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research article

Learning Electron Densities in the Condensed Phase

Lewis, Alan M.
•
Grisafi, Andrea  
•
Ceriotti, Michele  
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November 9, 2021
Journal of Chemical Theory and Computation

We introduce a local machine-learning method for predicting the electron densities of periodic systems. The framework is based on a numerical, atom-centered auxiliary basis, which enables an accurate expansion of the all-electron density in a form suitable for learning isolated and periodic systems alike. We show that, using this formulation, the electron densities of metals, semiconductors, and molecular crystals can all be accurately predicted using symmetry-adapted Gaussian process regression models, properly adjusted for the nonorthogonal nature of the basis. These predicted densities enable the efficient calculation of electronic properties, which present errors on the order of tens of meV/atom when compared to ab initio density-functional calculations. We demonstrate the key power of this approach by using a model trained on ice unit cells containing only 4 water molecules to predict the electron densities of cells containing up to 512 molecules and see no increase in the magnitude of the errors of derived electronic properties when increasing the system size. Indeed, we find that these extrapolated derived energies are more accurate than those predicted using a direct machine-learning model. Finally, on heterogeneous data sets SALTED can predict electron densities with errors below 4%.

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Type
research article
DOI
10.1021/acs.jctc.1c00576
Web of Science ID

WOS:000718183600042

Author(s)
Lewis, Alan M.
Grisafi, Andrea  
Ceriotti, Michele  
Rossi, Mariana
Date Issued

2021-11-09

Publisher

AMER CHEMICAL SOC

Published in
Journal of Chemical Theory and Computation
Volume

17

Issue

11

Start page

7203

End page

7214

Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

exchange

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
Available on Infoscience
December 18, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/183877
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