Toward High-Performance Energy and Power Battery Cells with Machine Learning-based Optimization of Electrode Manufacturing

The optimization of the electrode manufacturing process is important for upscaling the application of Lithium Ion Batteries (LIBs) to cater for growing energy demand. In particular, LIB manufacturing is very important to be optimized because it determines the practical performance of the cells when the latter are being used in applications such as electric vehicles. In this study, we tackled the issue of high-performance electrodes for desired battery application conditions by proposing a powerful data-driven approach supported by a deterministic machine learning (ML)-assisted pipeline for bi-objective optimization of the electrochemical performance. This ML pipeline allows the inverse design of the process parameters to adopt in order to manufacture electrodes for energy or power applications. The latter work is an analogy to our previous work that supported the optimization of the electrode microstructures for kinetic, ionic, and electronic transport properties improvement. An electrochemical pseudo-two-dimensional model is fed with the electrode properties characterizing the electrode microstructures generated by manufacturing simulations and used to simulate the electrochemical performances. Secondly, the resulting dataset was used to train a deterministic ML model to implement fast bi-objective optimizations to identify optimal electrodes. Our results suggested a high amount of active material, combined with intermediate values of solid content in the slurry and calendering degree, to achieve the optimal electrodes.

Catapults in SGD: spikes in the training loss and their impact on generalization through feature learning

In this paper, we first present an explanation regarding the common occurrence of spikes in the training loss when neural networks are trained with stochastic gradient descent (SGD). We provide evidence that the spikes in the training loss of SGD are "catapults", an optimization phenomenon originally observed in GD with large learning rates in [Lewkowycz et al. 2020]. We empirically show that these catapults occur in a low-dimensional subspace spanned by the top eigenvectors of the tangent kernel, for both GD and SGD. Second, we posit an explanation for how catapults lead to better generalization by demonstrating that catapults promote feature learning by increasing alignment with the Average Gradient Outer Product (AGOP) of the true predictor. Furthermore, we demonstrate that a smaller batch size in SGD induces a larger number of catapults, thereby improving AGOP alignment and test performance.

Aiming towards the minimizers: fast convergence of SGD for overparametrized problems

Modern machine learning paradigms, such as deep learning, occur in or close to the interpolation regime, wherein the number of model parameters is much larger than the number of data samples. In this work, we propose a regularity condition within the interpolation regime which endows the stochastic gradient method with the same worst-case iteration complexity as the deterministic gradient method, while using only a single sampled gradient (or a minibatch) in each iteration. In contrast, all existing guarantees require the stochastic gradient method to take small steps, thereby resulting in a much slower linear rate of convergence. Finally, we demonstrate that our condition holds when training sufficiently wide feedforward neural networks with a linear output layer.

On Emergence of Clean-Priority Learning in Early Stopped Neural Networks

When random label noise is added to a training dataset, the prediction error of a neural network on a label-noise-free test dataset initially improves during early training but eventually deteriorates, following a U-shaped dependence on training time. This behaviour is believed to be a result of neural networks learning the pattern of clean data first and fitting the noise later in the training, a phenomenon that we refer to as clean-priority learning. In this study, we aim to explore the learning dynamics underlying this phenomenon. We theoretically demonstrate that, in the early stage of training, the update direction of gradient descent is determined by the clean subset of training data, leaving the noisy subset has minimal to no impact, resulting in a prioritization of clean learning. Moreover, we show both theoretically and experimentally, as the clean-priority learning goes on, the dominance of the gradients of clean samples over those of noisy samples diminishes, and finally results in a termination of the clean-priority learning and fitting of the noisy samples.

ReLU soothes the NTK condition number and accelerates optimization for wide neural networks

Rectified linear unit (ReLU), as a non-linear activation function, is well known to improve the expressivity of neural networks such that any continuous function can be approximated to arbitrary precision by a sufficiently wide neural network. In this work, we present another interesting and important feature of ReLU activation function. We show that ReLU leads to: {\it better separation} for similar data, and {\it better conditioning} of neural tangent kernel (NTK), which are closely related. Comparing with linear neural networks, we show that a ReLU activated wide neural network at random initialization has a larger angle separation for similar data in the feature space of model gradient, and has a smaller condition number for NTK. Note that, for a linear neural network, the data separation and NTK condition number always remain the same as in the case of a linear model. Furthermore, we show that a deeper ReLU network (i.e., with more ReLU activation operations), has a smaller NTK condition number than a shallower one. Our results imply that ReLU activation, as well as the depth of ReLU network, helps improve the gradient descent convergence rate, which is closely related to the NTK condition number.

Quadratic models for understanding neural network dynamics

In this work, we propose using a quadratic model as a tool for understanding properties of wide neural networks in both optimization and generalization. We show analytically that certain deep learning phenomena such as the "catapult phase" from [Lewkowycz et al. 2020], which cannot be captured by linear models, are manifested in the quadratic model for shallow ReLU networks. Furthermore, our empirical results indicate that the behaviour of quadratic models parallels that of neural networks in generalization, especially in the large learning rate regime. We expect that quadratic models will serve as a useful tool for analysis of neural networks.

Transition to Linearity of General Neural Networks with Directed Acyclic Graph Architecture

In this paper we show that feedforward neural networks corresponding to arbitrary directed acyclic graphs undergo transition to linearity as their "width" approaches infinity. The width of these general networks is characterized by the minimum in-degree of their neurons, except for the input and first layers. Our results identify the mathematical structure underlying transition to linearity and generalize a number of recent works aimed at characterizing transition to linearity or constancy of the Neural Tangent Kernel for standard architectures.

Transition to Linearity of Wide Neural Networks is an Emerging Property of Assembling Weak Models

Wide neural networks with linear output layer have been shown to be near-linear, and to have near-constant neural tangent kernel (NTK), in a region containing the optimization path of gradient descent. These findings seem counter-intuitive since in general neural networks are highly complex models. Why does a linear structure emerge when the networks become wide? In this work, we provide a new perspective on this "transition to linearity" by considering a neural network as an assembly model recursively built from a set of sub-models corresponding to individual neurons. In this view, we show that the linearity of wide neural networks is, in fact, an emerging property of assembling a large number of diverse "weak" sub-models, none of which dominate the assembly.

Hyper-parameter optimization based on soft actor critic and hierarchical mixture regularization

Hyper-parameter optimization is a crucial problem in machine learning as it aims to achieve the state-of-the-art performance in any model. Great efforts have been made in this field, such as random search, grid search, Bayesian optimization. In this paper, we model hyper-parameter optimization process as a Markov decision process, and tackle it with reinforcement learning. A novel hyper-parameter optimization method based on soft actor critic and hierarchical mixture regularization has been proposed. Experiments show that the proposed method can obtain better hyper-parameters in a shorter time.

On the linearity of large non-linear models: when and why the tangent kernel is constant

The goal of this work is to shed light on the remarkable phenomenon of transition to linearity of certain neural networks as their width approaches infinity. We show that the transition to linearity of the model and, equivalently, constancy of the (neural) tangent kernel (NTK) result from the scaling properties of the norm of the Hessian matrix of the network as a function of the network width. We present a general framework for understanding the constancy of the tangent kernel via Hessian scaling applicable to the standard classes of neural networks. Our analysis provides a new perspective on the phenomenon of constant tangent kernel, which is different from the widely accepted "lazy training". Furthermore, we show that the transition to linearity is not a general property of wide neural networks and does not hold when the last layer of the network is non-linear. It is also not necessary for successful optimization by gradient descent.