Orbital-free density functional theory (OF-DFT) holds the promise to compute ground state molecular properties at minimal cost. However, it has been held back by our inability to compute the kinetic energy as a functional of the electron density only. We here set out to learn the kinetic energy functional from ground truth provided by the more expensive Kohn-Sham density functional theory. Such learning is confronted with two key challenges: Giving the model sufficient expressivity and spatial context while limiting the memory footprint to afford computations on a GPU; and creating a sufficiently broad distribution of training data to enable iterative density optimization even when starting from a poor initial guess. In response, we introduce KineticNet, an equivariant deep neural network architecture based on point convolutions adapted to the prediction of quantities on molecular quadrature grids. Important contributions include convolution filters with sufficient spatial resolution in the vicinity of the nuclear cusp, an atom-centric sparse but expressive architecture that relays information across multiple bond lengths; and a new strategy to generate varied training data by finding ground state densities in the face of perturbations by a random external potential. KineticNet achieves, for the first time, chemical accuracy of the learned functionals across input densities and geometries of tiny molecules. For two electron systems, we additionally demonstrate OF-DFT density optimization with chemical accuracy.
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Density functional theory (DFT) stands as a cornerstone method in computational quantum chemistry and materials science due to its remarkable versatility and scalability. Yet, it suffers from limitations in accuracy, particularly when dealing with strongly correlated systems. To address these shortcomings, recent work has begun to explore how machine learning can expand the capabilities of DFT; an endeavor with many open questions and technical challenges. In this work, we present Grad DFT: a fully differentiable JAX-based DFT library, enabling quick prototyping and experimentation with machine learning-enhanced exchange-correlation energy functionals. Grad DFT employs a pioneering parametrization of exchange-correlation functionals constructed using a weighted sum of energy densities, where the weights are determined using neural networks. Moreover, Grad DFT encompasses a comprehensive suite of auxiliary functions, notably featuring a just-in-time compilable and fully differentiable self-consistent iterative procedure. To support training and benchmarking efforts, we additionally compile a curated dataset of experimental dissociation energies of dimers, half of which contain transition metal atoms characterized by strong electronic correlations. The software library is tested against experimental results to study the generalization capabilities of a neural functional across potential energy surfaces and atomic species, as well as the effect of training data noise on the resulting model accuracy.
Human cognition operates on a "Global-first" cognitive mechanism, prioritizing information processing based on coarse-grained details. This mechanism inherently possesses an adaptive multi-granularity description capacity, resulting in computational traits such as efficiency, robustness, and interpretability. The analysis pattern reliance on the finest granularity and single-granularity makes most existing computational methods less efficient, robust, and interpretable, which is an important reason for the current lack of interpretability in neural networks. Multi-granularity granular-ball computing employs granular-balls of varying sizes to daptively represent and envelop the sample space, facilitating learning based on these granular-balls. Given that the number of coarse-grained "granular-balls" is fewer than sample points, granular-ball computing proves more efficient. Moreover, the inherent coarse-grained nature of granular-balls reduces susceptibility to fine-grained sample disturbances, enhancing robustness. The multi-granularity construct of granular-balls generates topological structures and coarse-grained descriptions, naturally augmenting interpretability. Granular-ball computing has successfully ventured into diverse AI domains, fostering the development of innovative theoretical methods, including granular-ball classifiers, clustering techniques, neural networks, rough sets, and evolutionary computing. This has notably ameliorated the efficiency, noise robustness, and interpretability of traditional methods. Overall, granular-ball computing is a rare and innovative theoretical approach in AI that can adaptively and simultaneously enhance efficiency, robustness, and interpretability. This article delves into the main application landscapes for granular-ball computing, aiming to equip future researchers with references and insights to refine and expand this promising theory.
Normal modal logics extending the logic K4.3 of linear transitive frames are known to lack the Craig interpolation property, except some logics of bounded depth such as S5. We turn this `negative' fact into a research question and pursue a non-uniform approach to Craig interpolation by investigating the following interpolant existence problem: decide whether there exists a Craig interpolant between two given formulas in any fixed logic above K4.3. Using a bisimulation-based characterisation of interpolant existence for descriptive frames, we show that this problem is decidable and coNP-complete for all finitely axiomatisable normal modal logics containing K4.3. It is thus not harder than entailment in these logics, which is in sharp contrast to other recent non-uniform interpolation results. We also extend our approach to Priorean temporal logics (with both past and future modalities) over the standard time flows-the integers, rationals, reals, and finite strict linear orders-none of which is blessed with the Craig interpolation property.
