Search

Interfacial defects between perovskite and adjacent charge transport layers present a significant obstacle, hindering the enhancement of power conversion efficiency (PCE) and stability in perovskite solar cells (PSCs). To address this challenge, a dual‐interface modification is proposed to aim at improving the performance of mixed‐halide PSCs. Specifically, the hole‐collecting side is modified with 5‐Aminopyridine‐2‐carboxylic Acid (APC), while the electron‐collecting side is modified with 2‐thiopheneethylammonium chloride (TEACl). The multifunctional APC enhances charge transfer by tailoring the interface between the perovskite and poly(triarylamine) (PTAA) through multiple bonding interactions, thereby suppressing interfacial nonradiative recombination. Density functional theory studies reveal that APC on the perovskite surface induces uniform adsorption energy, promoting homogenous crystallization without residual stress. Additionally, APC interlayer eliminates the localized edge states induced by the iodine vacancies near the conduction band edge. Further improvement in the device performance is achieved by passivating the top perovskite surface with TEACl, leading to well‐matched energy bands and reduced vacancy trap states. As a result, champion cell achieves a PCE of 24.87% with an open‐circuit voltage of 1.188 V. Furthermore, The dual‐interface modification improves thermal stability due to enhanced ion‐migration activation energy. [ABSTRACT FROM AUTHOR]

Herein, we synthesized two donor‐acceptor (D‐A) type small organic molecules with self‐assembly properties, namely MPA‐BT‐BA and MPA‐2FBT‐BA, both containing a low acidity anchoring group, benzoic acid. After systematically investigation, it is found that, with the fluorination, the MPA‐2FBT‐BA demonstrates a lower highest occupied molecular orbital (HOMO) energy level, higher hole mobility, higher hydrophobicity and stronger interaction with the perovskite layer than that of MPA‐BT‐BA. As a result, the device based‐on MPA‐2FBT‐BA displays a better crystallization and morphology of perovskite layer with larger grain size and less non‐radiative recombination. Consequently, the device using MPA‐2FBT‐BA as hole transport material achieved the power conversion efficiency (PCE) of 20.32 % and remarkable stability. After being kept in an N2 glove box for 116 days, the unsealed PSCs' device retained 93 % of its initial PCE. Even exposed to air with a relative humidity range of 30±5 % for 43 days, its PCE remained above 91 % of its initial condition. This study highlights the vital importance of the fluorination strategy combined with a low acidity anchoring group in SAMs, offering a pathway to achieve efficient and stable PSCs. [ABSTRACT FROM AUTHOR]

Metal–organic framework (MOF)–derived materials have been extensively studied for water splitting applications; however, their direct utilization suffers from the limited activity. Herein, atom doping strategy is demonstrated to activate the electrocatalysis performance of nickel foam–supported Co-BDC (BDC: terephthalic acid) MOF by introducing Ir dopants. It is found that Ir doping induces benefits of modulated electronic structure, enhanced catalysis kinetics and charge transfer, and more catalysis sites for electrocatalysis. The prepared CoIr-BDC exhibits impressive activities for oxygen evolution in alkaline media (308 mV at a current density of 100 mA cm−2) and hydrogen evolution in all pH conditions (overpotentials of 90, 140, and 226 mV in acidic, alkaline, and neutral solutions at 100 mA cm−2). For overall electrolysis, the alkaline electrolyzer with CoIr-BDC as bifunctional catalysts delivers low voltage of 1.89 V at 400 mA cm−2. This study provides insight to boost the catalysis activity of MOF materials by incorporating metal atoms. [ABSTRACT FROM AUTHOR]

Multicomponent metal selenides with heterostructures are believed to effectively activate the surface pseudocapacitive contribution and improve the electrochemical dynamics, thus achieving high-performance anodes for sodium ion batteries (SIBs). Herein, a carbon coated CoSe2/Sb2Se3 heterojunction (CoSe2/Sb2Se3@C) is designed and constructed via an ion-exchange reaction between Co and Sb, and the subsequent selenization step. It is found that the hetero-structure and carbon shell effectively boost the charge transfer in the CoSe2/Sb2Se3@C composite electrode. The highly pseudocapacitive Na+ storage contribution is acquired due to the structural benefits of the heterojunction. Therefore, the CoSe2/Sb2Se3@C anode affords good cycling stability (264.5 mA h g−1 after 1000 cycles at 2 A g−1) and excellent rate capability (266.0 mA h g−1 at 5 A g−1). This study supplies a reference for developing an advanced anode with multicomponent and heterojunction structures for energy storage. [ABSTRACT FROM AUTHOR]

