Chen Weijie

Various diammonium spacer cations are used to construct 2D/3D perovskite. The mechanism of molecular configuration-induced regulation of crystal orientation and carrier dynamics is investigated. 2D/3D perovskite solar cells based on 2,2′-(ethylenedioxy)bis(ethylamine) achieve a device efficiency of 22.68 % and excellent moisture stability, retaining 82 % of initial efficiency after aging at 50±5 % relative humidity for 1560 h.

Abstract

The effects from the molecular configuration of diammonium spacer cations on 2D/3D perovskite properties are still unclear. Here, we investigated systematically the mechanism of molecular configuration-induced regulation of crystallization kinetic and carrier dynamics by employing various diammonium molecules to construct Dion-Jacobson (DJ)-type 2D/3D perovskites to further facilitating the photovoltaic performance. The minimum average Pb-I-Pb angle leads to the smallest octahedral tilting of [PbX₆]⁴⁻ lattice in optimal diammonium molecule-incorporated DJ-type 2D/3D perovskite, which enables suitable binding energy and hydrogen-bonding between spacer cations and inorganic [PbX₆]⁴⁻ cages, thus contributing to the formation of high-quality perovskite film with vertical crystal orientation, mitigatory lattice distortion and efficient carrier transportation. As a consequence, a dramatically improved device efficiency of 22.68 % is achieved with excellent moisture stability.

The quality of buried interfaces in inverted perovskite solar cells is improved via constructing hole-transporting materials with deep HOMO levels, high wetting, and passivation capabilities. By systematically regulating the linking-site of pyridine unit, high efficiencies exceeding 22% (0.09 cm²) and 20% (1 cm²) are achieved.

Abstract

Inverted-structured perovskite solar cells (PSCs) mostly employ poly-triarylamines (PTAAs) as hole-transporting materials (HTMs), which generally result in low-quality buried interface due to their hydrophobic nature, shallow HOMO levels, and absence of passivation groups. Herein, the authors molecularly engineer the structure of PTAA via removing alkyl groups and incorporating a multifunctional pyridine unit, which not only regulates energy levels and surface wettability, but also passivates interfacial trap-states, thus addressing above-mentioned issues simultaneously. By altering the linking-site on pyridine unit from ortho- (o-PY) to meta- (m-PY) and para-position (p-PY), they observed a gradually improved hydrophilicity and passivation efficacy, mainly owing to increased exposure of the pyridine-nitrogen as well as its lone electron pair, which enhances the contact and interactions with perovskite. The open-circuit voltage and power conversion efficiency (PCE) of inverted-structured PSCs based on these HTMs increased with the same trend. Consequently, the optimal p-PY as HTM enables facile deposition of uniform perovskite films without complicated interlayer optimizations, delivering a remarkably high PCE exceeding 22% (0.09 cm²). Moreover, when enlarging device area tenfold, a comparable PCE of over 20% (1 cm²) can be obtained. These results are among the highest efficiencies for inverted PSCs, demonstrating the high potential of p-PY for future applications.

Organic solar cell active layers with A-DAD-A (A = acceptor; D = donor) non-fullerene acceptors (NFAs) having different extents of end group fluorination are systematically characterized in terms of film crystallinity, donor-acceptor depth distribution, charge carrier transport, and cell performance. The most fluorinated NFA, BT-BO-L4F, has optimal hierarchical morphology and vertical phase gradation, affording a power conversion efficiency of 16.81%.

Abstract

Non-fullerene acceptor (NFA) end group (EG) functionalization, especially by fluorination, affects not only the energetics but also the morphology of bulk-heterojunction (BHJ) organic solar cell (OSC) active layers, thereby influencing the power conversion efficiency (PCE) and other metrics of NFA-based OSCs. However, a quantitative understanding of how varying the degrees of NFA fluorination influence the blend morphological and photovoltaic properties remains elusive. Here a series of three A-DAD-A type NFAs (D = π-donor group and A = π-acceptor EG) which systematically increase the degree of EG fluorination and comprehensively investigate the resulting blends with the polymer donor PM6 in terms of optical properties, electronic structure, film crystallinity, charge carrier transport, and OSC performance is reported. The results indicate that the most highly fluorinated NFA, BT-BO-L4F, achieves an optimal BHJ hierarchical morphology where enhanced NFA molecule intermolecular π–π stacking and optimal vertical phase gradation are achieved in the BHJ blend. These factors also promote optimum NFA-cathode contact, more balanced electron and hole mobility, and suppress both monomolecular and bimolecular recombination. As a result, both the short-circuit current density and fill factor in this OSC series progressively increase with increasing EG fluorine density, and the resulting PCEs increase from 9 to 16.8%.

