Ligang Yuan

A narrow‐bandgap polymer acceptor L14 with an acceptor–acceptor (A–A) backbone is synthesized, showing lower‐lying frontier molecular orbitals, higher electron mobility, and larger absorption coefficient without sacrificing photovoltage compared to its donor–acceptor (D–A) analog polymer, L11. When applied in all‐polymer solar cells, L14 yields an outstanding efficiency of 14.3%.

Abstract

Narrow‐bandgap polymer semiconductors are essential for advancing the development of organic solar cells. Here, a new narrow‐bandgap polymer acceptor L14, featuring an acceptor–acceptor (A–A) type backbone, is synthesized by copolymerizing a dibrominated fused‐ring electron acceptor (FREA) with distannylated bithiophene imide. Combining the advantages of both the FREA and the A–A polymer, L14 not only shows a narrow bandgap and high absorption coefficient, but also low‐lying frontier molecular orbital (FMO) levels. Such FMO levels yield improved electron transfer character, but unexpectedly, without sacrificing open‐circuit voltage (V _oc), which is attributed to a small nonradiative recombination loss (E _loss,nr) of 0.22 eV. Benefiting from the improved photocurrent along with the high fill factor and V _oc, an excellent efficiency of 14.3% is achieved, which is among the highest values for all‐polymer solar cells (all‐PSCs). The results demonstrate the superiority of narrow‐bandgap A–A type polymers for improving all‐PSC performance and pave a way toward developing high‐performance polymer acceptors for all‐PSCs.

The inclusion of a novel in situ polymerizable ionic liquid, 1,3‐bis(4‐vinylbenzyl)imidazolium chloride ([bvbim]Cl), allows perovskite films to be manufactured under humid environments, conferring improved materials quality, higher power conversion efficiency, and long‐term stability.

Abstract

Despite the excellent photovoltaic properties achieved by perovskite solar cells at the laboratory scale, hybrid perovskites decompose in the presence of air, especially at high temperatures and in humid environments. Consequently, high‐efficiency perovskites are usually prepared in dry/inert environments, which are expensive and less convenient for scale‐up purposes. Here, a new approach based on the inclusion of an in situ polymerizable ionic liquid, 1,3‐bis(4‐vinylbenzyl)imidazolium chloride ([bvbim]Cl), is presented, which allows perovskite films to be manufactured under humid environments, additionally leading to a material with improved quality and long‐term stability. The approach, which is transferrable to several perovskite formulations, allows efficiencies as high as 17% for MAPbI₃ processed in air % relative humidity (RH) ≥30 (from an initial 15%), and 19.92% for FAMAPbI₃ fabricated in %RH ≥50 (from an initial 17%), providing one of the best performances to date under similar conditions.

A formamidinium (FA)‐based quasi‐2D Ruddlesden–Popper (RP) perovskite, namely, (ThMA)₂(FA) _{n −1}Pb _n I_{3 n +1} (nominal n = 5), is successfully demonstrated with high photovoltaic performance by using an organic‐salt‐assisted crystal growth method. The optimized device exhibits a champion efficiency of 19.06%, which is a record for quasi‐2D RP perovskite solar cells with nominal n‐value lower than 6.

Abstract

Quasi‐2D Ruddlesden–Popper (RP) perovskite solar cells (PSCs) have drawn significant attention due to their appealing environmental stability compared to their 3D counterparts. However, the relatively low power conversion efficiency (PCE) greatly limits their applications. Here, high photovoltaic performance is demonstrated for quasi‐2D RP PSCs using 2‐thiophenemethylammonium as spacer with nominal n‐value of 5, which is based on the stoichiometry of the precursors. The incorporation of formamidinium (FA) in quasi‐2D RP perovskites reduces the bandgap and improves the light absorption ability, resulting in enlarged photocurrent and an increased PCE of 16.18%, which is higher than that of reported analogous methylammonium (MA)‐based quasi‐2D PSC (≈15%). A record high PCE of 19.06% is further demonstrated by using an organic salt, namely, 4‐(trifluoromethyl)benzylammonium iodide, assisted crystal growth (OACG) technique, which can induce the crystal growth and orientation, tune the surface energy levels, and suppress the charge recombination losses. More importantly, the devices based on OACG‐processed quasi‐2D RP perovskites show remarkable environmental stability and thermal stability, for example, the PCE retaining ≈96% of its initial value after storage at 80 °C for 576 h, while only ≈37% of the original efficiency left for FAPbI₃‐based

3D PSCs.

