(Chemical Equation Presented) A long-standing dream in the large scale application of solar energy conversion is the fabrication of solar cells with high-efficiency and long-term stability at low cost. The realization of such practical goals depends on the architecture, process and key materials because solar cells are typically constructed from multilayer heterostructures of light harvesters, with electron and hole transporting layers as a major component. Recently, inorganic-organic hybrid lead halide perovskites have attracted significant attention as light absorbers for the fabrication of low-cost and high-efficiency solar cells via a solution process. This mainly stems from long-range ambipolar charge transport properties, low exciton binding energies, and suitable band gap tuning by managing the chemical composition. In our pioneering work, a new photovoltaic platform for efficient perovskite solar cells (PSCs) was proposed, which yielded a high power conversion efficiency (PCE) of 12%. The platform consisted of a pillared architecture of a three-dimensional nanocomposite of perovskites fully infiltrating mesoporous TiO 2 , resulting in the formation of continuous phases and perovskite domains overlaid with a polymeric hole conductor. Since then, the PCE of our PSCs has been rapidly increased from 3% to over 20% certified efficiency. The unprecedented increase in the PCE can be attributed to the effective integration of the advantageous attributes of the refined bicontinuous architecture, deposition process, and composition of perovskite materials. Specifically, the bicontinuous architectures used in the high efficiency comprise a layer of perovskite sandwiched between mesoporous metal-oxide layer, which is a very thinner than that of used in conventional dye-sensitized solar cells, and hole-conducting contact materials with a metal back contact. The mesoporous scaffold can affect the hysteresis under different scan direction in measurements of PSCs. The hysteresis also greatly depends on the cell architecture and perovskite composition. In this Account, we will describe what we do with major aspects including (1) the film morphology through the development of intermediate chemistry retarding the rapid reaction between methylammonium or formamidinium iodide and lead halide (PbI 2 ) for improved perovskite film formation; (2) the phase stability and band gap tuning of the perovskite layer through the materials engineering; (3) the development of electron and hole transporting materials for carrier-selective contacting layers; and (4) the adoption of p-i-n and n-i-p architectures depending on the position of the electron or hole conducting layer in front of incident light. Finally, we will summarize the recent incredible achievements in PSCs, and finally provide challenges facing the future development and commercialization of PSCs.
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