A polymeric hole-transport material (HTM) based on the phenanthrocarbazole derivative PC6 features a two-dimensionally conjugated phenanthrocarbazole and S-O noncovalent conformational locking. Perovskite solar cells employing PC6 as a dopant-free HTM afforded an excellent power conversion efficiency (PCE) of 22.2 % and long-term stability.

Abstract

Adequate hole mobility is the prerequisite for dopant-free polymeric hole-transport materials (HTMs). Constraining the configurational variation of polymer chains to afford a rigid and planar backbone can reduce unfavorable reorganization energy and improve hole mobility. Herein, a noncovalent conformational locking via S–O secondary interaction is exploited in a phenanthrocarbazole (PC) based polymeric HTM, PC6, to fix the molecular geometry and significantly reduce reorganization energy. Systematic studies on structurally explicit repeats to targeted polymers reveals that the broad and planar backbone of PC remarkably enhances π–π stacking of adjacent polymers, facilitating intermolecular charge transfer greatly. The inserted “Lewis soft” oxygen atoms passivate the trap sites efficiently at the perovskite/HTM interface and further suppress interfacial recombination. Consequently, a PSC employing PC6 as a dopant-free HTM offers an excellent power conversion efficiency of 22.2 % and significantly improved longevity, rendering it as one of the best PSCs based on dopant-free HTMs.

Publication date: 15 December 2021

Source: Joule, Volume 5, Issue 12

Author(s): Ian Marius Peters, Jens Hauch, Christoph Brabec, Parikhit Sinha

Exploiting norbornenyl modified terminals endows the fused ring acceptor (SM16) with an unprecedentedly high photoluminescence quantum yield of 8.61%, thus leading to a very low nonradiative voltage loss of 0.145 V when blended with PBDB-T. A power conversion efficiency of 17.1% is achieved by using SM16 as the third component due to the boosting of open-circuit voltage and fill factor.

Abstract

Increasing the photoluminescence quantum yield (PLQY) of narrow bandgap acceptors is of critical importance to suppress the nonradiative voltage loss (ΔV _nr) in organic solar cells (OSCs). Herein, two acceptors, SM16 and SM16-R, with an identical backbone but different terminal groups (norbornenyl modified 1,1-dicyanomethylene-3-indanone and dimethyl substituted 1,1-dicyanomethylene-3-indanone) are designed and synthesized. Compared with SM16-R, SM16 displays better solubility, higher PLQY, and more favorable nanomorphology when blended with polymer donor PBDB-T. PBDB-T:SM16-based OSCs yield a ΔV _nr as low as 0.145 V. Using SM16 as the third component, a high power conversion efficiency of 17.1% is achieved in the ternary OSCs based on PBDB-T:Y14:SM16, considerably higher than that of the binary devices based on PBDB-T:Y14 or PBDB-T:SM16. These results highlight that enhancing the PLQY of low bandgap acceptor via terminal group engineering strategy is highly effective to reduce ΔV _nr of OSCs.

Three benzodipyrrole (BDP)-based molecules are designed and synthesized as hole transport material for perovskite solar cells. The combination of BDP core and 3-fluorophenyl unit as CB-2 creates highly planar conformation and effective defect passivation via interaction with Pb of the perovskite. Thus, CB-2 achieves improved solar cell performance and excellent long-term storage stability without degradation for over 6 months.

Three benzodipyrrole (BDP)-based organic small molecules with substituted 4-methoxyphenyl (CB-1), 3-fluorophenyl (CB-2), and 3-trifluoromethylphenyl (CB-3) are designed, synthesized, and used as a hole-transporting material (HTM) for perovskite solar cells (PSCs). The electrochemical, optical, thermal, electronic, and optoelectronic properties of the HTMs are characterized to verify their suitability for PSCs. The terminal functional groups of the HTMs having different heteroatoms mainly target effective defect passivation of perovskites. Photoluminescence studies and molecular dynamic simulations reveal that fluorine atoms within CB-2 and CB-3 can contribute to the defect passivation via interaction with Pb of the perovskite. In particular, a highly planar conformation of CB-2 on the perovskite surface can facilitate more efficient hole transfer at the interface. Thus, the PSCs employing CB-2 achieve the highest power conversion efficiency (PCE) of 18.23% while the devices using CB-1 and CB-3 exhibit a lower PCE of 16.78% and 16.74%, respectively. PSCs with the BDP-based HTMs demonstrate excellent long-term storage stability without degradation in their PCEs over 6 months. The highly planar geometry, defect passivation effect, and hydrophobicity of CB-2 show its great potential as an HTM for efficient and stable PSCs.

