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The past decade has witnessed the great success achieved by metal halide perovskites (MHPs) in photovoltaic and related fields. However, challenges still remain in further improving their performance, as well as, settling the stability issue for future commercialization. Recently, MHP/2D material heterostructures that combining MHPs with the low‐cost and solution‐processable 2D materials have demonstrated unprecedented improvement in both performance and stability due to the distinctive features at hetero‐interface. The diverse fabrication techniques of MHPs and 2D materials allow them to be assembled as heterostructures with different configurations in a variety of ways. Moreover, the large families of MHPs and 2D materials provide the opportunity for the rational design and modification on compositions and functionalities of MHP/2D materials heterostructures. Herein, a comprehensive review of MHP/2D material heterostructures from syntheses to applications is presented. First, various fabrication techniques for MHP/2D material heterostructures are introduced by classifying them into solid‐state methods and solution‐processed methods. Then the applications of MHP/2D heterostructures in various fields including photodetectors, solar cells, and photocatalysis are summarized in detail. Finally, current challenges for the development of MHP/2D material heterostructures are highlighted, and future opportunities for the advancements in this research field are also provided. [ABSTRACT FROM AUTHOR]

Layer‐by‐layer all‐polymer solar cells (LbL all‐PSCs) are prepared with PM6 and PY‐IT by using sequential spin coating method. The exciton dissociation efficiency in acceptor layer near electrode is rather low due to the limited exciton diffuse distance and impossible energy transfer from narrow bandgap acceptor to wide bandgap donor. In this study, less PM6 is incorporated into PY‐IT layer to enhance exciton dissociation in PY‐IT layer near electrode. A power conversion efficiency (PCE) of 17.45% is achieved in the LbL all‐PSCs incorporating 10 wt% PM6 into PY‐IT layer, which is much larger than 16.04% PCE of PM6/PY‐IT‐based LbL all‐PSCs. Over 8% PCE enhancement can be realized by incorporating 10 wt% PM6 into PY‐IT layer, which is attributed to the enhanced exciton utilization efficiency in PY‐IT layers near electrode. The enhanced exciton utilization efficiency in PY‐IT layer can be confirmed from the quenched photoluminescence (PL) emission in PY‐IT:PM6 films. Meanwhile, charge transport in acceptor layers can be optimized by incorporating less PM6, as confirmed from the optimized molecular arrangement. This study indicates that the strategy of incorporating less donor into acceptor layer has great potential in fabricating efficient LbL all‐PSCs by improving exciton utilization efficiency in acceptor layer near electrode. [ABSTRACT FROM AUTHOR]

Quasi‐2D perovskite solar cells have recently emerged as a highly prospective and inexpensive solution for sustainable energy due to their intrinsic optoelectronic properties and stability. The qualities of these promising quasi‐2D perovskite cells are generally affected by different intermediates derived from the precursor solution during film fabrication processing. However, efficient solutions to inhibit intermediates remain insufficient to date. Here, an effective strategy is prsented to inhibit the growth of 1D solvate intermediate during the fabricating process of quasi‐2D perovskite films by introducing a guanidinium thiocyanate (GUASCN) inhibitor. Theoretical calculations reveal that the SCN− anions spontaneously replace the iodide ions in the inorganic framework [PbI6]3− and induce the decomposition of the solvate intermediate. The resulted perovskite solar cells exhibit a significant improvement in power conversion efficiency (PCE), benefiting from the reduced trap‐state density and enhanced carrier mobilities. The unencapsulated devices retain 91% and 95% of the original PCEs under 45 ± 10% humidity in air or under continuous light irradiation at 100 mW cm−2 and 45 °C in a nitrogen atmosphere for 1000 h. Particularly, devices without electron‐transporting layers maintain 85% of the peak PCE under maximum power point tracking at 45 °C for 1000 h. [ABSTRACT FROM AUTHOR]

