We integrate theoretical, computational and data-driven approaches for the sake of understanding, design and discovery of metal based catalysts. Firstly, we develop theoretical frameworks for predicting electronic descriptors of transition and noble metal alloys, including a physics model of d-band center, and a tight-binding theory of d-band moments to systematically elucidate the distinct electronic structures of novel catalysts. Within this framework, the hybridization of semi-empirical theories with graph neural network and attribution analysis enables accurate prediction equipped with mechanistic insights. In addition, novel physics effect controlling surface reactivity beyond conventional understanding is uncovered. Secondly, we develop a computational and data-driven framework to model high entropy alloy (HEA) catalysis, incorporating thermodynamic descriptor-based phase stability evaluation, surface segregation modeling by deep learning potential-driven molecular simulation and activity prediction through machine learning-embedded electrokinetic model. With this framework, we successfully elucidate the experimentally observed improved activity of PtPdCuNiCo HEA in oxygen reduction reaction. Thirdly, a Bayesian optimization framework is employed to optimize racemic lactide polymerization by searching for stereoselective aluminum (Al) -complex catalysts. We identified multiple new Al-complex molecules that catalyzed either isoselective or heteroselective polymerization. In addition, feature attribution analysis uncovered mechanistically meaningful ligand descriptors that can access quantitative and predictive models for catalyst development. / Doctor of Philosophy / In addressing the critical issues of climate change, energy scarcity, and pollution, the drive towards a sustainable economy has made catalysis a key area of focus. Computational chemistry has revolutionized our understanding of catalysts, especially in identifying and analyzing their active sites. Furthermore, the integration of open-access data and advanced computing has elevated data science as a crucial component in catalysis research. This synergy of computational and data-driven approaches is advancing the development of innovative catalytic materials, marking a significant stride in tackling environmental challenges. In my PhD research, I mainly work on the development of computational and data-driven methods for better understanding, design and discovery of catalytic materials. Firstly, I develop physics models for people to intuitively understand the reactivity of transition and noble metal catalysts. Then I embed the physics models into deep learning models for accurate and insightful predictions. Secondly, for a class of complex metal catalysts called high-entropy alloy (HEA) which is hard to model, I develop a modeling framework by hybridizing computational and data-driven approaches. With this framework, we successfully elucidate the experimentally observed improved activity of PtPdCuNiCo HEA in oxygen reduction reaction which is a key reaction in fuel cell technology. Thirdly, I develop a framework to virtually screen catalyst molecules to optimize polymerization reaction and provide potential candidates to our experimental collaborator to synthesize. Our collaboration leads to the discovery of novel high-performance molecular catalysts.

<div>Neuromorphic systems promise a novel alternative to the standard von-Neumann architectures that are computationally expensive for analyzing big data, and are not efficient for learning and inference. This novel generation of computing aims at ``mimicking" the human brain based on deploying neural networks on event-driven hardware architectures. A key bottleneck in designing such brain-inspired architectures is the complexity of co-optimizing the algorithm’s speed and accuracy along with the hardware’s performance and energy efficiency. This complexity stems from numerous intrinsic hyperparameters in both software and hardware that need to be optimized for an optimum design.</div><div><br></div><div>In this work, we present a versatile hierarchical pseudo agent-based multi-objective hyperparameter optimization approach for automatically tuning the hyperparameters of several training algorithms (such as traditional artificial neural networks (ANN), and evolutionary-based, binary, back-propagation-based, and conversion-based techniques in spiking neural networks (SNNs)) on digital and mixed-signal neural accelerators. By utilizing the proposed hyperparameter optimization approach we achieve improved performance over the previous state-of-the-art on those training algorithms and close some of the performance gaps that exist between SNNs and standard deep learning architectures.</div><div><br></div><div>We demonstrate >2% improvement in accuracy and more than 5X reduction in the training/inference time for a back-propagation-based SNN algorithm on the dynamic vision sensor (DVS) gesture dataset. In the case of ANN-SNN conversion-based techniques, we demonstrate 30% reduction in time-steps while surpassing the accuracy of state-of-the-art networks on an image classification dataset (CIFAR10) on a simpler and shallower architecture. Further, our analysis shows that in some cases even a seemingly minor change in hyperparameters may change the accuracy of these networks by 5‑6X. From the application perspective, we show that the optimum set of hyperparameters might drastically improve the performance (52% to 71% for Pole-Balance control application). In addition, we demonstrate resiliency of different input/output encoding, training neural network, or the underlying accelerator modules in a neuromorphic system to the changes of the hyperparameters.</div>

