Nanometer-sized metal clusters are prime candidates for photoactivated catalysis, based on their unique tunable optical and electronic properties, combined with a large surface-to-volume ratio. Due to the very small optical cross sections of such nanoclusters, support-mediated plasmonic activation could potentially make activation more efficient. Our support is a semi-transparent gold film, optimized to work in a back-illumination geometry. It has a surface plasmon resonance excitable in the 510–540 nm wavelength range. Pt_n clusters (size distribution peaked at n = 46 atoms) have been deposited onto this support and investigated for photoactivated catalytic performance in the oxidative decomposition of methylene blue. The Pt cluster catalytic activity under illumination exceeds that of the gold support by more than an order of magnitude per active surface area. To further investigate the underlying mechanism of plasmon-induced catalysis, the clusters have been imaged with optically-assisted scanning tunneling microscopy under illumination. The photoactivation of the Pt clusters via plasmonic excitation of the support and subsequential electronic excitation of the clusters can be imaged with nanometer resolution. The light-induced tunneling current on the clusters is enhanced relative to the gold film support.

中文翻译：

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等离子体支持介导的1 nm铂簇的活化以进行催化

纳米尺寸的金属团簇具有独特的可调节的光学和电子特性，并具有大的表面体积比，是光活化催化的主要候选材料。由于此类纳米团簇的光学横截面非常小，因此载体介导的等离激元活化可潜在地提高活化效率。我们的支持是一块半透明的金膜，该膜经过优化可在背照式几何结构中工作。它具有在510-540 nm波长范围内激发的表面等离子体共振。Pt _n个簇（大小分布在n处达到峰值）＝ 46个原子）已沉积到该载体上，并研究了亚甲基蓝的氧化分解中的光活化催化性能。在光照下，Pt簇的催化活性比金载体的催化活性每活性表面积高出一个数量级以上。为了进一步研究等离激元诱导的催化的基本机制，已在光照射下用光辅助扫描隧道显微镜对簇进行了成像。可以通过纳米级的分辨率对经由载体的等离子体激发的Pt簇的光活化以及随后的簇的电子激发进行成像。相对于金膜支撑物，增强了簇上的光诱导隧穿电流。