Quantum Dot Photovoltaics in the Extreme Quantum Confinement Regime: The Surface-Chemical Origins of Exceptional Air- and Light-Stability

被引:335
作者
Tang, Jiang [1 ,2 ]
Brzozowski, Lukasz [2 ]
Barkhouse, D. Aaron R. [2 ]
Wang, Xihua [2 ]
Debnath, Ratan [2 ]
Wolowiec, Remigiusz [2 ]
Palmiano, Elenita [2 ]
Levina, Larissa [2 ]
Pattantyus-Abraham, Andras G. [2 ]
Jamakosmanovic, Damir [2 ]
Sargent, Edward H. [1 ,2 ]
机构
[1] Univ Toronto, Dept Mat Sci & Engn, Toronto, ON M5S 3E4, Canada
[2] Univ Toronto, Dept Elect & Comp Engn, Toronto, ON M5S 3G4, Canada
关键词
colloidal quantum dot photovoltaics; surface spectroscopy; oxidation products; optoelectronic device stability; traps; recombination; transport in colloidal quantum dot solids; COLLOIDAL NANOCRYSTALS; INFRARED PHOTOVOLTAICS; SOLAR-CELLS; PBS; PHOTODETECTORS; EFFICIENT; FILMS;
D O I
10.1021/nn901564q
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We report colloidal quantum dot (CQDs) photovoltaics having a similar to 930 nm bandgap. The devices exhibit AM1.5G power conversion efficiencies in excess of 2%. Remarkably, the devices are stable in air under many tens of hours of solar illumination without the need for encapsulation. We explore herein the origins of this orders-of-magnitude improvement in air stability compared to larger PbS dots. We find that small and large dots form dramatically different oxidation products, with small dots forming lead sulfite primarily and large dots, lead sulfate. The lead sulfite produced on small dots results in shallow electron traps that are compatible with excellent device performance; whereas the sulfates formed on large dots lead to deep traps, midgap recombination, and consequent catastrophic loss of performance. We propose and offer evidence in support of an explanation based on the high rate of oxidation of sulfur-rich surfaces preponderant in highly faceted large-diameter PbS colloidal quantum dots.
引用
收藏
页码:869 / 878
页数:10
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