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research article

Electronic Excited States from Physically Constrained Machine Learning

Cignoni, Edoardo
•
Suman, Divya  
•
Nigam, Jigyasa  
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March 27, 2024
ACS Central Science

Data-driven techniques are increasingly used to replace electronic-structure calculations of matter. In this context, a relevant question is whether machine learning (ML) should be applied directly to predict the desired properties or combined explicitly with physically grounded operations. We present an example of an integrated modeling approach in which a symmetry-adapted ML model of an effective Hamiltonian is trained to reproduce electronic excitations from a quantum-mechanical calculation. The resulting model can make predictions for molecules that are much larger and more complex than those on which it is trained and allows for dramatic computational savings by indirectly targeting the outputs of well-converged calculations while using a parametrization corresponding to a minimal atom-centered basis. These results emphasize the merits of intertwining data-driven techniques with physical approximations, improving the transferability and interpretability of ML models without affecting their accuracy and computational efficiency and providing a blueprint for developing ML-augmented electronic-structure methods.

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Type
research article
DOI
10.1021/acscentsci.3c01480
Scopus ID

2-s2.0-85186314995

Author(s)
Cignoni, Edoardo
Suman, Divya  

École Polytechnique Fédérale de Lausanne

Nigam, Jigyasa  

École Polytechnique Fédérale de Lausanne

Cupellini, Lorenzo
Mennucci, Benedetta
Ceriotti, Michele  

École Polytechnique Fédérale de Lausanne

Date Issued

2024-03-27

Published in
ACS Central Science
Volume

10

Issue

3

Start page

637

End page

648

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
FunderFunding(s)Grant NumberGrant URL

NCCR MARVEL

Samsung

European Research Council

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Available on Infoscience
January 16, 2025
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/242903
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