Abstract

A fundamental understanding of molecular structure and chemical reactivity at complex interfaces is key to many technological applications ranging from single molecule electronics to functionalized surfaces and light- and electron-enhanced heterogeneous catalysis. Predictive ab-initio electronic structure methods enable to gain such understanding through an accurate description of interface structure, spectroscopy, and reactivity. On prototypical example systems such as the photo-induced isomerization of metal-adsorbed molecules, I will explain the computational techniques and methodological underpinnings that enable a computational interface characterization and description of surface spectroscopy measurements and our recent efforts to translate this description to larger length and time scales. I will furthermore present recently developed coupled electron-nuclear dynamics simulation methods that enable a direct simulation of electron- and light-driven chemical transformations at surfaces.