Chen Weijie

Publication date: December 2020

Source: Nano Energy, Volume 78

Author(s): Enrique Hernández-Balaguera, Beatriz Romero, Belén Arredondo, Gonzalo del Pozo, Mehrdad Najafi, Yulia Galagan

A mixed lead precursor of halide lead source and nonhalide lead source is used to enable a low‐temperature, two‐step sequential deposition method for FAPbI₃ perovskite in triple‐mesoscopic solar cells. A power conversion efficiency of 16.21% is achieved.

The evolution from the original methylammonium (MA)‐ to formamidinium (FA)‐dominated perovskite makes a crucial contribution to improve the photoelectric performance of perovskite solar cells (PSCs) in a decade. However, to obtain α‐FAPbI₃, annealing temperature above 100 °C is essential. In addition, it is still challenging to deposit a uniform and high‐quality FA‐based perovskite absorber in printable triple‐mesoscopic PSC due to the complicated mesoscopic structure. Herein, a low‐temperature, two‐step sequential deposition method is used for pure FAPbI₃ perovskite in printable triple‐mesoscopic PSC. By using different lead sources, the crystallization and morphology of lead iodide (PbI₂) are finely controlled, which modulates the crystallization and pore filling of perovskite in mesoscopic structure. The improved interface contact promotes the transfer of charge carrier from perovskite to TiO₂. With the further introduction of cesium bromide (CsBr) into lead precursor, a power conversion efficiency of 16.24% is achieved. This study provides a deeper understanding of the pore filling and crystallization for both PbI₂ and perovskite, and helps explore and optimize the deposition process of perovskite in mesoscopic structure.

A novel BDT‐based random polymeric hole‐transporting layer (asy‐ranPBTBDT) is developed with irregularity from asymmetric substitution and random copolymerization. The resulting low crystallinity from the irregularity leads to superior solubility capacity and suppressed charge recombination and morphological changes. Therefore, the colloidal quantum dot solar cells using asy‐ranPBTBDT‐based device show highly efficient power conversion efficiency of 13.2% with superior operational stability.

Abstract

Next‐generation solution‐processed solar cells will hopefully be processed using green solvents, and will unite high performance with operating stability. Colloidal quantum dot/polymer hybrid solar cells are of interest for their harvest of the visible as well as the near infrared; however, today's best polymer hole‐transporting layers (HTLs) rely on processing using hazardous solvents such as chlorobenzene. This stems from the strong polymer–polymer attraction in polymeric p‐type materials, which accounts for their limited solubility. Here, a new random polymeric HTL (asy‐ranPBTBDT) is reported that is soluble in green solvents such as 2‐methylanisole without compromising ultimate device power conversion efficiency. The new polymer structure induces a strong π–π stacking face‐on orientation and less lateral grain growth compared to control asy‐PBTBDT, leading to reduced charge recombination and improved device stability. The resulting device exhibits a power conversion efficiency (PCE) of 13.2% and retains 89% of its initial efficiency after 120 h of continuous device operation at the maximum power point, compared to a PCE of 11.4% and 71% degradation for control devices.

To generate cost‐efficient and high‐performanced polymers, a simple chemical steric effect (SE) is introduced to benzothiophene (BDT)‐based side chains. The polymeric crystallinity and miscibility are rebalanced and a power conversion efficiency (PCE) of 14.53% is achieved. Thus, the SE applied in crystalline polymer pave an easier and cheaper route to realize the coordination of low‐cost fabrication and high‐performance.

Abstract

Low synthetic cost and high performance are becoming a new challenge in designing polymer donors for large‐scaled polymer solar cells (PSCs) fabrication; however, complicated synthetic routes and high material costs hamper the widespread commercial application of OPVs. Here, a simple and low‐cost chemical steric effect (SE) is introduced to BDT‐based side chains. Through adjusting alkyl side chains, the polymeric crystallinity and miscibility are rebalanced and subsequently the photovoltaic device based on the meta‐positioned alkyl polymer outperforms its para‐positioned counterpart. The champion device based on the polymer with the meta‐positioned side chains affords a PCE of 14.53% without sacrificing its high fill factor of 0.77, which could be attributed to a more balanced charge‐carrier transport ability and optimized morphology. This is the highest PCE value reported in BTZ based polymer donors to date. Thus, it shows that the SE applied in high crystalline polymer could pave an easier and cheaper chemical route to realize the coordination of low‐cost fabrication and high‐performance.

