Mechanistic aspects of nonenzymatic RNA self-replication involving phosphoroimidazolide monomers were previously investigated with X-ray crystallography at different stages of the primer extension process . The acquired crystal structures confirmed the previous interpretation that the process involves the formation of imidazolium bridged dinucleotide intermediates and also offered information about the binding mode and conformation of activated guanosine nucleotides . However, X-ray crystallography does not offer any information about the dynamical behavior of the system and about minor conformations which might play an important role in the mechanism. Furthermore, it is limited to systems which can be readily crystallized, which is often challenging for nucleic acids with non-biological components . Therefore, to offer a comprehensive description of the mechanism of non-enzymatic RNA template copying, a more precise examination of the structures and dynamics of the binding of activated nucleotides to the template is necessary.