Christopher Phillip, Moskovits Martin
Department of Chemical and Environmental Engineering, University of California, Riverside, California 92521; email:
Department of Chemistry and Biochemistry, University of California, Santa Barbara, California 93106; email:
Annu Rev Phys Chem. 2017 May 5;68:379-398. doi: 10.1146/annurev-physchem-052516-044948. Epub 2017 Mar 16.
Surface plasmons have recently been harnessed to carry out processes such as photovoltaic current generation, redox photochemistry, photocatalysis, and photodetection, all of which are enabled by separating energetic (hot) electrons and holes-processes that, previously, were the domain of semiconductor junctions. Currently, the power conversion efficiencies of systems using plasmon excitation are low. However, the very large electron/hole per photon quantum efficiencies observed for plasmonic devices fan the hope of future improvements through a deeper understanding of the processes involved and through better device engineering, especially of critical interfaces such as those between metallic and semiconducting nanophases (or adsorbed molecules). In this review, we focus on the physics and dynamics governing plasmon-derived hot charge carrier transfer across, and the electronic structure at, metal-semiconductor (molecule) interfaces, where we feel the barriers contributing to low efficiencies reside. We suggest some areas of opportunity that deserve early attention in the still-evolving field of hot carrier transmission from plasmonic nanostructures to neighboring phases.
表面等离子体激元最近已被用于开展诸如光生电流产生、氧化还原光化学、光催化和光检测等过程,所有这些过程都是通过分离高能(热)电子和空穴来实现的,而此前这些过程是半导体结的领域。目前,利用等离子体激元激发的系统的功率转换效率较低。然而,在等离子体激元器件中观察到的每光子非常高的电子/空穴量子效率,燃起了人们通过更深入地理解所涉及的过程以及通过更好的器件工程,特别是对诸如金属和半导体纳米相(或吸附分子)之间的关键界面等进行改进,从而实现未来效率提升的希望。在本综述中,我们关注控制等离子体激元衍生的热电荷载流子在金属 - 半导体(分子)界面上转移以及该界面处电子结构的物理和动力学,我们认为导致低效率的障碍就存在于此。我们提出了一些在从等离子体激元纳米结构到相邻相的热载流子传输这个仍在不断发展的领域中值得早期关注的机会领域。