Extension of high-level electronic-structure methods to many-ion environments

Determine how coupled-cluster CCSD(T) and other correlated wavefunction methods can be extended to chemically complex, many-ion calcium carbonate environments relevant to nucleation and mineral carbonation.

Background

The study uses a revPBE-D3 density functional to construct a chemically diverse training set and access many-ion simulations. The paper notes that coupled-cluster CCSD(T) and related correlated wavefunction methods can provide more quantitatively accurate benchmarks for single ion-pair association, but their applicability to the larger, chemically heterogeneous systems relevant to nucleation and mineral carbonation is unresolved. Addressing this issue could reduce the trade-off between quantitative electronic-structure accuracy and access to collective many-ion behavior.

References

While such approaches provide a valuable benchmark for thermodynamic properties, it remains unclear how to extend them to the chemically complex, many-ion environments studied here, which are directly relevant to nucleation and mineral carbonation.

— Reactive calcium carbonate precipitation from an atomic cluster expansion potential and enhanced sampling  (2609.03044 - Ibrahim et al., 2 Sep 2026) in Discussion of limitations and future directions