Facilitate Carrier Transport Research Articles

Boosting thermoelectric performance of polycrystalline SnSe by controlled in-situ Ag2Se precipitates in grain boundaries

Boundary engineering has proven effective in enhancing the thermoelectric performance of materials. SnSe, known for its low thermal conductivity, has garnered significant interest; however, its application is hindered by poor electrical conductivity. Herein, the Ag8GeSe6 is introduced into the p-type polycrystalline SnSe matrix to optimize the thermoelectric performance, and the in-situ Ag2Se precipitates are formed in grain boundaries, which play dual roles, acting as an electron attraction center for improving hole concentration and a phonon scattering center for reducing lattice thermal conductivity. It effectively decouples the thermal and electrical transport properties to optimize the thermoelectric performance. Importantly, the amount of Ag2Se can be controlled by adjusting the amount of Ag8GeSe6 added to the SnSe matrix. The introduction of Ag8GeSe6 enhances electrical conductivity due to the increased hole carrier caused by the introduced Ag+ and the formed electron attraction center (in-situ Ag2Se precipitates). Based on the DFT calculations, the band gap of the Ag8GeSe6-doped samples is considerably decreased, facilitating carrier transport. As a result, the electrical transport properties increase to 808 μW m−1 K−2 at 823 K for SnSe + 0.5 wt% Ag8GeSe6. In addition, in-situ Ag2Se precipitates in grain boundaries strongly enhance phonon scattering, causing a decrease in lattice thermal conductivity. Furthermore, the presence of defects contributes to a reduction in lattice thermal conductivity. Specifically, the thermal conductivity of SnSe + 1.0 wt% Ag8GeSe6 decreases to 0.29 W m−1 K−1 at 823 K. Consequently, SnSe + 0.5 wt% Ag8GeSe6 obtains a high ZT value of 1.7 at 823 K and maintains a high average ZT value of 0.57 over the temperature range of 323−773 K. Additionally, the mechanical properties of Ag8GeSe6-doped also show an improvement. These advancements can be applied to energy supply applications during deep space exploration.

Impact of Structural Alterations from Chemical Doping on the Electrical Transport Properties of Conjugated Polymers.

Conjugated polymers (CPs) are widely used as conductive materials in various applications, with their conductive properties adjustable through chemical doping. While doping enhances the thermoelectric properties of CPs due to improved main-chain transport, overdoping can distort the polymer structure, increasing energy disorder and impeding intrinsic electrical transport. This study explored how different dopants affect the structural integrity and electrical transport properties of CPs. We found that dopants vary in their impact on CP structure, consequently altering their electrical transport capabilities. Specifically, ferric chloride (FeCl3)-doped indacenodithiophene-co-benzothiadiazole (IDTBT) shows superior electrical transport properties to triethyloxonium hexachloroantimonate (OA)-doped IDTBT due to enhanced backbone planarity and rigidity, which facilitate carrier transport and lower energetic disorder. These results highlight the critical role of dopant selection in optimizing CPs for advanced applications, suggesting that strategic dopant choices can significantly refine the charge transport characteristics of CPs, paving the way for their industrialization.

Creating electron traps in BiOBr nanosheet arrays by bulk-phase F doping to restrain carrier recombination for efficient photoelectrochemical water splitting system

Bismuth oxide semiconductors in the field of photoelectrochemical (PEC) water splitting face the problems of narrow photo response range and fast carrier compounding. On the basis of the above problems, we used a solvothermal method to prepare BiOBr nanosheet arrays (NSAs), which have a special structure that facilitates carrier transport. Subsequently, the F element was introduced into the bulk phase of BiOBr using a simple hydrothermal method. The results show that the BiOBr-F photoelectrode exhibits excellent photoelectrocatalysis performance under light and bias voltage. The photocurrent density of the BiOBr-F photoelectrode reached 28.35 μA cm−2 at 1.23 V vs. RHE, which is 2.01 times higher than that of the pure BiOBr, while a negative shift of the onset potential of 119 mV was obtained. The optical absorption tests show that the introduction of the F element forms an impurity energy level thereby extending the optical absorption range of BiOBr. Photoluminescence tests reveal that the introduction of F element effectively restricts the electron-hole pair recombination. This is due tothe fact that the F atoms replace some of the O atoms in BiOBr to create electron traps, thus forming a large number of electron-rich regions in the structure, which in turn reduces the electron-hole pair recombination. This work provides an effective solution to reduce the recombination between carriers by creating electron traps in semiconductor materials through bulk phase doping.

