Partitioning the electronic wave function using deep variational Monte Carlo

Fuente: arXiv
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Main Authors: Mezera, Matěj, Erdman, Paolo A., Schätzle, Zeno, Szabó, P. Bernát, Noé, Frank
Format: Preprint
Published: 2025
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author Mezera, Matěj
Erdman, Paolo A.
Schätzle, Zeno
Szabó, P. Bernát
Noé, Frank
author_facet Mezera, Matěj
Erdman, Paolo A.
Schätzle, Zeno
Szabó, P. Bernát
Noé, Frank
contents We propose a novel wave function partitioning method that integrates deep-learning variational Monte Carlo with ansätze based on generalized product functions. This approach effectively separates electronic wave functions (WFs) into multiple partial WFs representing, for example, the core and valence domains or different electronic shells. Although our ansätze do not explicitly include correlations between individual electron groups, we show that they accurately reproduce the underlying physics and chemical properties, such as dissociation curve, dipole moment, reaction energy, ionization energy, or atomic sizes. We identify the optimal number of core electrons and define physical core sizes for Li to Mg atoms. Our results demonstrate that core electrons can be effectively decoupled from valence electrons. We show that the core part of the WF remains nearly constant across different molecules and their geometries, enabling the transfer and reuse of the core part in WFs of more complex systems. This work provides a general framework for WF decomposition, offering potential advantages in computing and studying larger systems, and possibly paving the way for ab-initio development of effective core potentials. Though currently limited to small molecules due to scaling, we highlight several directions for extending our method it to larger systems.
format Preprint
id arxiv_https___arxiv_org_abs_2506_18574
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Partitioning the electronic wave function using deep variational Monte Carlo
Mezera, Matěj
Erdman, Paolo A.
Schätzle, Zeno
Szabó, P. Bernát
Noé, Frank
Chemical Physics
Quantum Physics
We propose a novel wave function partitioning method that integrates deep-learning variational Monte Carlo with ansätze based on generalized product functions. This approach effectively separates electronic wave functions (WFs) into multiple partial WFs representing, for example, the core and valence domains or different electronic shells. Although our ansätze do not explicitly include correlations between individual electron groups, we show that they accurately reproduce the underlying physics and chemical properties, such as dissociation curve, dipole moment, reaction energy, ionization energy, or atomic sizes. We identify the optimal number of core electrons and define physical core sizes for Li to Mg atoms. Our results demonstrate that core electrons can be effectively decoupled from valence electrons. We show that the core part of the WF remains nearly constant across different molecules and their geometries, enabling the transfer and reuse of the core part in WFs of more complex systems. This work provides a general framework for WF decomposition, offering potential advantages in computing and studying larger systems, and possibly paving the way for ab-initio development of effective core potentials. Though currently limited to small molecules due to scaling, we highlight several directions for extending our method it to larger systems.
title Partitioning the electronic wave function using deep variational Monte Carlo
topic Chemical Physics
Quantum Physics
url https://arxiv.org/abs/2506.18574