Wu Kaifeng, Liang Guijie, Kong Degui, Chen Jinquan, Chen Zheyuan, Shan Xinhe, McBride James R, Lian Tianquan
Department of Chemistry , Emory University , 1515 Dickey Drive, NE , Atlanta , Georgia 30322 , USA . Email:
Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices , Hubei University of Arts and Science , Xiangyang 441053 , Hubei Province , P. R. China.
Chem Sci. 2016 Feb 1;7(2):1238-1244. doi: 10.1039/c5sc03715h. Epub 2015 Nov 12.
Ternary chalcopyrite CuInS quantum dots (QDs) have been extensively studied in recent years as an alternative to conventional QDs for solar energy conversion applications. However, compared with the well-established photophysics in prototypical CdSe QDs, much less is known about the excited properties of CuInS QDs. In this work, using ultrafast spectroscopy, we showed that both conduction band (CB) edge electrons and copper vacancy (V) localized holes were susceptible to surface trappings in CuInS QDs. These trap states could be effectively passivated by forming quasi-type II CuInS/CdS core/shell QDs, leading to a single-exciton (with electrons delocalized among CuInS/CdS CB and holes localized in V) half lifetime of as long as 450 ns. Because of reduced electron-hole overlap in quasi-type II QDs, Auger recombination of multiple excitons was also suppressed and the bi-exciton lifetime was prolonged to 42 ps in CuInS/CdS QDs from 10 ps in CuInS QDs. These demonstrated advantages, including passivated trap states, long single and multiple exciton lifetimes, suggest that quasi-type II CuInS/CdS QDs are promising materials for photovoltaic and photocatalytic applications.
近年来,三元黄铜矿型硫化铜铟(CuInS)量子点(QDs)作为传统量子点在太阳能转换应用中的替代品,受到了广泛研究。然而,与典型的硒化镉(CdSe)量子点中已确立的光物理性质相比,人们对硫化铜铟量子点的激发特性了解较少。在这项工作中,我们利用超快光谱表明,硫化铜铟量子点中的导带(CB)边缘电子和铜空位(V)局域化空穴都容易受到表面俘获的影响。通过形成准II型硫化铜铟/硫化镉(CuInS/CdS)核壳量子点,可以有效地钝化这些陷阱态,从而使单激子(电子在CuInS/CdS导带中离域,空穴局域在V中)的半衰期长达450纳秒。由于准II型量子点中电子 - 空穴重叠减少,多激子的俄歇复合也受到抑制,并且硫化铜铟/硫化镉量子点中的双激子寿命从硫化铜铟量子点中的10皮秒延长至42皮秒。这些已证明的优势,包括钝化的陷阱态、长的单激子和多激子寿命,表明准II型硫化铜铟/硫化镉量子点是用于光伏和光催化应用有前景的材料。