Surface Engineering Enables Efficient AgBiS2 Quantum Dot Solar Cells.

Surface ligand chemistry is vital to control the synthesis, diminish surface defects, and improve the electronic coupling of quantum dots (QDs) toward emerging applications in optoelectronic devices. Here, we successfully develop highly homogeneous and dispersed AgBiS2 QDs, focus on the control of interdot spacing, and substitute the long-chain ligands with ammonium iodide in solution. This results in improved electronic coupling of AgBiS2 QDs with excellent surface passivation, which greatly facilitates carrier transport within the QD films. Based on the stable AgBiS2 QD dispersion with the optimal ligand state, a homogeneous and densely packed QD film is prepared by a facile one-step coating process, delivering a champion power conversion efficiency of approximately 8% in the QD solar cells with outstanding shelf life stability. The proposed surface engineering strategy holds the potential to become a universal preprocessing step in the realm of high-performance QD optoelectronic devices.

Van der Waals mid-wavelength infrared detector linear array for room temperature passive imaging.

Passive imaging for mid-wave infrared (MWIR) is resistant to atmospheric pollutants, guaranteeing image clarity and accuracy. Arrayed photodetectors can simultaneously perform radiation sensing to improve efficiency. Room temperature van der Waals (vdWs) photodetectors without lattice matching have evolved rapidly with optimized stacking methods, primarily for single-pixel devices. The urgent need to implement arrayed devices aligns with practical demands. Here, we present an 8 by 1 black phosphorus/molybdenum sulfide (BP/MoS2) vdWs photodetector linear array with a fill-factor of ~77%, fabricated using a temperature-assisted sloping transfer method. The flat interface and uniform thickness facilitate carrier transport and minimize pixel nonuniformities, showing an average peak detectivity (D*) of 2.34 × 109 cm·Hz1/2·W-1 in the mid-wave infrared region. Compared to a single pixel, push-broom scanning passive imaging is eight times more efficient and further enhanced through mean filtering and fast Fourier transform filtering for strip noise correction. Our study offers guidance on vdWs arrayed devices for engineering applications.

Photoelectrochemical catalytic CO2 reduction enhanced by In-doped GaN and combined with vibration energy harvester driving CO2 reduction

Photoelectrochemical (PEC) technology seamlessly integrates and optimizes the merits of photocatalysis and electrocatalysis, facilitating charge separation and enhancing solar conversion efficiency. It stands out as a promising approach for CO2 treatment. GaN as III-Ⅴ semiconductor, has garnered substantial attention in the realm of PEC CO2 reduction reactions (RR). In this study, GaN and In/GaN micro-rods were prepared via straightforward hydrothermal synthesis. Attaining a current density of approximately 10 mA/cm2 and CO Faradaic Efficiency (FE) of ∼45 % at −0.75 VRHE (Reversible Hydrogen Electrode, RHE), In/GaN exhibited exceptional stability over a 2 h PEC CO2 RR. The introduction of In into GaN significantly augmented CO2 adsorption capacity and light harvesting. Additionally, Density Functional Theory (DFT) calculations elucidated that In-doped GaN can diminish the adsorption of intermediate CO, favoring subsequent CO desorption. Furthermore, the N-vacancy increased with In doping, resulting in a rise in the number of unpaired electrons, facilitating carrier transport. Herein, vibration energy harvester was introduced to drive CO2 RR, marking a significant advancement in development of PEC CO2 RR for future green energy applications.

Tailoring interfacial states for improved n-type bismuth telluride thermoelectrics

Efforts to enhance the thermoelectric (TE) efficiency of n-type bismuth telluride (BTS) have focused on leveraging 2D nanostructures, as they have been proven effective in inhibiting phonon transport and simultaneously improving electrical properties. Herein, we introduce g-C3N4 as a suitable candidate for disrupting phonon transport, with the potential to finely tune charge carrier mobility. Crucially, our investigation provides insights into the potential of externally introduced conducting states as a feasible strategy for facilitating carrier transport at heterogeneous interfaces. In contrast, the carrier scattering and localization events play an inverse role. By carefully modulating the competition, we effectively increase carrier mobility, boosting electrical conductivity and optimizing the power factor. This orchestrated strategy leads to a high figure of merit (ZT) of 1.29 at 400 K and an average ZT (ZTave) of 1.20 within 300–500 K. At temperature difference ∆T = 180 K, a maximum power output Pmax = 0.91 W and a 6.2 % conversion efficiency (η) can be achieved over the fabricated TE module. Our findings underscore the potential of 2D nanomaterials and interfacial engineering (IE) as a promising avenue for unlocking the full potential of n-type thermoelectric materials, advancing sustainable and efficient TE power generation.

