The thermochemical data Δ H0n-1, n and Δ S0n-1, n for clustering reactions CH +3(Ar) n-1 + Ar⇌CH +3(Ar) n were determined with a pulsed electron beam high-pressure mass spectrometer. It was found that (1) the bond energy of CH +3(Ar) n with n = 1 (-Δ H00,1 = 11.3 kcal/mol) is much higher than that with n = 2 (-ΔH 01,2 = 2.26 kcal/mol); (2) -Δ H01,2 is slightly greater than -Δ H02,3 (1.97 kcal/mol), and (3) the -Δ H0n-1, n values with n = 3-8 are almost n-independent. The structures of CH +3(Ar) n with n = 1-3 were determined by ab initio MO calculations. The theoretical calculations predict some participation of covalent bond (charge transfer) in CH +3(Ar) n with n = 1 and 2. The nature of bonding in the complex with n ⩾ 3 is almost entirely electrostatic.
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