Matrix of orthogonalized atomic orbital coefficients representation for radicals and ions


Chemical (molecular, quantum) machine learning relies on representing molecules in unique and informative ways. Here, we present the matrix of orthogonalized atomic orbital coefficients (MAOC) as a quantum-inspired molecular and atomic representation containing both structural (composition and geometry) and electronic (charge and spin multiplicity) information. MAOC is based on a cost-effective localization scheme that represents localized orbitals via a predefined set of atomic orbitals. The latter can be constructed from such small atom-centered basis sets as pcseg-0 and STO-3G in conjunction with guess (non-optimized) electronic configuration of the molecule. Importantly, MAOC is suitable for representing monatomic, molecular, and periodic systems and can distinguish compounds with identical compositions and geometries but distinct charges and spin multiplicities. Using principal component analysis, we constructed a more compact but equally powerful version of MAOC—PCX-MAOC. To test the performance of full and reduced MAOC and several other representations (CM, SOAP, SLATM, and SPAHM), we used a kernel ridge regression machine learning model to predict frontier molecular orbital energy levels and ground state single-point energies for chemically diverse neutral and charged, closed- and open-shell molecules from an extended QM7b dataset, as well as two new datasets, N-HPC-1 (N-heteropolycycles) and REDOX (nitroxyl and phenoxyl radicals, carbonyl, and cyano compounds). MAOC affords accuracy that is either similar or superior to other representations for a range of chemical properties and systems.


Filename: 2023_Llenga_JCP.pdf 

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DOI: 10.1063/5.0151122

Research Groups: Computational Carbon Chemistry

Publication type: Journal

Journal: The Journal of Chemical Physics

Citation: The Journal of Chemical Physics 158(21),214116

Date Published: 7th Jun 2023

Registered Mode: by DOI

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Llenga, S., & Gryn’ova, G. (2023). Matrix of orthogonalized atomic orbital coefficients representation for radicals and ions. In The Journal of Chemical Physics (Vol. 158, Issue 21). AIP Publishing.

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Created: 4th Jun 2023 at 22:06

Last updated: 11th Mar 2024 at 13:34

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