Enhanced thermoelectric properties of carbon nanotubes/polyaniline fibers through engineering doping level and orientation

The rapid progress of miniaturized wearable electronics has put forward great requirements for organic fiber-based thermoelectric (TE) generators. Despite polyaniline (PANI) exhibits many outstanding attributes such as facile synthesis and low cost, as well as good environmental and thermal stability, only a few PANI-based fibers were fabricated and their TE efficiency needs to be further improved. In this work, the TE performance of wet-spun carbon nanotubes (CNTs)/PANI fibers was improved by synergistic engineering doping level of PANI and orientation of the fibers. The doping degree was optimized by varying coagulation baths, bath durations, and dopant loadings in the spinning solution, followed by fixing process during air drying to decrease shrinkage and enhance orientation of the fiber. Hexane coagulated CNTs/PANI fibers exhibited a higher doping degree of PANI compared to that of acetone and ethyl acetate, resulting in a maximum TE power factor of 77.4 μW m−1K−2 for 71 wt% CNTs/PANI fibers at PANI/dopant molar ratio of 2:1.25. Further fixing process induced a more oriented structure along the fibers, facilitating carrier transport and contributing to a significantly increased conductivity of 2155 S cm−1. Consequently, the CNTs/PANI fibers reached an optimal power factor of 91.8 μW m−1K−2. With outstanding TE performance and mechanical properties, the resultant fibers were assembled to fabricate a flexible TE generator, which generated a high output power of 2.5 nW with a temperature gradient of 10 K. These results demonstrate the potential of high-performance CNTs/PANI fibers to harvest body heat for the power supply of the wearable electronics.

Solar-Driven Conversion of CO2 to C2 Products by the 3d Transition Metal Intercalates of Layered Lead Iodides.

Photocatalytic CO2 reduction to high-value-added C2+ products presents significant challenges, which is attributed to the slow kinetics of multi-e- CO2 photoreduction and the high thermodynamic barrier for C-C coupling. Incorporating redox-active Co2+/Ni2+ cations into lead halide photocatalysts has high potentials to improve carrier transport and introduce charge polarized bimetallic sites, addressing the kinetic and thermodynamic issues, respectively. In this study, a coordination-driven synthetic strategy is developed to introduce 3d transition metals into the interlamellar region of layered organolead iodides with atomic precision. The resultant bimetallic halide hybrids exhibit selective photoreduction of CO2 to C2H5OH using H2O vapor at the evolution rates of 24.9-31.4µmol g-1h-1 and high selectivity of 89.5-93.6%, while pristine layered lead iodide yields only C1 products. Band structure calculations and photoluminescence studies indicate that the interlayer Co2+/Ni2+ species greatly contribute to the frontier orbitals and enhance exciton dissociation into free carriers, facilitating carrier transport between adjacent lead iodide layers. In addition, Bader charge distribution calculations and in situ experimental spectroscopic studies reveal that the asymmetric Ni-O-Pb bimetallic catalytic sites exhibit intrinsic charge polarization, promoting C-C coupling and leading to the formation of the key *OC-CHO intermediate.

Chemical Reaction of FA Cations Enables Efficient and Stable Perovskite Solar Cells.

Organometal halide perovskite solar cells (PSCs) have received great attention owing to a rapid increase in power conversion efficiency (PCE) over the last decade. However, the deficit of long-term stability is a major obstacle to the implementation of PSCs in commercialization. The defects in perovskite films are considered as one of the primary causes. To address this issue, isocyanic acid (HNCO) is introduced as an additive into the perovskite film, in which the added molecules form covalent bonds with FA cations via a chemical reaction. This chemical reaction gives rise to an efficient passivation on the perovskite film, resulting in an improved film quality, a suppressed non-radiation recombination, a facilitated carrier transport, and optimization of energy band levels. As a result, the HNCO-based PSCs achieve a high PCE of 24.41% with excellent storage stability both in an inert atmosphere and in air. Different from conventional passivation methods based on coordination effects, this work presents an alternative chemical reaction for defect passivation, which opens an avenue toward defect-mitigated PSCs showing enhanced performance and stability.

