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Equivariant representations for molecular Hamiltonians

Jigyasa Nigam1,2*, Michael J. Willatt1, Michele Ceriotti1,2*

1 Laboratory of Computational Science and Modeling, IMX, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland

2 National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland

* Corresponding authors emails: jigyasa.nigam@epfl.ch, michele.ceriotti@epfl.ch
DOI10.24435/materialscloud:2d-3e [version v1]

Publication date: Dec 09, 2021

How to cite this record

Jigyasa Nigam, Michael J. Willatt, Michele Ceriotti, Equivariant representations for molecular Hamiltonians, Materials Cloud Archive 2021.217 (2021), doi: 10.24435/materialscloud:2d-3e.


The application of machine learning to the modeling of materials and molecules has proven to be extremely successful in accelerating the understanding, design, and characterization of materials. A major factor in this success has been the development of representations of atomic structures that reflect physics-based symmetries of the underlying interactions. Most of the descriptions of atomic properties or even global observables rely on decompositions into atomic contributions that are subsequently learnt in an atom-centered framework. However, many quantities associated with quantum mechanical calculations, such as the single-particle Hamiltonian matrices written in an atomic-orbital basis, are associated with multiple atom-centers. Following the introduction of equivariant N-center structural descriptors, in the reference below, that generalize the very successful atom-centered density correlation features to the problem of learning properties indexed by N atoms, we present benchmarks showing how the construction can be applied to efficiently learn the matrix elements of the (effective) single-particle Hamiltonian in an atom-centered orbital basis. In this record, we include the dataset comprising the Fock and overlap matrices in the def2-SVP of 1000 distorted water molecules, up to 4500 ethanol structures, and a subset of QM7-CHNO molecules. We also provide scripts to generate the two-center representations and fit linear and sparse kernel models for the Hamiltonians.

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File name Size Description
7.4 GiB Folder containing benchmarks for machine learning for datasets of water, ethanol and QM7-CHNO and commented scripts to reproduce the same.
889 Bytes Description of data source and availability of code


Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.
Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Journal reference (Manuscript where the data and methods are described)


ERC MARVEL EPFL H2020 N-center-representations machine learning hamiltonians equivariant representations hamiltonian learning

Version history:

2021.217 (version v1) [This version] Dec 09, 2021 DOI10.24435/materialscloud:2d-3e