Computational catalysis is playing an increasingly significant role in the design of catalysts across a wide range of applications. A common task for many computational methods is the need to accurately compute the minimum binding energy - the adsorption energy - for an adsorbate and a catalyst surface of interest. Traditionally, the identification of low energy adsorbate-surface configurations relies on heuristic methods and researcher intuition. As the desire to perform high-throughput screening increases, it becomes challenging to use heuristics and intuition alone. In this paper, we demonstrate machine learning potentials can be leveraged to identify low energy adsorbate-surface configurations more accurately and efficiently. Our algorithm provides a spectrum of trade-offs between accuracy and efficiency, with one balanced option finding the lowest energy configuration, within a 0.1 eV threshold, 86.63% of the time, while achieving a 1387x speedup in computation. To standardize benchmarking, we introduce the Open Catalyst Dense dataset containing nearly 1,000 diverse surfaces and 87,045 unique configurations.
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機器學習（Machine Learning）是一個研究計算學習方法的國際論壇。該雜志發表文章，報告廣泛的學習方法應用于各種學習問題的實質性結果。該雜志的特色論文描述研究的問題和方法，應用研究和研究方法的問題。有關學習問題或方法的論文通過實證研究、理論分析或與心理現象的比較提供了堅實的支持。應用論文展示了如何應用學習方法來解決重要的應用問題。研究方法論文改進了機器學習的研究方法。所有的論文都以其他研究人員可以驗證或復制的方式描述了支持證據。論文還詳細說明了學習的組成部分，并討論了關于知識表示和性能任務的假設。
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During the past decades, evolutionary computation (EC) has demonstrated promising potential in solving various complex optimization problems of relatively small scales. Nowadays, however, ongoing developments in modern science and engineering are bringing increasingly grave challenges to the conventional EC paradigm in terms of scalability. As problem scales increase, on the one hand, the encoding spaces (i.e., dimensions of the decision vectors) are intrinsically larger; on the other hand, EC algorithms often require growing numbers of function evaluations (and probably larger population sizes as well) to work properly. To meet such emerging challenges, not only does it require delicate algorithm designs, but more importantly, a high-performance computing framework is indispensable. Hence, we develop a distributed GPU-accelerated algorithm library -- EvoX. First, we propose a generalized workflow for implementing general EC algorithms. Second, we design a scalable computing framework for running EC algorithms on distributed GPU devices. Third, we provide user-friendly interfaces to both researchers and practitioners for benchmark studies as well as extended real-world applications. Empirically, we assess the promising scalability of EvoX via a series of benchmark experiments with problem dimensions/population sizes up to millions. Moreover, we demonstrate the easy usability of EvoX by applying it to solving reinforcement learning tasks on OpenAI Gym. To the best of our knowledge, this is the first library supporting distributed GPU computing in the EC literature. The code of EvoX is available at //github.com/EMI-Group/EvoX.
Stein thinning is a promising algorithm proposed by (Riabiz et al., 2022) for post-processing outputs of Markov chain Monte Carlo (MCMC). The main principle is to greedily minimize the kernelized Stein discrepancy (KSD), which only requires the gradient of the log-target distribution, and is thus well-suited for Bayesian inference. The main advantages of Stein thinning are the automatic remove of the burn-in period, the correction of the bias introduced by recent MCMC algorithms, and the asymptotic properties of convergence towards the target distribution. Nevertheless, Stein thinning suffers from several empirical pathologies, which may result in poor approximations, as observed in the literature. In this article, we conduct a theoretical analysis of these pathologies, to clearly identify the mechanisms at stake, and suggest improved strategies. Then, we introduce the regularized Stein thinning algorithm to alleviate the identified pathologies. Finally, theoretical guarantees and extensive experiments show the high efficiency of the proposed algorithm.
Energy modelling can enable energy-aware software development and assist the developer in meeting an application's energy budget. Although many energy models for embedded processors exist, most do not account for processor-specific configurations, neither are they suitable for static energy consumption estimation. This paper introduces a set of comprehensive energy models for Arm's Cortex-M0 processor, ready to support energy-aware development of edge computing applications using either profiling- or static-analysis-based energy consumption estimation. We use a commercially representative physical platform together with a custom modified Instruction Set Simulator to obtain the physical data and system state markers used to generate the models. The models account for different processor configurations which all have a significant impact on the execution time and energy consumption of edge computing applications. Unlike existing works, which target a very limited set of applications, all developed models are generated and validated using a very wide range of benchmarks from a variety of emerging IoT application areas, including machine learning and have a prediction error of less than 5%.
With the growth of data, it is more important than ever to develop an efficient and robust method for solving the consistent matrix equation AXB=C. The randomized Kaczmarz (RK) method has received a lot of attention because of its computational efficiency and low memory footprint. A recently proposed approach is the matrix equation relaxed greedy RK (ME-RGRK) method, which greedily uses the loss of the index pair as a threshold to detect and avoid projecting the working rows onto that are too far from the current iterate. In this work, we utilize the Polyak's and Nesterov's momentums to further speed up the convergence rate of the ME-RGRK method. The resulting methods are shown to converge linearly to a least-squares solution with minimum Frobenius norm. Finally, some numerical experiments are provided to illustrate the feasibility and effectiveness of our proposed methods. In addition, a real-world application, i.e., tensor product surface fitting in computer-aided geometry design, has also been presented for explanatory purpose.
