Ferroelectric phase transition in group-IV monochalcogenides from an equivariant machine learned force field

Mihm, Tina N.; Trerayapiwat, Kasidet Jing; Darancet, Pierre; Sharifzadeh, Sahar

doi:10.1103/t63g-4zp3

Ferroelectric phase transition in group-IV monochalcogenides from an equivariant machine learned force field

Journal Article · Thu Oct 09 20:00:00 EDT 2025 · Physical Review Materials

DOI:https://doi.org/10.1103/t63g-4zp3· OSTI ID:2998493

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Boston Univ., MA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

Group-IV monochalcogenides are a class of layered ferroelectric semiconductors that have demonstrated spontaneous intrinsic polarization above room temperature. Here, in this study, we use the multi-atomic cluster expansion (MACE) machine learning architecture to train and test a force field capable of modeling the structural properties and second-order ferroelectric-to-paraelectric phase transition in a Group-IV monochalcogenide, GeSe. The model captures the double-well potential energy surface associated with the onset of macroscopic polarization in bulk GeSe within 12.5 meV/atom, as well as near-equilibrium properties like the phonon dispersion. The development of this quantitatively accurate force field enables long-time molecular dynamics simulations, which predict the critical temperature of the ferroelectric-to-paraelectric phase transition in bulk GeSe to be T_c = 600 K. This study demonstrates the capabilities of equivariant force-fields to accurately describe phenomena associated with structural symmetry breaking.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC02-06CH11357; SC0023402; AC02-05CH11231

OSTI ID:: 2998493

Alternate ID(s):: OSTI ID: 3011356

Journal Information:: Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 10 Vol. 9; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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