Energy Level Alignment Research Articles

Zwitterion additive-assisted crystal growth regulation and defect passivation for high-performance inorganic perovskite solar cells

Inorganic CsPbI2Br perovskites solar cells (PSCs) have attracted extensive interest owing to their outstanding optoelectronic properties. Nevertheless, the undesirable perovskite film quality and severe charge recombination dramatically restrict their performance improvement. Herein, we propose an additive strategy to modulate the CsPbI2Br crystallization process and reduce the defect density by adding 3-(1-pyridinio)-1-propanesulfonate (PPS) zwitterionic molecules into the perovskite precursor solution. The incorporation of PPS zwitterion can not only retard the crystal growth rate of CsPbI2Br with uniform morphology and enlarged grain size, but also effectively passivate defects via interacting with the uncoordinated sites in the perovskite film. In addition, the PPS zwitterion greatly ameliorates the energy level alignments at the interface. Thus, the photogenerated carriers are more efficiently extracted, and the nonradiative recombination is significantly suppressed. With these benefits, the optimized PPS-based CsPbI2Br device delivers a champion efficiency of 16.37% with high open-circuit voltage (VOC) of 1.302 V in contrast to the pristine device with an inferior efficiency of 14.26% (VOC of 1.183 V). In addition, the unencapsulated device with PPS presents improved long-term stability by preserving ∼85% of the initial efficiency after 760 h storage in ambient atmosphere. These findings provided important insights into the additive strategy of using zwitterionic materials for constructing efficient and stable inorganic PSCs.

PCBM Constructing Heterojunction for Efficient CsPbI3 Perovskite Quantum Dot Solar Cells.

CsPbI3 perovskite quantum dots (PQDs) have emerged as promising photovoltaic materials for third-generation solar cells, owing to their superior optoelectronic properties. Nevertheless, the performance of CsPbI3 PQD solar cells is primarily hindered by low carrier extraction efficiency, largely due to the insulative ligands. In this study, we introduced a semiconductor molecule, [6,6]-phenyl C61 butyric acid methyl ester (PCBM), onto the surfaces of CsPbI3 PQDs as surface ligands to enhance photogenerated charge extraction. The results indicate that PCBM accelerates carrier separation in CsPbI3 PQDs by forming a type II heterojunction, and also modulates the energy level of CsPbI3 PQDs by altering surface dipole moments. Additionally, we established an energy-level gradient alignment in the PCBM/CsPbI3 PQD heterojunction absorber layer, which was found to effectively promote carrier extraction and reduce carrier recombination loss in PQD solar cells. Ultimately, the PQD solar cells incorporating this novel structure achieved a power conversion efficiency of 14.23%, a significant improvement compared to 12.69% achieved by solar cells with a traditional structure, thus demonstrating the strong potential of this approach for high-performance PQD solar cells.

Highly Efficient and Stable Perovskite Solar Cells by Introducing a Multifunctional Surface Modulator

Simultaneously passivating the perovskite surface defects (VI, Pbi) and suppressing Li+ ions diffusion of hole transport layer (HTL) are still challenging issues. Herein, we report an effective “ three birds with one stone ” strategy by utilizing sodium 4,4'‐(1,4‐phenylenebis(oxy))bis(butane‐1‐sulfonate) (ZR3) containing sulfonic acid groups (SO3−) and Na+ ions as a multifunctional surface treatment modulator to simultaneously address the above issues. It is found that ZR3 is not only capable of passivating the Pb‐related defects at the surface of perovskite by the SO3‐ group, but also possesses the remarkable ability to passivate the halide defects with Na+ ions. Meanwhile, ZR3 treatment enables the enhanced exciton dissociation of perovskite, better energy level alignment with hole transport layer (HTL), improved hole extraction/transfer from perovskite layer into HTL, and reduced charge carrier recombination in device. Therefore, it results in the enhanced power conversion efficiency (PCE) of 25.34% in ZR3‐based n‐i‐p device from 22.97% for the control device. Specifically, p‐i‐n PSCs with ZR3 also achieves an improved PCE of 25.96% with respect to the pristine one (23.99%), proving the universality of ZR3 for PSCs. Moreover, the stabilities of ZR3‐treated devices are significantly enhanced owing to Li+ ions migration suppressing and perovskite defects reduction.

Highly Efficient and Stable Perovskite Solar Cells by Introducing a Multifunctional Surface Modulator.

