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High‐level G4 calculations show that the strength of chalcogen interactions is enhanced dramatically if chalcogen compounds simultaneously form alkaline‐earth bonds. This phenomenon is studied by exploring binary YX2⋅⋅⋅N‐Base complexes and two types of ternary MCl2⋅⋅⋅YX2⋅⋅⋅N‐Base, YX2⋅⋅⋅N‐Base⋅⋅⋅MCl2 complexes, in which YX2 is a chalcogen compound (Y=S, Se; X=F, Cl), the N‐Bases are sp, sp2, and sp...
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