Maxwell-Amp\`{e}re-Nernst-Planck (MANP) equations were recently proposed to model the dynamics of charged particles. In this study, we enhance a numerical algorithm of this system with deep learning tools. The proposed hybrid algorithm provides an automated means to determine a proper approximation for the dummy variables, which can otherwise only be obtained through massive numerical tests. In addition, the original method is validated for 2-dimensional problems. However, when the spatial dimension is one, the original curl-free relaxation component is inapplicable, and the approximation formula for dummy variables, which works well in a 2-dimensional scenario, fails to provide a reasonable output in the 1-dimensional case. The proposed method can be readily generalised to cases with one spatial dimension. Experiments show numerical stability and good convergence to the steady-state solution obtained from Poisson-Boltzmann type equations in the 1-dimensional case. The experiments conducted in the 2-dimensional case indicate that the proposed method preserves the conservation properties.
Finite-dimensional truncations are routinely used to approximate partial differential equations (PDEs), either to obtain numerical solutions or to derive reduced-order models. The resulting discretized equations are known to violate certain physical properties of the system. In particular, first integrals of the PDE may not remain invariant after discretization. Here, we use the method of reduced-order nonlinear solutions (RONS) to ensure that the conserved quantities of the PDE survive its finite-dimensional truncation. In particular, we develop two methods: Galerkin RONS and finite volume RONS. Galerkin RONS ensures the conservation of first integrals in Galerkin-type truncations, whether used for direct numerical simulations or reduced-order modeling. Similarly, finite volume RONS conserves any number of first integrals of the system, including its total energy, after finite volume discretization. Both methods are applicable to general time-dependent PDEs and can be easily incorporated in existing Galerkin-type or finite volume code. We demonstrate the efficacy of our methods on two examples: direct numerical simulations of the shallow water equation and a reduced-order model of the nonlinear Schrodinger equation. As a byproduct, we also generalize RONS to phenomena described by a system of PDEs.
We discuss avoidance of sure loss and coherence results for semicopulas and standardized functions, i.e., for grounded, 1-increasing functions with value $1$ at $(1,1,\ldots, 1)$. We characterize the existence of a $k$-increasing $n$-variate function $C$ fulfilling $A\leq C\leq B$ for standardized $n$-variate functions $A,B$ and discuss the method for constructing this function. Our proofs also include procedures for extending functions on some countably infinite mesh to functions on the unit box. We provide a characterization when $A$ respectively $B$ coincides with the pointwise infimum respectively supremum of the set of all $k$-increasing $n$-variate functions $C$ fulfilling $A\leq C\leq B$.
Penalizing complexity (PC) priors is a principled framework for designing priors that reduce model complexity. PC priors penalize the Kullback-Leibler Divergence (KLD) between the distributions induced by a ``simple'' model and that of a more complex model. However, in many common cases, it is impossible to construct a prior in this way because the KLD is infinite. Various approximations are used to mitigate this problem, but the resulting priors then fail to follow the designed principles. We propose a new class of priors, the Wasserstein complexity penalization (WCP) priors, by replacing KLD with the Wasserstein distance in the PC prior framework. These priors avoid the infinite model distance issues and can be derived by following the principles exactly, making them more interpretable. Furthermore, principles and recipes to construct joint WCP priors for multiple parameters analytically and numerically are proposed and we show that they can be easily obtained, either numerically or analytically, for a general class of models. The methods are illustrated through several examples for which PC priors have previously been applied.
We extend the use of piecewise orthogonal collocation to computing periodic solutions of renewal equations, which are particularly important in modeling population dynamics. We prove convergence through a rigorous error analysis. Finally, we show some numerical experiments confirming the theoretical results, and a couple of applications in view of bifurcation analysis.
Neufeld and Wu (arXiv:2310.12545) developed a multilevel Picard (MLP) algorithm which can approximately solve general semilinear parabolic PDEs with gradient-dependent nonlinearities, allowing also for coefficient functions of the corresponding PDE to be non-constant. By introducing a particular stochastic fixed-point equation (SFPE) motivated by the Feynman-Kac representation and the Bismut-Elworthy-Li formula and identifying the first and second component of the unique fixed-point of the SFPE with the unique viscosity solution of the PDE and its gradient, they proved convergence of their algorithm. However, it remained an open question whether the proposed MLP schema in arXiv:2310.12545 does not suffer from the curse of dimensionality. In this paper, we prove that the MLP algorithm in arXiv:2310.12545 indeed can overcome the curse of dimensionality, i.e. that its computational complexity only grows polynomially in the dimension $d\in \mathbb{N}$ and the reciprocal of the accuracy $\varepsilon$, under some suitable assumptions on the nonlinear part of the corresponding PDE.
We introduce a family of identities that express general linear non-unitary evolution operators as a linear combination of unitary evolution operators, each solving a Hamiltonian simulation problem. This formulation can exponentially enhance the accuracy of the recently introduced linear combination of Hamiltonian simulation (LCHS) method [An, Liu, and Lin, Physical Review Letters, 2023]. For the first time, this approach enables quantum algorithms to solve linear differential equations with both optimal state preparation cost and near-optimal scaling in matrix queries on all parameters.
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