Knecht Peter, Reichert Joachim, Deimel Peter S, Feulner Peter, Haag Felix, Allegretti Francesco, Garnica Manuela, Schwarz Martin, Auwärter Willi, Ryan Paul T P, Lee Tien-Lin, Duncan David A, Seitsonen Ari Paavo, Barth Johannes V, Papageorgiou Anthoula C
Physics Department E20, Technical University of Munich, James Franck Straße 1, 85748, Garching, Germany.
Current address: Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA-Nanociencia), Cantoblanco, 28049, Madrid, Spain.
Angew Chem Int Ed Engl. 2021 Jul 19;60(30):16561-16567. doi: 10.1002/anie.202104075. Epub 2021 Jun 22.
We assess the crucial role of tetrapyrrole flexibility in the CO ligation to distinct Ru-porphyrins supported on an atomistically well-defined Ag(111) substrate. Our systematic real-space visualisation and manipulation experiments with scanning tunnelling microscopy directly probe the ligation, while bond-resolving atomic force microscopy and X-ray standing-wave measurements characterise the geometry, X-ray and ultraviolet photoelectron spectroscopy the electronic structure, and temperature-programmed desorption the binding strength. Density-functional-theory calculations provide additional insight into the functional interface. We unambiguously demonstrate that the substituents regulate the interfacial conformational adaptability, either promoting or obstructing the uptake of axial CO adducts.
我们评估了四吡咯柔韧性在一氧化碳与原子尺度清晰的 Ag(111) 基底上负载的不同钌卟啉进行配位时所起的关键作用。我们利用扫描隧道显微镜进行的系统实空间可视化和操纵实验直接探测了配位过程，而键分辨原子力显微镜和 X 射线驻波测量表征了其几何结构，X 射线和紫外光电子能谱表征了电子结构，程序升温脱附表征了结合强度。密度泛函理论计算为功能界面提供了更多见解。我们明确证明，取代基调节界面构象适应性，促进或阻碍轴向一氧化碳加合物的摄取。
