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Recent Advances in the Inverted Planar Structure of Perovskite Solar

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Recent Advances in the Inverted Planar Structure of Perovskite Solar Article pubs.acs.org/accounts Recent Advances in the Inverted Planar Structure of Perovskite Solar Cells Published as part of the Accounts of Chemical Research special issue “Lead Halide Perovskites for Solar Energy Conversion”. † † ‡ § † Lei Meng, Jingbi You,*, , Tzung-Fang Guo, and Yang Yang*, † Department of Material Science and Engineering, University of California, Los Angeles, Los Angeles, California 90095, United States ‡ Key Lab of Semiconductor Materials Science, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, P. R. China § Department of Photonics, Advanced Optoelectronic Technology Center, National Cheng Kung University, Tainan, Taiwan 701, ROC CONSPECTUS: Inorganic−organic hybrid perovskite solar cells research could be traced back to 2009, and initially showed 3.8% efficiency. After 6 years of efforts, the efficiency has been pushed to 20.1%. The pace of development was much faster than that of any type of solar cell technology. In addition to high efficiency, the device fabrication is a low-cost solution process. Due to these advantages, a large number of scientists have been immersed into this promising area. In the past 6 years, much of the research on perovskite solar cells has been focused on planar and mesoporous device structures employing an n-type TiO2 layer as the bottom electron transport layer. These architectures have achieved champion device efficiencies. However, they still possess unwanted features. Mesoporous structures require a high temperature ° ff (>450 C) sintering process for the TiO2 sca old, which will increase the cost and also not be compatible with flexible substrates. While the planar ff − structures based on TiO2 (regular structure) usually su er from a large degree of J V hysteresis. Recently, another emerging structure, referred to as an “inverted” planar device structure (i.e., p-i-n), uses p-type and n-type materials as bottom and top charge transport layers, respectively. This structure derived from organic solar cells, and the charge transport layers used in organic photovoltaics were successfully transferred into perovskite solar cells. The p-i-n structure of perovskite solar cells has shown efficiencies as high as 18%, lower temperature processing, flexibility, and, furthermore, negligible J−V hysteresis effects. In this Account, we will provide a comprehensive comparison of the mesoporous and planar structures, and also the regular and inverted of planar structures. Later, we will focus the discussion on the development of the inverted planar structure of perovskite solar cells, including film growth, band alignment, stability, and hysteresis. In the film growth part, several methods for obtaining high quality perovskite films are reviewed. In the interface engineering parts, the effect of hole transport layer on subsequent perovskite film growth and their interface band alignment, and also the effect of electron transport layers on charge transport and interface contact will be discussed. As concerns stability, the role of charge transport layers especially the top electron transport layer in the devices stability will be concluded. In the hysteresis part, possible reasons for hysteresis free in inverted planar structure are provided. At the end of this Account, future development and possible solutions to the remaining challenges facing the commercialization of perovskite solar cells are discussed. ■ INTRODUCTION recombination.5 After 6 years of efforts, the power conversion efficiency (PCE) of perovskite solar cells has risen from about Inorganic−organic hybrid perovskite solar cells have attracted − 3% to over 20%,1,6 15 which is close to that of traditional solar great attention due to their solution processing and high 1,2 cell technologies such as Si, CIGS, and CdTe. performance. Organic halide perovskites have ABX3 crystal structures, where A, B, and X are organic cation, metal cation and ■ PLANAR STRUCTURE VERSUS MESOPOROUS halide anion, respectively (Figure 1a), where the band gap can be STRUCTURE (TiO SYSTEM) tuned from the ultraviolet to infrared region through varying 2 − these components (Figure 1b).2 4 This family of materials The hybrid perovskite solar cell was initially discovered in a dye 1 exhibits a myriad of properties ideal for PV such as high dual sensitized solar cell (DSSC) using a mesoporous TiO2 structure. fi electron and hole mobility, large absorption coefficients result- Miyasaka and co-workers were the rst to utilize the perovskite ing from sp antibonding coupling, a favorable band gap, a strong defect tolerance and shallow point defects, benign Received: September 3, 2015 grain boundary recombination effects, and reduced surface © XXXX American Chemical Society A DOI: 10.1021/acs.accounts.5b00404 Acc. Chem. Res. XXXX, XXX, XXX−XXX