A Stochastic Cluster Expansion for Electronic Correlation in Large Systems
. By combining correlation contributions from randomly sampled environment orbitals with an exactly treated subspace of interest, the method reproduces total energies for nonreacting and reactive systems while drastically reducing computational cost. The approach also provides a quantitative diagnostic for molecule-solvent correlation, guiding principled embedding decisions. This framework enables systematically improvable many-body calculations in extended systems, opening the door to high-accuracy studies of chemical processes in condensed phase environments.
Authors
- Anthony J. Dominic
- Andrés Montoya−Castillo (ORCID: https://orcid.org/0000-0003-3037-3695)
- Libor Veis (ORCID: https://orcid.org/0000-0002-4229-6335)
- Vojtěch Vlček (ORCID: https://orcid.org/0000-0002-2836-7619)
- Annabelle Canestraight (ORCID: https://orcid.org/0000-0001-6473-3762)
Institutions
- University of Colorado Boulder (US)
- Czech Academy of Sciences (CZ)
- University of Colorado System (US)
- University of California System (US)
- Material (Belgium) (BE)
- Czech Academy of Sciences, J. Heyrovský Institute of Physical Chemistry (CZ)
Publication Details
- Journal
- The Journal of Physical Chemistry Letters
- Published
- 2026-04-16
- DOI
- https://doi.org/10.1021/acs.jpclett.6c00563
- Primary Topic
- Machine Learning in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Grantová Agentura České Republiky
- National Institute of General Medical Sciences
- Division of Materials Research
- Wellcome Leap