The commercially available pyridinedicarboxylic acid (PDA) molecule with one pyridine and two carboxylic acid groups is used as a passivating agent to cure the defects at both the surfaces and grain boundaries of MAPbI₃ perovskites. A champion power conversion efficiency (PCE) approaching 19% with optimized long‐term stability and thermal stability is achieved in PDA‐passivated perovskite solar cells (PSCs).

Electronic defects and grain boundaries of perovskite films will significantly deteriorate both the efficiency and the stability of perovskite solar cells (PSCs), and various methods aimed to reduce these defects are proposed. Herein, an organic solid molecule of pyridinedicarboxylic acid (PDA) with one pyridine and two carboxylic acid groups is used as a passivating agent to cure the defects by regulating the perovskite microstructures in a multiple manner. The defects located at both the surfaces and grain boundaries of polycrystalline MAPbI₃ perovskites are simultaneously passivated through the multiple coordination effects between the used functional groups and uncoordinated Pb²⁺, regardless of the substitution sites of the carboxylic acid and pyridine. Impressively, the PDA‐passivated inverted PSCs achieve remarkably enhanced power conversion efficiencies (PCEs) from 16.43% to nearly 19% and maintain over 90% of its original PCE after 1300 h under an inert environment. These findings indicate that the commercially available PDA molecule emerges as an efficient passivating agent of perovskite defects capable of stimulating the combined effects of the multiple functional groups, which is highly promising for the practical applications of PSCs with both high efficiency and good stability.

Inorganic CsPbI3 perovskite is the most competitive candidate to hybrid perovskites. However, its poor phase stability, hydrophobicity and high‐density defects have limited the development of CsPbI3 perovskite solar cells (PSCs). To overcome these obstacles for achieving high‐performance CsPbI3 PSCs, additive engineering has been widely employed. Herein, the progress of additive engineering in CsPbI3 PSCs is systematically reviewed.

All‐inorganic perovskite solar cells (PSCs) have attracted a lot of attention in the past few years because of their preeminent thermal stability compared with organic–inorganic hybrid PSCs. Among all kinds of all‐inorganic perovskites, CsPbI₃ perovskite with a proper bandgap of ≈1.7 eV becomes the most competitive candidate. However, its poor phase stability, hydrophobicity, and high‐density defects have limited the development of CsPbI₃ PSCs. To overcome these obstacles for achieving high‐performance CsPbI₃ PSCs, additive engineering has been widely used, which has rapidly promoted the power conversion efficiency (PCE) to over 19%. Herein, the progress of additive engineering in CsPbI₃ PSCs is systematically reviewed. First, the roles of additives in CsPbI₃ PSCs are introduced, including improving phase stability, increasing moisture resistance, and passivating defects. Then, the additive engineering is categorized (additive engineering in perovskites and at perovskite/hole transport layer interfaces) and reviewed in detail. Finally, future research directions on additive engineering are suggested for further enhancing stability and improving PCE.

A methylammonium chloride (MACl) additive is used to synthesize FA_1–x MA _x PbI₃ films. The best molar fraction of this additive is determined. The MA content in thin films actually used in solar cells is x = 0.06. This amount is thermodynamically the best for the stabilization of this highly efficient perovskite. The perovskite solar cell achieves a stabilized power conversion efficiency as high as 22.06%.

