How Thermodynamically Accessible are Quaternary Mixed-Metal Chalcohalides?
Abstract
Quaternary mixed-metal chalcohalides (MMCHs) are a promising mixed-anion semiconductor family, but their thermodynamic accessibility remains largely unexplored. We combine density functional theory with the Alexandria Materials Database to carry out a rapid and reliable evaluation of the thermodynamic accessibility of 54 M(II)2M(III)Ch2X3 compounds. All evaluated MMCHs are predicted to be thermodynamically unstable, but a considerable fraction of MMCHs lie within computational uncertainty of the convex hull. Their predicted decomposition follows five distinct reaction pathways, most commonly into M(III)2Ch3, M(II)X2, and M(II)Ch. Solution processing of six Sn-based MMCHs supports our analysis. Notably, this includes the first synthesis of the previously unreported Sn2InS2Br3 in a multiphase film. Our approach identifies convex hull proximity and competing phase formation as key constraints on MMCH synthetic accessibility during solution processing, thereby guiding future MMCH exploration.
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BibTeX
@misc{henkel2026thermodynamically,
title = {{How Thermodynamically Accessible are Quaternary Mixed-Metal Chalcohalides?}},
author = {Pascal Henkel and G. Krishnamurthy Grandhi and Jarno Laakso and David Rovira Ferrer and Edgardo Saucedo and Jingrui Li and Paola Vivo and Miguel A. L. Marques and Patrick Rinke},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.38125},
eprint = {2609.38125},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.38125},
}
RIS
TY - UNPB
TI - How Thermodynamically Accessible are Quaternary Mixed-Metal Chalcohalides?
AU - Pascal Henkel
AU - G. Krishnamurthy Grandhi
AU - Jarno Laakso
AU - David Rovira Ferrer
AU - Edgardo Saucedo
AU - Jingrui Li
AU - Paola Vivo
AU - Miguel A. L. Marques
AU - Patrick Rinke
PY - 2026
DA - 2026/09/29
PB - arXiv
DO - 10.48550/arxiv.2609.38125
UR - https://arxiv.org/abs/2609.38125
AB - Quaternary mixed-metal chalcohalides (MMCHs) are a promising mixed-anion semiconductor family, but their thermodynamic accessibility remains largely unexplored. We combine density functional theory with the Alexandria Materials Database to carry out a rapid and reliable evaluation of the thermodynamic accessibility of 54 M(II)_2M(III)Ch_2X_3 compounds. All evaluated MMCHs are predicted to be thermodynamically unstable, but a considerable fraction of MMCHs lie within computational uncertainty of the convex hull. Their predicted decomposition follows five distinct reaction pathways, most commonly into M(III)_2Ch_3, M(II)X_2, and M(II)Ch. Solution processing of six Sn-based MMCHs supports our analysis. Notably, this includes the first synthesis of the previously unreported Sn_2InS_2Br_3 in a multiphase film. Our approach identifies convex hull proximity and competing phase formation as key constraints on MMCH synthetic accessibility during solution processing, thereby guiding future MMCH exploration.
ER -