Journal
ACS NANO
Volume 13, Issue 10, Pages 11800-11808Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b05774
Keywords
low-band-gap perovskites; Sn-Pb-based perovskites; photodiodes; near-infrared imaging; room-temperature crystallization; CMOS-compatible metal/silicon substrates
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Funding
- University Grant Council of the University of Hong Kong [201611159194, 201511159225]
- Research Grants Council of Hong Kong Special Administrative Region, China [17211916, 17204117, 17200518]
- Ohio Research Scholar Program
- National Key Research and Development Program of China [2016YFB0700700]
- National Natural Science Foundation of China [11674237, 51602211]
- Natural Science Foundation of Jiangsu Province of China [BK20160299]
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Although Sn-Pb perovskites sensing nearultraviolet-visible-near-infrared light could be an attractive alternative to silicon in photodiodes and imaging, there have been no clear studies on such devices constructed on metal/silicon substrates, hindering their direct integration with complementary metal-oxide semiconductor (CMOS) and silicon electronics. Typically, high surface roughness and severe pinholes of Sn-rich binary perovskites make it difficult for them to fulfill the requirements of efficient photodiodes and imaging. These issues cause inherently high dark current and poor (dark and photo-) current uniformity. Herein, we propose and demonstrate the room-temperature crystallization in the Sn-rich binary perovskite system to effectively control film crystallization kinetics. With experimental and theoretical studies of the crystallization mechanism, we successfully tune the density and location of nanocrystals in precursor films to achieve compact nanocrystals, which coalesce into high-quality (smooth, dense, and pinhole-free) perovskites with intensified preferred orientation and decreased trap density. The high-quality perovskites reduce dark current and improve (dark and photo-) current uniformity of perovskite photodiodes on CMOS-compatible metal/silicon substrates. Meanwhile, self-powered devices achieve a high responsivity of 0.2 A/W at 940 nm, a large dynamic range of 100 dB, and a fast fall time of 2.27 mu s, exceeding those of most silicon-based imaging sensors. Finally, a 6 x 6 pixel integrated photodiode array is successfully demonstrated to realize the imaging application. The work contributes to understanding the fundamentals of the crystallization of Sn-rich binary perovskites and advancing perovskite integration with Si-based electronics.
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