Optically nonlinear energy transfer in light-harvesting dendrimers

Andrews, David L. and Bradshaw, David S. ORCID: https://orcid.org/0000-0002-6458-432X (2004) Optically nonlinear energy transfer in light-harvesting dendrimers. The Journal of Chemical Physics, 121 (5). pp. 2445-2454. ISSN 1089-7690

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Dendrimeric polymers are the subject of intense research activity geared towards their implementation in nanodevice applications such as energy harvesting systems,organic light-emitting diodes, photosensitizers, low-threshold lasers, and quantum logic elements, etc. A recent development in this area has been the construction of dendrimers specifically designed to exhibit novel forms of optical nonlinearity, exploiting the unique properties of these materials at high levels of photon flux. Starting from a thorough treatment of the underlying theory based on the principles of molecular quantum electrodynamics, it is possible to identify and characterize several optically nonlinear mechanisms for directed energy transfer and energy pooling in multichromophore dendrimers. Such mechanisms fall into two classes: first, those where two-photon absorption by individual donors is followed by transfer of the net energy to an acceptor; second, those where the excitation of two electronically distinct but neighboring donor groups is followed by a collective migration of their energy to a suitable acceptor. Each transfer process is subject to minor dissipative losses. In this paper we describe in detail the balance of factors and the constraints that determines the favored mechanism, which include the excitation statistics, structure of the energy levels, laser coherence factors, chromophore selection rules and architecture, possibilities for the formation of delocalized excitons, spectral overlap, and the overall distribution of donors and acceptors. Furthermore, it transpires that quantum interference between different mechanisms can play an important role. Thus, as the relative importance of each mechanism determines the relevant nanophotonic characteristics, the results reported here afford the means for optimizing highly efficient light-harvesting dendrimer devices.

Item Type: Article
Uncontrolled Keywords: energy transfer,excitation energies,materials properties,laser optical systems,nonlinear optical materials
Faculty \ School: Faculty of Science > School of Chemistry
UEA Research Groups: Faculty of Science > Research Groups > Centre for Photonics and Quantum Science
Faculty of Science > Research Groups > Chemistry of Light and Energy
Faculty of Science > Research Groups > Physical and Analytical Chemistry (former - to 2017)
Depositing User: Rachel Smith
Date Deposited: 27 Oct 2010 14:48
Last Modified: 02 Mar 2023 12:30
URI: https://ueaeprints.uea.ac.uk/id/eprint/10693
DOI: 10.1063/1.1769354


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