Nowadays, complex chemistry and precursor solution compositions are developed to stabilize hybrid perovskite films and boost the efficiency of perovskite solar cells (PSCs). In this context, determining the actual composition of these layers, especially in organic cations, and understanding the chemistry behind is challenging. Herein, the introduction of methylammonium (MA⁺) in formamidinium lead iodide (FAPbI₃) 3D perovskite is considered to stabilize the α‐phase, whose quantity must be minimized to reduce the material hydrophilicity and its possible destabilization by degassing. The key effects of methylammonium chloride (MACl) additive on the growth of FA_1–x MA _x PbI₃ perovskite layers are studied. Liquid nuclear magnetic resonance (NMR) is used to analyze the photovoltaic layers. NMR peaks and their origin are identified. The MA and FA content in films actually used in PSCs is reliably measured and prepared over a large additive molar concentration ratio. x is quantified at 0.06 ± 0.01 for pure films, which corresponds to the best entropic compound stabilization. It results in PSCs with a stabilized power conversion efficiency as high as 22.06%. These PSCs are shown to be highly stable under solar irradiation and high moisture.

High‐temperature degradation of perovskite solar cells with spiro‐OMeTAD hole transport layer is investigated. The postdoping of the spiro‐OMeTAD layer by iodine released from an iodine‐containing perovskite layer at high temperature is discovered as one reason for the high‐temperature degradation. Using an iodine‐free perovskite absorber, thermally stable perovskite solar cells are demonstrated.

Organic–inorganic halide perovskites are promising as the light absorber of solar cells because of their efficient solar power conversion. An issue frequently occurring in perovskite solar cells (PSCs) with a hole transport layer of N,N‐di(4‐methoxyphenyl)amino]‐9,9′‐spirobifluorene (spiro‐OMeTAD) is a quick performance degradation at high temperature. Herein, it is discovered that postdoping of the spiro‐OMeTAD layer by iodine released from the perovskite layer is one possible mechanism for the high‐temperature PSC degradation. Iodine doping leads to the highest occupied molecular orbital level of the spiro‐OMeTAD layer becoming deeper and, therefore, induces the formation of an energy barrier for hole extraction from the perovskite layer. It is demonstrated that it is possible to suppress the high‐temperature degradation by using an iodine‐blocking layer or an iodine‐free perovskite in PSCs. These findings will guide the way for the realization of thermally stable perovskite optoelectronic devices in the future.

The impact of SnF₂ on FA_{0 . 83}Cs_{0 . 17}Sn _x Pb_{1− x} I₃ perovskite thin films is examined for additive amounts varying between 0.1% and 20%. Structural distortion from lattice strain is reduced by SnF₂ addition. Lower background hole doping, longer photoluminescence lifetimes, and higher charge‐carrier mobilities are observed with as little as 1% SnF₂ added. Larger quantities of the additive introduce defects alongside these beneficial effects.

Abstract

Mixed tin‐lead halide perovskites are promising low‐bandgap absorbers for all‐perovskite tandem solar cells that offer higher efficiencies than single‐junction devices. A significant barrier to higher performance and stability is the ready oxidation of tin, commonly mitigated by various additives whose impact is still poorly understood for mixed tin‐lead perovskites. Here, the effects of the commonly used SnF₂ additive are revealed for FA_{0 . 83}Cs_{0 . 17}Sn _x Pb_{1− x} I₃ perovskites across the full compositional lead‐tin range and SnF₂ percentages of 0.1–20% of precursor tin content. SnF₂ addition causes a significant reduction in the background hole density associated with tin vacancies, yielding longer photoluminescence lifetimes, decreased energetic disorder, reduced Burstein–Moss shifts, and higher charge‐carrier mobilities. Such effects are optimized for SnF₂ addition of 1%, while for 5% SnF₂ and above, additional nonradiative recombination pathways begin to appear. It is further found that the addition of SnF₂ reduces a tetragonal distortion in the perovskite structure deriving from the presence of tin vacancies that cause strain, particularly for high tin content. The optical phonon response associated with inorganic lattice vibrations is further explored, exhibiting a shift to higher frequency and significant broadening with increasing tin fraction, in accordance with lower effective atomic metal masses and shorter phonon lifetimes.

