LAUSR

Abstract Bilayer assembly is important for energy conversion devices such as the photoelectrochemical water-splitting system, in which a second layer such as the catalyst is required to deposit onto a functional self-assembled monolayer. In this manuscript, we employ first principles calculations to reveal the nanoscopic structures and properties of a long alkyl chain stabilized bilayer assembly on metal oxide substrate. The calculation confirms the viability of employing the long alkyl chain as an effective anchoring method to stabilize the self-assembled bilayer. The calculation constructs the potential energy surface and identifies a charge transfer character induced by the long alkyl chain interactions. We expect that the long alkyl chains could facilitate the preparation of more advanced surface structures for energy conversion devices which rely on self-assembled multilayers. This study helps the fundamental understanding of photoelectrochemical photoelectrodes and optoelectronic devices with the multi-layer molecular assembly.