The planarity of two new small-molecule acceptors, based on diketopyrrolopyrrole, is achieved by noncovalent intramolecular interactions. These molecules show broad absorption in the visible and near-infrared region. Binary solar cells built together with a polymer display power conversion efficiency as high as 14.12%.

A simple synthesis of highly planar extended π-electron molecules is of particular interest for the development of efficient nonfullerene acceptors in organic solar cells with high light absorption and high mobility. Herein, two small-molecule acceptors (MPU7 and MPU8) with a diketopyrrolopyrrole core connected to CPTCN end-capping groups (A₂) via thienylethynylselenophene (MPU7) or thienylethynylthiophene (MPU8) linkers are conceived and synthesized. Planarity of the conjugated skeleton is achieved in both molecules, thanks to the existence of four (Se⋯O or S⋯O) noncovalent, through-space intramolecular interactions. Both nonfullerene small-molecule acceptors show broad absorption in the visible and near-infrared region (up to 930 nm). As a result, the binary solar cells constructed together with a polymer donor (P) display power conversion efficiencies as high as 14.12%. Devices built with MPU7 (containing the selenophene) show better film morphology, electron mobility, and higher efficiency than those containing thiophene (MPU8).

For the first time, it is demonstrated that an organic solar cell (OSC) using the Dawson-type polyoxometalate as hole collection material can exhibit superior photovoltaic efficiency to the device modified by classic interlayer PEDOT:PSS. The results herein suggest that the Dawson-type polyoxometalates can be used as low-cost and effective anode interlayers for the future manufacturing of OSCs.

Interfacial layer materials play an important role in performance enhancement of organic solar cells (OSCs). Herein, the utilization of mixed-metal Dawson-type polyoxometalates, namely P₂Mo₃W₁₅O₆₂ (POM-1) and P₂Mo₉W₉O₆₂ (POM-2), as anode interlayer (AIL) materials, for efficiently collecting holes to boost the photovoltaic efficiency of OSCs, is explored. The increase in molybdenum substitution in the mixed-metal POMs can lower the conduction band level and increase the reduction potential. Meanwhile, the high work function of POMs helps to remove the energy barrier in the hole collection, which solves the serious problem of V _oc loss in OSCs. As a result, OSCs modified by POM-2 can exhibit superior photovoltaic performance with power conversion efficiency of 14.8%. The results of Mott−Schottky analysis, current density−light intensity dependence, and excitons dissociation probability indicate the efficient hole collection and the depressed charge recombination in the POM-2-based OSC device. By means of fabricating OSCs, the effect of the two POM-based AILs on various photoactive layers is also investigated, and POM-2 exhibits excellent hole collection capability. Moreover, the advantages of low-cost and solution-processable conduct make POM-2 a promising candidate as the AIL material for future mass production of OSCs.

Ternary organic solar cells (OSCs) are high-performance solar cells based on photovoltaic technologies that have emerged as potential energy technologies. The active layers of ternary OSCs comprise donor/acceptor host components and a third component. This review categorizes and describes the effects that the role and function of the third component have on the efficiency and stability of ternary OSCs.

Ternary organic solar cells (OSCs) have attracted much attention due to them being high-performance solar cells. Ternary OSCs represent an efficient strategy to gain both the benefits of enhanced photon energy harvesting using multiple organic materials, similar to that in tandem OSCs, and the easy fabrication of simple single-junction device structures. The properties of ternary OSCs are closely related to their complex energy/charge dynamics mechanisms and unique thermodynamic features of blend morphology and crystallinity. Hence, there is much more to introducing a third component into a binary blend than the simple superposition of individual components. Herein, the role of the third component is mainly discussed to provide in-depth insights into ternary OSCs. This review categorizes and describes the effects that the role and function of the third component have on the efficiency and stability of ternary OSCs. Finally, in addition to a summary on the current research progress, outlooks for future research directions are also addressed.

Phenethylamine halides (PEAX) coated on perovskite layers either form 2D perovskites or dipole moments. High-performance perovskite solar cells are realized mainly due to the formation of dipole moments caused by PEAX leading to high open-circuit voltages. This implies that direct contact of PEAX with the perovskite layer is not necessary for further improvements.