Simultaneously passivating the perovskite surface defects (VI, Pbi) and suppressing Li+ ions diffusion of hole transport layer (HTL) are still challenging issues. Herein, we report an effective " three birds with one stone " strategy by utilizing sodium 4,4'-(1,4-phenylenebis(oxy))bis(butane-1-sulfonate) (ZR3) containing sulfonic acid groups (SO3-) and Na+ ions as a multifunctional surface treatment modulator to simultaneously address the above issues. It is found that ZR3 is not only capable of passivating the Pb-related defects at the surface of perovskite by the SO3- group, but also possesses the remarkable ability to passivate the halide defects with Na+ ions. Meanwhile, ZR3 treatment enables the enhanced exciton dissociation of perovskite, better energy level alignment with hole transport layer (HTL), improved hole extraction/transfer from perovskite layer into HTL, and reduced charge carrier recombination in device. Therefore, it results in the enhanced power conversion efficiency (PCE) of 25.34% in ZR3-based n-i-p device from 22.97% for the control device. Specifically, p-i-n PSCs with ZR3 also achieves an improved PCE of 25.96% with respect to the pristine one (23.99%), proving the universality of ZR3 for PSCs. Moreover, the stabilities of ZR3-treated devices are significantly enhanced owing to Li+ ions migration suppressing and perovskite defects reduction.

Fluorination Strategy for Benzimidazole Core Based Electron Acceptors Achieving over 19% Efficiency for Ternary Organic Solar Cells.

The expansion of two-dimensional conjugated systems in nonfullerene electron acceptors (NFAs) has significantly advanced the molecular design and efficiency potential of organic solar cells (OSCs). This study introduces a novel class of NFAs featuring a benzimidazole core with varying degrees of peripheral fluorination, designated as YIS-4F, YIS-6F, and YIS-8F, respectively. Through systematic modulation of fluorine content, we observed that OSCs incorporating YIS-6F achieved the highest power conversion efficiency (PCE) of 17.28%, surpassing those with YIS-4F and YIS-8F. Notably, the incorporation of YIS-6F in a ternary blend with D18/N3 yielded a remarkable PCE of 19.43%. The enhanced performance of YIS-6F-based devices is attributed to the optimized energy level alignment and optimized crystallinity, which collectively facilitate efficient exciton dissociation, accelerated charge transport, and minimized charge recombination, culminating in an exceptional fill factor and PCE. Our findings underscore the pivotal role of fluorination of NFAs at the central benzimidazole core in optimizing molecular packing, and consequently enhancing the performance of OSCs.

Enhancing FAPbI3 Perovskite Solar Cell Performance and Stability Through Bespoke Graphene Quantum Dots

ABSTRACTA novel approach to enhancing the efficiency and long‐term stability of perovskite solar cells (PSCs) is presented through strategic interfacial modification using bespoke graphene quantum dots (GQDs). GQDs with controlled alkylamine chain lengths, such as butylamine (C4), octylamine (C8), and dodecylamine (C12), were customized to have the proper optical and electronic properties toward specific interfaces within the PSCs. The incorporation of C4‐GQDs significantly improved the energy level alignment and conductivity of the SnO2 electron transport layer (ETL), while C12‐GQDs effectively reduced trap density on the perovskite surface, leading to enhanced defect passivation. These modifications resulted in a substantial increase in power conversion efficiency of 24.41% in a unit cell and 18.91% in a mini‐module, respectively. Notably, the maximum power point tracked perovskite mini‐module retained 89% of its initial efficiency during 1000 h of continuous light soaking condition at 25°C under 35% relative humidity. This work highlights the potential of bespoke GQDs to advance both the performance and durability of PSCs, providing a scalable approach for future photovoltaic applications. image

Construction of ultra-smooth and void-free buried interface via bilateral chemical bridging for efficient and hysteresis-suppressed perovskite solar cells

The surface properties are vital aspects in improving photovoltaic performance of perovskite solar cells (PSCs). Except for the upper surface of perovskite, the hidden buried interface which supports the beginning of perovskite film crystallization is of equal great importance for the construction of high-efficiency PSCs. Herein, we use urea phosphate (UPP) to build a bilateral chemical bridge in the buried interface under perovskite layer, to simultaneously improve the properties of SnO2 ETL and the upper perovskite. On one hand, the interaction between UPP and SnO2 passivates the defects of the SnO2 and facilitates the formation of ultra-smooth surface for superior interfacial contact. On the other hand, the chemical interaction between UPP and perovskite contributes to the optimization of crystal nucleation and growth, which improves the crystalline quality of perovskite, inhibits the formation of voids at the buried interface and reduces the defects of the grain boundary. Benefiting from the optimized buried interfacial contact, suppressed defects, accelerated charge extraction and modified energy level alignment, the UPP-processed device delivers an improved power conversion efficiency of 24.54 %, with effective suppression of hysteresis. Moreover, the stability of device is also improved owing to the reduction of trap defects. This work provides a feasible strategy to tune the buried interface between the charge transfer layer and perovskite layer for fabrication of efficient and stable PSCs.