Ruddlesden–Popper phase 2D perovskite solar cells (PSCs) exhibit improved lifetime while still facing challenges such as phase alignment and up‐scaling to module‐level devices. Herein, polyelectrolytes are explored to tackle this issue. The contact between perovskite and hole‐transport layer (HTL) is important for decreasing interfacial non‐radiative recombination and scalable fabrication of uniform 2D perovskite films. Through exploring compatible butylamine cations, we first demonstrate poly(3‐(4‐carboxybutyl)thiophene‐2,5‐diyl)‐butylamine (P3CT‐BA) as an efficient HTL for 2D PSCs due to its great hydrophilicity, relatively high hole mobility and uniform surface. More importantly, the tailored P3CT‐BA has an anchoring effect and acts as the buried passivator for 2D perovskites. Consequently, a best efficiency approaching 18 % was achieved and we further first report large‐area (2×3 cm2, 5×5 cm2) 2D perovskite minimodules with an impressive efficiency of 14.81 % and 11.13 %, respectively. [ABSTRACT FROM AUTHOR]

Ruddlesden–Popper phase 2D perovskite solar cells (PSCs) exhibit improved lifetime while still facing challenges such as phase alignment and up‐scaling to module‐level devices. Herein, polyelectrolytes are explored to tackle this issue. The contact between perovskite and hole‐transport layer (HTL) is important for decreasing interfacial non‐radiative recombination and scalable fabrication of uniform 2D perovskite films. Through exploring compatible butylamine cations, we first demonstrate poly(3‐(4‐carboxybutyl)thiophene‐2,5‐diyl)‐butylamine (P3CT‐BA) as an efficient HTL for 2D PSCs due to its great hydrophilicity, relatively high hole mobility and uniform surface. More importantly, the tailored P3CT‐BA has an anchoring effect and acts as the buried passivator for 2D perovskites. Consequently, a best efficiency approaching 18 % was achieved and we further first report large‐area (2×3 cm2, 5×5 cm2) 2D perovskite minimodules with an impressive efficiency of 14.81 % and 11.13 %, respectively. [ABSTRACT FROM AUTHOR]

All‐inorganic CsPbX3 (X = Cl, Br, I, or mixed halides) perovskite quantum dots (QDs) exhibit tunable optical bandgaps and narrow emission peaks, which have received worldwide interest in the field of both photovoltaics (PVs) and light‐emitting diodes (LEDs). Herein, it is reported a discovery that CsPbI3 perovskite QD solar cell can simultaneously deliver high PV performance and intense electroluminescence. In specific, the multifunctional CsPbI3 QD film is fabricated through a simple yet efficient solid‐state‐ligand exchange process using a tailored organic ligand triphenyl phosphite (TPPI). The function of QD surface manipulation using TPPI here is proven to be twofold, balancing the carrier transport and effectively passivating the QD surface to produce conductive and emissive QD film. The CsPbI3 perovskite QD solar cell delivers a champion efficiency of 15.21% with improved open circuit voltage and high fill factor. Concurrently functioning as a red LED, the CsPbI3 perovskite QD solar cell outputs electric power to light conversion efficiency approaching 4%, a record value for QD electroluminescent PVs. The results here indicate that these versatile perovskite QDs may be a promising candidate for fabricating multifunctional optoelectronic devices. [ABSTRACT FROM AUTHOR]

The surface chemistry of colloidal quantum dots (CQD) play a crucial role in fabricating highly efficient and stable solar cells. However, as‐synthesized PbS CQDs are significantly off‐stoichiometric and contain inhomogeneously distributed S and Pb atoms at the surface, which results in undercharged Pb atoms, dangling bonds of S atoms and uncapped sites, thus causing surface trap states. Moreover, conventional ligand exchange processes cannot efficiently eliminate these undesired atom configurations and defect sites. Here, potassium triiodide (KI3) additives are combined with conventional PbX2 matrix ligands to simultaneously eliminate the undercharged Pb species and dangling S sites via reacting with molecular I2 generated from the reversible reaction KI3 ⇌ I2 + KI. Meanwhile, high surface coverage shells on PbS CQDs are built via PbX2 and KI ligands. The implementation of KI3 additives remarkably suppresses the surface trap states and enhances the device stability due to the surface chemistry optimization. The resultant solar cells achieve the best power convention efficiency of 12.1% and retain 94% of its initial efficiency under 20 h continuous operation in air, while the control devices with KI additive deliver an efficiency of 11.0% and retains 87% of their initial efficiency under the same conditions. [ABSTRACT FROM AUTHOR]