High‐performance quasi‐2D perovskite solar cells (PVSCs) are demonstrated via heat–light co‐treatment. The optimized quasi‐2D PVSC presents a maximum PCE of 18.24% with excellent stability. The underlying mechanism of the light and heat co‐treatment in improving the device performance lies in its synergistic effect in reducing the trap states and improving the charge transport.

Abstract

2D perovskite solar cells (2D PVSCs) show good stability for commercialization. However, their power conversion efficiency (PCE) is relatively low. In this work, a post‐treatment strategy by simultaneously applying light and heat to quasi‐2D PVSCs, obtaining a record PCE of 18.24% is developed. It is found that heat‐treating PVSCs in the dark slightly increases the device performance over time at temperatures below 75 °C, whereas the performance deteriorates rapidly at temperatures above 100 °C. Upon illumination, the device efficiency is significantly improved, particularly when the thermal‐treatment temperature is increased to 100 °C. A comprehensive carrier dynamic study reveals that the enhanced performance can be attributed to the reduced quasi‐2D perovskite defect states and improved charge collection. In addition, this strategy enables better stability, and an unencapsulated device can retain 90% of its original PCE after 1340 h of direct exposure to air with a humidity of 50 ± 5%. Thus, the strategy paves the way for the commercialization of quasi‐2D PVSCs.

Nature Energy, Published online: 05 October 2020; doi:10.1038/s41560-020-00705-5

A new fluorinated organic ammonium halide salt, 4‐trifluoromethyl phenethylammonium iodide (CFPEAI), is utilized to passivate the surface of CsPbI₂Br perovskite for solar cells with enhanced efficiency as well as improved stability.

Surface modification is demonstrated as an efficient strategy to enhance the efficiency and stability of perovskite solar cells (PVSCs). Fluorinated organic ammonium salts featuring a strong hydrophobic nature are seldom used as passivation agents for the surface modification of CsPbI₂Br perovskites. Herein, a fluorinated organic ammonium halide salt, 4‐trifluoromethyl phenethylammonium iodide (CFPEAI), is incorporated into the surface of CsPbI₂Br perovskite for the first time. After the CFPEAI modification, the defects of CsPbI₂Br perovskite are significantly passivated with reduced trap densities. The best‐performance PVSC with CFPEAI modification shows an excellent power conversion efficiency (PCE) of 16.07% with a high fill factor (FF) of 84.65%, a short‐circuit current density (J _SC) of 15.45 mA cm⁻², and an open‐circuit voltage (V _OC) of 1.23 V. In contrast, the control PVSCs without the surface modification exhibit a lower PCE of 14.50% with a FF of 80.56%, a J _SC of 15.05 mA cm⁻², and a V _OC of 1.20 V. With CFPEAI passivation, the CsPbI₂Br perovskite film exhibits enhanced hydrophobicity, thereby leading to improved stability for the corresponding PVSC in comparison with the control PVSC without any surface modification.

Publication date: 18 November 2020

Source: Joule, Volume 4, Issue 11

Author(s): Fabrizio Gota, Malte Langenhorst, Raphael Schmager, Jonathan Lehr, Ulrich W. Paetzold

A new DPP‐based alternating D–A copolymer (PD2FCT‐29DPP) is developed for use as a hole‐transport layer. PD2FCT‐29DPP addresses the different requirements for an HTL, offering favorable energetics, near‐infrared absorption, and efficient charge transfer. Therefore, a PD2FCT‐29DPP‐based device achieves a remarkable FF of 70% and the highest PCE of 14.0% among PbS CQD‐SCs.

