The current energy infrastructure generating and transporting electrical energy is inefficient: between conversion inefficiencies and transmission losses, approximately 30% of electricity produced is lost to the environment without being consumed. Further, the best photovoltaic devices have not exceeded 45% efficiency and industrial panels have even lower yields. This paper focuses on a scalable method for using Hamiltonians like those proposed by K�ppel, Domcke, and Cederbaum, where the system is described in an electronic vibronic product basis, to simulate non-adiabatic energy conversion and transportation processes in molecules and materials. Using spectroscopic measurements to validate the applied model is emphasized. Initially, small diphenylalkanes will be simulated using parameters obtained from ab-initio calculations and the resulting spectra will be compared to resonant two photon ionization and laser induced fluorescence spectra obtained by Zwier and co-workers (Zwier, private communications) (Figure 1). Following the validation of this model, we will proceed to apply the method to larger systems such as the photosynthetic Fenna-Matthews-Olson complex. Parameters for this system will be found using scalable ab-initio calculations, such as the Fragment Molecular Orbital and Effective Fragment Potential methodologies. Exploration of this prototypical multi-chromophore complex will then be used to obtain an intuitive picture of the effects of electronic-vibronic coupling on energy transport in biological systems through wave function visualization and analysis, aiding in the development of the next generation of energy harvesting and transporting materials.

Understanding non-adiabatic effects in molecules and materials with scalable ab-initio methods and KDC-like Hamiltonians

248th National Meeting (2014)

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