The stability improvement of photoelectrochemical solar cells with Bi2S3 quantum dots sensitized photoanodes

Bi2S3, Bi2MoO6 and TiO2 composite photoanodes were fabricated using three different preparation routes to improve its photoelectrochemical (PEC) stability. The microstructure of three photoanodes are distinct significantly according to the results of XRD, SEM and TEM. The ordered TiO2 nanorod arrays (NRAs) and thinner Bi2MoO6 sheet crystals in flower-ball structure facilitate carrier transport and suppresses electron-hole recombination efficiently. The results of PEC tests indicate that the photoanode with Bi2MoO6 sheet crystals in flower-ball structure and TiO2 NRAs shows significant enhancement in PEC performance stability due to its ordered microstructure facilitating carrier transport and transfer and also good adherence of photoanode layer on FTO glass substrate. This photoanode in Bi2S3 quantum dots/Bi2MoO6@TiO2 NRAs structure exhibits satisfactory properties, achieving a PEC stability of 86.41% after 48 h.

Hig‐Performance Green Quasi‐2D Perovskite Light‐Emitting Diodes via Passivated Defects

AbstractIn next generation semiconductors, metal halide perovskite materials would replace traditional light‐emitting materials since their exceptional photoelectronic characteristics. The future development of perovskite light‐emitting diodes have generated challenges such as abundant surface or interfacial defects and exciton quenching. To overcome these challenges, the light‐emitting layer is modified utilizing benzimidazole/phosphine oxide hybrid 1,3,5‐tris(1‐(4‐(diphenylphenylphosphoryl)phenyl)‐1H‐benzo[d]imidazol‐2‐yl)benzene (TPOB) and 1,3,5‐tris(diphenylphosphoryl)benzene (TPO) with high triple energy state. It is demonstrated by X‐ray photoelectron spectroscopy results that the oxygen atoms in the P = O functional group of TPOB and TPO provided lone electron pairs coordinate to the unsaturated Pb2+ in turn led to a decrease in the electron cloud density of Pb2+ and Br‐, which can suppress defects. Additionally, this technique improved the morphology of film, reduced surface roughness, and facilitated carrier transport, all of which are crucial for achieving high‐emission efficiency. As a result, the optimal devices has EQEs of 16.20 (TPOB) and 20.48% (TPO), respectively. Furthermore, the devices demonstrated excellent reproducibility. Excitingly, the champion EQE value for the optimal device is 22.64%. Simultaneously, it can increase the stability of the devices and the lifetimes are increased from 1231 s (Pristine) to 5421 (TPOB) and 5631 s (TPO).

Nonstoichiometric In–S group yielding efficient carrier transfer pathway in In2S3 photoanode for solar water oxidation

AbstractThe construction of high‐efficiency photoanodes is essential for developing outstanding photoelectrochemical (PEC) water splitting cells. Furthermore, insufficient carrier transport capabilities and sluggish surface water oxidation kinetics limit its application. Using a solvothermal annealing strategy, we prepared a nonstoichiometric In–S (NS) group on the surface of an In2S3 photoanode in situ and unexpectedly formed a type II transfer path of carrier, thereby reducing the interfacial recombination and promoting the bulk separation. First‐principles calculations and comprehensive characterizations demonstrated NS group as an excellent oxygen evolution cocatalyst (OEC) that effectively facilitated carrier transport, lowered the surface overpotential, increased the surface active site, and accelerated the surface oxygen evolution reaction kinetics by precisely altering the rate‐determining steps of * to *OH and *O to *OOH. These synergistic effects remarkably enhanced the PEC performance, with a high photocurrent density of 5.02 mA cm−2 at 1.23 V versus reversible hydrogen electrode and a negative shift in the onset potential by 310 mV. This work provides a new strategy for the in situ preparation of high‐efficiency OECs and provides ideas for constructing excellent carrier transfer and transport channels.

Electronically Manipulated Molecular Strategy Enabling Highly Efficient Tin Perovskite Photovoltaics.

Buried interface modification can effectively improve the compatibility between interfaces. Given the distinct interface selections in perovskite solar cells (PSCs), the applicability of a singular modification material remains limited. Consequently, in response to this challenge, we devised a tailored molecular strategy based on the electronic effects of specific functional groups. Therefore, we prepared three distinct silane coupling agents, and due to the varying inductive effects of these functional groups, the electronic distribution and molecular dipole moments of the coupling agents are correspondingly altered. Among them, trimethoxy (3,3,3-trifluoropropyl)-silane (F3 -TMOS), which possesses electron-withdrawing groups, generates a molecular dipole moment directed toward the hole transport layer (HTL). This approach changes the work function of the HTL, optimizes the energy level alignment, reduces the open-circuit voltage loss, and facilitates carrier transport. Furthermore, through the buffering effect of the coupling agent, the interface strain and lattice distortion caused by annealing the perovskite are reduced, enhancing the stability of the tin-based perovskite. Encouragingly, tin PSCs treated with F3 -TMOS achieved a champion efficiency of 14.67 %. This strategy provides an expedient avenue for the design of buried interface modification materials, enabling precise molecular adjustments in accordance with distinct interfacial contexts to ameliorate mismatched energetics and enhance carrier dynamics.

