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Layered materials span a very broad range of solids ranging from van derWaals materials to highly complex crystal structures such as clays. They arecommonly believed to have highly anisotropic properties, which is essentiallyattributed to weak interlayer interactions. The layered Mg3Sb2 structure iscurrently being intensely scrutinized due to its outstanding thermoelectricproperties. Based on quantitative chemical bonding analysis we unravel thatMg3Sb2 exhibits a nearly isotropic three-dimensional (3D) bonding network withthe interlayer and intralayer bonds being surprisingly similar, and theseunique chemical bonding features are the origin of the nearly isotropicstructural and thermal properties. The isotropic 3D bonding network is found tobe broadly applicable to many Mg-containing compounds with the layeredCaAl2Si2-type structure. Intriguingly, a parameter based on the electrondensity can be used as an indicator measuring the anisotropy of lattice thermalconductivity in layered structures. This work extends our understanding ofstructure and properties based on chemical bonding analysis, and it will guidethe search for, and design of, layered materials with tailored anisotropicproperties.

Relating chemical bonding to physical properties: The origin of unexpected isotropic properties in layered materials