论文标题
环境修饰的三体能量转移
Environment-modified three-body energy transfer
论文作者
论文摘要
从供体到受体的共振能量转移是原子系统和分子系统之间最基本的相互作用之一。在现实生活中，捐助者和受体不是孤立的，而是实际上与他们的环境以及其他原子和分子结合在一起。第三身体的存在可以以独特和复杂的方式改变供体和受体之间的能量转移速率，尤其是当三个站点系统本身与较大的宏观背景（例如溶剂）相互作用时。该速率可以触及扰动，通常需要大量类似Feynman的图。在这里，我们演示了一种基于规范扰动理论的方法，该方法使我们能够减少所需的计算工作，并使用此技术来推导背景环境中三体共振能量传递速率的公式。作为原理证明，我们将其应用于位于介电界面附近的二聚体的情况，并具有遥远的第三分子来控制速率，从而根据系统参数找到了增强或抑制速率。
Resonant energy transfer from a donor to an acceptor is one of the most basic interactions between atomic and molecular systems. In real-life situations, the donor and acceptor are not isolated but in fact coupled to their environment and to other atoms and molecules. The presence of a third body can modify the rate of energy transfer between donor and acceptor in distinctive and intricate ways, especially when the three-site system is itself interacting with a larger macroscopic background such as a solvent. The rate can be calculated perturbatively, which ordinarily requires the summation of very large numbers of Feynman-like diagrams. Here we demonstrate a method based on canonical perturbation theory that allows us to reduce the computational effort required, and use this technique to derive a formula for the rate of three-body resonance energy transfer in a background environment. As a proof-of-principle, we apply this to the situation of a dimer positioned near a dielectric interface, with a distant third molecule controlling the rate, finding both enhancement or suppression of the rate depending on system parameters.