As next-generation bioelectronic devices, organic electrochemical transistors (OECTs) have attracted great interest in health monitoring and early diagnosis because of their high sensitivity, easy integration, high flexibility, and light weight. However, costly gold electrodes fabricated by lithography are commonly used in traditional OECTs and the devices are usually composed of rigid materials, limiting their flexibility and cost effectiveness. To improve the flexibility and cost efficiency, we design and fabricate an all-carbon OECT by using laser-induced graphene (LIG) as the electrode. A high output performance is achieved because of the porous structure on the LIG surface. The obtained OECT has a high normalized transconductance of 30.1 ± 3.2 S cm−1. In addition, our LIG-based OECT possesses high stability and flexibility. After being integrated with a microfluidic chip, the LIG-based OECT demonstrates sensitive detection of glucose in artificial sweat and on human skin. We envision that the simple and cost-effective LIG-based OECT will advance the development of flexible bioelectronics. [ABSTRACT FROM AUTHOR]

The increasing amount of space debris poses a major threat to the security of space assets. The timely acquisition of space debris orbital data through observations is essential. We established a mathematical model of optical satellite constellations for space debris observation, designed a high-quality constellation configuration, and designed a space debris tracking observation scheduling algorithm. These tools can realize the efficient networking of space debris from a large number of optical satellite observation facilities. We designed a constellation consisting of more than 20 low-Earth orbit (LEO) satellites, mainly dedicated to the observation of LEO space objects. According to the observation scheduling method, the satellite constellation can track and observe more than 93% of the targets every day, increase the frequency of orbital data updates, and provide support for the realization of orbital space debris cataloguing. Designing optical satellite constellations to observe space debris can help realize the advance perception of dangerous collisions, timely detect dangerous space events, make key observations about high-risk targets, greatly reduce the false alarm rate of collisions, and provide observational data support for space collisions. [ABSTRACT FROM AUTHOR]

The reaction efficiency of reactants near plasmonic nanostructures can be enhanced significantly because of plasmonic effects. Herein, we propose that the catalytic activity of molecular catalysts near plasmonic nanostructures may also be enhanced dramatically. Based on this proposal, we develop a highly efficient and stable photocatalytic system for the hydrogen evolution reaction (HER) by compositing a molecular catalyst of cobalt porphyrin together with plasmonic gold nanoparticles, around which plasmonic effects of localized electromagnetic field, local heating, and enhanced hot carrier excitation exist. After optimization, the HER rate and turn-over frequency (TOF) reach 3.21 mol g−1 h−1 and 4650 h−1, respectively. In addition, the catalytic system remains stable after 45-hour catalytic cycles, and the system is catalytically stable after being illuminated for two weeks. The enhanced reaction efficiency is attributed to the excitation of localized surface plasmon resonance, particularly plasmon-generated hot carriers. These findings may pave a new and convenient way for developing plasmon-based photocatalysts with high efficiency and stability. The reaction efficiency of reactants near plasmonic nanostructures can be enhanced under illumination. Here, the authors show that the activity of a Co porphyrin molecular catalyst bound to Au nanoparticles is enhanced by plasmonic effects, yielding a high photocatalytic hydrogen generation rate. [ABSTRACT FROM AUTHOR]

Herein, a very simple but efficient method is developed to concurrently improve the quality of perovskite film and enhance the interfaces of perovskite solar cells (PSCs) concurrently via partially replacing dimethyl sulfoxide (DMSO) with N‐methyl‐2‐pyrrolidinone (NMP) in inverted planar PSCs. With the systematic investigations, it is found that the perovskite films fabricated with this simple method demonstrate higher crystallinity, larger grain size with less grain boundaries, and better perovskite–substrate interface with very rare voids. All of these lead to efficient all‐round defects suppression and high performance of the corresponding PSCs. As a result, the tri‐mixed solvent (DMF:DMSO:NMP = 4:0.75:0.25) processing renders a power conversion efficiency (PCE) of 21.53%, which is much higher than that of PSCs fabricated with traditional bi‐mixed solvent (DMF:DMSO = 4:1) (only 17.05%). Notably, the simple‐method‐fabricated PSCs demonstrate remarkable humidity and thermal stabilities even without any encapsulation (90.6% and 75.2% of initial PCE are retained after more than 511 h in air with relative humidity (RH) ≈ 50% at room temperature and 216 h in air with RH 70% at continuous heating of 70 °C, respectively). All these results demonstrate that the simple method by partially replacing DMSO with NMP is very efficient to improve the quality of perovskite layer and yield high‐performance PSCs. [ABSTRACT FROM AUTHOR]