This study reports the deposition of a TiO₂ electron transporting layer for perovskite solar cells by spray coating using a stable TiO₂ colloidal aqueous solution, which is synthesized via the self‐condensation of a titanium peroxide complex under hydrothermal conditions. Although the whole fabrication process for the cells is performed at 100 °C, 22.7% efficiency is achieved.

Abstract

TiO₂ is one of the most efficient and widely used materials for electron‐transporting layer (ETLs) in perovskite solar cells (PSCs). The formation of efficient TiO₂ layers is generally carried out at high temperature by baking at a temperature >400 °C or by vacuum deposition (e.g., atomic layer deposition and E‐beam). In this study, the preparation of a TiO₂ ETL for PSCs is reported with excellent properties at low temperatures based on the synthesis of a stable TiO₂ colloidal aqueous solution and spray coating. The prepared TiO₂ colloids are able to produce a dense and uniform ETL even if it is simply dried at 100 °C after spray coating. It is believed that this is owing to the peroxo functional group remaining on the surface of the TiO₂ colloids. The TiO₂ ETLs, combined with the TiO₂ underlayer formed by chemical bath deposition, and the sprayed TiO₂ colloids allowed the fabrication of PSCs with performance similar to those of PSCs produced by annealing at 450 °C with a TiO₂ paste. The PSCs fabricated entirely at 100 °C demonstrated power conversion efficiency of 22.7% in small cells, and 19.0% in mini‐modules.

Stable and pure α‐FAPbI₃ phase is successfully obtained by a printed method in the ambient atmosphere. The scalable and fully printed perovskite solar cell with a carbon top electrode provides a stable PCE of 16.4%, which is the highest performance of full printed FAPbI₃ PSCs reported to date.

Abstract

Manufacturing commercially viable perovskite solar cells still requires appropriate low‐temperature and scalable deposition processes to be developed. While α‐phase FAPbI₃ has higher thermal stability and broader absorption than MAPbI₃, there still is no report of a pure α‐phase FAPbI₃ perovskite film obtained by a scalable printing method. Moreover, spontaneous conversion of the α‐phase to non‐perovskite δ‐phase under ambient conditions poses a serious challenge for practical applications. Herein, a scalable and fully solution based printing method for the fabrication of pure α‐phase FAPbI₃ perovskite solar cells is reported. Through adding N‐methyl pyrrolidone and methylammonium chloride to the dimethylformamide based precursor solution to control the crystallization, and vacuum or air‐flow assisted film drying, pure α‐FAPbI₃ phase is obtained by doctor blading. The resulting α‐FAPbI₃ film is highly stable, with no δ‐FAPbI₃ phase being formed even after keeping it in an ambient atmosphere over a period of 200 days without encapsulation. In addition, a fully solution processed PSC with a PCE of 16.1% is processed by the vacuum assisted method, and 17.8% by the air‐flow assisted method. Replacing silver with a printed carbon electrode provides a stable PCE up to 15% for the vacuum assisted and 16.4% for the air‐flow assisted method, which is the highest performance of FAPbI₃ solar cells to date. Compared with MAPbI₃, the fully printed FAPbI₃ perovskite devices exhibit a remarkable thermal stability in humid atmospheres which makes them a promising candidate for scalable production and commercialization.

An inorganic CsPbI₂Br perovskite solar cell employing organic ligands armored ZnO as the electron transport materials achieves a maximum power conversion efficiency of 16.84%, with superior photo‐ and thermal‐ stabilities.

