Ultrahigh sensitive Raman spectroscopy for subnanoscience: Direct observation of tin oxide clusters
Ultrahigh sensitive Raman spectroscopy for subnanoscience: Direct observation of tin oxide clusters
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DOI：
10.1126/sciadv.aax6455
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发表时间：
2019-12-01
期刊：
影响因子：
13.6
通讯作者：
Yamamoto, Kimihisa
中科院分区：
文献类型：
--
作者：
Kuzume, Akiyoshi;Ozawa, Miyu;Yamamoto, Kimihisa
亚纳米金属簇表现出异常催化活性，表明作为下一代材料的创新应用，尽管由于传统分析方法的信号强度严重弱，在原子细节上识别和表征这些亚纳米材料仍然是一个巨大的挑战。在这里，我们报告了一种基于表面增强拉曼光谱建立的亚纳米敏感振动技术，首次展示了亚纳米材料的详细振动表征。此外，结合密度泛函理论计算，我们揭示了氧化锡亚纳米团簇的固有表面结构决定了这些团簇的特定尺寸光谱和催化特性。这里阐述的高灵敏度表征方法可以提供对亚纳米材料的化学和结构性质的全面理解，这有助于在原子尺度上合理设计亚纳米材料的实际应用，例如催化剂、生物传感器和电子产品。
Subnanometric metal clusters exhibit anomalous catalytic activity, suggesting innovative applications as next-generation materials, although identifying and characterizing these subnanomaterials in atomic detail remains a substantial challenge because of the severely weak signal intensity for the conventional analytical methods. Here, we report a subnanosensitive vibrational technique established based on the surface-enhanced Raman spectroscopy, demonstrating the first-ever detailed vibrational characterization of subnanomaterials. Furthermore, combining with density functional theory calculations, we reveal that inherent surface structures of the tin oxide subnanoclusters determine the size-specific spectral and catalytic characteristics of these clusters. The high-sensitivity characterization methodology elaborated here can provide a comprehensive understanding of the chemical and structural natures of subnanomaterials, which facilitate the rational design of subnanomaterials on the atomic scale for practical applications, such as in catalysts, biosensors, and electronics.