Primary Photonic Processes in Energy Harvesting: Quantum Dynamical Analysis of Exciton Energy Transfer over Three-Dimensional Dendrimeric Geometries

Andrews, DL and Jones, GA (2011) Primary Photonic Processes in Energy Harvesting: Quantum Dynamical Analysis of Exciton Energy Transfer over Three-Dimensional Dendrimeric Geometries. MRS Proceedings, 1325. ISSN 1946-4274

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Abstract

In molecular solar energy harvesting systems, quantum mechanical features may be apparent in the physical processes involved in the acquisition and migration of photon energy. With a sharply declining distance-dependence in transfer efficiency, the excitation energy generally takes a large number of steps en route to the site of its utilization; quantum features are rapidly dissipated in an essentially stochastic process. In the case of engineered dendrimeric polymers, each such step usually takes the form of an inward hop between chromophores in neighboring generation shells. A physically intuitive, structure-determined adjacency matrix formulation of the energy flow affords insights into the key harvesting and inward funneling processes. A numerical method based on this analytic approach has now been developed and is able to deliver results on significantly larger dendrimeric polymers, with the help of large multi-processor computers. Central to this study is the interpretation of key features such as the relevance of a spectroscopic gradient and the presence of traps or irregularities due to conformational changes and folding. With the objective of fine-tune the funneling process, this model now allows the incorporation of parameters derived from quantum chemical calculations, affording new insights into the detailed operation of the harvesting process in a variety of dendrimer systems.

Item Type: Article
Faculty \ School: Faculty of Science > School of Chemistry
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Depositing User: Users 2731 not found.
Date Deposited: 10 Jan 2012 16:30
Last Modified: 17 Sep 2020 23:30
URI: https://ueaeprints.uea.ac.uk/id/eprint/36071
DOI: 10.1557/opl.2011.846

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