Obtaining accurate solutions to the Schrödinger equation is the key challenge in computational quantum chemistry. Deep-learning-based Variational Monte Carlo (DL-VMC) has recently outperformed conventional approaches in terms of accuracy, but only at large computational cost. Whereas in many domains models are trained once and subsequently applied for inference, accurate DL-VMC so far requires a full optimization for every new problem instance, consuming thousands of GPUhs even for small molecules. We instead propose a DL-VMC model which has been pre-trained using self-supervised wavefunction optimization on a large and chemically diverse set of molecules. Applying this model to new molecules without any optimization, yields wavefunctions and absolute energies that outperform established methods such as CCSD(T)-2Z. To obtain accurate relative energies, only few fine-tuning steps of this base model are required. We accomplish this with a fully end-to-end machine-learned model, consisting of an improved geometry embedding architecture and an existing SE(3)-equivariant model to represent molecular orbitals. Combining this architecture with continuous sampling of geometries, we improve zero-shot accuracy by two orders of magnitude compared to the state of the art. We extensively evaluate the accuracy, scalability and limitations of our base model on a wide variety of test systems.

Finding accurate solutions to the Schrödinger equation is the key unsolved challenge of computational chemistry. Given its importance for the development of new chemical compounds, decades of research have been dedicated to this problem, but due to the large dimensionality even the best available methods do not yet reach the desired accuracy.Recently the combination of deep learning with Monte Carlo methods has emerged as a promising way to obtain highly accurate energies and moderate scaling of computational cost. In this paper we significantly contribute towards this goal by introducing a novel deep-learning architecture that achieves 40-70% lower energy error at 6x lower computational cost compared to previous approaches. Using our method we establish a new benchmark by calculating the most accurate variational ground state energies ever published for a number of different atoms and molecules.We systematically break down and measure our improvements, focusing in particular on the effect of increasing physical prior knowledge.We surprisingly find that increasing the prior knowledge given to the architecture can actually decrease accuracy.

This paper develops fundamental limits of deep neural network learning by characterizing what is possible if no constraints are imposed on the learning algorithm and on the amount of training data. Concretely, we consider Kolmogorov-optimal approximation through deep neural networks with the guiding theme being a relation between the complexity of the function (class) to be approximated and the complexity of the approximating network in terms of connectivity and memory requirements for storing the network topology and the associated quantized weights. The theory we develop establishes that deep networks are Kolmogorov-optimal approximants for markedly different function classes, such as unit balls in Besov spaces and modulation spaces. In addition, deep networks provide exponential approximation accuracy-i.e., the approximation error decays exponentially in the number of nonzero weights in the network-of the multiplication operation, polynomials, sinusoidal functions, and certain smooth functions. Moreover, this holds true even for one-dimensional oscillatory textures and the Weierstrass function-a fractal function, neither of which has previously known methods achieving exponential approximation accuracy. We also show that in the approximation of sufficiently smooth functions finite-width deep networks require strictly smaller connectivity than finite-depth wide networks.

We present a deep learning algorithm for the numerical solution of parametric families of high-dimensional linear Kolmogorov partial differential equations (PDEs). Our method is based on reformulating the numerical approximation of a whole family of Kolmogorov PDEs as a single statistical learning problem using the Feynman-Kac formula. Successful numerical experiments are presented, which empirically confirm the functionality and efficiency of our proposed algorithm in the case of heat equations and Black-Scholes option pricing models parametrized by affine-linear coefficient functions. We show that a single deep neural network trained on simulated data is capable of learning the solution functions of an entire family of PDEs on a full space-time region. Most notably, our numerical observations and theoretical results also demonstrate that the proposed method does not suffer from the curse of dimensionality, distinguishing it from almost all standard numerical methods for PDEs.

