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Resonance energy transfer: the unified theory revisited

机译:共振能量转移:统一理论再探

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Resonance energy transfer (RET) is the principal mechanism for the intermolecular or intramolecular redistribution of electronic energy following molecular excitation. In terms of fundamental quantum interactions, the process is properly described in terms of a virtual photon transit between the pre-excited donor and a lower energy (usually ground-state) acceptor. The detailed quantum amplitude for RET is calculated by molecular quantum electrodynamical techniques with the observable, the transfer ate, derived via application of the Fermi golden rule. In the treatment reported here, recently devised state-sequence techniques and a novel calculational protocol is applied to RET and shown to circumvent problems associated with the usual method. The second-rank tensor describing virtual photon behavior evolves from a Green's function solution to the Helmholtz equation, and special functions are employed to realize the coupling tensor. The method is used to derive a new result for energy transfer systems sensitive to both magnetic- and electric-dipole transitions. The ensuing result is compared to that of pure electric-dipole-electric-dipole coupling and is analyzed with regard to acceptable transfer separations. Systems are proposed where the electric-dipole-magentic-dipole term is the leading contribution to the overall rate.
机译:共振能量转移(RET)是分子激发后分子间或分子内电子能量重新分布的主要机制。在基本的量子相互作用方面,该过程以预激发供体与较低能级(通常为基态)受体之间的虚拟光子跃迁进行了适当描述。 RET的详细量子振幅是通过分子量子电动力学技术计算得到的,其可观察到的转移速率是通过应用费米黄金定律得出的。在这里报道的治疗中,最近设计的状态序列技术和新颖的计算协议被应用于RET,并被证明可以规避与常规方法相关的问题。描述虚拟光子行为的第二张量从格林函数解演化为亥姆霍兹方程,并使用特殊函数来实现耦合张量。该方法用于为对磁偶极和电偶极跃迁都敏感的能量传输系统得出新结果。将所得结果与纯电偶极-电偶极耦合的结果进行比较,并就可接受的转移间隔进行分析。提出了系统,其中电偶极子-磁偶极子项是总速率的主要贡献。

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