derived, which accounts for both surface and bulk reactions. Lambert W functions are used to obtain closed form solutions to the integrated rate laws for the multiphase kinetics; similar to previous expressions that describe Michaelis-Menten enzyme kinetics. Together these equations couple interface and bulk processes over a wide range of conditions and do not require many of the limiting assumptions needed to apply resistor model formulations to explain trace gas uptake and reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Machine learning using host/guest energy histograms to predict adsorption in metal–organic frameworks: Application to short alkanes and Xe/Kr mixtures

A machine learning (ML) methodology that uses a histogram of interaction energies has been applied to predict gas adsorption in metal–organic frameworks (MOFs) using results from atomistic grand canonical Monte Carlo (GCMC) simulations as training and test data. In this work, the method is first extended to binary mixtures of spherical species, in particular, Xe and Kr. In addition, it is shown that single-component adsorption of ethane and propane can be predicted in good agreement with GCMC simulation using a histogram of the adsorption energies felt by a methyl probe in conjunction with the random forest ML method. Here, the results for propane can be improved by including a small number of MOF textural properties as descriptors. We also discuss the most significant features, which provides physical insight into the most beneficial adsorption energy sites for a given application.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Bringing chemical structures to life with augmented reality, machine learning, and quantum chemistry

Visualizing 3D molecular structures is crucial to understanding and predicting their chemical behavior. However, static 2D hand-drawn skeletal structures remain the preferred method of chemical communication. Here, we combine cutting-edge technologies in augmented reality (AR), machine learning, and computational chemistry to develop MolAR, an open-source mobile application for visualizing molecules in AR directly from their hand-drawn chemical structures. Users can also visualize any molecule or protein directly from its name or protein data bank ID and compute chemical properties in real time via quantum chemistry cloud computing. MolAR provides an easily accessible platform for the scientific community to visualize and interact with 3D molecular structures in an immersive and engaging way.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Toward Guided Mutagenesis: Gaussian Process Regression Predicts MHC Class II Antigen Mutant Binding

Antigen-specific immunotherapies (ASI) require successful loading and presentation of antigen peptides into the major histocompatibility complex (MHC) binding cleft. One route of ASI design is to mutate native antigens for either stronger or weaker binding interaction to MHC. Exploring all possible mutations is costly both experimentally and computationally. To reduce experimental and computational expense, here we investigate the minimal amount of prior data required to accurately predict the relative binding affinity of point mutations for peptide-MHC class II (pMHCII) binding. Using data from different residue subsets, we interpolate pMHCII mutant binding affinities by Gaussian process (GP) regression of residue volume and hydrophobicity. We apply GP regression to an experimental data set from the Immune Epitope Database, and theoretical data sets from NetMHCIIpan and Free Energy Perturbation calculations. We find that GP regression can predict binding affinities of nine neutral residues from a six-residue subset with an average R 2 coefficient of determination value of 0.62 ± 0.04 (±95% CI), average error of 0.09 ± 0.01 kcal/mol (±95% CI), and with an receiver operating characteristic (ROC) AUC value of 0.92 for binary classification of enhanced or diminished binding affinity. Similarly, metrics increase to an R2 value of 0.69 ± 0.04, average error of 0.07 ± 0.01 kcal/mol, and an ROC AUC value of 0.94 for predicting seven neutral residues from an eight-residue subset. Our work finds that prediction is most accurate for neutral residues at anchor residue sites without register shift. This work holds relevance to predicting pMHCII binding and accelerating ASI design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Improving the reliability of machine learned potentials for modeling inhomogeneous liquids

The atomic-scale response of inhomogeneous fluids at interfaces and surrounding solute particles plays a critical role in governing chemical, electrochemical, and biological processes. Classical molecular dynamics simulations have been applied extensively to simulate the response of fluids to inhomogeneities directly, but are limited by the accuracy of the underlying interatomic potentials. Here, we use neural network potentials (NNPs) trained to ab initio simulations to accurately predict the inhomogeneous responses of two distinct fluids: liquid water and molten NaCl. Although NNPs can be readily trained to model complex bulk systems across a range of state points, we show that to appropriately model a fluid's response at an interface, relevant inhomogeneous configurations must be included in the training data. In order to sufficiently sample appropriate configurations of such inhomogeneous fluids, we develop protocols based on molecular dynamics simulations in the presence of external potentials. We demonstrate that NNPs trained on inhomogeneous fluid configurations can more accurately predict several key properties of fluids—including the density response, surface tension and size-dependent cavitation free energies—for liquid water and molten NaCl, compared to both empirical interatomic potentials and NNPs that are not trained on such inhomogeneous configurations. This work therefore provides a first demonstration and framework to extract the response of inhomogeneous fluids from first principles for classical density-functional treatment of fluids free from empirical potentials.

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