Indiana University-Purdue University Indianapolis (IUPUI) / In the last years, lithium-ion batteries (LIBs) have become the most important energy storage system for consumer electronics, electric vehicles, and smart grids. The development of lithium-ion batteries (LIBs) based on current practice allows an energy density increase estimated at 10% per year. However, the required power for portable electronic devices is predicted to increase at a much faster rate, namely 20% per year. Similarly, the global electric vehicle battery capacity is expected to increase from around 170 GWh per year today to 1.5 TWh per year in 2030--this is an increase of 125% per year. Without a breakthrough in battery design technology, it will be difficult to keep up with the increasing energy demand. To that end, a design methodology to accelerate the LIB development is needed. This can be achieved through the integration of electro-chemical numerical simulations and machine learning algorithms. To help this cause, this study develops a design methodology and framework using Simcenter Battery Design Studio® (BDS) and Bayesian optimization for design and optimization of cylindrical cell type 18650. The materials of the cathode are Nickel-Cobalt-Aluminum (NCA)/Nickel-Manganese-Cobalt-Aluminum (NMCA), anode is graphite, and electrolyte is Lithium hexafluorophosphate (LiPF6). Bayesian optimization has emerged as a powerful gradient-free optimization methodology to solve optimization problems that involve the evaluation of expensive black-box functions. The black-box functions are simulations of the cyclic performance test in Simcenter Battery Design Studio. The physics model used for this study is based on full system model described by Fuller and Newman. It uses Butler-Volmer Equation for ion-transportation across an interface and solvent diffusion model (Ploehn Model) for Aging of Lithium-Ion Battery Cells. The BDS model considers effects of SEI, cell electrode and microstructure dimensions, and charge-discharge rates to simulate battery degradation. Two objectives are optimized: maximization of the specific energy and minimization of the capacity fade. We perform global sensitivity analysis and see that thickness and porosity of the coating of the LIB electrodes that affect the objective functions the most. As such the design variables selected for this study are thickness and porosity of the electrodes. The thickness is restricted to vary from 22microns to 240microns and the porosity varies from 0.22 to 0.54. Two case studies are carried out using the above-mentioned objective functions and parameters. In the first study, cycling tests of 18650 NCA cathode Li-ion cells are simulated. The cells are charged and discharged using a constant 0.2C rate for 500 cycles. In the second case study a cathode active material more relevant to the electric vehicle industry, Nickel-Manganese-Cobalt-Aluminum (NMCA), is used. Here, the cells are cycled for 5 different charge-discharge scenarios to replicate charge-discharge scenario that an EVs battery module experiences. The results show that the design and optimization methodology can identify cells to satisfy the design objective that extend and improve the pareto front outside the original sampling plan for several practical charge-discharge scenarios which maximize energy density and minimize capacity fade.

No description available.

Ces travaux sur la stabilisation de la Ligne de Visée d’un dispositif optronique s’inscrivent dans le contexte actuel de durcissement des exigences de stabilisation et de réduction du temps accordé à la synthèse des lois de commande.Ils incluent dans un premier temps l’amélioration de la performance intrinsèque de stabilisation du système. La solution proposée ici est l’ajout d’un étage de stabilisation supplémentaire à une structure de stabilisation existante. L’architecture de ce nouvel étage est définie. Les composants sont choisis parmi les technologies existantes puis caractérisés expérimentalement. Un modèle complet du système à deux étages de stabilisation est ensuite proposé.L’objectif de ces travaux comprend également la simplification des procédures d’élaboration des lois de commande par l’utilisation d’une fonction de coût F incluant notamment la Fonction de Transfert de Modulation (qui quantifie le flou introduit par l’erreur de stabilisation dans l’image) en lieu et place ducritère dérivé usuel qui nécessite des vérifications supplémentaires et qui peut s’avérer conservatif.L’évaluation de F étant coûteuse en temps de calcul, un algorithme d’optimisation bayésienne, adapté à l’optimisation des fonctions coûteuses, permet la synthèse des lois de commande du système dans un temps compatible avec les contraintes industrielles, à partir de la modélisation du système précédemment proposée. / The presented work on the Line of Sight stabilization of an optronic device meets the heightened demands regarding stabilization performances that come with the reduction of the time allowed to controller tuning.It includes the intrinsinc improvement of the system stabilization. The proposed solution features a double stabilization stage built from a single stabilization stage existing system. The new architecture is specified and the new components are chosen among the existing technology and experimentally characterized. A complete double stabilization stage model is then proposed.The simplification of the controller tuning process is another goal. The designed cost function F includes a high-level optronic criterion, the Modulation Transfer Function (that quantifies the level of blur broughtinto the image by the residual motion of the platform) instead of the usual low-level and potentially conservative criterion.The function F is costly to evaluate. In order to tune the controller parameters within industrial time constraints, a Bayesian algorithm, adapted to optimization with a reduced budget of evaluations, is implemented.Controllers of both stabilization stages are simultaneously tuned thanks to the previously developped system model.