The original article can be found online at https://doi.org/10.1038/s41467-023-37271-9.Correction to: Nature Communicationshttps://doi.org/10.1038/s41467-023-37271-9, published online 18 March 2023In this article, fig. 1d and fig.1e X axis read 'Binging Energy' and should have read 'Binding Energy'. The original article has been corrected.By Huixiang Sheng; Jin Wang; Juhui Huang; Zhuoyao Li; Guozhang Ren; Linrong Zhang; Liuyingzi Yu; Mengshuai Zhao; Xuehui Li; Gongqiang Li; Ning Wang; Chen Shen and Gang LuReported by Author; Author; Author; Author; Author; Author; Author; Author; Author; Author; Author; Author; Author [Extracted from the article]

As one of the cheapest photovoltaic polymers, poly(3-hexylthiophene) (P3HT) has been considered as one of the prospective donor materials for commercial application. Thus, various non-fullerene acceptors (NFAs), especially A2–A1–D–A1–A2 type molecules comprising one electron-donating (D) unit and two electron-withdrawing (A) units have been designed to improve the photovoltaic performance of P3HT. So far, the central D unit has been dominated by large conjugated heterocycles fused with thiophene and benzene rings. Herein, indacenodiselenophene (IDSe) and benzo[d][1,2,3]triazole (BTA) were utilized as the central D part and bridged A1 unit respectively, to synthesize two novel A2–A1–D–A1–A2 type NFAs BTA46 and BTA47. To modulate the molecular planarity, absorption spectra and energy levels, 3-benzyl-rhodanine (R-Bn) and 3-benzyl-2-(1,1-dicyanomethylene)rhodanine (RCN-Bn) were used as the terminal units. P3HT:BTA47 combination demonstrates a higher PCE of 7.12% benefiting from the more efficient charge generation and transport in comparison with P3HT:BTA46 blend, which exhibits an inferior PCE of 3.99%. Detailed photoelectric properties and charge generation process analysis indicate that IDSe is a promising central core for A2–A1–D–A1–A2 type NFAs to combine with P3HT. [ABSTRACT FROM AUTHOR]

Solution-processed metal halide perovskites have been recognized as one of the most promising semiconductors, with applications in light-emitting diodes (LEDs), solar cells and lasers. Various additives have been widely used in perovskite precursor solutions, aiming to improve the formed perovskite film quality through passivating defects and controlling the crystallinity. The additive's role of defect passivation has been intensively investigated, while a deep understanding of how additives influence the crystallization process of perovskites is lacking. Here, we reveal a general additive-assisted crystal formation pathway for FAPbI3 perovskite with vertical orientation, by tracking the chemical interaction in the precursor solution and crystallographic evolution during the film formation process. The resulting understanding motivates us to use a new additive with multi-functional groups, 2-(2-(2-Aminoethoxy)ethoxy)acetic acid, which can facilitate the orientated growth of perovskite and passivate defects, leading to perovskite layer with high crystallinity and low defect density and thereby record-high performance NIR perovskite LEDs (~800 nm emission peak, a peak external quantum efficiency of 22.2% with enhanced stability). Additives have been widely used for passivating defects in perovskite semiconductors, yet the role of additive and their interaction is not clear. Here, the authors reveal an additive-assisted crystal formation in FAPbI3 perovskite by tracking the chemical interaction in the precursor solution and crystallographic evolution using multi-functional additives. [ABSTRACT FROM AUTHOR]

Organic–inorganic hybrid perovskites (OIHPs) are becoming appealing for photodetectors due to their excellent optoelectronic properties, but the drawbacks of the commonly used interfacial layers in OIHP photodetectors such as the necessity of doping, high cost and stability issues hinder the further development of this technology. Herein, a star-shaped small molecule with a triazine core unit named Triazine-Th-OMeTAD was synthesized and employed as a dopant-free hole transporting layer in an OIHP photodetector. The Triazine-Th-OMeTAD provided a low-trap-density perovskite film, efficient charge extraction and a large electron injection barrier. As a result, the optimized OIHP photodetector with the Triazine-Th-OMeTAD HTL exhibited a low dark current of 1.09 nA cm−2, a high responsivity of 0.47 A W−1, and a high specific detectivity of over 8.2 × 1012 Jones at zero bias. Remarkably, a response speed of 18 ns was obtained at a large active area of 11 mm2. The high-performance OIHP photodetector demonstrated here acts as a promising candidate for low-cost and high-performance near-ultraviolet-visible photodetection, which is applicable in quick frame rate visible imagers, optical communications and many more. [ABSTRACT FROM AUTHOR]

