Predicting the phase stability of BaZrS3 using a range of approaches: from harmonic lattice dynamics to the neuroevolution-potential framework

Chalcogenide perovskite materials are highly robust, non-toxic and show strong light absorption but device development is hindered by the high-temperatures typically required for synthesis [1]. I will present our research, based on first-principles calculations and machine learnt interatomic potentials, which explores the thermodynamics of BaZrS3 phase formation [2,3,5]. I will consider stability against competing binary phases as a function of temperature and sulfur partial pressure [2], and compare our computational predictions against recent experimental measurements. I will also highlight the presence of low-dimensional Ruddlesden- Popper materials Ban+1ZrnS3n+1, and discuss how first-principles predictions of Raman spectra can be used to support their experimental characterisation [3]. Finally, I will share our latest work using the Neuroevolution Potential framework [4] and molecular dynamics to explore octahedral-tilt driven phase transitions in BaZrS3 [5].

[1] K. Sopiha, C. Comparotto, J. A. Márquez et al., Advanced Optical Materials, 2022, 10 (3), 2101704

[2] P. Kayastha, G. Longo, L.D Whalley et al., Solar RRL, 2023, 7 (9), 2201078

[3] P. Kayastha, G. Longo, L. D. Whalley, ACS Applied Energy Materials, 2024, ASAP article, DOI: 10.1021/acsaem.3c03208

[4] Z. Fan, Z. Zeng, C. Zhang et al., Physical Review B, 2021, 104 (10), 104309

[5] P. Kayastha, E. Fransson, P. Erhart, L.D. Whalley, In Prep.

Bio: Lucy's research uses first-principles methods to predict the properties of energy materials and link macroscopic observables (such as open circuit voltage or thermodynamic stability) with microscopic processes (such as electron capture or electron-phonon coupling). She is an Assistant Professor in Physics at Northumbria University and an Associate Editor at the Journal of Open Source Software.