<p>  </p> <p>In the last years, lithium-ion batteries (LIBs) have become the most important energy storage system for consumer electronics, electric vehicles, and smart grids. The development of lithium-ion batteries (LIBs) based on current practice allows an energy density increase estimated at 10% per year. However, the required power for portable electronic devices is predicted to increase at a much faster rate, namely 20% per year. Similarly, the global electric vehicle battery capacity is expected to increase from around 170 GWh per year today to 1.5 TWh per year in 2030--this is an increase of 125% per year. Without a breakthrough in battery design technology, it will be difficult to keep up with the increasing energy demand. To that end, a design methodology to accelerate the LIB development is needed. This can be achieved through the integration of electro-chemical numerical simulations and machine learning algorithms.</p> <p><br></p> <p>To help this cause, this study develops a design methodology and framework using Simcenter Battery Design Studio® (BDS) and Bayesian optimization for design and optimization of cylindrical cell type 18650. The materials of the cathode are Nickel-Cobalt-Aluminum (NCA)/Nickel-Manganese-Cobalt-Aluminum (NMCA), anode is graphite, and electrolyte is Lithium hexafluorophosphate (LiPF6). Bayesian optimization has emerged as a powerful gradient-free optimization methodology to solve optimization problems that involve the evaluation of expensive black-box functions. The black-box functions are simulations of the cyclic performance test in Simcenter Battery Design Studio. </p> <p>The physics model used for this study is based on full system model described by Fuller and Newman. It uses Butler-Volmer Equation for ion-transportation across an interface and solvent diffusion model (Ploehn Model) for Aging of Lithium-Ion Battery Cells. The BDS model considers effects of SEI, cell electrode and microstructure dimensions, and charge-discharge rates to simulate battery degradation. Two objectives are optimized: maximization of the specific energy and minimization of the capacity fade. We perform global sensitivity analysis and see that thickness and porosity of the coating of the LIB electrodes that affect the objective functions the most. As such the design variables selected for this study are thickness and porosity of the electrodes. The thickness is restricted to vary from 22 micron to 240 microns and the porosity varies from 0.22 to 0.54. </p> <p>Two case studies are carried out using the above-mentioned objective functions and parameters. In the first study, cycling tests of 18650 NCA cathode Li-ion cells are simulated. The cells are charged and discharged using a constant 0.2C rate for 500 cycles. In the second case study a cathode active material more relevant to the electric vehicle industry, Nickel-Manganese-Cobalt-Aluminum (NMCA), is used. Here, the cells are cycled for 5 different charge-discharge scenarios to replicate charge-discharge scenario that an EVs battery module experiences. The results show that the design and optimization methodology can identify cells to satisfy the design objective that extend and improve the pareto front outside the original sampling plan for several practical charge-discharge scenarios which maximize energy density and minimize capacity fade. </p>

<p>The document describes the computational framework to optimize spring-driven Autoinjectors. It involves Bayesian Optimization for efficient and cost-effective design of Autoinjectors.</p>

