电子转移
纳米颗粒
等离子体子
纳米晶
拉曼光谱
光化学
材料科学
光诱导电子转移
小提琴手
限制
半导体
自组装
光谱学
纳米技术
化学
化学物理
光电子学
物理
光学
机械工程
工程类
量子力学
作者
Kamil Sokołowski,Junyang Huang,Tamás Földes,Jade A. McCune,David D. Xu,Bart de Nijs,Rohit Chikkaraddy,Sean M. Collins,Edina Rosta,Jeremy J. Baumberg,Oren A. Scherman
标识
DOI:10.1038/s41565-021-00949-6
摘要
Nature controls the assembly of complex architectures through self-limiting processes; however, few artificial strategies to mimic these processes have been reported to date. Here we demonstrate a system comprising two types of nanocrystal (NC), where the self-limiting assembly of one NC component controls the aggregation of the other. Our strategy uses semiconducting InP/ZnS core-shell NCs (3 nm) as effective assembly modulators and functional nanoparticle surfactants in cucurbit[n]uril-triggered aggregation of AuNCs (5-60 nm), allowing the rapid formation (within seconds) of colloidally stable hybrid aggregates. The resultant assemblies efficiently harvest light within the semiconductor substructures, inducing out-of-equilibrium electron transfer processes, which can now be simultaneously monitored through the incorporated surface-enhanced Raman spectroscopy-active plasmonic compartments. Spatial confinement of electron mediators (for example, methyl viologen (MV2+)) within the hybrids enables the direct observation of photogenerated radical species as well as molecular recognition in real time, providing experimental evidence for the formation of elusive σ-(MV+)2 dimeric species. This approach paves the way for widespread use of analogous hybrids for the long-term real-time tracking of interfacial charge transfer processes, such as the light-driven generation of radicals and catalysis with operando spectroscopies under irreversible conditions.
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