Abstract

Inorganic perovskite solar cells (PSCs) have witnessed great progress in recent years due to their superior thermal stability. As a representative, CsPbI₂Br is attracting considerable attention as it can balance the high efficiency of CsPbI₃ and the stability of CsPbBr₃. However, most research employs doped charge transport materials or applies bilayer transport layers to obtain decent performance, which vastly complicates the fabrication process and scarcely satisfies the commercial production requirement. In this work, all‐layer‐doping‐free inorganic CsPbI₂Br PSCs using organic ligands armored ZnO as the electron transport materials achieve an encouraging performance of 16.84%, which is one of the highest efficiencies among published works. Meanwhile, both the ZnO‐based CsPbI₂Br film and device show superior photostability under continuous white light‐emitting diode illumination and improved thermal stability under 85 °C. The remarkable enhanced performance arises from the favorable organic ligands (acetate ions) residue in the ZnO film, which not only can conduce to maintain high crystallinity of perovskite, but also passivate traps at the interface through cesium/acetate interactions, thus suppressing the photo‐ and thermal‐ induced perovskite degradation.

The effects of Na doping on polycrystalline flexible Cu₂ZnSn(S,Se)₄ (CZTSSe) solar cells are analyzed. When doping is excessive, the device shows low contact potential difference and fill factor and selects a worse carrier transport path even though the built‐in potential becomes stronger. On the other hand, the optimized CZTSSe solar cell clearly shows the enhancing effect of Na doping.

Abstract

It is well‐known that the alkali doping of polycrystalline Cu₂ZnSn(S,Se)₄ (CZTSSe) and Cu(In,Ga)(Se,S)₂ has a beneficial influence on the device performance and there are various hypotheses about the principles of performance improvement. This work clearly explains the effect of Na doping on the fill factor (FF) rather than on all of the solar cell parameters (open‐circuit voltage, FF, and sometimes short circuit current) for overall performance improvement. When doping is optimized, the fabricated device shows sufficient built‐in potential and selects a better carrier transport path by the high potential difference between the intragrains and the grain boundaries. On the other hand, when doping is excessive, the device shows low contact potential difference and FF and selects a worse carrier transport path even though the built‐in potential becomes stronger. The fabricated CZTSSe solar cell on a flexible metal foil optimized with a 25 nm thick NaF doping layer achieves an FF of 62.63%, thereby clearly showing the enhancing effect of Na doping.

Stable and pure α‐FAPbI₃ phase is successfully obtained by a printed method in the ambient atmosphere. The scalable and fully printed perovskite solar cell with a carbon top electrode provides a stable PCE of 16.4%, which is the highest performance of full printed FAPbI₃ PSCs reported to date.

Abstract

Manufacturing commercially viable perovskite solar cells still requires appropriate low‐temperature and scalable deposition processes to be developed. While α‐phase FAPbI₃ has higher thermal stability and broader absorption than MAPbI₃, there still is no report of a pure α‐phase FAPbI₃ perovskite film obtained by a scalable printing method. Moreover, spontaneous conversion of the α‐phase to non‐perovskite δ‐phase under ambient conditions poses a serious challenge for practical applications. Herein, a scalable and fully solution based printing method for the fabrication of pure α‐phase FAPbI₃ perovskite solar cells is reported. Through adding N‐methyl pyrrolidone and methylammonium chloride to the dimethylformamide based precursor solution to control the crystallization, and vacuum or air‐flow assisted film drying, pure α‐FAPbI₃ phase is obtained by doctor blading. The resulting α‐FAPbI₃ film is highly stable, with no δ‐FAPbI₃ phase being formed even after keeping it in an ambient atmosphere over a period of 200 days without encapsulation. In addition, a fully solution processed PSC with a PCE of 16.1% is processed by the vacuum assisted method, and 17.8% by the air‐flow assisted method. Replacing silver with a printed carbon electrode provides a stable PCE up to 15% for the vacuum assisted and 16.4% for the air‐flow assisted method, which is the highest performance of FAPbI₃ solar cells to date. Compared with MAPbI₃, the fully printed FAPbI₃ perovskite devices exhibit a remarkable thermal stability in humid atmospheres which makes them a promising candidate for scalable production and commercialization.

