Metavalent or Hypervalent Bonding: Is There a Chance for Reconciliation?

超价或高价键合:还有和解的可能吗?

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Abstract

A family of solids including crystalline phase change materials such as GeTe and Sb(2) Te(3) , topological insulators like Bi(2) Se(3,) and halide perovskites such as CsPbI(3) possesses an unconventional property portfolio that seems incompatible with ionic, metallic, or covalent bonding. Instead, evidence is found for a bonding mechanism characterized by half-filled p-bands and a competition between electron localization and delocalization. Different bonding concepts have recently been suggested based on quantum chemical bonding descriptors which either define the bonds in these solids as electron-deficient (metavalent) or electron-rich (hypervalent). This disagreement raises concerns about the accuracy of quantum-chemical bonding descriptors is showed. Here independent of the approach chosen, electron-deficient bonds govern the materials mentioned above is showed. A detailed analysis of bonding in electron-rich XeF(2) and electron-deficient GeTe shows that in both cases p-electrons govern bonding, while s-electrons only play a minor role. Yet, the properties of the electron-deficient crystals are very different from molecular crystals of electron-rich XeF(2) or electron-deficient B(2) H(6) . The unique properties of phase change materials and related solids can be attributed to an extended system of half-filled bonds, providing further arguments as to why a distinct nomenclature such as metavalent bonding is adequate and appropriate for these solids.

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