Journal of Chemical Physics p. 8687 - 8696 (1994)
Update date:2022-08-11
Topics:
Tsuji, Masaharu
Matsumura, Ken-ichi
Kouno, Hiroyuki
Aizawa, Masato
Nishimura, Yukio
The product ion distributions and rate constants are determined for ion-molecule reactions of ArN2+ with C2Hn (n=2,4,6) and C3Hn (n=6,8) by using a thermal ion-beam apparatus.Although charge-transfer channels leading to parent ions and/or fragment ions are found, no displacement reaction leading to ArCmHn+ and N2CmHn+ is detected.A comparison of the product ion distributions with breakdown patterns of the parent ions suggests that fragment ions, formed through cleavage of C-H and/or C-C bonds, are produced via near-resonant ionic states in the 13.1-13.4 eV range.The branching ratios of parent ions for C2H4 (68percent) and C3H6 (20percent) are larger than those for C2H6 (5percent) and C3H8 (5percent).The large branching ratios of the parent ions for the unsaturated hydrocarbons are explained as due to a strong interaction of a vacant orbital of ArN2+ with the highest occupied ?C=C orbital of the unsaturated hydrocarbons which induces nonresonant charge transfer.The total rate constant for C2H2 is 6.8x10-10 cm3 s-1, while those for C2Hn (n = 4,6) and C3Hn (n = 6,8) are in the range (8.5-9.8)x10-10 cm3 s-1.The former and the latter values correspond to 69percent and 77percent-90percent of the calculated values from Langevin or average dipole orientation (ADO) theory.The smaller kobs/kcalc ratio for C2H2 is attributed to the lack of near-resonant ionic states with favorable Franck-Condon factors for ionization.
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