A multi-resolution systematically improvable quantum embedding scheme for large-scale surface chemistry calculations.

ABSTRACT: Predictive simulation of surface chemistry is critical in fields from catalysis to electrochemistry and clean energy generation. Ab-initio quantum many-body methods should offer deep insights into these systems at the electronic level but are limited by their steep computational cost. Here, we build upon state-of-the-art correlated wavefunctions to reliably reach 'gold standard' accuracy in quantum chemistry for extended surface chemistry. Efficiently harnessing graphics processing unit acceleration along with systematically improvable multi-resolution techniques, we achieve linear computational scaling up to 392 atoms. These large-scale simulations demonstrate the importance of converging to these extended system sizes, achieving consistency between simulations with different boundary con

SUBMITTER: Huang Z 

PROVIDER: S-EPMC12540692 | biostudies-literature | 2025 Oct

REPOSITORIES: biostudies-literature