Abstract

Surface modification of 3D hybrid perovskites using 2D perovskites, such as phenethylamine halides (PEAX), increases the overall power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs). The effect is based on a surface passivation phenomenon where PEAX is in direct contact with the perovskite and hole transport layer (HTL). However, it is herein observed that the PCE of PSCs containing PEAX increases significantly when they are not in direct contact with either the bottom layers (perovskites) or top layers (HTLs). Moreover, the highest PCE (>22%) is obtained for the PSCs when PEAX is not in contact with HTLs by using poly(methyl methacrylate) (PMMA). Photoemission measurements reveal that the shift of the highest occupied molecular orbital of the hole transporting material (a donor-acceptor-donor molecule synthesized for the study) to a deeper level results in an increased hole transfer at the perovskite/HTL interface leading to an improved device performance. It is proposed that PEAX acts as dipoles aligned between perovskite and HTL resulting in a shift in the energy levels. The combination of PEAX/PMMA at the interface enables high open-circuit voltage (1.19V) close to the Shockley–Queisser limit for the triple-cation (Cs-MA-FA) perovskites (bandgap, 1.51 eV).

Gradient self-doping within the micron scale is established based on an optimized two-step method in printable mesoscopic perovskite solar cells. The difference in the work function of the perovskite enhances the built-in electric field, thus promoting the transport and extraction of photogenerated holes. Reduced carrier recombination losses deliver an average V _OC improvement over 60 mV and a power conversion efficiency of 17.68%.

Abstract

The hole-conductor-free printable mesoscopic perovskite solar cells based on the inorganic scaffolds of mesoporous titania, mesoporous zirconia, and porous carbon have attracted much attention due to their excellent stability and low manufacturing cost. However, in such hole-conductor-free devices, the transport of the photogenerated holes is dominated by the diffusion-assisted charge carrier movement, while the driving force is insufficient. Reinforcing the built-in electric field (BEF) is an effective strategy to promote oriented carrier transport. Herein, by using an optimized two-step deposition method, the BEF is reinforced by creating a work function difference of perovskite (Δµ) in different layers via a gradient self-doping. The enhanced BEF improves the hole transport and extraction, and significantly reduces the carrier recombination losses in the device. As a result, an average open-circuit voltage improvement over 60 mV and a power conversion efficiency of 17.68% are achieved without any additives or complex processes. This strategy provides a new approach toward fabricating highly efficient printable mesoscopic perovskite solar cells with reduced carrier recombination losses.

Methyl 3-sulfamoyl-2-thiophenecarboxylate (MSTC), containing sulfonamides and carbonyl groups, is doped into a two-step precursor as an effective additive engineering strategy. MSTC can coordinate with PbI₂ or FAI precursor through coordination bonding, hydrogen bonding, and collaboration bonding, enhancing the performance effectively. The champion power conversion efficiency of solar cells is increased from 19.19% to 22.14%, with improved stability.

Intrinsic defects are key factors that would affect the performance and stability of perovskite solar cells (PSCs). Herein, a sulfonamides additive, methyl 3-sulfamoyl-2-thiophenecarboxylate (MSTC), is introduced into the PbI₂ or FAI/MACl/MABr precursor solution, to prepare high-quality PSCs with a two-step method. After the addition of MSTC, all the devices show enhanced performance. With optimized MSTC incorporated into PSCs, the champion power conversion efficiency (PCE) of the PSCs is increased from 19.19% to 22.14%, and the stability is also improved. The MSTC-FAI based device can still maintain 89% of its initial PCE compared to 68% of the control one after 15 days in ambient condition under relative humidity of 40–50% at room temperature in dark. Test results reveal that amido group in MSTC would coordinate with PbI₂ or FAI through hydrogen bonding (NH···I), thus effectively enhancing the performance of devices. Nevertheless, the sulfonyl and carbonyl groups in MSTC would coordinate with the FAI precursor through chemical bond of COS and COC. And with the hydrogen bonding connection between MSTC and FAI, the inherent defects in the MSTC-FAI based device are effectively suppressed, leading to the enhanced photovoltaic performance.

With the development from the printed thin-film devices to thick-film devices, the vertical component distribution are finely modulated by additives for the efficient charge transport, resulting in high-performance large-area thick-film organic solar cells.

