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用于超灵敏表面增强拉曼散射传感器的硫化锡纳米结构的形态工程以激发PICT共振

Morphology Engineering of SnS Nanostructures to Stimulate PICT Resonance for Ultra-Sensitive SERS Sensors.

作者信息

Peng Yusi, Zhang Weida, Xu Meimei, Zhao Shuai, Yang Lili, Li Dan, Tanemura Masaki, Huang Zhengren, Yang Yong

机构信息

State Key Laboratory of High-Performance Ceramics and Superfine Microstructures Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai People's Republic of China.

University of Chinese Academy of Sciences Beijing People's Republic of China.

出版信息

Exploration (Beijing). 2025 Feb 24;5(3):270016. doi: 10.1002/EXP.70016. eCollection 2025 Jun.

Abstract

Recent advances indicate the surface-enhanced Raman scattering (SERS) sensitivity of semiconductors is generally lower than that of noble metal substrates, and developing ultra-sensitive semiconductor SERS substrates is an urgent task. Here, SnS with better SERS performance is screened out from sulfides and selenides by density functional theory (DFT) calculations. Through adjusting the concentration of reactants to control the growth driving force without any surfactants or templates, SnS nanostrctures of stacked nanosheets (SNSs), microspheres (MSs) and microflowers (MFs) are developed, which all exhibit ultra-low limit of detections (LODs) of 10, 10, and 10 M, respectively. To the best of our knowledge, the SERS sensitivity of these three kinds of SnS nanostrctures are superior to most of the reported pure semiconductors and even can be parallel to the noble metals with a "hot spot" effect. This extraordinary SERS enhancement of SnS nanostrctures is originated from the dominated contribution of photo-induced charge transfer (PICT) resonance with different wavelength excitation lasers. Benefitting to the excellent SERS enhanced uniformity, generality, stability, ultra-high sensitivity of SnS nanostrctures, and the advantages that the PICT resonance enhancement excited for different probe molecules is not limited by its morphology, it is expected to provide a class of potential commercial SERS-active materials for the practical application of semiconductor-based SERS technology.

摘要

最新进展表明,半导体的表面增强拉曼散射(SERS)灵敏度通常低于贵金属基底,因此开发超灵敏的半导体SERS基底是一项紧迫任务。在此,通过密度泛函理论(DFT)计算从硫化物和硒化物中筛选出具有更好SERS性能的SnS。通过调节反应物浓度来控制生长驱动力,无需任何表面活性剂或模板,制备出了堆叠纳米片(SNSs)、微球(MSs)和微花(MFs)的SnS纳米结构,它们的检测限(LODs)分别低至10⁻¹²、10⁻¹¹和10⁻¹⁰ M。据我们所知,这三种SnS纳米结构的SERS灵敏度优于大多数已报道的纯半导体,甚至可与具有“热点”效应的贵金属相媲美。SnS纳米结构这种非凡的SERS增强源于不同波长激发激光下光致电荷转移(PICT)共振的主导贡献。得益于SnS纳米结构优异的SERS增强均匀性、通用性、稳定性、超高灵敏度,以及PICT共振增强对不同探针分子的激发不受其形态限制的优点,有望为基于半导体的SERS技术的实际应用提供一类潜在的商业SERS活性材料。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8904/12199321/4433a8bbaf67/EXP2-5-270016-g005.jpg

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