Wang Hui, Liu Wenxiu, Jin Sen, Zhang Xiaodong, Xie Yi
Hefei National Laboratory for Physical Sciences at the Microscale, CAS Centre for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
Institute of Energy, Hefei Comprehensive National Science Center, Hefei, Anhui 230031, P. R. China.
ACS Cent Sci. 2020 Jul 22;6(7):1058-1069. doi: 10.1021/acscentsci.0c00540. Epub 2020 Jun 5.
By virtue of their intriguing electronic structures and excellent surface properties, low-dimensional semiconductors hold great promise in the field of solar-driven artificial photosynthesis. However, owing to promoted structural confinement and reduced Coulomb screening, remarkable interactions between particles/quasiparticles, including electrons, holes, phonons, and excitons, can be expected in low-dimensional semiconductors, which endow the systems with distinctive excited-state properties that are distinctly different from those in the bulk counterparts. Consequently, these interactions determine not only the mechanisms but also quantum yields of photosynthetic energy utilization. In this Outlook, we review recent advances in studying the unique interactions in low-dimensional semiconductor-based photocatalysts. By highlighting the relevance of different interactions to excited-state properties, we describe the impacts of the interactions on photosynthetic energy conversion. Furthermore, we summarize the regulation of these interactions for gaining optimized photosynthetic behaviors, where the relationships between these interactions and structural factors/external fields are elaborated. Additionally, the challenges and opportunities in studying the interaction-related photosynthesis are discussed.
凭借其引人入胜的电子结构和优异的表面性质,低维半导体在太阳能驱动的人工光合作用领域具有巨大潜力。然而,由于结构限制增强和库仑屏蔽减弱,在低维半导体中可以预期粒子/准粒子之间会有显著的相互作用,包括电子、空穴、声子和激子,这赋予了系统与体相材料截然不同的独特激发态性质。因此,这些相互作用不仅决定了光合能量利用的机制,还决定了其量子产率。在本展望中,我们回顾了研究基于低维半导体的光催化剂中独特相互作用的最新进展。通过强调不同相互作用与激发态性质的相关性,我们描述了这些相互作用对光合能量转换的影响。此外,我们总结了为获得优化的光合行为而对这些相互作用进行的调控,阐述了这些相互作用与结构因素/外部场之间的关系。此外,还讨论了研究与相互作用相关的光合作用所面临的挑战和机遇。