Beck M, Bornhauser P, Visser Bradley, Knopp G, Bokhoven J A van, Radi P P
Photon Science Division, Paul Scherrer Institute, 5232, Villigen, Switzerland.
University of Applied Sciences and Arts, Northwestern Switzerland, 5610, Windisch, Switzerland.
Nat Commun. 2019 Jul 22;10(1):3270. doi: 10.1038/s41467-019-11156-2.
Transition metals, characterised by their partially filled d orbitals, provide the basis for many of the most relevant processes in chemistry, biology, and physics. Embedded as single atoms or in small clusters, they give rise to exceptional optical, chemical, and magnetic properties. So far, it has proven impossible to disentangle the complex network of excited quantum states, which greatly hinders prediction and control of material properties. Here, we apply two-colour resonant four-wave mixing to quantitatively resolve the quantum states of the neutral copper dimer. This allows us to unwind the individual spectral lines by isotopic composition and rotational quantum number and reveals a rich network of bright and perturbing dark states. While this work presents a road map for the experimental study of the bonding between and with transition metal atoms, it also provides experimental reference data for prospective quantum chemical approaches on handling systems with a high density of states.
过渡金属以其部分填充的d轨道为特征，为化学、生物学和物理学中许多最相关的过程提供了基础。作为单原子或小团簇嵌入时，它们会产生特殊的光学、化学和磁性能。到目前为止，已证明无法解开复杂的激发量子态网络，这极大地阻碍了对材料性能的预测和控制。在这里，我们应用双色共振四波混频来定量解析中性铜二聚体的量子态。这使我们能够通过同位素组成和转动量子数来解开各个光谱线，并揭示出丰富的亮态和扰动暗态网络。虽然这项工作为过渡金属原子之间以及与其他原子的键合实验研究提供了路线图，但它也为处理具有高态密度系统的前瞻性量子化学方法提供了实验参考数据。
