Efficient Exploratory Synthesis of Quaternary Cesium Chlorides Guided by In Silico Predictions

Area of Science:

• Solid-state chemistry
• Materials science
• Computational materials science

Background:

• Exploratory solid-state synthesis is crucial but time-consuming.
• Quaternary cesium chlorides (Cs₂A^IB^IIICl₆) are an underexplored class of materials.

Purpose of the Study:

• To develop an efficient strategy for exploring the synthesis of quaternary cesium chlorides.
• To bridge computational predictions with experimental synthesis and characterization.
• To identify new compounds and polymorphs within the Cs₂A^IB^IIICl₆ system.

Main Methods:

• Computational prediction of material stability.
• In situ synchrotron X-ray diffraction for assessing synthesizability.
• Laboratory synthesis and characterization using powder X-ray and neutron diffraction.
• Rietveld refinement for structural analysis.

Main Results:

• Successful synthesis of new polymorphs of Cs₂LiCrCl₆ and Cs₂LiRuCl₆.
• Discovery of a new compound, Cs₂LiIrCl₆.
• Demonstration of a strategy combining computational predictions and experimental validation.

Conclusions:

• The developed strategy efficiently guides exploratory solid-state synthesis.
• Computational predictions are valuable for identifying promising synthetic targets.
• New quaternary cesium chlorides and polymorphs expand the known materials landscape.