We are interested in the dynamic behavior of molecules, in addition to their static structures. In particular, we focus on molecules at surfaces and interfaces. These are the places where the spatially isolated electrons in molecules meet delocalized ones in substrates such as metals. Under such circumstances, molecules behave very differently from those in gas and liquid phases. Sometimes, totally unexpected molecular processes take place at surfaces and interfaces. Of course, there are many important applications where surfaces/interfaces play an important role, such as photovoltaic and catalytic applications. These all depend on specific complex interactions that are not always fully understood. Thus, our aim is to clarify such interactions and determine how they govern electron and nuclear dynamics at surfaces and interfaces.