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arXiv · 2605.19414

Octahedral Tilting in Halide Double Perovskites: Disentangling Lone-Pair Chemistry and Geometric Effects

Mehmet Baskurt·Erik Fransson·Madeleine Lindvik·Paul Erhart·Julia Wiktor
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Abstract

Halide double perovskites (HDPs) have emerged as promising alternatives to their lead-based counterparts. However, their structural dynamics is less explored than that of conventional halide perovskites. In this work, we investigate octahedral tilting at 0 K and the relative stability of tetragonal and cubic phases of a set of 57 halide double perovskites (HDPs). By combining structural and energetic descriptors with simple geometric metrics, we identify the main trends controlling the stabilization of one-tilt tetragonal phases across this family. We find that both the magnitude of the tilt angles and the energetic preference for tilted phases correlate primarily with the Goldschmidt tolerance factor $t$. The presence of stereochemically active lone-pair cations also correlates with enhanced tilting; however, this trend largely reflects that lone-pair chemistries in HDPs occur together with ionic sizes that shift $t$ away from unity. Consistent with this picture, we observe several compounds without lone pairs that nonetheless exhibit strong octahedral tilting. Finally, using machine-learned interatomic potentials, we connect the 0 K tilting energetics to finite-temperature behavior: compounds with more strongly stabilized tilt phases exhibit higher transition temperatures, and phonon spectra at 350 K reveal soft and broad modes that are consistent with the trends in tolerance factors, tilt angles, and tilt energies at 0 K. Our results provide a systematic reference for structure-stability relationships in HDPs and clarify when lone-pair chemistry is correlated with, rather than the primary cause of, octahedral tilting.

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Mehmet Baskurt, Erik Fransson, Madeleine Lindvik, Paul Erhart, Julia Wiktor. 2026-09-18. Octahedral Tilting in Halide Double Perovskites: Disentangling Lone-Pair Chemistry and Geometric Effects. https://arxiv.org/abs/2605.19414

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