Organic Solar Cell Materials toward Commercialization.

Bulk-heterojunction organic solar cells (OSCs) have received considerable attention with significant progress recently and offer a promising outlook for portable energy resources and building-integrated photovoltaics in the future. Now, it is urgent to promote the research of OSCs toward their commercialization. For the commercial application of OSCs, it is of great importance to develop high performance, high stability, and low cost photovoltaic materials. In this review, a comprehensive overview of the fundamental requirements of photoactive layer materials and interface layer materials toward commercialization is provided, mainly focusing on high performance, green manufacturing, simplifying device fabrication processes, stability, and cost issues. Furthermore, the perspectives and opportunities for this emerging field of materials science and engineering are also discussed.

Reducing Energy Disorder of Hole Transport Layer by Charge Transfer Complex for High Performance p-i-n Perovskite Solar Cells.

Solution-processed organic semiconductor charge-transport layers (OS-CTLs) with high mobility, low trap density, and energy level alignment have dominated the important progress in p-i-n planar perovskite solar cells (pero-SCs). Unfortunately, their inevitable long chains result in weak molecular stacking, which is likely to generate high energy disorder and deteriorate the charge-transport ability of OS-CTLs. Here, a charge-transfer complex (CTC) strategy to reduce the energy disorder in the OS-CTLs by doping an organic semiconductor, 4,4'-(4,8-bis(5-(trimethylsilyl)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene-2,6-diyl)bis(N,N-bis(4-methoxyphenyl)aniline) (BDT-Si), in a commercial hole-transport layer (HTL), poly[bis(4-phenyl) (2,4,6-trimethylphenyl)amine (PTAA), is proposed. The formation of the CTC makes the PTAA conjugated backbone electron-deficient, resulting in a quinoidal and stiffer character, which is likely to planarize the PTAA backbone and enhance the ordering of the film in nanoscale. The resultant HTL exhibits a reduced energy disorder, which simultaneously promotes hole transport in the HTL, hole extraction at the interface, energy level alignment, and quasi-Fermi level splitting in the device. As a result, the p-i-n planar pero-SCs with optimized HTL exhibit the best power conversion efficiency of 21.87% with good operating stability. This finding demonstrates that the CTC strategy is an effective way to reduce the energy disorder in HTLs and to improve the performance of planar pero-SCs.

Interfacial Molecular Doping of Metal Halide Perovskites for Highly Efficient Solar Cells.

Tailoring the doping of semiconductors in heterojunction solar cells shows tremendous success in enhancing the performance of many types of inorganic solar cells, while it is found challenging in perovskite solar cells because of the difficulty in doping perovskites in a controllable way. Here, a small molecule of 4,4',4″,4″'-(pyrazine-2,3,5,6-tetrayl) tetrakis (N,N-bis(4-methoxyphenyl) aniline) (PT-TPA) which can effectively p-dope the surface of FAx MA1- x PbI3 (FA: HC(NH2 )2 ; MA: CH3 NH3 ) perovskite films is reported. The intermolecular charge transfer property of PT-TPA forms a stabilized resonance structure to accept electrons from perovskites. The doping effect increases perovskite dark conductivity and carrier concentration by up to 4737 times. Computation shows that electrons in the first two layers of octahedral cages in perovskites are transferred to PT-TPA. After applying PT-TPA into perovskite solar cells, the doping-induced band bending in perovskite effectively facilitates hole extraction to hole transport layer and expels electrons toward cathode side, which reduces the charge recombination there. The optimized devices demonstrate an increased photovoltage from 1.12 to 1.17 V and an efficiency of 23.4% from photocurrent scanning with a stabilized efficiency of 22.9%. The findings demonstrate that molecular doping is an effective route to control the interfacial charge recombination in perovskite solar cells which is in complimentary to broadly applied defect passivation techniques.

Targeted Therapy for Interfacial Engineering Toward Stable and Efficient Perovskite Solar Cells.

The poor long-term stability of organic-inorganic hybrid halide perovskite solar cells (pero-SCs) remains a big challenge for their commercialization. Although strategies such as encapsulation, doping, and passivation have been reported, there remains a lack of understanding of the water resistance and thermal stability of pero-SCs. A fullerene derivative, [6,6]-phenyl-C61 -butyric acid-N,N-dimethyl-3-(2-thienyl)propanam ester (PCBB-S-N) containing a functional sulfur atom and C60, is synthesized and employed as electron transporting layer (ETL)/intermediary layer to targetedly heal the multitype defects in pero-SCs or assist the growth of ETL, such as [6,6]-phenyl-C61 -butyric acid methyl ester (PCBM), in planar p-i-n pero-SCs. The repaired pero-SCs can not only dramatically improve their power conversion efficiencies, but also address stability issues under moisture and high temperature. The corresponding mechanism of PCBB-S-N with targeted therapy effect in a device is systematically investigated by both experiments and theoretical calculation. This work demonstrates that the proposed fullerene derivative with finely tuned chemical structure can be a promising ETL candidate or intermediary to approach stable and efficient planar p-i-n pero-SCs.

Reconfiguration of interfacial energy band structure for high-performance inverted structure perovskite solar cells.

Charged defects at the surface of the organic-inorganic perovskite active layer are detrimental to solar cells due to exacerbated charge carrier recombination. Here we show that charged surface defects can be benign after passivation and further exploited for reconfiguration of interfacial energy band structure. Based on the electrostatic interaction between oppositely charged ions, Lewis-acid-featured fullerene skeleton after iodide ionization (PCBB-3N-3I) not only efficiently passivates positively charged surface defects but also assembles on top of the perovskite active layer with preferred orientation. Consequently, PCBB-3N-3I with a strong molecular electric dipole forms a dipole interlayer to reconfigure interfacial energy band structure, leading to enhanced built-in potential and charge collection. As a result, inverted structure planar heterojunction perovskite solar cells exhibit the promising power conversion efficiency of 21.1% and robust ambient stability. This work opens up a new window to boost perovskite solar cells via rational exploitation of charged defects beyond passivation.

A Semitransparent Inorganic Perovskite Film for Overcoming Ultraviolet Light Instability of Organic Solar Cells and Achieving 14.03% Efficiency.

Organic solar cells (OSCs) can be unstable under ultraviolet (UV) irradiation. To address this issue and enhance the power conversion efficiency (PCE), an inorganic-perovskite/organic four-terminal tandem solar cell (TSC) based on a semitransparent inorganic CsPbBr3 perovskite solar cell (pero-SC) as the top cell and an OSC as bottom cell is constructed. The high-quality CsPbBr3 photoactive layer of the planar pero-SC is prepared with a dual-source vacuum coevaporation method, using stoichiometric precursors of CsBr and PbBr2 with a low evaporation rate. The resultant opaque planar pero-SC exhibits an ultrahigh open-circuit voltage of 1.44 V and the highest reported PCE of 7.78% for a CsPbBr3 -based planar pero-SC. Importantly, the devices show no degradation after 120 h UV light illumination. The related semitransparent pero-SC can almost completely filter UV light and well maintain photovoltaic performance; it additionally shows an extremely high average visible transmittance. When it is used to construct a TSC, the top pero-SC acting as a UV filter can utilize UV light for photoelectric conversion, avoiding the instability problem of UV light on the bottom OSC that can meet the industrial standards of UV-light stability for solar cells, and leading to the highest reported PCE of 14.03% for the inorganic-perovskite/organic TSC.