Many algorithms today require a number of parameters to be set in order to perform well in a given application. The tuning of these parameters is often difficult and tedious to do manually, especially when the number of parameters is large. It is also unlikely that a human can find the best possible solution for difficult problems. To be able to automatically find good sets of parameters could both provide better results and save a lot of time. The prominent methods Bayesian optimization and Covariance Matrix Adaptation Evolution Strategy (CMA-ES) are evaluated for automatic parameter tuning in localization algorithms in this work. Both methods are evaluated using a localization algorithm on different datasets and compared in terms of computational time and the precision and recall of the final solutions. This study shows that it is feasible to automatically tune the parameters of localization algorithms using the evaluated methods. In all experiments performed in this work, Bayesian optimization was shown to make the biggest improvements early in the optimization but CMA-ES always passed it and proceeded to reach the best final solutions after some time. This study also shows that automatic parameter tuning is feasible even when using noisy real-world data collected from 3D cameras.

<div>Researchers and scientists across various areas face the perennial challenge of selecting experimental conditions or inputs for computer simulations in order to achieve promising results.</div><div> The aim of conducting these experiments could be to study the production of a material that has great applicability.</div><div> One might also be interested in accurately modeling and analyzing a simulation of a physical process through a high-fidelity computer code.</div><div> The presence of noise in the experimental observations or simulator outputs, called aleatory uncertainty, is usually accompanied by limited amount of data due to budget constraints.</div><div> This gives rise to what is known as epistemic uncertainty. </div><div> This problem of designing of experiments with limited number of allowable experiments or simulations under aleatory and epistemic uncertainty needs to be treated in a Bayesian way.</div><div> The aim of this thesis is to extend the state-of-the-art in Bayesian optimal design of experiments where one can optimize and infer statistics of the expensive experimental observation(s) or simulation output(s) under uncertainty.</div>

Ce travail de thèse porte sur le développement d’une méthodologie efficace pour la conception analogique, des algorithmes et des outils correspondants qui peuvent être utilisés dans la conception dynamique de fonctions linéaires à temps continu. L’objectif principal est d’assurer que les performances pour un système complet peuvent être rapidement investiguées, mais avec une précision comparable aux évaluations au niveau transistor.Une première direction de recherche a impliqué le développement de la méthodologie de conception basée sur le processus d'optimisation automatique de cellules au niveau transistor et la synthèse de macro-modèles analogiques de haut niveau dans certains environnements comme Mathworks - Simulink, VHDL-AMS ou Verilog-A. Le processus d'extraction des macro-modèles se base sur un ensemble complet d'analyses (DC, AC, transitoire, paramétrique, Balance Harmonique) qui sont effectuées sur les schémas analogiques conçues à partir d’une technologie spécifique. Ensuite, l'extraction et le calcul d'une multitude de facteurs de mérite assure que les modèles comprennent les caractéristiques de bas niveau et peuvent être directement régénéré au cours de l'optimisation.L'algorithme d'optimisation utilise une méthode bayésienne, où l'espace d’évaluation est créé à partir d'un modèle de substitution (krigeage dans ce cas), et la sélection est effectuée en utilisant le critère d’amélioration (Expected Improvement - EI) sujet à des contraintes. Un outil de conception a été développé (SIMECT), qui a été intégré comme une boîte à outils Matlab, employant les algorithmes d’extraction des macro-modèles et d'optimisation automatique. / The aim of this thesis is to establish an efficient analog design methodology, the algorithms and the corresponding design tools which can be employed in the dynamic conception of linear continuous-time (CT) functions. The purpose is to assure that the performance figures for a complete system can be rapidly investigated, but with comparable accuracy to the transistor-level evaluations. A first research direction implied the development of the novel design methodology based on the automatic optimization process of transistor-level cells using a modified Bayesian Kriging approach and the synthesis of robust high-level analog behavioral models in environments like Mathworks – Simulink, VHDL-AMS or Verilog-A.The macro-model extraction process involves a complete set of analyses (DC, AC, transient, parametric, Harmonic Balance) which are performed on the analog schematics implemented on a specific technology process. Then, the extraction and calculus of a multitude of figures of merit assures that the models include the low-level characteristics and can be directly regenerated during the optimization process.The optimization algorithm uses a Bayesian method, where the evaluation space is created by the means of a Kriging surrogate model, and the selection is effectuated by using the expected improvement (EI) criterion subject to constraints.A conception tool was developed (SIMECT), which was integrated as a Matlab toolbox, including all the macro-models extraction and automatic optimization techniques.