Annealing‐free solution‐processable aqueous MoO _x are developed and applied in bulk‐heterojunction polymer solar cells based on non‐fullerene system PBDB‐T‐2F:Y6. The solar cells with aqueous MoO _x exhibit higher efficiencies and better stabilities without high‐temperature annealing compared to the solar cells with PEDOT:PSS.

Abstract

A charge transport layer based on transition metal‐oxides prepared by an anhydrous sol–gel method normally requires high‐temperature annealing to achieve the desired quality. Although annealing is not a difficult process in the laboratory, it is definitely not a simple process in mass production, such as roll‐to‐roll, because of the inevitable long cooling step that follows. Therefore, the development of an annealing‐free solution‐processable metal‐oxide is essential for the large‐scale commercialization. In this work, a room‐temperature processable annealing‐free “aqueous” MoO _x solution is developed and applied in non‐fullerene PBDB‐T‐2F:Y6 solar cells. By adjusting the concentration of water in the sol–gel route, an annealing‐free MoO _x with excellent electrical properties is successfully developed. The PBDB‐T‐2F:Y6 solar cell with the general MoO _x prepared by the anhydrous sol–gel method shows a low efficiency of 7.7% without annealing. If this anhydrous MoO _x is annealed at 200 °C, the efficiency is recovered to 17.1%, which is a normal value typically observed in conventional structure PBDB‐T‐2F:Y6 solar cells. However, without any annealing process, the solar cell with aqueous MoO _x exhibits comparable performance of 17.0%. In addition, the solar cell with annealing‐free aqueous MoO _x exhibits better performance and stability without high‐temperature annealing compared to the solar cells with PEDOT:PSS.

A series of copolymers via a random copolymerization approach are designed and synthesized. The well‐defined fibril interpenetrating morphology with appropriate phase separation in PT2‐based blends can efficiently suppress the unfavorable aggregation, resulting in excellent morphological stability and high efficiency. The work demonstrates the importance of optimization of fibril network morphology in realizing high‐efficiency and ambient‐stable polymer solar cells.

Abstract

Morphological stability is crucially important for the long‐term stability of polymer solar cells (PSCs). Many high‐efficiency PSCs suffer from metastable morphology, resulting in severe device degradation. Here, a series of copolymers is developed by manipulating the content of chlorinated benzodithiophene‐4,8‐dione (T1‐Cl) via a random copolymerization approach. It is found that all the copolymers can self‐assemble into a fibril nanostructure in films. By altering the T1‐Cl content, the polymer crystallinity and fibril width can be effectively controlled. When blended with several nonfullerene acceptors, such as TTPTT‐4F, O‐INIC3, EH‐INIC3, and Y6, the optimized fibril interpenetrating morphology can not only favor charge transport, but also inhibit the unfavorable molecular diffusion and aggregation in active layers, leading to excellent morphological stability. The work demonstrates the importance of optimization of fibril network morphology in realizing high‐efficiency and ambient‐stable PSCs, and also provides new insights into the effect of chemical structure on the fibril network morphology and photovoltaic performance of PSCs.

N‐functionalized conjugation engineering is explored for the design of 2D asymmetric nonfullerene acceptors (NFAs). Endowed with high charge transport and good nanofibrous phase separation with PBDB‐T, the best‐performing NFA contributes a champion power conversion efficiency of 14.02% in solar cells. Excellent thermal aging and light soaking stability are observed for the corresponding solar cells.

Abstract

The charge transport and morphology of active layers are key considerations for device performance and stability in organic solar cells (OSCs). Such properties can be fine‐tuned via elaborate molecular design of fused‐ring electron acceptors (FREAs), especially conjugation extension and side chain engineering. In this work, N‐functionalized conjugation is explored in the design of high‐efficient asymmetric FREAs. The twisting of N‐conjugated side chains from backbone endows three FREAs with similar energy levels and light absorptions (≈850 nm edge). Their blends with PBDB‐T exhibit high charge carrier mobility and ordered phase separation. Excitingly, IPT2F‐TT based OSCs yield a champion power conversion efficiency (PCE) of 14.02% with a fill factor (FF) of 75.06%, outperforming PBDB‐T devices with IPT2F‐Th (12.52%, 71.20%), IPT2F‐Ph (13.13%, 72.11%), and octylated IPT‐2F (13.70%, 71.50%). The PCE over 14% and FF over 75% are among the highest values for 2D FREAs OSCs reported to date. More importantly, outstanding thermal stability and light soaking stability are observed with PCE over 12% maintained after thermal or light aging for 100 h. This work demonstrates N‐conjugated FREAs design as an effective strategy to simultaneously improve the photovoltaic performance and device stability for the OSCs.

