受限电磁场中的电子转移
Electron transfer in confined electromagnetic fields
摘要:
由于纳米光子学的快速发展,分子(原子)电子与反射腔的真空场之间的相互作用引起了人们的极大兴趣。这种相互作用属于腔量子电动力学的范畴,可以对分子系统的输运性质产生重大影响。本文研究了腔模存在下的非绝热电子转移过程。本文提出了一个广义的带电分子系统与腔体量子化电磁场相互作用的理论框架,并将其应用于封闭真空电磁场中施主与受主之间的电子转移问题。有效系统的哈密顿量对应于一个统一的拉比和自旋玻色子模型,其中包括一个自偶极能量项。两个限制的情况下被认为是:一个电子被假定为远快于腔模式和另一个在其中的电子隧穿时间是显着大于模式周期。在这两种情况下,一个显着的速率增强可以通过耦合到马库斯反转区的腔模。这项工作的结果提供了新的可能性控制电子转移过程中使用可见光和红外等离子体
英文摘要:
The interaction between molecular (atomic) electron(s) and the vacuum field of a reflective cavity generates a significant interest thanks to the rapid developments in nanophotonics. Such interaction which lies within the realm of cavity quantum electrodynamic can substantially affect transport properties of molecular systems. In this work we consider non-adiabatic electron transfer process in the presence of a cavity mode. We present a generalized framework for the interaction between a charged molecular system and a quantized electromagnetic field of a cavity and apply it to the problem of electron transfer between a donor and an acceptor placed in a confined vacuum electromagnetic field. The effective system Hamiltonian corresponds to a unified Rabi and spin-boson model which includes a self-dipole energy term. Two limiting cases are considered: one where the electron is assumed much faster than the cavity mode and another in which the electron tunneling time is significantly larger than the mode period. In both cases a significant rate enhancement can be produced by coupling to the cavity mode in the Marcus inverted region. The results of this work offer new possibilities for controlling electron transfer processes using visible and infrared plasmonics
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