For non-fullerene acceptors (NFAs) with linear A2-A1-D-A1-A2 backbone, there are three kinds of possible intermolecular interaction, A1-A1, A1-A2 and A2-A2 stacking. Hence, it is a huge challenge to control this interaction and investigate the effect of intermolecular stacking model on the photovoltaic performance. Here, we adopt a feasible strategy, by utilizing different substituent groups on terminal A2 unit of dicyanomethylene rhodanine (RCN), to modulate this stacking model. According to theoretical calculation results, the molecule BTA3 with ethyl substituent packs via heterogeneous interaction between A2 and A1 unit in neighboring molecules. Surprisingly, the benzyl group can effectively transform the aggregation of BTA5 into homogeneous packing of A2-A2 model, which might be driven by the strong interaction between benzyl and A1 (benzotriazole) unit. However, different with benzyl, phenyl end group impedes the intermolecular interaction of BTA4 due to the large steric hindrance. When using a BTA-based D-π-A polymer J52-F as donor according to "Same-A-Strategy", BTA3-5 could achieve ultrahigh open-circuit voltage (VOC) of 1.17–1.21 V. Finally, BTA5 with benzyl groups realized an improved power conversion efficiency (PCE) of 11.27%, obviously higher than that of BTA3 (PCE=9.04%) and BTA4 (PCE=5.61%). It is also worth noting that the same trend can be found when using other four classic p-type polymers of P3HT, PTB7, PTB7-Th and PBDB-T. This work not only investigates the intermolecular interaction of A2-A1-D-A1-A2 type NFAs for the first time, but also provides a straightforward and universal method to change the interaction model and improve the photovoltaic performance. [ABSTRACT FROM AUTHOR]

Two saddle‐shaped hole‐transporting materials (HTMs), α, β‐COTh‐Ph‐OMeTAD and β, β‐COTh‐Ph‐OMeTAD are designed with a strategy of flexible core with tunable conformation (FCTC) and applied in inverted planar perovskite solar cells (PSCs) as dopant‐free HTMs. As a result, the device based on α, β‐COTh‐Ph‐OMeTAD demonstrates a high power conversion efficiency (PCE) of 17.59% with Jsc = 21.32 mA cm−2, Voc = 1.02 V, and FF = 80.75%, and the one based on β, β‐COTh‐Ph‐OMeTAD yields a higher PCE of 18.53% with Jsc = 22.68 mA cm−2, Voc = 1.04 V, and FF = 78.48%. Moreover, the green‐solvent‐processed PSCs are also fabricated by dissolving the HTMs in ethyl acetate. Without any encapsulation, the devices based on both HTMs retain 80% of their initial PCEs after storage for 150 days in a glove box, and 60% of their initial PCEs after storing for 300 h in ambient air with 40% relative humidity. All these results demonstrate that the materials α, β‐COTh‐Ph‐OMeTAD and β, β‐COTh‐Ph‐OMeTAD based on FCTC strategy are promising HTMs for highly efficient and stable PSCs. [ABSTRACT FROM AUTHOR]

The mode selection and resource allocation are important issues in Device-to-Device (D2D) communication, which have been investigated in single Base Station (BS) cellular network. However, the joint problem of the base station selection, mode selection and resource allocation is a challenging issue. Because the mode selection, base station and resource allocation are inter-coupled with each other. The joint problem of D2D User Equipments (DUEs) mode selection, base station selection, channel allocation and power allocation remains an open problem. In this paper, the scenario with multiple BSs in D2D heterogeneous networks is considered, and the joint problem of DUEs mode selection, base station selection, channel allocation and power allocation is studied. The objective is to maximize the system energy efficiency. We consider the DUEs multiplex the cellular user uplink resource. Meanwhile, the constraint of the total transmission power of the DUEs, and the constraint of the load balancing of the BSs are considered. The joint problem of mode selection, base station selection and resource allocation is formulated. The formulated problem is a non-convex mixed-integer optimization problem. In order to handle the formulated problem, a joint mode selection, base station selection and resource allocation algorithm based on particle swarm optimization is proposed. Numerical results demonstrate that the proposed algorithm can improve the system energy efficiency and obtain the desired target. [ABSTRACT FROM AUTHOR]

