Argonne-Northwestern Solar Energy Research Center, Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208, USA.
Rep Prog Phys. 2012 Sep;75(9):096402. doi: 10.1088/0034-4885/75/9/096402. Epub 2012 Aug 30.
Plasmon-molecule interactions are widely believed to involve photo-induced interferences between the localized excitation of individual electrons in molecules and the large collective excitation of conduction electrons in metal particles. The intrinsic multi-scale characteristics of plasmon-molecule interactions not only offer great opportunities for realizing precise top-down control of the optical properties of individual molecules, but also allow for accurate bottom-up manipulation of light polarization and propagation as a result of molecular excitation. However, the temporal and spatial complexity of plasmon-molecule experiments severely limits our interpretation and understanding of interactions that have important applications in dye-sensitized solar cells, single-molecule detectors, photoconductive molecular electronics, all-optical switching and photo-catalytic water splitting. This review aims to outline recent progress in experimental practice and theory for probing and exploiting the subtle coupling between discrete molecular orbitals and continuous metallic bands. For each experimental technique or theoretical model, the fundamental mechanisms and relevant applications are discussed in detail with specific examples. In addition, the experimental validation of theoretical models and the computational design of functional devices are both highlighted. Finally, a brief summary is presented together with an outlook for potential future directions of this emerging interdisciplinary research field.
等离子体-分子相互作用被广泛认为涉及分子中单个电子的局域激发与金属颗粒中传导电子的大集体激发之间的光诱导干扰。等离子体-分子相互作用的固有多尺度特性不仅为实现对单个分子光学性质的精确自上而下控制提供了巨大的机会，而且由于分子激发，还可以实现对光偏振和传播的精确自下而上操纵。然而，等离子体-分子实验的时间和空间复杂性严重限制了我们对在染料敏化太阳能电池、单分子探测器、光电导分子电子学、全光开关和光催化水分解等具有重要应用的相互作用的解释和理解。本综述旨在概述探测和利用离散分子轨道与连续金属能带之间微妙耦合的实验实践和理论的最新进展。对于每种实验技术或理论模型，都通过具体实例详细讨论了其基本机制和相关应用。此外，还强调了理论模型的实验验证和功能器件的计算设计。最后，给出了简短的总结，并展望了这一新兴交叉学科研究领域的未来发展方向。
