title: Generalized quantum kinetic expansion: Higher-order corrections to multichromophoric Förster theory.
abstract: 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.
authors: Physics Department, Zhejiang University, 38 Zheda Road, Hangzhou, Zhejiang 310027, China.
authors: Jianlan
authors: J
authors: Wu
authors: Physics Department, Zhejiang University, 38 Zheda Road, Hangzhou, Zhejiang 310027, China.
authors: Zhihao
authors: Z
authors: Gong
authors: Physics Department, Zhejiang University, 38 Zheda Road, Hangzhou, Zhejiang 310027, China.
authors: Zhoufei
authors: Z
authors: Tang
mesh_terms: D001426:Bacterial Proteins / Q000737:chemistry; D001429:Bacteriochlorophylls / Q000737:chemistry; D031541:Fluorescence Resonance Energy Transfer; D007700:Kinetics; D045342:Light-Harvesting Protein Complexes / Q000737:chemistry; D008956:Models, Chemical; D011789:Quantum Theory
chemical_list: D001426:Bacterial Proteins; D001429:Bacteriochlorophylls; C086320:FMO bacteriochlorophyll protein, Bacteria; D045342:Light-Harvesting Protein Complexes