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research article

Atom-density representations for machine learning

Willatt, Michael J.  
•
Musil, Félix  
•
Ceriotti, Michele  
2019
The Journal of Chemical Physics

This has led to a proliferation of alternative ways to convert an atomic structure into an input for a machine-learning model. We introduce an abstract definition of chemical environments that is based on a smoothed atomic density, using a bra-ket notation to emphasize basis set independence and to highlight the connections with some popular choices of representations for describing atomic systems. The correlations between the spatial distribution of atoms and their chemical identities are computed as inner products between these feature kets, which can be given an explicit representation in terms of the expansion of the atom density on orthogonal basis functions, that is equivalent to the smooth overlap of atomic positions power spectrum, but also in real space, corresponding to n-body correlations of the atom density. This formalism lays the foundations for a more systematic tuning of the behavior of the representations, by introducing operators that represent the correlations between structure, composition, and the target properties. It provides a unifying picture of recent developments in the field and indicates a way forward toward more effective and computationally affordable machine-learning schemes for molecules and materials.

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Type
research article
DOI
10.1063/1.5090481
Web of Science ID

WOS:000465442100014

Author(s)
Willatt, Michael J.  
Musil, Félix  
Ceriotti, Michele  
Date Issued

2019

Published in
The Journal of Chemical Physics
Volume

150

Issue

15

Article Number

154110

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
FunderGrant Number

H2020

ERC 677013-HBMAP

Available on Infoscience
November 19, 2019
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/163204
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