Abstract

The need for optoelectronic and chemical compatibility between the layers in colloidal quantum dot (CQD) photovoltaic devices remains a bottleneck in further increasing performance. Conjugated polymers are promising candidates as new hole‐transport layer (HTL) materials in CQD solar cells (CQD‐SCs) owing to the highly tunable optoelectronic properties and compatible chemistries. A diketopyrrolopyrrole‐based polymer with benzothiadiazole derivatives (PD2FCT‐29DPP) as an HTL in these devices is reported. The energy level, molecular orientation, and hole mobility of this HTL are manipulated through molecular engineering. By levering the polymer's optical absorption spectrum complementary to that of the CQD active layer, EQE across the visible and near‐infrared regions is maximized. As a result, a PD2FCT‐29DPP‐based device exhibits a fill factor of 70% and approximately 35% efficiency enhancement compared to a PTB7‐based device.

Publication date: 16 December 2020

Source: Joule, Volume 4, Issue 12

Author(s): Anyi Mei, Yusong Sheng, Yue Ming, Yue Hu, Yaoguang Rong, Weihua Zhang, Shulin Luo, Guangren Na, Chengbo Tian, Xiaomeng Hou, Yuli Xiong, Zhihui Zhang, Shuang Liu, Satoshi Uchida, Tae-Woong Kim, Yongbo Yuan, Lijun Zhang, Yinhua Zhou, Hongwei Han

Novel interface polarization induced field‐effect passivation based on amorphous transition metal oxide is developed for efficient and ambient‐air‐stable perovskite solar cells. Comprehensive insights into the interaction between the field‐effect passivation, interface polarities, and the performance of the device have been elucidated in detail.

Abstract

Organolead halide hybrid perovskite solar cells (PSCs) have become a shining star in the renewable devices field due to the sharp growth of power conversion efficiency; however, interfacial recombination and carrier‐extraction losses at heterointerfaces between the perovskite active layer and the carrier transport layers remain the two main obstacles to further improve the power conversion efficiency. Here, novel field‐effect passivation has been successfully induced to effectively suppress the interfacial recombination and improve interfacial charge transfer by incorporating interfacial polarization via inserting a high work function interlayer between perovskite and holes transport layer. The charge dynamics within the device and the mechanism of the field‐effect passivation are elucidated in detail. The unique interfacial dipoles reinforce the built‐in field and prevent the photogenerated charges from recombining, resulting in power conversion efficiency up to 21.7% with negligible hysteresis. Furthermore, the hydrophobic interlayer also suppresses the perovskite decomposition by preventing the moisture penetration, thereby improving the humidity stability of the PSCs (>91% of the initial power conversion efficiency (PCE) after 30 d in 65 ± 5% humidity). Finally, several promising research perspectives based on field‐effect passivation are also suggested for further conversion efficiency improvements and photovoltaic applications.

Herein, novel Ruddlesden–Popper Cs₂PbI₂Cl₂ nanosheets are synthesized and creatively employed as a multifunctional interface optimization material to improve the performance of CsPbI₂Br solar cells. Based on the heterostructured NSs/CsPbI₂Br/NSs inorganic film, an efficiency of 16.65% is obtained, which is one of the best reported for CsPbI₂Br solar cells, along with much‐enhanced UV, air, and thermal stabilities.

Abstract

Inorganic CsPbI₂Br perovskite solar cells (PSCs) have gained enormous research interest due to their excellent thermal and light stabilities. However, their unsatisfactory power‐conversion efficiency and poor intrinsic phase stability remain roadblocks to their further development. Herein, Cs₂PbI₂Cl₂ nanosheets (NSs) with the Ruddlesden–Popper (RP) structure are synthesized, and an NSs/CsPbI₂Br/NSs heterostructure is employed to enhance both the stability and efficiency of CsPbI₂Br solar cells. The novel Cs₂PbI₂Cl₂ NSs can not only passivate the top and bottom surfaces of the perovskite film and top surface of the TiO₂ film but also enhance the stability of the perovskite film. Based on the heterostructured NSs/CsPbI₂Br/NSs inorganic perovskite film, the efficiency of the CsPbI₂Br PSCs is improved from 15.02% to 16.65%. Moreover, the unencapsulated CsPbI₂Br devices with the NSs/CsPbI₂Br/NSs heterostructure sustain over 90% of their original efficiencies after being exposed to ambient conditions (≈25 °C and ≈35% RH) for 648 h. Both the UV‐light‐soaking stability (100 mW cm⁻¹ 365 nm UV light) and thermal stability (T = 85 °C) of the optimized devices are dramatically improved in comparison with their counterparts with only a 3D active layer. Therefore, this work promotes the application of RP inorganic perovskite nanocrystals in a range of perovskite optoelectronic devices.