Accounts of Chemical Research Article Figure 1. (a) Crystal structure of the halide perovskite material: A site is typically CH3NH3I (MAI), NH2CH NH2I (FAI), Cs; B site is commonly Pb, ff Sn; X site could be Cl, Br or I. (b) Absorption of FAPbIyBr3‑y with di erent ratios of Br and I. Reprinted with permission from ref 4. Copyright 2014 Royal Society of Chemistry ff Figure 2. (a) Plot of exciton di usion length versus PL lifetime quenching ratios for CH3NH3PbI3. Reprinted with permission from ref 16. Copyright 2013 American Association for the Advancement of Science. (b) Time-resolved PL of the mixed halide perovskite (CH3NH3PbI3−xClx) with quenching.Reprinted with permission from ref 17. Copyright 2013 American Association for the Advancement of Science. Figure 3. Three typical device structures of perovskite solar cells: (a) mesoporous, (b) regular planar structure, and (c) inverted planar structure. fi (CH3NH3PbI3 and CH3NH3PbBr3) nanocrystal as absorbers in structure was feasible. The rst successful demonstration of the DSSC structure, achieving an efficiency of 3.8% in 2009.1 In 2012, planar structure can be traced back to the perovskite/fullerene Park and Gratzel et al. reported a solid state perovskite solar cell structure reported by Guo et al.,19 showing a 4% efficiency. The by using the solid hole transport layer to improve stability.7 After low efficiency reported at that time was due to the inferior film that, several milestones in device performance have been achieved quality and inadequate absorption of the perovskite film.19 The − by using mesoporous structure.6 15 However, these mesoporous breakthrough of the planar perovskite structure was obtained devices need a high temperature sintering of TiO2 layer that could by using a dual source vapor deposition, providing dense and increase the processing time and cost of cell production. high quality perovskite films that achieved 15.4% efficiency.20 Sum et al. and Snaith et al. independently reported that the Recently, the efficiency of the planar structure was pushed over methylammonium-based perovskites own long charge carrier 19% through interface engineering.12 These results showed that ff ∼ ∼ di usion lengths ( 100 nm for CH3NH3PbI3 and 1000 nm for the planar structure could achieve similar device performance 16,17 CH3NH3PbI3−xClx, Figure 2). Recently, single crystals of as the mesoporous structure. The evolution of the structure of ff CH3NH3PbI3 were found to reach di usion lengths larger than perovskite is shown in Figure 3. 175 um.18 Further studies demonstrated that perovskites exhibit The planar structure can be divided into two categories ambipolar behavior, indicating that the perovskite materials depending on which selective contact is used on the bottom, that themselves can transport both of electrons and holes between is, regular (n-i-p) and inverted (p-i-n); the device structures are the cell terminals.16 All of these results indicated that a planar shown in Figure 3b and c, respectively. The regular n-i-p structure B DOI: 10.1021/acs.accounts.5b00404 Acc. Chem. Res. XXXX, XXX, XXX−XXX Accounts of Chemical Research Article Figure 4. (a) Device structure of the first inverted planar structure of perovskite solar cell. (b) band alignment. Reprinted with permission from ref 19. Copyright 2013 Wiley-VCH. (c) Thin perovskite film (<100 nm) as the absorber. Reprinted with permission from ref 21. Copyright 2014 Royal Society of Chemistry. (d) Thicker film (about 300 nm) as the absorber. Reprinted with permission from ref 22. Copyright 2014 American Chemical Society. Table 1. Several Representative Devices Performances of Inverted Planar Structured Perovskite Solar Cells 2 perovskite processing HTL ETL Voc (V) Jsc (mA/cm ) FF (%) PCE (%) stability ref one-step PEDOT:PSS PC61BM/BCP 0.60 10.32 63 3.9 19 two-step PEDOT:PSS PC61BM 0.91 10.8 76 7.4 21 one-step (Cl) PEDOT:PSS PC61BM 0.87 18.5 72 11.5 22 one-step (Cl) PEDOT:PSS PC61BM/TiOx 0.94 15.8 66 9.8 23 solvent engineering PEDOT:PSS PC61BM/LiF 0.87 20.7 78.3 14.1 26 one-step (moisture, Cl) PEDOT:PSS PC61BM/PFN 1.05 20.3 80.2 17.1 11 one-step (hot-casting, Cl) PEDOT:PSS PCBM 0.94 22.4 83 17.4 27 one-step (HI additive) PEDOT:PSS PC61BM 1.1 20.9 79 18.2 28 coevaporation PEDOT:PSS/Poly-TPD PC61BM 1.05 16.12 67 12.04 24 coevaporation PEDOT:PSS/PCDTBT PC61BM/LiF 1.05 21.9 72 16.5 31 two-step spin-coating PTAA PCBM/C60/BCP 1.07 22.0 76.8 18.1 29 one-step solvent PEDOT:PSS C60 0.92 21.07 80 15.44 39 one-step (Cl) PEDOT:PSS PC61BM/ZnO 0.97 20.5 80.1 15.9 140 h 41 one-step (Cl) PEDOT:PSS PC61BM/ZnO 1.02 22.0 74.2 16.8 60 days 42 one-step NiOx PC61BM/BCP 0.92 12.43 68 7.8 33 one-step NiOx:Cu PC61BM/C60-bis surfcant 1.11 19.01 73 15.4 244 h 35 solvent engineering NiOx PC61BM/LiF 1.06 20.2 81.3 17.3 36 two-step NiOx ZnO 1.01 21.0 76 16.1 >60 days 30 has been extensively studied and could be traced back to dye poly(3,4-ethylenedioxythiophene):poly(styrenesulfonic acid) sensitized solar cells.
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