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research article

Physics-based representations for machine learning properties of chemical reactions

van Gerwen, Puck  
•
Fabrizio, Alberto  
•
Wodrich, Matthew D.  
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December 1, 2022
Machine Learning-Science And Technology

Physics-based representations constructed using only atomic positions and nuclear charges (also known as quantum machine learning, QML) allow for the reliable and efficient inference of molecular properties from training data. Chemistry is a science rooted in chemical reactions, naturally involving multiple molecular species. Here, we extend QML's capabilities to include the prediction of reaction properties by defining reaction representations: representations taking as input multiple molecules participating in a reaction, each represented by their corresponding atomic charges and three-dimensional coordinates. Several reaction representations are constructed from established molecular ones and benchmarked on four datasets representative of thermodynamic or kinetic reaction properties. One of these, the Hydroform-22-TS dataset (2350 energy barriers), is introduced as part of this work. The relevant ingredients for a high-performing reaction representation are extracted and used to construct the Bond-Based Reaction Representation ((BR2)-R-2) for the prediction of quantum-chemical properties of chemical reactions. Finally, variations of (BR2)-R-2 with varying representation size vs. performance are provided.

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Type
research article
DOI
10.1088/2632-2153/ac8f1a
Web of Science ID

WOS:000869457000001

Author(s)
van Gerwen, Puck  
Fabrizio, Alberto  
Wodrich, Matthew D.  
Corminboeuf, Clemence  
Date Issued

2022-12-01

Published in
Machine Learning-Science And Technology
Volume

3

Issue

4

Article Number

045005

Subjects

Computer Science, Artificial Intelligence

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Computer Science, Interdisciplinary Applications

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Multidisciplinary Sciences

•

Computer Science

•

Science & Technology - Other Topics

•

chemical reactions

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quantum machine learning

•

physics-based representation

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reaction-based representation

•

molecular-orbital methods

•

basis-sets

•

design

•

atoms

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LCMD  
RelationURL/DOI

IsNewVersionOf

https://infoscience.epfl.ch/record/307768
Available on Infoscience
November 7, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/191881
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