期刊
CHEMISTRY OF MATERIALS
卷 28, 期 3, 页码 802-812出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.5b04019
关键词
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资金
- National Key Basic Research Program of China [2012CB921403, 2015CB921001]
- National Natural Science Foundation of China [11222431, 11574365]
- Chinese Academy of Sciences [XDB07030100]
- US National Science Foundation
- Army Research Office
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1205734] Funding Source: National Science Foundation
Organometal halide perovskite solar cells (PSCs) have emerged as one of the most promising photovoltaic technologies with efficiencies exceeding 20.3%. However, device stability problems including hysteresis in current voltage scans must be resolved before the commercialization of PSCs. Transient absorption measurements and first-principles calculations indicate that the migration of oxygen vacancies in the TiO2 electrode under electric field during voltage scans contributes to the anomalous hysteresis in PSCs. The accumulation of oxygen vacancies at the electrode/perovskite interface slows down charge extraction while significantly speeding up charge recombination at the interface. Moreover, nonadiabatic molecular dynamics simulations reveal that the charge recombination rates at the interface depend sensitively (with 1 order of magnitude difference) on the locations of oxygen vacancies. By intentionally reducing oxygen vacancies in the TiO2 electrode, we substantially suppress unfavorable hysteresis in the PSC devices. This work establishes a firm link between microscopic interfacial structure and macroscopic device performance of PSCs, providing important clues for future device design and optimization.
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