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.

中文翻译：

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用于宽带光驱动催化的可调谐等离子体核壳异质结构设计†

人们投入了大量的精力来操纵金属纳米结构的光学吸收以适应不同的应用。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。在这里，我们报告了一种混合两种概念上不同的光学模型以实现金属纳米颗粒（NP）的宽带吸收增强的新策略，这是通过构建核壳异质结构来实现的，该异质结构由金属纳米粒子夹层覆盖的球形介电核和可调谐半导体壳。这种方法集成了界面光子管理、金属纳米粒子的光激发以及将热载流子注入半导体壳中，从而显着增强了热载流子的产生和转移，从而促进了广谱光驱动催化。全面研究和优化了异质结构的结构-等离子体-催化相互作用。通过改变金属纳米颗粒和支撑介质的类型，这种概念验证被证明是普遍可行的，为控制材料的光电性能开辟了一条新途径。