In the bottom-up approach to nanotechnology, molecular-scale devices are constructed by designing their components to self-assemble and realize a desired structure or complex. In this context, the self-assembly process often occurs in the vicinity of a solid substrate. Theoretical investigations of surface self-assembly can be extremely useful counterparts to experimental studies, but can be challenging to pursue. One main issue is that while ultimately, quantum level information about the molecules, the surface and their interactions is essential to understand, the representative size of the system is more amenable to bulk simulations. This presentation will describe some of our group's efforts to advance the theoretical understanding of molecular self-assembly and behaviour on solid surfaces. Our studies of chiral structure formation at adsorption and its relationship to molecular structure will be discussed in some detail, with emphasis on both thiol adsorption on chiral facets, and the self-assembly of small chiral amino acids. The second part of the talk will present our investigations of field-response properties of nanostructured materials.