量子效应进入基于半导体的 SERS：多共振 MoO3·xH2O 量子点实现对无机小分子的直接、灵敏 SERS 检测,Analytical Chemistry

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量子效应进入基于半导体的 SERS：多共振 MoO3·xH2O 量子点实现对无机小分子的直接、灵敏 SERS 检测
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-03-17 , DOI: 10.1021/acs.analchem.1c05142
Ge Song _{1,

2} , Hongzhao Sun _{1,

2} , Jian Chen _{1,

2} , Zhigang Chen ₂ , Boyang Liu ₃ , Zhenghui Liu ₃ , Shan Cong _{1,

4,

5} , Zhigang Zhao _{1,

2,

4}

Affiliation

由于它们对许多探针分子的选择性和对复杂场景应用的适用性，人们对构建高效的基于半导体的表面增强拉曼散射 (SERS) 平台有着浓厚的研究兴趣。然而，由于在半导体中产生足够的 SERS 增强的挑战，目前的调谐方法尚未成功地为小无机分子创建基于半导体的 SERS 传感器。在这里，我们演示了 MoO ₃ · x H _2的使用O 量子点 (QD)，用于实现无机物种肼的直接和灵敏指纹识别，这是基于半导体的 SERS 研究以及各种其他探针分子的首次尝试。由此产生的使用平均尺寸为 2.2 nm 的 QD 的 SERS 平台可以成功检测肼的信号，检测限估计约为 4 × 10 ^–5M，显着降低可检测浓度至少 1000 倍，与 10 和 100 nm 粒子的弱性能形成鲜明对比，表明由低于玻尔半径的小粒径触发的量子尺寸效应是高 SERS 活性的关键原因。_{显着增强的 SERS 活性是由量子尺寸 MoO 3} · x H ₂ O中的能态发散引起的振动耦合多路径、高效电荷转移共振的结果。这是开发的概念验证演示量子尺寸效应，显着增强基于半导体的 SERS 材料的本征 SERS 活性。

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Quantum Effects Enter Semiconductor-Based SERS: Multiresonant MoO3·xH2O Quantum Dots Enabling Direct, Sensitive SERS Detection of Small Inorganic Molecules

There is keen research interest in building highly effective semiconductor-based surface-enhanced Raman scattering (SERS) platforms, due to their selectivity for many probe molecules and suitability for complex scenario applications. However, current tuning approaches have not yet been successful in creating semiconductor-based SERS sensors for small inorganic molecules, due to the challenge of creating sufficient SERS enhancement in semiconductors. Here, we demonstrate the use of MoO₃·xH₂O quantum dots (QDs), to achieve direct and sensitive fingerprinting of the inorganic species hydrazine, which is a first attempt in semiconductor-based SERS research, as well as various other probe molecules. The resulting SERS platform that uses QDs with average size of 2.2 nm could successfully detect the signal of hydrazine with a limit of detection estimated to be around 4 × 10^–5 M, significantly lowering the detectable concentration by at least 1000-fold, in sharp contrast to the weak performance of 10 and 100 nm particles, demonstrating that quantum size effect triggered by small particle size below the Bohr radius is crucially responsible for high SERS activity. The significantly enhanced SERS activity is a result of vibronically coupled multipathway, highly efficient charge-transfer resonances induced by the divergence of energy states in quantum-sized MoO₃·xH₂O. This is a proof-of-concept demonstration of the exploitation of quantum size effect, toward significantly enhanced intrinsic SERS activity in semiconductor-based SERS materials.

更新日期：2022-03-17

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