In this contribution, the photovoltaic performance of methylammonium‐free perovskite solar cells is enhanced by constructing interfacial capping layers with a pair of alkylammonium halides. The structure and composition of the interfacial layers are comprehensively investigated and their correlation with the device performance is described in terms of defect passivation efficacy, energy level alignment, and hydrophobicity for moisture resistance.

Abstract

The methylammonium (MA)‐free perovskite solar cells (PSCs) have drawn broad attention due to their excellent thermostability. However, the efficiency of these devices is inferior to most state‐of‐the‐art PSCs. Herein, the photovoltaic performance of the MA‐free PSCs is enhanced by constructing interfacial capping layers with a pair of alkylammonium halides, n‐propylammonium (PA) iodide and propane‐1,3‐diammonium (PDA) iodide. The structure and composition of the interfacial layers are comprehensively investigated and their correlation with the device performance is presented in terms of defect passivation efficacy, energy level alignment, and hydrophobicity for moisture resistance. The PSC devices based on the PAI and PDAI₂ treated MA‐free perovskite films demonstrate better power conversion efficiencies (PCEs) and stabilities than the reference devices without the interfacial layers. Although the PAI‐treated devices exhibit the highest PCE of 21.1%, the PDAI₂‐treated PSCs demonstrate the exceptional thermal and humidity stabilities.

As crystallized powders, hybrid perovskites (HP) show highly sensitive mechanochromic luminescence properties. Composites consisting of monolayered 2D and 3D HP components exhibit reversible tunable color emission upon mechanical strain: bright green emission originates from the 3D HP after efficient energy funneling from the multi‐layered 2D HP produced at the 2D/3D interface by the mechanical treatment.

Abstract

Hybrid perovskite (HP) materials are of interest in photovoltaics and lighting applications. Here we report that hybrid perovskite composites, as crystallized powders, can behave as intelligent materials showing highly sensitive and reversible mechanochromic luminescence (MCL). Composites consisting of monolayered 2D HP and 3D HP components exhibit reversible tunable color emission upon mechanical strain. The bluish‐whitish emission of the 2D HP turns into orange in the composite owing to an energy transfer process. The bright green emission, observed as soon as the composite is slightly crushed, originates from the 3D HP after efficient energy funneling from the multi‐layered 2D HP produced at the 2D/3D interface by the mechanical treatment. Besides highlighting the key role of the interfaces in light emission of HP, our findings pave the way for hybrid perovskites as highly sensitive MCL smart materials for mechanosensors, security papers, or optical storage applications.

CsSn_0.6Ge_0.4I₃ nanocrystals have been synthesized for the first time by a B‐site co‐alloying strategy. The introduction of Ge effectively decreases the high density of intrinsic Sn defects, resulting in an extended excitonic lifetime and enhanced solar cell performance. The stability of the new nanocrystals also improves owing to the effective protection of Sn²⁺ against oxidation.

Abstract

Colloidal lead‐free perovskite nanocrystals have recently received extensive attention because of their facile synthesis, the outstanding size‐tunable optoelectronic properties, and less or no toxicity in their commercial applications. Tin (Sn) has so far led to the most efficient lead‐free solar cells, yet showing highly unstable characteristics in ambient conditions. Here, we propose the synthesis of all‐inorganic mixture Sn‐Ge perovskite nanocrystals, demonstrating the role of Ge²⁺ in stabilizing Sn²⁺ cation while enhancing the optical and photophysical properties. The partial replacement of Sn atoms by Ge atoms in the nanostructures effectively fills the high density of Sn vacancies, reducing the surface traps and leading to a longer excitonic lifetime and increased photoluminescence quantum yield. The resultant Sn‐Ge nanocrystals‐based devices show the highest efficiency of 4.9 %, enhanced by nearly 60 % compared to that of pure Sn nanocrystals‐based devices.

