Speaker
Description
Isolated gas phase clusters of atoms and molecules serve as well established proxys for the characterization of elementary steps and intermediates within complex reactions at ambient or industrial conditions. In this context, the charge states of such clusters are subject of debate ever since. We have developed and applied a cryo trapping technique [1] that allowed us to characterize size selected transition metal clusters and their adsorbates for their kinetic and spectroscopic properties, and we have applied this technique to clusters of several transition metals and some of their alloys [2-8]. Electronic characterization arose through novel X-ray techniques which we have brought to application at our gas phase clusters [9]. On the basis of our wide spread results from these experiments we have recently started a systematic quantum chemical survey of charge states and shifts along the N2 activating reaction pathways of some selected clusters [10], and the conceptual findings of this survey shall be presented, and their implications and the outreach shall be discussed.
[1] DOI: 10.1016/B978-0-12-814013-0.00019-3; [3] DOI: 10.1039/c5cp00047e; [2] DOI: 10.1021/acs.jpcc.6b12167; 10.1063/1.4997403 ; 10.1063/1.4997407; [5] DOI: 10.1007/s11244-017-0865-2 ; 10.1080/00268976.2021.1953172; [4] DOI: 10.1063/5.0064965 ; 10.1063/5.0064966; [5] DOI: 10.1063/5.0075289 ; 10.1063/5.0075286; [7] DOI: 10.1039/D0CP06208A ; 10.1063/5.0157218 ; 10.1063/5.0157217; [8] DOI: 10.1021/acs.jpclett.8b00093 ; submitted to Helv. Chim. Act.; [9] DOI: 10.1103/PhysRevLett.107.233401 ; 10.1039/C5CP01923K ; 10.1063/1.4929482; [10] to be published