AI 中文总结
本文推导了包含延迟效应的集体ICD理论，证实其可在气体中发生，明确物种激发后永久偶极矩变化是该过程的关键要素。
AI 中文摘要
分子间库仑衰变（Intermolecular Coulombic Decay，ICD）是自然界与实验室中广泛存在的现象，供体的多余能量会被用于电离邻近的受体。若多余能量不足以触发ICD，两个或更多供体可共同转移其总多余能量以电离受体。实验表明，这种集体ICD竟能在气体中发生。近期研究证实，由于 retardation（ retardation 译为 retardation，即延迟效应）的存在，标准ICD可在供体与受体间距较大时高效发生。本文推导了包含延迟效应的集体ICD理论，采用量子电动力学（Quantum Electrodynamics，QED）微扰论，通过引入包含延迟效应的两体相互作用势，大幅简化了该理论，同时提升了其可解释性。本文推导了集体ICD速率的显式公式，将该速率用可测量量和几何因子表达以作解释，还证实了物种激发后永久偶极矩的变化是集体ICD的相关要素。
英文摘要
Intermolecular Coulombic decay (ICD) is a widely spread phenomenon in nature and laboratory in which the excess energy of a donor is utilized to ionize a nearby acceptor. If the excess energy is insufficiently large to enable ICD, two (or more) donors can collectively transfer their combined excess energy to ionize the acceptor. Experiments show that this collective ICD is, surprisingly, operative in gases. Recently, it has been demonstrated that standard ICD can efficiently take place at large distances between the donors and acceptors due to retardation. Here, we derive the theory of collective ICD including retardation. Quantum electrodynamics (QED) perturbation theory is used and it is shown that the theory can be substantially simplified and the process also made more amenable to interpretation by introducing two-body interaction potentials which include retardation. Explicit formulas for the rate of collective ICD are derived and interpreted by expressing the rate in terms of measurable quantities and geometric factors. It is demonstrated that the change of the permanent dipole moments of the species upon excitation is a relevant ingredient in collective ICD.
Comments50 pages, 3 figures