The development of highly efficient dye‐sensitized solar cells (DSSCs) is greatly hindered by the lack of a reliable and understandable quantitative structure–property relationship (QSPR) model. Herein, an accurate, robust, and interpretable QSPR model is established by combining the machine learning technique and computational quantum chemistry, and with this model, virtual screening as well as the assessment of synthetic accessibility is performed to identify new efficient and synthetically accessible organic dyes for DSSCs. Finally, eight promising organic dyes with high power conversion efficiency and synthetic accessibility are screened out from ≈10 000 candidates. Meanwhile, the interpretability of the model is used for deducing reasonable chemical rules for high‐performance organic dyes, which are expected to contribute to further innovations for the practical applications of DSSCs. [ABSTRACT FROM AUTHOR]

Two novel donor–accepter–donor structured hole‐transporting materials based on fluorine‐substituted benzotriazole (BTA) core building blocks (2FBTA‐1 and 2FBTA‐2) are designed and synthesized through molecular regulation. Applying these materials into perovskite solar cells, power conversion efficiencies of 7.55% and 17.94% are obtained for 2FBTA‐1 and 2FBTA‐2, respectively. The better photovoltaic performance of 2FBTA‐2 is attributed to its more suitable energy level, more planar molecular configurations, and higher hole mobility. Moreover, the devices with 2FBTA‐2 as hole transport material (HTM) show good stability in air. The results indicate that BTA is a promising building block for future HTM design. [ABSTRACT FROM AUTHOR]

Poly(3-hexylthiophene) (P3HT) is one of the most used semiconducting polymers for organic photovoltaics because it has potential for commercialization due to its easy synthesis and stability. Although the rapid development of the small molecular non-fullerene acceptors (NFAs) have largely improved the power conversion efficiency (PCE) of organic solar cells (OSCs) based on other complicated p-type polymers, the PCE of P3HT-based OSCs is still low. In addition, the design principle and structure-properties correlation for the NFAs matching well with P3HT are still unclear and need to be investigated in depth. Here we designed a series of NFAs comprised of acceptor (A) and donor (D) units with an A2-A1-D-A1-A2 configuration. These NFAs are abbreviated as Qx3, Qx3b and Qx3c, where indaceno[1,2-b:5,6-b′]dithiophene (IDT), quinoxaline (Qx) and 2-(1,1-dicyanomethylene)rhodanine serve as the middle D, bridged A1 and the end group A2, respectively. By subtracting the phenyl side groups appended on both IDT and Qx skeletons, the absorption spectra, energy levels and crystallinity could be regularly modulated. When paired with P3HT, three NFAs show totally different photovoltaic performance with PCEs of 3.37% (Qx3), 6.37% (Qx3b) and 0.03% (Qx3c), respectively. From Qx3 to Qx3b, the removing of phenyl side chain in the middle IDT unit results in the increase of crystallinity and electron mobility. However, after subtracting all the grafted phenyl side groups on both IDT and Qx units, the final molecule Qx3c exhibits the lowest PCE of only 0.03%, which is mainly attributed to the serious phase-separation of the blend film. These results demonstrate that optimizing the substituted position of phenyl side groups for A2-A1-D-A1-A2 type NFAs is vital to regulate the optoelectronic property of molecule and morphological property of active layer for high performance P3HT-based OSCs. [ABSTRACT FROM AUTHOR]

In the last three years, the A2–A1–D–A1–A2 skeleton has become increasingly popular in the design of non-fullerene acceptors (NFAs), and it could match particularly well with the classic p-type polymer of poly(3-hexylthiophene) (P3HT). In this manuscript, we successfully synthesized three NFAs with this skeleton, named BTA100, BTA101 and BTA103, where BTA units were substituted by methoxy groups and used as the middle electron-accepting unit (A1). To fine-tune the energy levels of the final BTA-based NFAs, three different electron-deficient building blocks, thiazolidine-2,4-dione (TD), rhodanine (R) and 2-(1,1-dicyanomethylene)rhodanine (RCN), were used as the end groups (A2), respectively. The introduction of methoxy groups into BTA can upshift the lowest unoccupied molecular orbital (LUMO) energy level of NFAs and realize high open-circuit voltage (VOC) organic solar cells. In addition, the O atom shows a weak interaction with the S atom in the neighbouring thiophene ring, which might be able to facilitate intramolecular charge transfer. The organic solar cell (OSC) device based on P3HT:BTA103 shows a high PCE of 5.31% with a VOC of 0.94 V, a JSC of 8.56 mA cm−2 and a FF of 0.66. In addition, it is worth noting that the VOC of P3HT:BTA100 reached 1.34 V, which is one of the highest values for P3HT based solar cells. These results indicate that RCN is also an effective end group to construct NFAs and methoxy substitution is a simple method to improve the VOC for P3HT-based OSC devices. [ABSTRACT FROM AUTHOR]

