This proposal consists of three subprojects that are related to each other and offer broad synergies. In project A we continue to investigate modern template surfaces for molecular self-assembly based on hexagonal boron nitride or graphene layers on transition metals. In order to connect molecule arrays formed on these templates to the macroscopic world we will implement two new experimental techniques: the detection of light-emission from individual molecules in scanning tunneling microscope junctions and the in-situ resistance measurement in thin metal films covered by templated molecular layers. The choice of molecules is driven by the specific questions that are addressed, like e.g. how negatively charged molecules are immobilized on sp2 templates, or how single electron spins can be controlled in an sp2 templated molecular nanostructure. A second activity will explore new approaches for the formation of double layers, with one particular focus being the growth of graphene / boron nitride heterostructures. With the implementation of the mu-metal shielding around the detector, our spin-resolved photoemission end station at the SLS has become a successful and unique facility for studying spin systems on surfaces. In project B the focus lies primarily on momentum dependent spin-structures in low dimensional systems, induced by the Rashba effect and related spin-orbit-interaction induced effects. Specifically, the tuning of the spin splitting in quantum well states in few monolayer thick Pb films on Si(111) by interface engineering will be studied, as well as the influence of alloying Bi, Pb and Sb on Ag(111) surfaces on the resulting spin structures of the surface states.In project C, transient processes occurring on a femtosecond timescale on surfaces are studied by means of time-resolved photoelectron spectroscopy. This research focuses on the phenomenon of ultrafast magnetization dynamics in thin ferromagnetic films, exploiting the constant energy surface mapping capabilities of an electron display analyzer for pump-probe experiments; this project includes the final setup of the display analyzer and the development of a high-harmonic generation setup for UV-pulses. Moreover, the properties and dynamics of negative electron affinity surfaces, in particular diamondoid layers on pre-patterned surfaces like the boron nitride nanomesh will be investigated.