Electronically Manipulated Molecular Strategy Enabling Highly Efficient Tin Perovskite Photovoltaics

AbstractBuried interface modification can effectively improve the compatibility between interfaces. Given the distinct interface selections in perovskite solar cells (PSCs), the applicability of a singular modification material remains limited. Consequently, in response to this challenge, we devised a tailored molecular strategy based on the electronic effects of specific functional groups. Therefore, we prepared three distinct silane coupling agents, and due to the varying inductive effects of these functional groups, the electronic distribution and molecular dipole moments of the coupling agents are correspondingly altered. Among them, trimethoxy (3,3,3‐trifluoropropyl)‐silane (F3‐TMOS), which possesses electron‐withdrawing groups, generates a molecular dipole moment directed toward the hole transport layer (HTL). This approach changes the work function of the HTL, optimizes the energy level alignment, reduces the open‐circuit voltage loss, and facilitates carrier transport. Furthermore, through the buffering effect of the coupling agent, the interface strain and lattice distortion caused by annealing the perovskite are reduced, enhancing the stability of the tin‐based perovskite. Encouragingly, tin PSCs treated with F3‐TMOS achieved a champion efficiency of 14.67 %. This strategy provides an expedient avenue for the design of buried interface modification materials, enabling precise molecular adjustments in accordance with distinct interfacial contexts to ameliorate mismatched energetics and enhance carrier dynamics.

A regulation strategy of self-assembly molecules for achieving efficient inverted perovskite solar cells.

Self-assembled monolayers (SAMs) have been successfully employed to enhance the efficiency of inverted perovskite solar cells (PSCs) and perovskite/silicon tandem solar cells due to their facile low-temperature processing and superior device performance. Nevertheless, depositing uniform and dense SAMs with high surface coverage on metal oxide substrates remains a critical challenge. In this work, we propose a holistic strategy to construct composite hole transport layers (HTLs) by co-adsorbing mixed SAMs (MeO-2PACz and 2PACz) onto the surface of the H2O2-modified NiOx layer. The results demonstrate that the conductivity of the NiOx bulk phase is enhanced due to the H2O2 modification, thereby facilitating carrier transport. Furthermore, the hydroxyl-rich NiOx surface promotes uniform and dense adsorption of mixed SAM molecules while enhancing their anchoring stability. In addition, the energy level alignment at the interface is improved due to the utilization of mixed SAMs in an optimized ratio. Furthermore, the perovskite film crystal growth is facilitated by the uniform and dense composite HTLs. As a result, the power conversion efficiency of PSCs based on composite HTLs is boosted from 22.26% to 23.16%, along with enhanced operational stability. This work highlights the importance of designing and constructing NiOx/SAM composite HTLs as an effective strategy for enhancing both the performance and stability of inverted PSCs.

The anti-correlation effect of alkyl chain size on the photovoltaic performance of centrally extended non-fullerene acceptors.

Contrary to previous results, a unique anti-correlation effect of the alkyl chain size on the photovoltaic performance of acceptors was observed. For a centrally-extended acceptor, replacing linear alkyl chains (n-undecyl for CH-BBQ) on the thienothiophene unit with branched ones (2-butyloctyl for CH-BO) leads to a plunge in the power conversion efficiency of organic solar cells (18.12% vs. 11.34% for binary devices), while the largely shortened ones (n-heptyl for CH-HP) bring a surge in performance (18.74%/19.44% for binary/ternary devices). Compared with CH-BO, the more compact intermolecular packing of CH-HP facilitates carrier transport. The characterization of organic field effect transistors and carrier dynamics also echoes the above results. Molecular dynamics simulations indicate that the encounter of the branched alkyl chains and the extended central core hinders the effective interfacial interaction of polymer donors and acceptors, thus deteriorating the device performance. This work suggests that the conventional strategy for alkyl chain engineering of Y-series acceptors might need to be reconsidered in other molecular systems.