Iterative methods are ubiquitous in large-scale scientific computing applications, and a number of approaches based on meta-learning have been recently proposed to accelerate them. However, a systematic study of these approaches and how they differ from meta-learning is lacking. In this paper, we propose a framework to analyze such learning-based acceleration approaches, where one can immediately identify a departure from classical meta-learning. We show that this departure may lead to arbitrary deterioration of model performance. Based on our analysis, we introduce a novel training method for learning-based acceleration of iterative methods. Furthermore, we theoretically prove that the proposed method improves upon the existing methods, and demonstrate its significant advantage and versatility through various numerical applications.
We consider optimal sensor placement for a family of linear Bayesian inverse problems characterized by a deterministic hyper-parameter. The hyper-parameter describes distinct configurations in which measurements can be taken of the observed physical system. To optimally reduce the uncertainty in the system's model with a single set of sensors, the initial sensor placement needs to account for the non-linear state changes of all admissible configurations. We address this requirement through an observability coefficient which links the posteriors' uncertainties directly to the choice of sensors. We propose a greedy sensor selection algorithm to iteratively improve the observability coefficient for all configurations through orthogonal matching pursuit. The algorithm allows explicitly correlated noise models even for large sets of candidate sensors, and remains computationally efficient for high-dimensional forward models through model order reduction. We demonstrate our approach on a large-scale geophysical model of the Perth Basin, and provide numerical studies regarding optimality and scalability with regard to classic optimal experimental design utility functions.
Bayesian model comparison (BMC) offers a principled approach for assessing the relative merits of competing computational models and propagating uncertainty into model selection decisions. However, BMC is often intractable for the popular class of hierarchical models due to their high-dimensional nested parameter structure. To address this intractability, we propose a deep learning method for performing BMC on any set of hierarchical models which can be instantiated as probabilistic programs. Since our method enables amortized inference, it allows efficient re-estimation of posterior model probabilities and fast performance validation prior to any real-data application. In a series of extensive validation studies, we benchmark the performance of our method against the state-of-the-art bridge sampling method and demonstrate excellent amortized inference across all BMC settings. We then use our method to compare four hierarchical evidence accumulation models that have previously been deemed intractable for BMC due to partly implicit likelihoods. In this application, we corroborate evidence for the recently proposed L\'evy flight model of decision-making and show how transfer learning can be leveraged to enhance training efficiency. Reproducible code for all analyses is provided.
Guided diffusion is a technique for conditioning the output of a diffusion model at sampling time without retraining the network for each specific task. One drawback of diffusion models, however, is their slow sampling process. Recent techniques can accelerate unguided sampling by applying high-order numerical methods to the sampling process when viewed as differential equations. On the contrary, we discover that the same techniques do not work for guided sampling, and little has been explored about its acceleration. This paper explores the culprit of this problem and provides a solution based on operator splitting methods, motivated by our key finding that classical high-order numerical methods are unsuitable for the conditional function. Our proposed method can re-utilize the high-order methods for guided sampling and can generate images with the same quality as a 250-step DDIM baseline using 32-58% less sampling time on ImageNet256. We also demonstrate usage on a wide variety of conditional generation tasks, such as text-to-image generation, colorization, inpainting, and super-resolution.
The industrialization of catalytic processes is of far more importance today than it has ever been before and kinetic models are essential tools for their industrialization. Kinetic models affect the design, the optimization and the control of catalytic processes, but they are not easy to obtain. Classical paradigms, such as mechanistic modeling require substantial domain knowledge, while data-driven and hybrid modeling lack interpretability. Consequently, a different approach called automated knowledge discovery has recently gained popularity. Many methods under this paradigm have been developed, where ALAMO, SINDy and genetic programming are notable examples. However, these methods suffer from important drawbacks: they require assumptions about model structures, scale poorly, lack robust and well-founded model selection routines, and they are sensitive to noise. To overcome these challenges, the present work constructs two methodological frameworks, Automated Discovery of Kinetics using a Strong/Weak formulation of symbolic regression, ADoK-S and ADoK-W, for the automated generation of catalytic kinetic models. We leverage genetic programming for model generation, a sequential optimization routine for model refinement, and a robust criterion for model selection. Both frameworks are tested against three computational case studies of increasing complexity. We showcase their ability to retrieve the underlying kinetic rate model with a limited amount of noisy data from the catalytic system, indicating a strong potential for chemical reaction engineering applications.
This paper focuses on the expected difference in borrower's repayment when there is a change in the lender's credit decisions. Classical estimators overlook the confounding effects and hence the estimation error can be magnificent. As such, we propose another approach to construct the estimators such that the error can be greatly reduced. The proposed estimators are shown to be unbiased, consistent, and robust through a combination of theoretical analysis and numerical testing. Moreover, we compare the power of estimating the causal quantities between the classical estimators and the proposed estimators. The comparison is tested across a wide range of models, including linear regression models, tree-based models, and neural network-based models, under different simulated datasets that exhibit different levels of causality, different degrees of nonlinearity, and different distributional properties. Most importantly, we apply our approaches to a large observational dataset provided by a global technology firm that operates in both the e-commerce and the lending business. We find that the relative reduction of estimation error is strikingly substantial if the causal effects are accounted for correctly.
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