Bridged Carbolong Modulating Interfacial Charge Transfer Enhancement for High-Performance Inverted Perovskite Solar Cells.

Efficient regulation of perovskite/C60 interface is crucial to improving the long-term stability of the inverted perovskite solar cells (PSCs). However, precise methods for controlling the perovskite/C60 interface have yet to be thoroughly explored. Herein, we develop a carbolong chemical manipulation strategy to improve the interface contact of perovskite/C60 due to versatile functional groups and excellent optoelectronic properties of carbolong metallaaromatics. And constructing an electron-transfer bridge enhances the interfacial interaction and accelerates interfacial electron transfer. The carbolong manipulation results in optimized energy level alignment, suppressed nonradiative recombination, and improved electronic contact. An impressive efficiency of 25.80% is demonstrated, with open-circuit voltage and fill factor of 1.19 V and 84.53%, respectively. The unsealed devices retain more than 98% of their original efficiency after 1400 h of maximum power point tracking under illumination and demonstrate remarkable thermal stability, maintaining 93% of their initial efficiency after 2500 h at 85°C in a nitrogen atmosphere. And the encapsulated carbolong-modified module achieved a high efficiency of 20.72% (active area of 25.25 cm²) with robust operation stability.

Tuning the morphology and energy levels in organic solar cells with metal–organic framework nanosheets

Metal–organic framework nanosheets (MONs) have proved themselves to be useful additives for enhancing the performance of a variety of thin film solar cell devices. However, to date only isolated examples have been reported. In this work we take advantage of the modular structure of MONs in order to resolve the effect of their different structural and optoelectronic features on the performance of organic photovoltaic (OPV) devices. Three different MONs were synthesized using different combinations of two porphyrin-based ligands meso-tetracarboxyphenyl porphyrin (TCPP) or tetrapyridyl-porphyrin (TPyP) with either zinc and/or copper ions and the effect of their addition to polythiophene-fullerene (P3HT-PC71BM) OPV devices was investigated. The power conversion efficiency (PCE) of devices was found to approximately double with the addition of MONs of Zn2(ZnTCPP) -4.7% PCE, 10.45 mA/cm2 short-circuit current density (JSC), 0.69 open-circuit voltage (VOC), 64.20% fill-factor (FF), but was unchanged with the addition of Cu2(ZnTPyP) (2.6% PCE, 3.68 mA/cm2JSC, 0.59 VOC, 46.27% FF) and halved upon the addition of Cu2(CuTCPP) (1.24% PCE, 6.72 mA/cm2JSC, 0.59 VOC, 56.24% FF) compared to devices without nanosheets (2.6% PCE, 6.61 mA/cm2JSC, 0.58 VOC, 56.64% FF). Our analysis indicates that there are three different mechanisms by which MONs can influence the photoactive layer – light absorption, energy level alignment, and morphological changes. Analysis of external quantum efficiency, UV–vis and photoelectron spectroscopy data found that MONs have similar effects on light absorption and energy level alignment. However, atomic force and Raman microscopy studies revealed that the nanosheet thickness and lateral size are crucial parameters in enabling the MONs to act as beneficial additives resulting in an improvement of the OPV device performance. We anticipate this study will aid in the design of MONs and other 2D materials for future use in other light harvesting and emitting devices.

Enhanced Hole-Injecting Interface for High-Performance Deep-Blue Perovskite Light-Emitting Diodes Using Dipole-Controlled Self-Assembled Monolayers.