Due to the poor morphology and crystallinity of Sn–Pb mixed perovskites, it is found that the addition of potassium thiocyanate (KSCN) can effectively reduce the bulk defects and carrier recombination through optimizing the process of film formation and the perovskite film quality. Therefore, a whole improvement of device performance can be achieved under the optimization effect of KSCN doping.

The organic–inorganic Sn–Pb mixed perovskite has achieved great progress during the last 10 years and is considered as one of the most promising low‐bandgap photovoltaic materials. It has lower toxicity, outstanding optoelectrical properties, and achieved remarkable performance. However, there are still plenty of challenges in controlling the morphology, crystallinity, and defects of the Sn–Pb mixed perovskite film because of the inferior chemical stability of Sn compared with Pb. Herein, it is found that the synergistic effect of potassium thiocyanate (KSCN) in the Sn–Pb mixed perovskites can enlarge the grain size, enhance the crystallization, improve the film morphology, and obtain high‐quality perovskite films which effectively eliminate the bulk defects and smooth carrier transportation of Sn–Pb mixed perovskite solar cells. Through optimizing the concentration of KSCN, a high‐performance MA_0.5FA_0.5Pb_0.5Sn_0.5I₃ solar cell with an efficiency of 15.14% and improved stability is obtained. This work lays a key foundation for the fabrication of efficient and stable Sn‐based or Sn–Pb mixed perovskite solar devices.

Lead‐free CsSnX₃ (X=Cl, Br, and I) NCs are synthesized by using SnC₂O₄, Cs₂CO₃, and NH₄X as precursors. Highly stable CsSnX₃ NCs can be prepared employing antioxidative SnC₂O₄ as the Sn^II precursor. The stability improvement is mainly due to the oxalate in the SnC₂O₄ precursor that not only inhibits the oxidation of Sn²⁺ during synthesis but also caps on the surface of NCs as a bidentate ligand to protect the NCs.

Abstract

Lead‐free CsSnX₃ perovskite NCs are becoming a promising alternative to CsPbX₃ (X=Cl, Br, I), but suffer from extremely poor stability. Herein, we highlight the significant effect of Sn^II precursors used in the synthesis on the stability of the resultant CsSnX₃ NCs. A method is proposed for synthesizing CsSnX₃ NCs using Cs₂CO₃, SnC₂O₄, and NH₄X as corresponding constituent precursors, wherein the ratio of reactants can be easily adjusted. Stable CsSnX₃ NCs can be obtained with the use of antioxidative SnC₂O₄ as the Sn^II precursor. Experimental results show that the improvement of NCs stability is mainly ascribed to the role of oxalate in the SnC₂O₄ precursor. Oxalate ion has a strong antioxidative ability and can effectively inhibit the oxidation of Sn^II during the synthesis. Besides, oxalate as a bidentate capping ligand is shown to be coordinated on the surface of formed NCs. This can not only passivate the uncoordinated Sn on the surface but also prevent the oxidation of the NCs.

An electrospray printing technique is developed to continuously print the TiO₂ electron transport layer, perovskite layer, and carbon layer, enabling a cost‐effective device. The electrospray technique is capable of printing uniform, compact, and high adhesion layers with controllable dimensions and patterns. This work demonstrates a fully printed low‐cost solar cell and provides a feasible process for perovskite solar cells to initial industrialization.

