首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Laser-Induced Formation, Fragmentation, Coalescence, and Delayed Ionization of the C_(59)N Heterofullerene
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Laser-Induced Formation, Fragmentation, Coalescence, and Delayed Ionization of the C_(59)N Heterofullerene

机译:激光诱导的C_(59)N杂富勒烯的形成,断裂,聚结和延迟电离

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The formation of the nitrogen heterofullerene, C_(59)N, following the ablation of a variety of fullerene derivatives, all of which possess organic ligands bound to the carbon cage through a nitrogen atom, has been investigated utilizing laser desorption/ionization mass spectrometry. Investigating the formation of cationic and anionic C_(59)N~(+/-), this approach is found to be a new and very efficient way to implement the initially exohedral nitrogen atom into the carbon cage. The laser-induced heterofullerene formation is discussed in terms of the structure and the charge stage dependency of the target material. In further experiments, the coalescence reactivity, leading toward the formation of larger clusters has been examined following laser ablation of thin films of the (C_(59)N)_2 dimer. Coalescence leads to two major reaction products, consisting of larger C_(n - 1)N~+ clusters which retain the nitrogen atom networked into a larger carbon cage and pure C_n~+ (n = even) carbon clusters. The C_(n - 1)N~+ cluster formation is accompanied by abundant metastable transitions caused by the loss of CN and the resulting implications for the coalescence mechanism are discussed. Finally, evidence is presented for the delayed electron emission of C_(59)N·. The observation of delayed ionization of heterofullerenes is unprecedented, revealing a similar resistance toward fragmentation as the case of their all-carbon fullerene analogues.
机译:已经通过激光解吸/电离质谱研究了各种富勒烯衍生物的烧蚀后形成的氮杂富勒烯C_(59)N,所有这些富勒烯衍生物均具有通过氮原子与碳笼结合的有机配体。研究阳离子和阴离子C_(59)N〜(+/-)的形成,发现这种方法是将最初的外表面氮原子引入碳笼的一种非常有效的新方法。根据靶材料的结构和电荷级依赖性,讨论了激光诱导的异富勒烯形成。在进一步的实验中,在激光烧蚀(C_(59)N)_2二聚体薄膜之后,研究了导致较大簇形成的聚结反应性。聚结产生两个主要的反应产物,它们由较大的C_(n-1)N〜+团簇和纯C_n〜+(n =偶数)团簇组成,这些团簇保留了连接到较大碳笼中的氮原子。 C_(n-1)N〜+团簇的形成伴随着大量CN的损失引起的亚稳态跃迁,并讨论了其对聚结机理的影响。最后,给出了电子延迟发射C_(59)N·的证据。对异富勒烯进行延迟电离的观察是前所未有的,与它们的全碳富勒烯类似物一样,其对碎片的抵抗力相似。

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