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.

The use of the atomic layer deposition (ALD) ultrathin TiO _x to modify the interface layer in both opaque and semitransparent organic solar cells is reported. The modification effectively passivates the interface, reduces the series resistance, and improves the charge transport, which leads to increased power conversion efficiency (PCE) with enhanced stability in the device.

Organic solar cells (OSCs) are considered to have reached a second golden age with profoundly improved power conversion efficiency (PCE) and device stability in recent years. The modification of the interface layer plays a significant role in achieving performance enhancement in OSCs. Herein, the use of the atomic layer deposition (ALD) ultrathin TiO _x to modify the interface layer in OSCs is reported. The modification with only two TiO _x ALD cycles not only effectively passivates the interface between the ZnO electron transport layer (ETL) and the active layer, but also reduces the series resistance and improves the charge transport process in the device. An absolute 1% increase in PCE with enhanced device stability for modified OSCs is achieved. Semitransparent OSCs are also fabricated by applying this interface modification strategy. The modification with two TiO _x ALD cycles increases the electrical device performance without affecting the optical properties of the semitransparent device. An average PCE of 10.46% with an average visible transmittance (AVT) of 19.61% and a color rendering index (CRI) close to 100 is demonstrated for the fabricated semitransparent device with the modification. The ALD‐assisted interface modification provides a straightforward way to realize high‐performance semitransparent OSCs.

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.

Herein, a one‐step solution‐processing of [MA_0.9Cs_0.1Pb(I_0.6Br_0.4)₃] wide‐bandgap perovskite using phenylhydrazine iodide with amino groups to successfully passivate the trap density within grain boundaries and increase the perovskite grain size is demonstrated. The reinforced morphology and grain boundaries treatment considerably enhance the power conversion efficiency from 12.16% for pristine to 14.63% for the treated devices.

Due to the attraction of fabricating highly efficient tandem solar cells, wide‐bandgap perovskite solar cells (PSCs) have attracted substantial interest in recent years. However, polycrystalline perovskite thin‐films show the existence of trap states at grain boundaries which diminish the optoelectronic properties of the perovskite and thus remains a challenge. Here, a one‐step solution‐processing of [ MA0.9Cs0.1Pb(I0.6Br0.4)3] wide‐bandgap perovskite using phenylhydrazine iodide with amino groups is demonstrated to successfully passivate the trap density within grain boundaries and increase the perovskite grain size. The reinforced morphology and grain boundaries treatment considerably enhanced the power conversion efficiency (PCE) from 12.16% for pristine to 14.63% for the treated devices. This strategy can be easily adopted to other perovskites and help realize highly efficient perovskite solar cells.

As crystallized powders, hybrid perovskites (HP) show highly sensitive mechanochromic luminescence properties. Composites consisting of monolayered 2D and 3D HP components exhibit reversible tunable color emission upon mechanical strain: bright green emission originates from the 3D HP after efficient energy funneling from the multi‐layered 2D HP produced at the 2D/3D interface by the mechanical treatment.

Abstract

Hybrid perovskite (HP) materials are of interest in photovoltaics and lighting applications. Here we report that hybrid perovskite composites, as crystallized powders, can behave as intelligent materials showing highly sensitive and reversible mechanochromic luminescence (MCL). Composites consisting of monolayered 2D HP and 3D HP components exhibit reversible tunable color emission upon mechanical strain. The bluish‐whitish emission of the 2D HP turns into orange in the composite owing to an energy transfer process. The bright green emission, observed as soon as the composite is slightly crushed, originates from the 3D HP after efficient energy funneling from the multi‐layered 2D HP produced at the 2D/3D interface by the mechanical treatment. Besides highlighting the key role of the interfaces in light emission of HP, our findings pave the way for hybrid perovskites as highly sensitive MCL smart materials for mechanosensors, security papers, or optical storage applications.