Identification and finite-temperature relevance of metastable defect basins

Determine which metastable defect basins and local minima are relevant at finite temperature, particularly in molecular systems and chemically complex materials with enormous basin multiplicity.

Background

The constrained Bayesian Adaptive Biasing Force (BABFc) framework computes a restricted formation free energy once a metastable basin and a confinement strategy have been specified. However, the method does not automatically enumerate all possible basins or determine which minima contribute meaningfully to finite-temperature behavior. In the reported study, this upstream discovery task is delegated to the ARTn database, harmonic screening, minimum-covariance-determinant analysis, and random subsampling. The authors explicitly identify the more general problem of basin identification and finite-temperature relevance as unresolved, with greater difficulty expected for molecular and chemically complex materials because of their very large number of possible basins.

References

Firstly, identifying basins and deciding which minima are relevant at finite temperature is an open problem in general (and it becomes acute for molecular systems or chemically complex materials where basin multiplicity is enormous).

— Systematic and accurate anharmonic formation free energies of metastable defects via a constrained Bayesian Adaptive Biasing Force framework  (2608.20902 - Lapointe et al., 21 Aug 2026) in Discussions and Conclusion, paragraph beginning “This viewpoint clarifies both the strengths and limitations.”