Theory and modelling of energy transport in quantum nanostructures

This thesis is concerned with quantum properties of excitonic energy transport in nanostructures that are embedded in a noisy environment. Of principal interests are ways to exploit this environment to facilitate the transport of energetic excitations. The first research chapter deals with an extension to the 'standard' open quantum system picture, where the Hilbert space is split into three: system, environment, and a wider universe. This division is natural for many biological and artificial nanostructures. A new analytical method, based on a phase space representation of the density matrix, is developed for studying such division. The effects of the wider universe are shown to be captured by a simple correction of the environmental response function. The second research chapter addresses the question: when do second-order perturbative approaches to open quantum systems, which are intuitive and simple to compute, provide adequate accuracy? A simple analytical criterion is developed, and its validity is verified for the case of the much-studied FMO dynamics as well as the canonical spin-boson model. In the third research chapter, an intuitive model of a photocell is studied. The model comprises two light-absorbing molecules coupled to an idealised reaction centre, showing asymmetric dimers are capable of providing a significant enhancement of light-to-current conversion under ambient conditions. This is done by 'parking' the energy of an absorbed photon in a dark state which neither absorbs nor emits light. In the final research chapter, a basic model for what can be thought as a "quantum brachistochrone" problem is investigated. Exotic energy configurations are found to yield considerable enhancement to the exciton’s transfer probability, due to similar mechanisms studied in the previous chapter.