423 research outputs found
Quantum-Chemical Insights from Interpretable Atomistic Neural Networks
With the rise of deep neural networks for quantum chemistry applications, there is a pressing need for architectures that, beyond delivering accurate predictions of chemical properties, are readily interpretable by researchers. Here, we describe interpretation techniques for atomistic neural networks on the example of Behler–Parrinello networks as well as the end-to-end model SchNet. Both models obtain predictions of chemical properties by aggregating atom-wise contributions. These latent variables can serve as local explanations of a prediction and are obtained during training without additional cost. Due to their correspondence to well-known chemical concepts such as atomic energies and partial charges, these atom-wise explanations enable insights not only about the model but more importantly about the underlying quantum-chemical regularities. We generalize from atomistic explanations to 3d space, thus obtaining spatially resolved visualizations which further improve interpretability. Finally, we analyze learned embeddings of chemical elements that exhibit a partial ordering that resembles the order of the periodic table. As the examined neural networks show excellent agreement with chemical knowledge, the presented techniques open up new venues for data-driven research in chemistry, physics and materials science.EC/H2020/792572/EU/Machine Learning for Catalytic Carbon Dioxide Activation/MachineCatBMBF, 01IS14013A, Verbundprojekt: BBDC - Berliner Kompetenzzentrum für Big DataBMBF, 01IS18037A, Verbundprojekt BIFOLD-BZML: Berlin Institute for the Foundations of Learning and DataEC/H2020/725291/EU/Beyond Static Molecules: Modeling Quantum Fluctuations in Complex Molecular Environments/BeStM
SchNet - a deep learning architecture for molecules and materials
Deep learning has led to a paradigm shift in artificial intelligence,
including web, text and image search, speech recognition, as well as
bioinformatics, with growing impact in chemical physics. Machine learning in
general and deep learning in particular is ideally suited for representing
quantum-mechanical interactions, enabling to model nonlinear potential-energy
surfaces or enhancing the exploration of chemical compound space. Here we
present the deep learning architecture SchNet that is specifically designed to
model atomistic systems by making use of continuous-filter convolutional
layers. We demonstrate the capabilities of SchNet by accurately predicting a
range of properties across chemical space for \emph{molecules and materials}
where our model learns chemically plausible embeddings of atom types across the
periodic table. Finally, we employ SchNet to predict potential-energy surfaces
and energy-conserving force fields for molecular dynamics simulations of small
molecules and perform an exemplary study of the quantum-mechanical properties
of C-fullerene that would have been infeasible with regular ab initio
molecular dynamics
Band gap prediction for large organic crystal structures with machine learning
Machine-learning models are capable of capturing the structure-property
relationship from a dataset of computationally demanding ab initio
calculations. Over the past two years, the Organic Materials Database (OMDB)
has hosted a growing number of calculated electronic properties of previously
synthesized organic crystal structures. The complexity of the organic crystals
contained within the OMDB, which have on average 82 atoms per unit cell, makes
this database a challenging platform for machine learning applications. In this
paper, the focus is on predicting the band gap which represents one of the
basic properties of a crystalline materials. With this aim, a consistent
dataset of 12 500 crystal structures and their corresponding DFT band gap are
released, freely available for download at https://omdb.mathub.io/dataset. An
ensemble of two state-of-the-art models reach a mean absolute error (MAE) of
0.388 eV, which corresponds to a percentage error of 13% for an average band
gap of 3.05 eV. Finally, the trained models are employed to predict the band
gap for 260 092 materials contained within the Crystallography Open Database
(COD) and made available online so that the predictions can be obtained for any
arbitrary crystal structure uploaded by a user.Comment: 10 pages, 6 figure
Representations of molecules and materials for interpolation of quantum-mechanical simulations via machine learning
Computational study of molecules and materials from first principles is a cornerstone of physics, chemistry and materials science, but limited by the cost of accurate and precise simulations. In settings involving many simulations, machine learning can reduce these costs, sometimes by orders of magnitude, by interpolating between reference simulations. This requires representations that describe any molecule or material and support interpolation. We review, discuss and benchmark state-of-the-art representations and relations between them, including smooth overlap of atomic positions, many-body tensor representation, and symmetry functions. For this, we use a unified mathematical framework based on many-body functions, group averaging and tensor products, and compare energy predictions for organic molecules, binary alloys and Al-Ga-In sesquioxides in numerical experiments controlled for data distribution, regression method and hyper-parameter optimization
Atomistic Line Graph Neural Network for Improved Materials Property Predictions
Graph neural networks (GNN) have been shown to provide substantial
performance improvements for representing and modeling atomistic materials
compared with descriptor-based machine-learning models. While most existing GNN
models for atomistic predictions are based on atomic distance information, they
do not explicitly incorporate bond angles, which are critical for
distinguishing many atomic structures. Furthermore, many material properties
are known to be sensitive to slight changes in bond angles. We present an
Atomistic Line Graph Neural Network (ALIGNN), a GNN architecture that performs
message passing on both the interatomic bond graph and its line graph
corresponding to bond angles. We demonstrate that angle information can be
explicitly and efficiently included, leading to improved performance on
multiple atomistic prediction tasks. We use ALIGNN models for predicting 52
solid-state and molecular properties available in the JARVIS-DFT, Materials
project, and QM9 databases. ALIGNN can outperform some previously reported GNN
models on atomistic prediction tasks by up to 85 % in accuracy with better or
comparable model training speed
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