The Blue electroluminescence (EL) with high brightness and spectral stability is imperative for full-color perovskite display technologies meeting the Rec. 2020 standard. However, deep-blue perovskite light-emitting diodes (PeLEDs) lag behind their green- or red-emitting counterparts in brightness, quantum efficiency, and operational stability. Additionally, the Cl-/Br- mixed-halide perovskites with wide bandgap typically designed for deep-blue emitters are prone to degradation quickly under high operating bias due to low energy for halide migrations and vacancies formation, posing a significant challenge to spectral/operative stabilities. To address these issues, high-performance deep-blue PeLEDs are demonstrated by tuning the interface properties with Br-2ETP, a self-assembled monolayer (SAM) molecule engineered for a high dipole moment. The Br-2EPT-based hole-injecting interface facilitates favorable energy level alignment between indium tin oxide and the deep-lying valence band of the perovskite layer, suppressing the hole-injecting barrier and non-radiative charge recombination. Excellent perovskite film morphologies are observed at the top and buried surfaces by Br-2EPT, improving the balance of carrier injection for light emission efficiency. Consequently, the devices exhibit deep-blue electroluminescence at 457nm, with an external quantum efficiency of 6.56% and spectral/operative stabilities.

Planar Structure of Organic Photodetector for Low Dark Current

Abstract The focus of this study is on investigating the vanadyl 2,9,16,23-tetraphenoxy-29H,31H-phthalocyanine (VOPcPhO) and its blend with o-xylenyl C60 bis-adduct (OXCBA), for use as a lateral ultraviolet organic photodetector. The research focuses on improving dark current reduction, which is a challenge in lateral organic photodetector. By integrating the OXCBA, low dark current values of 4.83 nAcm-2 (D shot * = 1.414 × 1011 Jones) have been achieved as compared to the stand-alone VoPcPhO device of 14.06 nAcm-2. The major contributing factors to dark current reduction are due to the efficient charge transfer at the photoactive-electrode interface, the deep highest occupied molecular orbital (HOMO) level of OXCBA, which leads to favourable energy level alignments hindering hole injection, and the occurrence of bulk heterojunction vertical phase segregation between VOPcPhO and OXCBA. These findings shed light on the relationship between the organic photoconductor's material composition, morphology, and performance metrics and open new avenues for metal phthalocyanine-based lateral ultraviolet organic photodetectors with low dark current and enhanced performance.

Energy Level Alignment Regulation and Carrier Management in Perovskite Solar Cells with Various Bandgaps Using Tailored Metal‐Organic Frameworks

Energy Level Alignment Regulation and Carrier Management in Perovskite Solar Cells with Various Bandgaps Using Tailored Metal‐Organic Frameworks

Reconstruction of Hole Transport Layer via Co‐Self‐Assembled Molecules for High‐Performance Inverted Perovskite Solar Cells

AbstractAdjusting the hole transport layer (HTL) to optimize its interface with perovskite is crucial for minimizing interface recombination, enhancing carrier extraction, and achieving efficient and stable inverted perovskite solar cells (PSCs). However, as a commonly used HTL, the self‐assemble layer (SAM) of [2‐(3,6‐dimethoxy‐9H‐carbazol‐9‐yl)ethyl] phosphonic acid (MeO‐2PACz) tends to form clusters and micelles during the deposition process, leading to inadequate coverage of the ITO substrate. Here, a Co‐SAM strategy is employed by incorporating 4‐mercaptobenzoic acid (SBA) and 4‐trifluoromethyl benzoic acid (TBA) as additives into MeO‐2PACz to fabricate a Co‐SAM‐based HTL. The introduced additive can interact with MeO‐2PACz, facilitating cluster dispersion and thereby enabling better deposition on ITO for improved HTL coverage. Moreover, Co‐SAM exhibits superior energy level alignment with perovskite to enhance interfacial contact and improve carrier extraction efficiency as well as promote growth of bottom perovskite grains. As a result, an impressive increase of the power conversion efficiency (PCE) from 21.34% to 23.31% is achieved in the inverted device based on the Co‐SAM HTL of MeO‐2PACz+TBA while maintaining ≈90% of its initial efficiency under continuous operation at 1‐sun.

Stable Surface Contact with Tailored Alkylamine Pyridine Derivatives for High-Performance Inverted Perovskite Solar Cells.