Highly stable and sensitive photoelectrochemical photodetectors based on a ZnO nanorod/monolayer MoS2 nanosheets heterostructure

Construction of type-II heterostructures between metal oxide nanorod arrays and narrow band gap semiconductors is a proven strategy for enlarging the surface area, shortening the diffusion length, broadening the light harvesting ability, and facilitating carrier transport, which are of great significance for photoelectrochemical (PEC) photodetectors. A ZnO/MoS2 heterostructure was designed and fabricated via a facile hydrothermal process accompanied by chemical vapor deposition method. The ZnO nanorod/monolayer MoS2 nanosheet heterostructure was revealed with scanning electron microscopy, transmission electron microscopy, and Raman spectroscopy. These heterojunction-based PEC photodetectors showed higher photoresponsivity (4.2 mA/W) than those of ZnO (∼0.9 mA/W) and MoS2 photodetectors (∼0.007 mA/W) due to its fast interfacial charge transfer and efficient light capture. Furthermore, the ZnO/MoS2 heterostructural photodetectors exhibited a maximum photoresponsivity of approximately 5.0 mA/W at 420 nm and long-term stability even over 6 h. Our work paves the way to rationally designed heterostructures for high-performance and stable photodetectors and beyond.

(Poster Award - 1st Place) Emerging Effect of Vertical-Oriented WSe2 Interfacial Layers in the CIGSe Thin Film Solar Cells

Copper indium gallium selenide (CIGSe) thin film solar cells become popular due to their potential as a solution for green energy and space technology recently. These solar cells have a similar electrical performance to traditional silicon solar cells, making them ideal for light, flexible, and high-performance applications. Molybdenum is a popular material for the rear electrode due to its conductivity and low cost. During the selenizing process of the absorber layer, MoSe2 will be formed between Mo and CIGSe layer, which improves adhesion between Mo and CIGSe and facilitates carrier transport from the absorber layer to the rear electrode. Therefore, previous studies show that oxides or nitride-based materials, such as Titanium Nitride and Alumina, are used as the passivation layer at the back contact to address the trade-off of the critical thickness of the MoSe2 layer. That is, designing a nanostructure and creating a contact hole can attract carriers and avoid current blocking. Similarly, Oxide-based material interfacial layers, such as Molybdenum oxide and tungsten oxide, can also play a role in the obstacle of selenium diffusion and modify the band structure. In this work, a few layers of WSe2 interfacial layer were introduced between the CIGSe absorber layer and Mo electrode. First, 20 nm WOx was deposited on Mo by E-beam evaporation. Second, WOx was selenized by a vertical furnace with ICP coils plasma system to form WSe2. By tuning the substrate temperature of plasma-enhanced selenization process, the full vertically lamellar-oriented WSe2 was formed on Mo. The results show that inserting a few layers of WSe2 improved the efficiency of the CIGS solar cell from 12.5 to 14.3%, with a significant increase in short circuit current density up to 38mA/cm2. This improvement was attributed to the improved carrier transportation through the backside interface, facilitated by the specific vertically lamellar-orientated WSe2 and the induced Gallium gradient measured by TEM, SIMS, and XPS. The remarkable enhancement by WSe2 provides the potential for further applications. Figure 1

Dual Role of Rapid Transport and Efficient Passivation in Inverted Methylammonium‐Free Perovskite Solar Cells Utilizing a Self‐Assembled Porous Insulating Layer

AbstractIn recent years, the surface modification of perovskite by wide band‐gap insulating materials has been one of the main strategies to achieve efficient and stable perovskite solar cells (PSCs). Unfortunately, a significant hurdle in this approach is the dilemma surrounding the quality of passivation and the transport of charges. Here, this trade‐off is overcome by introducing self‐assembled diphenylphosphinic acid (DPPA) porous layer. Applying highly concentrated DPPA solution on the perovskite surface not only provides excellent passivation of entire surface, but also the excess DPPA will form a self‐assembled porous insulating layer (PIL), which forms random submicron‐sized openings at the interface of the insulating layer for accelerated charge transport. In addition, the energy level of the perovskite surface can be modulated by this insulating material to facilitate carrier transport. As a result, an impressive power conversion efficiency (PCE) over 24% has been achieved in methylammonium‐free p‐i‐n devices with an ultrahigh fill factor (FF) of 84.7%. The unencapsulated devices exhibit excellent thermal and operational stability. This work paves a way for establishment of an effective passivation and facilitated transport simultaneously.