Hot-electron-transfer enhancement for the efficient energy conversion of visible light.
Hot-electron-transfer enhancement for the efficient energy conversion of visible light.
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DOI：
10.1002/anie.201405598
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发表时间：
2014-10
影响因子：
--
通讯作者：
Sungju Yu;Yong Hwa Kim;S. Y. Lee;H. Song;J. Yi
中科院分区：
文献类型：
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作者：
Sungju Yu;Yong Hwa Kim;S. Y. Lee;H. Song;J. Yi
在利用半导体中的等离子体纳米结构来提高太阳能转换方面取得了长足的进步。然而，由于等离子体诱导的超热电子的超快衰变，目前的等离子体纳米结构的产生仍然有些低效。目前的研究表明，通过与硫化镉量子点的强耦合和与钙钛矿型钛酸锶纳米粒子的肖特基结，可以显著地降低热电子在金纳米粒子中的超快衰减。稳态和时间分辨光致发光光谱表明，所设计的具有三个不同组分的等离子体纳米结构能够实现热电子辅助的电子转移能级联，即CDS→Au→SrTiO 3。因此，热电子转移能够有效地从水中生产氢气，并在不同波长的可见光照射下显著地收集电子。这些发现为克服通常与等离子体纳米结构相关的低效率提供了一种新的方法。
Great strides have been made in enhancing solar energy conversion by utilizing plasmonic nanostructures in semiconductors. However, current generation with plasmonic nanostructures is still somewhat inefficient owing to the ultrafast decay of plasmon-induced hot electrons. It is now shown that the ultrafast decay of hot electrons across Au nanoparticles can be significantly reduced by strong coupling with CdS quantum dots and by a Schottky junction with perovskite SrTiO3 nanoparticles. The designed plasmonic nanostructure with three distinct components enables a hot-electron-assisted energy cascade for electron transfer, CdS→Au→SrTiO3, as demonstrated by steady-state and time-resolved photoluminescence spectroscopy. Consequently, hot-electron transfer enabled the efficient production of H2 from water as well as significant electron harvesting under irradiation with visible light of various wavelengths. These findings provide a new approach for overcoming the low efficiency that is typically associated with plasmonic nanostructures.