Formamidinium-cesium lead triiodide (FA1-xCsxPbI3) perovskite holds great promise for perovskite solar cells (PSCs) with both high efficiency and stability. However, the defective perovskite surfaces induced by defects and residual tensile strain largely limit the photovoltaic performance of the corresponding devices. Here, the passivation capability of alkylamine-modified pyridine derivatives for the surface defects of FA1-xCsxPbI3 perovskite is systematically studied. Among the studied surface passivators, 3-(2-aminoethyl)pyridine (3-PyEA) with the suitable size is demonstrated to be the most effective in reducing surface iodine impurities and defects (VI and I2) through its strong coordination with Npyridine. Additionally, the tail amino group (─NH2) from 3-PyEA can react with FA+ cations to reduce the surface roughness of perovskite films, and the reaction products can also passivate FA vacancies (VFA), and further strengthen their binding interaction to perovskite surfaces. These merits lead to suppressed nonradiative recombination loss, the release of residual tensile stress for the perovskite films, and a favorable energy-level alignment at the perovskite/[6,6]-phenyl-C61-butyric acid methyl ester interface. Consequently, the resulting inverted FA1-xCsxPbI3 PSCs obtain an impressive power conversion efficiency (PCE) of 25.65% (certified 25.45%, certified steady-state efficiency 25.06%), along with retaining 96.5% of the initial PCE after 1800 h of 1-sun operation at 55 °C in air.

Heterojunction interface engineering enabling high transmittance and record efficiency in Sb2S3 semitransparent solar cell

Antimony sulfide (Sb2S3) is an auspicious contender for semitransparent and tandem solar cells owing to its exceptional optoelectronic characteristics. Yet, complex bulk and heterojunction defects hinder achieving optimal power conversion efficiency (PCE). Although CdS is an established electron transport layer (ETL) in Sb-chalcogenide solar cells benefitting from its exceptional electron mobility (350 cm2V–1s−1) and energy level alignments, its potential contribution has been deplorably overlooked in Sb2S3 semitransparent photovoltaics (STPV). Herein, an optimized TiO2/CdS double ETL strategy is embraced to counteract CdS absorption loss and mitigate the “deep cliff” conduction band off-set at TiO2/Sb2S3 heterojunction. Subsequently, an evolved chemical bath deposition strategy is proposed to deposit a uniform, faster, and comparatively more transparent Sb2S3 absorber layer. A systematic investigation of the absorber layer and in-depth analysis of carrier dynamics at heterojunctions advocate for the mitigation of charge accumulation and recombination at the interface, thereby pledging superior carrier transport. The advantageous gradient energy band alignment of TiO2/CdS/Sb2S3 realized a record PCE of 5.61 % for STPV. Furthermore, the semitransparent device is innovatively employed as a window, enabling transmitted light to be harvested by subsequent Sb2S3 solar cells. It maintains 18 % of its standalone PCE, thereby setting new benchmarks for its practical submissions.

A Stepwise Melting-Polymerizing Molecule for Hydrophobic Grain-Scale Encapsulated Perovskite Solar Cell.

Despite the ongoing increase in the efficiency of perovskite solar cells, the stability issues of perovskite have been a significant hindrance to its commercialization. In response to this challenge, a stepwise melting-polymerizing molecule (SMPM) is designed as an additive into FAPbI3 perovskite. SMPM undergoes a three-stage phase transition during the perovskite annealing process: initially melting from solid to liquid state, followed by overflowing grain boundaries, and finally self-polymerizing to form a hydrophobic grain-scale encapsulation in perovskite solar cells, providing protection against humidity-induced degradation. With this unique property, coupled with the advantages of improved crystallization, diminished non-radiative recombination, and energy level alignment, FAPbI3-based perovskite solar cells with a 25.21% (small-area) and 22.94% (1 cm2) power conversion efficiency and over 2000 h T95% stability under 85% relative humidity is achieved. Furthermore, the SMPM-based perovskite solar cells without external encapsulations sustain impressive stability during underwater operation, in which the black FAPbI3 phase is maintained and Pb-leakage is also effectively suppressed. Therefore, the SMPM strategy can offer a sustainable settlement in both stability and environmental issues for the commercialization of perovskite solar cells.

Light‐Emitting Perovskite Solar Cells: Genesis to Recent Drifts

Perovskite, a star material with extraordinary opto‐electronic properties has shown promising results in both perovskite solar cells (PSCs) and perovskite light‐emitting diodes (PeLEDs). Taking advantage of the similar configuration of PSCs and PeLEDs, next generation devices with dual functionality of light‐harvesting and light‐emission can be realized. Such devices hold enormous application prospects. However, the necessary tradeoff resulted from the opposite working principles required for each mode of operation and challenges such as non‐radiative recombination loss resulted from bulk and surface defects in perovskite films and mismatched energy levels have hindered mass production. To provide a roadmap for rationally designing efficient light emitting perovskite solar cells (LEPSCs), a comprehensive review focusing on operating principle, device architecture, recent developments and limitations is required. We begin with a brief overview of the basic principles underlying the working mechanism of LEPSCs such as photon to electricity conversion and viceversa. The focus of this review then shift towards deligently combining and overviewing the important breakthroughs reported in this newly developed field such as morphology optimization, defect passivation, interface engineering, energy level alignment and dimensional control. Finally, this work concludes with discussing future challenges and providing a roadmap for rational design of efficient and stable LEPSCs.

