发表机构
Université Caen Normandie, ENSICAEN, CNRS, CEA, Normandie Univ, CIMAP UMR6252; Lund University; University of Gothenburg; Institute of Physical Chemistry, Polish Academy of Sciences（卡昂诺曼底大学，ENSICAEN，法国国家科学研究中心，法国原子能和替代能源委员会; 隆德大学; 哥德堡大学; 波兰科学院物理化学研究所）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过质谱和量子化学计算，发现keV离子轰击金刚烷团簇引发广泛脱氢和分子间共价键形成，将弱结合团簇转化为特定结构的碳质物种，揭示了电离驱动的分子生长机制。
AI 中文摘要
我们研究了在初始中性气相金刚烷团簇（最简单的金刚烷型分子，Ad，C$_{10}$H$_{16}$）中，由keV离子诱导的碎裂和分子生长过程。通过结合飞行时间质谱和量子化学计算，我们发现完整的团簇阳离子经历了广泛的脱氢反应。我们还观察到单电荷产物的明显分布，其质量主要介于金刚烷单体和二聚体阳离子之间。我们将这些物种归因于离子诱导的生长产物，并利用量子化学计算，考虑最小的团簇阳离子[Ad]$_2^+$来解释它们的形成。我们的结果表明，电离强烈地重构了二聚体的几何结构，促进了H$_2$的消除和分子间共价C--C键的形成。弱结合的金刚烷团簇由此转变为共价结合的碳质物种，并强烈偏好特定的分子结构。这些发现为饱和烃系统中电离驱动的分子生长提供了新的见解，有助于理解分子复杂化，对化学物理和天体化学具有重要意义。
英文摘要
We investigate fragmentation and molecular growth induced by keV ions in initially neutral gas-phase adamantane clusters, the simplest diamondoid molecule (Ad, C$_{10}$H$_{16}$). Using time-of-flight mass spectrometry in combination with quantum-chemical calculations, we find that intact cluster cations undergo extensive dehydrogenation. We also observe a distinct distribution of singly charged products with masses predominantly between those of the adamantane monomer and dimer cations. We attribute these species to ion-induced growth products and interpret their formation considering the smallest cluster cation, [Ad]$_2^+$, using quantum-chemical calculations. Our results demonstrate that ionization strongly reorganizes the dimer geometry, facilitating H$_2$ elimination and intermolecular covalent C--C bond formation. Weakly bound adamantane clusters are thereby transformed into covalently bound carbonaceous species with a strong preference for specific molecular structures. These findings provide new insight into ionization-driven molecular growth in saturated hydrocarbon systems contributing to the understanding of molecular complexification, with implications for chemical physics and astrochemistry.
CommentsArticle is submitted to "The Journal of Physical Chemistry Letters"