The crystalline cooperativity of the donor and acceptor segment in double‐cable conjugated polymers plays an important role in the nanophase separation and photovoltaic performance in single‐component organic solar cells (SCOSCs). Two double‐cable conjugated polymers with the same conjugated backbone and perylene bisimide (PBI) side units were designed in which PBIs were positioned symmetrically and perpendicularly (P1) and asymmetrically and slantingly (P2) along the conjugated backbones. After thermal annealing, both conjugated backbones and PBI side units in P1 tend to form ordered nanostructures, while PBI side units in P2 dominated the crystallization and hamper the crystallization of conjugated backbones. P1 showed good crystalline cooperativity between conjugated backbones and PBI side units, resulting in improved power conversion efficiencies (PCEs) up to 3.43 % in SCOSCs, while P2 with poor crystalline cooperativity exhibited PCEs below 2.42 %. [ABSTRACT FROM AUTHOR]

The crystalline cooperativity of the donor and acceptor segment in double‐cable conjugated polymers plays an important role in the nanophase separation and photovoltaic performance in single‐component organic solar cells (SCOSCs). Two double‐cable conjugated polymers with the same conjugated backbone and perylene bisimide (PBI) side units were designed in which PBIs were positioned symmetrically and perpendicularly (P1) and asymmetrically and slantingly (P2) along the conjugated backbones. After thermal annealing, both conjugated backbones and PBI side units in P1 tend to form ordered nanostructures, while PBI side units in P2 dominated the crystallization and hamper the crystallization of conjugated backbones. P1 showed good crystalline cooperativity between conjugated backbones and PBI side units, resulting in improved power conversion efficiencies (PCEs) up to 3.43 % in SCOSCs, while P2 with poor crystalline cooperativity exhibited PCEs below 2.42 %. [ABSTRACT FROM AUTHOR]

Abstract: Nonfullerene polymer solar cells (PSCs) are fabricated by using one wide bandgap donor PBDB‐T and one ultranarrow bandgap acceptor IEICO‐4F as the active layers. One medium bandgap donor PTB7‐Th is selected as the third component due to the similar highest occupied molecular orbital level compared to that of PBDB‐T and their complementary absorption spectra. The champion power conversion efficiency (PCE) of PSCs is increased from 10.25% to 11.62% via incorporating 20 wt% PTB7‐Th in donors, with enhanced short‐circuit current (JSC) of 24.14 mA cm−2 and fill factor (FF) of 65.03%. The 11.62% PCE should be the highest value for ternary nonfullerene PSCs. The main contribution of PTB7‐Th can be summarized as the improved photon harvesting and enhanced exciton utilization of PBDB‐T due to the efficient energy transfer from PBDB‐T to PTB7‐Th. Meanwhile, PTB7‐Th can also act as a regulator to adjust PBDB‐T molecular arrangement for optimizing charge transport, resulting in the enhanced FF of ternary PSCs. This experimental result may provide new insight for developing high‐performance ternary nonfullerene PSCs by selecting two well‐compatible donors with different bandgap and one ultranarrow bandgap acceptor. [ABSTRACT FROM AUTHOR]

Back Cover: Tailoring Phase Alignment and Interfaces via Polyelectrolyte Anchoring Enables Large-Area 2D Perovskite Solar Cells (Angew. 2D Perovskites, Polyelectrolytes, Ruddelsden-Popper Phase, Solar Cells The tailored polyelectrolyte has an anchoring effect and acts as a passivator for 2D perovskites, which can improve 2D perovskite phase alignment and interfacial charge transfer efficiency, and finally enables high-efficiency and large-area 2D perovskite solar cells. [Extracted from the article]

Keywords: 2D Perovskites; Polyelectrolytes; Ruddelsden-Popper Phase; Solar Cells EN 2D Perovskites Polyelectrolytes Ruddelsden-Popper Phase Solar Cells 1 1 1 09/01/22 20220905 NES 220905 B Eine Polyelektrolyt-Lochtransportschicht b für 2D-Perowskit-Solarzellen unter Verwendung eines kompatiblen Butylamin-Kations wurde von Jianyu Yuan und Mitarbeitern in ihrem Forschungsartikel untersucht (e202205111). Rücktitelbild: Tailoring Phase Alignment and Interfaces via Polyelectrolyte Anchoring Enables Large-Area 2D Perovskite Solar Cells (Angew. 2D Perovskites, Polyelectrolytes, Ruddelsden-Popper Phase, Solar Cells. [Extracted from the article]