Suppressing the Dark Current Under Forward Bias for Dual‐Mode Organic Photodiodes

AbstractTremendous research efforts are developed to suppress the reverse dark current (Jd) and enhance the responsivity of organic photodiodes (OPDs). The functional layers of traditional OPDs usually follow the principle of energy level alignment to make unobstructed photo‐carriers transport under reverse bias, but this inevitably leads to a large forward Jd. Herein, a universal strategy is proposed to manipulate the carrier dynamics and effectively suppress the forward Jd of OPDs, that is, tuning the energy level and electron traps of the anode interface layers (AILs). The bandgap and electron traps of typical organometallic chelate AIL (PEIE‐Co) can be well controlled by adjusting the component ratio of PEIE and metal ions. The wide bandgap increases the carrier injection barrier under reverse and forward bias, endowing OPD with a much lower Jd; the electron traps induce hole tunneling injection by capturing photo‐generated electrons under forward bias, thereby enabling the photomultiplication effect. The obtained OPD exhibits photoconductive/photomultiplication working mode at reverse/forward bias and the specific detectivity approaches ≈1013/1012 Jones, showing promise for adaptively detecting faint and strong light. This study presents an intelligent strategy to achieve dual‐mode OPDs, paving the way for the multifunctional development of photodetectors.

In-Device Ballistic-Electron-Emission Spectroscopy for Accurately In Situ Mapping Energy Level Alignment at Metal-Organic Semiconductors Interface.

Energy level alignment at metal/organic semiconductors (OSCs) interface governs electronic processes in organic electronics devices, making its precise determination essential for understanding carrier transport behaviors and optimizing device performance. However, it is proven that accurately characterizing the energy barrier at metal/OSC interface under operational conditions remains challenging due to the technical limitations of traditional methods. Herein, through integrating highly-improved device constructions with an ingenious derivative-assisted data processing method, this study demonstrates an in-device ballistic-electron-emission spectroscopy using hot-electron transistors to accurately characterize the energy barrier at metal/OSC interface under in-operando conditions. This technique is found that a remarkable improvement in measurement accuracy, reaching up to ±0.03eV, can be achieved-surpassing previous techniques (±0.1-0.2eV). The high accuracy allows us to monitor subtle changes in energy barriers at metal/OSC interface caused by variations in the aggregation state of OSCs, a phenomenon that is theoretically possible but failed to be directly demonstrated through conventional methods. Moreover, this study makes demonstration that this technology is universally applicable to various metal/OSC interfaces consisting of electron-transporting, hole-transporting, and ambipolar OSCs. These findings manifest the great potential of this method to advance both theoretical exploration and technical applications in organic electronics.

Boosting Carrier Transport in Quasi-2D/3D Perovskite Heterojunction for High-Performance Perovskite/Organic Tandems.

Wide-bandgap (WBG) perovskites are continuously in the limelight owing to their applicability in tandem solar cells. The main bottlenecks of WBG perovskites are interfacial non-radiative recombination and carrier transport loss caused by interfacial defects and large energy-level offsets, which induce additional energy losses when WBG perovskites are stacked with organic solar cells in series because of unbalanced carrier recombination in interconnecting layer (ICL). To solve these issues, 1,3-propanediammonium iodide (PDADI) is incorporated to form Dion-Jacobson -phase quasi-2D perovskites with mixed high-n-values in WBG perovskites. PDADI simultaneously repairs the shallow/deep defects and establishes a Type-II energy-level alignment between quasi-2D/3D and 3D perovskites for rapid carrier extraction. More importantly, the short-chain diammonium cation in quasi-2D perovskite with high n-values results in a short Pb-I inorganic layer spacing, which enhances the interlayer electronic coupling and weakens the quantum-well confinement effect that restricts carrier transport. The suppressed transport loss increases the electron concentration in the ICL for balanced carrier recombination. The 0.0628 and 1.004 cm2 perovskite/organic tandems achieve remarkable efficiencies of 25.92% and 24.63%, respectively. The quasi-2D capping layer can inhibit ion migration, allowing perovskite/organic tandems to show excellent operational stability (T85 >1000h).