Neural network training is usually accomplished by solving a non-convex optimization problem using stochastic gradient descent. Although one optimizes over the networks parameters, the main loss function generally only depends on the realization of the neural network, i.e. the function it computes. Studying the optimization problem over the space of realizations opens up new ways to understand neural network training. In particular, usual loss functions like mean squared error and categorical cross entropy are convex on spaces of neural network realizations, which themselves are non-convex. Approximation capabilities of neural networks can be used to deal with the latter non-convexity, which allows us to establish that for sufficiently large networks local minima of a regularized optimization problem on the realization space are almost optimal. Note, however, that each realization has many different, possibly degenerate, parametrizations. In particular, a local minimum in the parametrization space needs not correspond to a local minimum in the realization space. To establish such a connection, inverse stability of the realization map is required, meaning that proximity of realizations must imply proximity of corresponding parametrizations. We present pathologies which prevent inverse stability in general, and, for shallow networks, proceed to establish a restricted space of parametrizations on which we have inverse stability w.r.t. to a Sobolev norm. Furthermore, we show that by optimizing over such restricted sets, it is still possible to learn any function which can be learned by optimization over unrestricted sets.

Many practical machine learning tasks employ very deep convolutional neural networks. Such large depths pose formidable computational challenges in training and operating the network. It is therefore important to understand how fast the energy contained in the propagated signals (a.k.a. feature maps) decays across layers. In addition, it is desirable that the feature extractor generated by the network be informative in the sense of the only signal mapping to the all-zeros feature vector being the zero input signal. This “trivial null-set” property can be accomplished by asking for “energy conservation” in the sense of the energy in the feature vector being proportional to that of the corresponding input signal. This paper establishes conditions for energy conservation (and thus for a trivial null-set) for a wide class of deep convolutional neural network-based feature extractors and characterizes corresponding feature map energy decay rates. Specifically, we consider general scattering networks employing the modulus non-linearity and we find that under mild analyticity and high-pass conditions on the filters (which encompass, inter alia, various constructions of Weyl-Heisenberg filters, wavelets, ridgelets, (α)-curvelets, and shearlets) the feature map energy decays at least polynomially fast. For broad families of wavelets and Weyl-Heisenberg filters, the guaranteed decay rate is shown to be exponential. Moreover, we provide handy estimates of the number of layers needed to have at least ((1-ε) 100)% of the input signal energy be contained in the feature vector.

Many practical machine learning tasks employ very deep convolutional neural networks. Such large depths pose formidable computational challenges in training and operating the network. It is therefore important to understand how many layers are actually needed to have most of the input signal's features be contained in the feature vector generated by the network. This question can be formalized by asking how quickly the energy contained in the feature maps decays across layers. In addition, it is desirable that none of the input signal's features be “lost” in the feature extraction network or, more formally, we want energy conservation in the sense of the energy contained in the feature vector being proportional to that of the corresponding input signal. This paper establishes conditions for energy conservation for a wide class of deep convolutional neural networks and characterizes corresponding feature map energy decay rates. Specifically, we consider general scattering networks, and find that under mild analyticity and high-pass conditions on the filters (which encompass, inter alia, various constructions of Weyl-Heisenberg filters, wavelets, ridgelets,(α)-curvelets, and shearlets) the feature map energy decays at least polynomially. For broad families of wavelets and Weyl-Heisenberg filters, the guaranteed decay rate is shown to be exponential. Our results yield handy estimates of the number of layers needed to have at least ((1 − ε) · 100)% of the input signal energy be contained in the feature vector.

First steps towards a mathematical theory of deep convolutional neural networks for feature extraction were made—for the continuous-time case—in Mallat, 2012, and Wiatowski and Bölcskei, 2015. This paper considers the discrete case, introduces new convolutional neural network architectures, and proposes a mathematical framework for their analysis. Specifically, we establish deformation and translation sensitivity results of local and global nature, and we investigate how certain structural properties of the input signal are reflected in the corresponding feature vectors. Our theory applies to general filters and general Lipschitz-continuous non-linearities and pooling operators. Experiments on handwritten digit classification and facial landmark detection—including feature importance evaluation—complement the theoretical findings.

Wiatowski and Bölcskei, 2015, proved that deformation stability and vertical translation invariance of deep convolutional neural network-based feature extractors are guaranteed by the network structure per se rather than the specific convolution kernels and non-linearities. While the translation invariance result applies to square-integrable functions, the deformation stability bound holds for band-limited functions only. Many signals of practical relevance (such as natural images) exhibit, however, sharp and curved discontinuities and are hence not band-limited. The main contribution of this paper is a deformation stability result that takes these structural properties into account. Specifically, we establish deformation stability bounds for the class of cartoon functions introduced by Donoho, 2001.