Poly(3‐hexylthiophene) (P3HT)‐based organic solar cells (OSCs) have attracted much attention due to their advantages of low‐cost production and matured roll‐to‐roll manufacture. However, the efficiency of P3HT‐based OSCs lag much behind the non‐P3HT ones due to their negligible absorption of long wavelengths of light over 650 nm, high‐lying highest occupied molecular orbitals (HOMO), and difficulty of controlling morphology. In this study, the alkyl chains of the nonfullerene acceptors are replaced with alkoxy chains to achieve synergistic enhancement of all three parameters ( short circuit current density (JSC), open circuit voltage (VOC), and fill factor (FF)) and thus significant increase of power conversion efficiency for P3HT‐based OSCs. As a result, the OSCs exhibit a maxima efficiency of 6.6%. The P3HT‐based systems are systematically studied with optical spectroscopy, photoluminescence, cyclic voltametry, space charge limit current, grazing incident wide‐angle X‐ray scattering, transient absorption spectroscopy, transmission electron microscope, and atomic force microscopy to probe the mechanism, which reveal that introducing alkoxy chains simultaneously increases the energy levels of the HOMO and the lowest unoccupied molecular orbitals, enhances the light absorption, improves the rigidity of the backbone and charge transport mobility, and tunes the molecular orientation and film morphology, thus improving the photovoltaic performance. This contribution provides an important guidance in the design of novel nonfullerene acceptors for high‐performance P3HT‐based OSCs. Replacement of alkyl chains with alkoxyl chains of the backbone of nonfullerene acceptors successfully increases the energy levels, enhances the light absorption, and improves charge transport mobility, which simultaneously enhances three parameters (short circuit current density (JSC), open circuit voltage (VOC), and fill factor (FF)), resulting in a highest efficiency for poly(3‐hexylthiophene) (P3HT)‐based organic solar cells (OSCs) (6.6%). [ABSTRACT FROM AUTHOR]

Efficient ternary polymer solar cells (PSCs) are prepared with poly‐[4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)benzo[1,2‐b:4,5‐b′] dithiophene‐co‐3fluorothieno[3,4‐b]thiophene‐2‐carboxylate] (PTB7‐Th):COi8DFIC as host system and medium bandgap material BDTThIT‐4F as the third component. The power conversion efficiency of PSCs can be increased from 11.47% to 13.08% by incorporating 20 wt% BDTThIT‐4F in acceptors, along with the simultaneously improved three key photovoltaic parameters. The absorption edge of ternary blend films can be tilted up in long wavelength range by incorporating appropriate BDTThIT‐4F, although the bandgap of BDTThIT‐4F is wider than that of COi8DFIC, leading to the extended external quantum efficiency spectra of ternary PSCs. The tilted up absorption edge of blend films should be attributed to the variation of COi8DFIC molecular arrangement, which can be well demonstrated from the transient and steady absorption spectra of blend films with different donors and acceptors. A new ground state bleach signal can be clearly observed in transient absorption spectra of the optimized ternary blend films, which may be due to the varied COi8DFIC molecular energy levels by incorporating BDTThIT‐4F. Meanwhile, the lifetimes on excited states are increased in the ternary blend films, which is beneficial to exciton dissociation for improving the performance of ternary PSCs. Efficient ternary non‐fullerene polymer solar cells (PSCs) are fabricated with poly‐[4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)benzo[1,2‐b:4,5‐b′] dithiophene‐co‐3‐fluorothieno[3,4‐b]thiophene‐2‐carboxylate] (PTB7‐Th):COi8DFIC:BDTThIT‐4F as active layers. The power conversion efficiency is increased from 11.47% to 13.08% by incorporating 20 wt% BDTThIT‐4F in acceptors, which is attributed to the tilted up absorption edge and the optimized phase separation of ternary active layers. [ABSTRACT FROM AUTHOR]