Jasík Juraj, Zabka Jan, Feketeova Linda, Ipolyi Imre, Märk Tilmann D, Herman Zdenek
V. Cermak Laboratory, J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, Dolejskova 3, 182 23 Prague 8, Czech Republic.
J Phys Chem A. 2005 Nov 17;109(45):10208-15. doi: 10.1021/jp053064a.
Interaction of C2Hn+ (n = 2-5) hydrocarbon ions and some of their isotopic variants with room-temperature and heated (600 degrees C) highly oriented pyrolytic graphite (HOPG) surfaces was investigated over the range of incident energies 11-46 eV and an incident angle of 60 degrees with respect to the surface normal. The work is an extension of our earlier research on surface interactions of CHn+ (n = 3-5) ions. Mass spectra, translational energy distributions, and angular distributions of product ions were measured. Collisions with the HOPG surface heated to 600 degrees C showed only partial or substantial dissociation of the projectile ions; translational energy distributions of the product ions peaked at about 50% of the incident energy. Interactions with the HOPG surface at room temperature showed both surface-induced dissociation of the projectiles and, in the case of radical cation projectiles C2H2+* and C2H4+, chemical reactions with the hydrocarbons on the surface. These reactions were (i) H-atom transfer to the projectile, formation of protonated projectiles, and their subsequent fragmentation and (ii) formation of a carbon chain build-up product in reactions of the projectile ion with a terminal CH3-group of the surface hydrocarbons and subsequent fragmentation of the product ion to C3H3+. The product ions were formed in inelastic collisions in which the translational energy of the surface-excited projectile peaked at about 32% of the incident energy. Angular distributions of reaction products showed peaking at subspecular angles close to 68 degrees (heated surfaces) and 72 degrees (room-temperature surfaces). The absolute survival probability at the incident angle of 60 degrees was about 0.1% for C2H2+, close to 1% for C2H4+* and C2H5+, and about 3-6% for C2H3+.
研究了C2Hn+(n = 2 - 5)烃离子及其一些同位素变体与室温及加热至600℃的高度取向热解石墨(HOPG)表面在11 - 46 eV的入射能量范围以及相对于表面法线60°的入射角下的相互作用。这项工作是我们早期关于CHn+(n = 3 - 5)离子表面相互作用研究的扩展。测量了产物离子的质谱、平动能分布和角分布。与加热到600℃的HOPG表面的碰撞仅显示出弹丸离子的部分或大量解离;产物离子的平动能分布在入射能量的约50%处达到峰值。在室温下与HOPG表面的相互作用既显示出弹丸的表面诱导解离,对于自由基阳离子弹丸C2H2+和C2H4+,还显示出与表面烃类的化学反应。这些反应包括:(i)氢原子转移到弹丸上,形成质子化弹丸,随后它们发生碎片化;(ii)在弹丸离子与表面烃类的末端CH3基团反应中形成碳链增长产物,随后产物离子碎片化生成C3H3+。产物离子是在非弹性碰撞中形成的,其中表面激发弹丸的平动能在入射能量的约32%处达到峰值。反应产物的角分布在接近68°(加热表面)和72°(室温表面)的亚镜面角处出现峰值。对于C2H2+*,在60°入射角下的绝对存活概率约为0.1%,对于C2H4+*和C2H5+接近1%,对于C2H3+约为3 - 6%。