Strong-coupling between light and matter produces hybridized states (polaritons) whose delocalization and electromagnetic character allow for novel modifications in spectroscopy and chemical reactivity of molecular systems. Recent experiments have demonstrated remarkable distance-independent long-range energy transfer between molecules strongly coupled to optical microcavity modes. To shed light on the mechanism of this phenomenon, we present the first comprehensive theory of polariton-assisted remote energy transfer (PARET) based on strong-coupling of donor and/or acceptor chromophores to surface plasmons. Application of our theory demonstrates that PARET up to a micron is indeed possible. In particular, we report two regimes for PARET: in one case, strong-coupling to a single type of chromophore leads to transfer mediated largely by surface plasmons while in the other case, strong-coupling to both types of chromophores creates energy transfer pathways mediated by vibrational relaxation. Importantly, we highlight conditions under which coherence enhances or deteriorates these processes. For instance, while exclusive strong-coupling to donors can enhance transfer to acceptors, the reverse turns out not to be true. However, strong-coupling to acceptors can shift energy levels in a way that transfer from acceptors to donors can occur, thus yielding a chromophore role-reversal or “carnival effect”. This theoretical study demonstrates the potential for confined electromagnetic fields to control and mediate PARET, thus opening doors to the design of remote mesoscale interactions between molecular systems.

中文翻译：

---

极化子辅助的远程能量传输理论†

光与物质之间的强耦合产生了杂化态（极化子），其离域和电磁特性使光谱学和分子系统的化学反应性发生了新的变化。最近的实验表明，在与光学微腔模式强烈耦合的分子之间，非凡的距离无关的远距离能量转移。为了阐明这种现象的机理，我们提出了基于供体和/或受体生色团与表面等离子体激元的强耦合的极化辅助远程能量转移（PARET）的第一个综合理论。我们理论的应用表明，最大可能达到PARET的微米。特别是，我们报告了P​​ARET的两种制度：在一种情况下，与单一类型生色团的强耦合导致转移主要由表面等离激元介导，而在另一种情况下，与两种类型生色团的强耦合产生由振动弛豫介导的能量转移途径。重要的是，我们强调了一致性会增强或恶化这些过程的条件。例如，虽然与供体的排他性强耦合可以增强向受体的转移，但事实并非如此。但是，与受体的强耦合可以改变能级，从而发生从受体到供体的转移，从而产生生色团的作用反转或“狂欢节效应”。这项理论研究证明了受限电磁场控制和调解PARET的潜力，