MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter, School of Physics, Xi'an Jiaotong University, Xi'an, 710049, China.
Institute of Atomic and Molecular Physics, Jilin University, Changchun, 130012, China.
Nat Commun. 2022 Sep 10;13(1):5335. doi: 10.1038/s41467-022-33032-2.
Intermolecular interactions involving aromatic rings are ubiquitous in biochemistry and they govern the properties of many organic materials. Nevertheless, our understanding of the structures and dynamics of aromatic clusters remains incomplete, in particular for systems beyond the dimers, despite their high presence in many macromolecular systems such as DNA and proteins. Here, we study the fragmentation dynamics of benzene trimer that represents a prototype of higher-order aromatic clusters. The trimers are initially ionized by electron-collision with the creation of a deep-lying carbon 2s state or one outer-valence and one inner-valence vacancies at two separate molecules. The system can thus relax via ultrafast intermolecular decay mechanisms, leading to the formation of C[Formula: see text]C[Formula: see text]C[Formula: see text] trications and followed by a concerted three-body Coulomb explosion. Triple-coincidence ion momentum spectroscopy, accompanied by ab-initio calculations and further supported by strong-field laser experiments, allows us to elucidate the details on the fragmentation dynamics of benzene trimers.
分子间涉及芳环的相互作用在生物化学中无处不在，它们控制着许多有机材料的性质。然而，尽管它们在许多大分子体系如 DNA 和蛋白质中大量存在，我们对芳族团簇的结构和动力学的理解仍然不完整，特别是对于二聚体以外的体系。在这里，我们研究了苯三聚体的碎裂动力学，它代表了更高阶芳族团簇的原型。三聚体最初通过与电子碰撞而被电离，在两个不同的分子中形成一个深埋的碳 2s 态或一个外价和一个内价空位。因此，该体系可以通过超快的分子间弛豫机制进行松弛，导致 C[Formula: see text]C[Formula: see text]C[Formula: see text] 三正离子的形成，并随后协同进行三体库仑爆炸。三重符合离子动量谱学，伴随着从头算计算，并进一步得到强场激光实验的支持，使我们能够阐明苯三聚体碎裂动力学的细节。
