Han Chuang, Li Shao-Hai, Tang Zi-Rong, Xu Yi-Jun
State Key Laboratory of Photocatalysis on Energy and Environment , College of Chemistry , Fuzhou University , Fuzhou , 350116 , China . Email:
College of Chemistry , New Campus , Fuzhou University , Fuzhou , 350116 , China.
Chem Sci. 2018 Nov 15;9(48):8914-8922. doi: 10.1039/c8sc04479a. eCollection 2018 Dec 28.
Considerable effort has been devoted to manipulating the optical absorption of metal nanostructures for diverse applications. However, it still remains a challenge to develop a general and flexible method to promote broadband absorption of metal nanostructures without changing their size and shape. Here, we report a new strategy of hybridizing two conceptually different optical models to realize broadband absorption enhancement of metal nanoparticles (NPs), which is enabled by constructing a core-shell heterostructure, consisting of a spherical dielectric core covered by a metal NPs interlayer and tunable semiconductor shell. This approach integrates the interfacial photon management, photoexcitation of metal NPs and injection of hot charge carriers into the semiconductor shell, and results in distinctly enhanced hot charge carrier generation and transfer, thereby boosting the broad-spectrum light driven catalysis. The structure-plasmon-catalysis interplay of the heterostructure is comprehensively studied and optimized. This proof-of-concept proves to be generally feasible by varying the type of both metal NPs and support medium, opening a new avenue to control the optoelectronic properties of materials.
为了实现各种应用，人们在操控金属纳米结构的光吸收方面付出了巨大努力。然而，开发一种通用且灵活的方法来促进金属纳米结构的宽带吸收而不改变其尺寸和形状，仍然是一个挑战。在此，我们报告了一种将两种概念上不同的光学模型相结合的新策略，以实现金属纳米颗粒（NPs）的宽带吸收增强，这是通过构建一种核壳异质结构来实现的，该结构由一个球形介电核、覆盖在其上的金属NPs中间层以及可调谐半导体壳组成。这种方法整合了界面光子管理、金属NPs的光激发以及热载流子注入到半导体壳中，从而显著增强了热载流子的产生和转移，进而推动了广谱光驱动催化。对异质结构的结构 - 等离子体 - 催化相互作用进行了全面研究和优化。通过改变金属NPs和支撑介质的类型，这一概念验证被证明总体上是可行的，为控制材料的光电特性开辟了一条新途径。
