Quantum chemical calculations are carried out in order to investigate the heterodimers of NF3 with isoelectronic and isostructure species of N2O and CO2 in gas phase within the MP2 (Møller–Plesset perturbation) and CCSD(T) levels. Three and four minima are located on the potential energy surfaces of NF3–CO2 and NF3–N2O systems at the MP2/aug–cc–PVDZ level, respectively. Single-point energy calculations at the MP2/aug–cc–PVTZ and CCSD(T)/aug–cc–PVDZ levels confirm results obtained at the MP2/aug–cc–PVDZ level show that atmospheric roles of NF3–N2O and NF3–CO2 systems are similar. The atom in molecules theory was applied to analyse the nature of intermolecular interactions. Also, natural bond orbital (NBO) analysis has been used in order to obtain charge transfer quota among heterodimers.