Abstract

With the power conversion efficiencies of perovskite solar cells (PSCs) exceeding 25%, the PSCs are a step closer to initial industrialization. Prior to transferring from laboratory fabrication to industrial manufacturing, issues such as scalability, material cost, and production line compatibility that significantly impact the manufacturing remain to be addressed. Here, breakthroughs on all these fronts are reported. Carbon‐based PSCs with architecture fluorine doped tin oxide (FTO)/electron transport layer/perovskite/carbon, that eliminate the need for the hole transport layer and noble metal electrode, provide ultralow‐cost configuration. This PSC architecture is manufactured using a scalable and industrially compatible electrospray (ES) technique, which enables continuous printing of all the cell layers. The ES deposited electron transport layer and perovskite layer exhibit properties comparable to that of the laboratory‐scale spin coating method. The ES deposited carbon electrode layer exhibits superior conductivity and interfacial microstructure in comparison to films synthesized using the conventional doctor blading technique. As a result, the fully ES printed carbon‐based PSCs show a record 14.41% power conversion efficiency, rivaling the state‐of‐the‐art hole transporter‐free PSCs. These results will immediately have an impact on the scalable production of PSCs.

An ionic liquid, 1,3‐dimethyl‐3‐imidazolium hexafluorophosphate (DMIMPF₆), was used to passivate a perovskite to decrease the defects of Pb‐cluster and Pb‐I antisite, thereby reducing the energy barrier between the perovskite and hole transport layer. A perovskite solar cell attained a 23.25 % efficiency with a high stability due to hydrophobic DMIMPF₆.

Abstract

Surface defects have been a key constraint for perovskite photovoltaics. Herein, 1,3‐dimethyl‐3‐imidazolium hexafluorophosphate (DMIMPF₆) ionic liquid (IL) is adopted to passivate the surface of a formamidinium‐cesium lead iodide perovskite (Cs_0.08FA_0.92PbI₃) and also reduce the energy barrier between the perovskite and hole transport layer. Theoretical simulations and experimental results demonstrate that Pb‐cluster and Pb‐I antisite defects can be effectively passivated by [DMIM]⁺ bonding with the Pb²⁺ ion on the perovskite surface, leading to significantly suppressed non‐radiative recombination. As a result, the solar cell efficiency was increased to 23.25 % from 21.09 %. Meanwhile, the DMIMPF₆‐treated perovskite device demonstrated long‐term stability because the hydrophobic DMIMPF₆ layer blocked moisture permeation.

Aided by theoretical calculation, a multifunctional 2,2‐difluoropropanediamide (DFPDA) molecule that bears carbonyl, amino, and fluorine groups is first introduced into the perovskite precursor, serving as a crystal growth mitigator, grain boundaries passivator, and surface protection material. With the help of the combined effects of multifunctional groups in DFPDA, the perovskite cells deliver an efficiency of 22.21% and improved stability.

Abstract

With a certified efficiency as high as 25.2%, perovskite has taken the crown as the highest efficiency thin film solar cell material. Unfortunately, serious instability issues must be resolved before perovskite solar cells (PSCs) are commercialized. Aided by theoretical calculation, an appropriate multifunctional molecule, 2,2‐difluoropropanediamide (DFPDA), is selected to ameliorate all the instability issues. Specifically, the carbonyl groups in DFPDA form chemical bonds with Pb²⁺ and passivate under‐coordinated Pb²⁺ defects. Consequently, the perovskite crystallization rate is reduced and high‐quality films are produced with fewer defects. The amino groups not only bind with iodide to suppress ion migration but also increase the electron density on the carbonyl groups to further enhance their passivation effect. Furthermore, the fluorine groups in DFPDA form both an effective barrier on the perovskite to improve its moisture stability and a bridge between the perovskite and HTL for effective charge transport. In addition, they show an effective doping effect in the HTL to improve its carrier mobility. With the help of the combined effects of these groups in DFPDA, the PSCs with DFPDA additive achieve a champion efficiency of 22.21% and a substantially improved stability against moisture, heat, and light.