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The reaction of Au+(1S,3D) with CS2 has been investigated at the B3LYP and CCSD(T) levels of theory.The identified reaction pathways revealed that the experimentally observed products,AuS+ and AuCS+,can be produced by the insertion of Au+ into C-S bond.The calculated energetics shows that the reactions on singlet surface lead to excited-state products,AuS+(1Σ) + 1CS and AuCS+(1Σ) + 1S,and have notable energy barriers,whereas the reactions on triplet surface producing the ground state products of AuS+(3Σ) + 1CS and AuCS+(1Σ) + 3S are energetically much more favorable.This result suggests that the minor formations of AuS+ and AuCS+ observed in the previous experiment under room-temperature condition should result from the reactions of excited-state Au+(3D) with CS2.Further,the possibility for singlet-triplet surface crossing was also discussed by approximately determining the crossing region.
The reaction of Au + (1S, 3D) with CS2 has been investigated at the B3LYP and CCSD (T) levels of theory. The identified reaction pathways revealed that the experimentally observed products, AuS + and AuCS +, can be produced by the insertion of Au + into CS bond.The calculated energetics shows that the reactions on singlet surface lead to excited-state products, AuS + (1Σ) + 1CS and AuCS + (1Σ) + 1S, and have notable energy barriers, while the reactions on triplet surface producing the ground state products of AuS + (3Σ) + 1CS and AuCS + (1Σ) + 3S are energetically much more favorable. This result suggests that the minor formations of AuS + and AuCS + observed in the previous experiment under room-temperature conditions should result from the reactions of excited- state Au + (3D) with CS2.Further, the possibility for singlet-triplet surface crossing was also discussed about undetermined the crossing region.