Two types of cyclopentadithiophene dyes with different linking modes with an N-annulated perylene (NP) donor were designed and synthesized. These new dyes were applied in Co(ii)/(iii) based dye-sensitized solar cells and an efficiency up to 7.8% could be obtained for peri-NP linked CPD-1. The effect of the linking mode on the material properties and device performance was discussed. [ABSTRACT FROM AUTHOR]

Fusion of two N-annulated perylene (NP) units with a fused porphyrin dimer along the S0-S1 electronic transition moment axis has resulted in new near-infrared (NIR) dyes 1 a/ 1 b with very intense absorption (ε>1.3×105 M−1 cm−1) beyond 1250 nm. Both compounds displayed moderate NIR fluorescence with fluorescence quantum yields of 4.4×10−6 and 6.0×10−6 for 1 a and 1 b, respectively. The NP-substituted porphyrin dimers 2 a/ 2 b have also been obtained by controlled oxidative coupling and cyclodehydrogenation, and they showed superimposed absorptions of the fused porphyrin dimer and the NP chromophore. The excited-state dynamics of all of these compounds have been studied by femtosecond transient absorption measurements, which revealed porphyrin dimer-like behaviour. These new chromophores also exhibited good nonlinear optical susceptibility with large two-photon absorption cross-sections in the NIR region due to extended π-conjugation. Time-dependent density functional theory calculations have been performed to aid our understanding of their electronic structures and absorption spectra. [ABSTRACT FROM AUTHOR]

A dithienobenzodithiophene‐based π‐conjugated polymer consisting of fluorinated benzotriazole and benzothiadiazole is successfully applied through anti‐solvent method to passivate the defects of perovskite crystals. The fluorinated polymer interacts with under coordinated Pb2+ ions in the perovskite crystals to form Pb‐F bond which effectively passivates the defects. The trap density is reduced and the charge carrier transfer between the perovskite film and Spiro‐OMeTAD is also improved after passivation with the polymer. As a result, a power conversion efficiency (PCE) of 18.03% is achieved in the champion cell. After storing in an ambient environment with 60% relative humidity for 1000 h, the device still retains 90% of the original PCE. These results demonstrate that dithienobenzodithiophene‐based π‐conjugated polymers are promising materials for passivation of perovskite films to further improve the performance and stability of perovskite solar cells. [ABSTRACT FROM AUTHOR]

Herein, a new bifunctional saddle‐shaped organic small molecule named 2,2′,7,7′‐tetrakis(N, N‐di‐p‐methoxyphenyl‐aniline)‐α, β‐cycloocta[1,2‐b:4,3‐b′:5,6‐b′:8,7‐b″′]tetrathiophenyl (α, β‐COTh‐Ph‐OMeTAD) is synthesized. When compared with spiro‐OMeTAD, a star hole transporting material (HTM) for highly efficient perovskite solar cells, the new material has a deeper highest occupied molecular orbital (HOMO) energy level of −5.30 eV, and a higher hole mobility of 2.88 × 10−4 cm2 V−1 s−1. With dopant‐free α, β‐COTh‐Ph‐OMeTAD as a HTM and an interfacial layer combinined with chlorobenzene (CB) as the anti‐solvent, mesoporous perovskite solar cells (PSCs) are fabricated, which exhibit a power conversion efficiency (PCE) of 17.22% under AM 1.5 conditions, which is a little higher than that of devices based‐on doped spiro‐OMeTAD under the same conditions, which is 16.83%. Notably, the PSCs devices with dopant‐free α, β‐COTh‐Ph‐OMeTAD as both the HTM and interfacial layer show better stability, and after being stored in dark and dry air without encapsulation for nearly 800 h, the PCE can still be maintained at 86% of the maximum. This opens a new avenue for efficient and stable PSCs by exploring new dopant‐free materials as alternatives to spiro‐OMeTAD. [ABSTRACT FROM AUTHOR]