Generalized quantum kinetic expansion: Higher-order corrections to multichromophoric Förster theory
For a general two-cluster energy transfer network, a new methodology of the generalized quantum kinetic expansion (GQKE) method is developed, which predicts an exact time-convolution equation for the cluster population evolution under the initial condition of the local cluster equilibrium state. The...
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Veröffentlicht in: | The Journal of chemical physics 2015-08, Vol.143 (7), p.074102-074102 |
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Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | For a general two-cluster energy transfer network, a new methodology of the generalized quantum kinetic expansion (GQKE) method is developed, which predicts an exact time-convolution equation for the cluster population evolution under the initial condition of the local cluster equilibrium state. The cluster-to-cluster rate kernel is expanded over the inter-cluster couplings. The lowest second-order GQKE rate recovers the multichromophoric Förster theory (MCFT) rate. The higher-order corrections to the MCFT rate are systematically included using the continued fraction resummation form, resulting in the resummed GQKE method. The reliability of the GQKE methodology is verified in two model systems, revealing the relevance of higher-order corrections. |
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ISSN: | 0021-9606 1089-7690 |
DOI: | 10.1063/1.4928634 |