Thick active layers in organic solar cells (OSCs) have a great promise of enhancing light absorption and providing pinhole-free films for large-scale fabrication. Since charge carriers in thick films need a longer transporting path in the vertical direction to the electrode than in thin films, modulation of the active layer morphology in thick films is highly required for effective charge transport. Herein, thin-film (≈110 nm) and thick-film (≈300 nm) OSCs based on a PM6:IT-4 F film are fabricated by blade coating with various additive contents. It is found that the optimized thick-film device needs more additives than the optimized thin-film device. The addition of more additives in thick-films promotes vertical component distribution and enhances the crystallization, resulting in efficient charge transport with reduced charge recombination and electron (or hole) accumulation within the thick active layer. These results are also confirmed by PM6:Y6-based devices, in which optimized thin-film and thick-film devices exhibit power conversion efficiency (PCE) of 16.69% and 14.91% at the additive contents of 0.3% and 0.6%, respectively. Encouragingly, thick-film device with 0.6% additive has a narrow distribution of PCE values, and high PCEs of 13.94% and 13.05% are obtained for the large-area (1 cm²) rigid and flexible thick-film OSCs, showing great application prospect.

The grain boundaries in perovskite films play a major role in restricting the performance and stability of perovskite photovoltaics by allowing moisture permeation and ion migration. Herein, Cu₂NiSn(S,Se)₄ nanocrystals effectively passivate the surface and enhance the hole extraction from active layer to hole transport layer, yielding an efficiency of 20.8% with outstanding stability by retaining over 85% of initial performance.

Despite the rapid progress of perovskite materials in emerging perovskite photovoltaic devices, they still suffer from the polycrystalline nature associated with grain boundaries (GBs) which are vulnerable to moisture permeation and/or ion migration. Besides, charge carrier recombination of GBs through defect states plays a crucial role in restricting the performance and stability of perovskite photovoltaics. To address such detrimental issues, quinary kesterite nanocrystals, namely Cu₂NiSn(S,Se)₄ (CNTSSe), having narrow size distribution below 10 nm by a facile hot-casting method are rationally designed and employed as a passivation agent for the GBs/surface of perovskite films. This passivation strategy greatly reduces defect states at perovskite GBs and promotes continuity between adjacent grains, resulting in accelerated hole transport ability and suppressed interfacial recombination. Thereupon, champion power conversion efficiency of 20.8% (20.5 ± 0.3% in average) (Cs_0.05(FA_0.90MA_0.10)_0.95Pb(I_0.90Br_0.10)₃), 18.9% (MAPbI₃), and 18.7% (FAPbI₃) is achieved with a negligible hysteresis and outstanding stability by retaining over 85% of initial performance under ambient conditions with continuous illumination over 900 h. Herein, not only a universal approach to effectively passivate the GBs of the perovskite films by inorganic nanocrystals is presented, but also a deep understanding of detrimental defects on the photovoltaic performance and stability of perovskite solar cells is ensured.

Hydrothermal-synthesized Cu-doped Ga₂O₃ nanocrystals are used as the hole transport material of inverted perovskite solar cells. Cu dopants remarkably improve the performance of devices, which is related to the additional hole transport channels from impurity levels.

In inverted perovskite solar cells (PSCs), metal oxides become kind of promising hole transport layers for their facile synthesis and low cost. For conventional hole transport materials, the valence band match between metal oxides and perovskite layers is usually necessary for the hole extraction process. Ga₂O₃ is an emerging semiconductor material with ultrawide bandgap, but a significant energy level mismatch exists at Ga₂O₃/perovskite interfaces. In this work, Cu-doped Ga₂O₃ (Ga₂O₃:Cu) nanocrystals are synthesized by the hydrothermal method and used as the hole transport material of inverted PSCs for the first time. It is found that Cu dopants can substantially improve the performance of Ga₂O₃ layers, and the efficiency of PSCs is increased from 7.6% to 19.5%. This improvement can be attributed to the additional hole transport channels from impurity levels of Cu dopants, which exactly match with the valence band of perovskite layers. As a consequence, Ga₂O₃:Cu layers can effectively extract holes and inhibit the recombination in perovskite layers. This work also provides an alternative route for the design of hole transport materials.

Near-infrared (NIR) electron acceptors can absorb low-energy photons for large short-circuit current density, which can enable significant efficiency enhancements of organic solar cells by molecular design to balance open-circuit voltage. Further development of NIR acceptors toward higher performance and practicality needs to take core innovation, materials stability and cost into considerations.

Materials with intense near-infrared (NIR) absorption, especially electron acceptors, play crucial roles in the development of organic solar cells (OSCs) due to their capability in harvesting low-energy photons to enable high photocurrent. Herein, the NIR nonfullerene acceptors (NFAs) are focused by briefly reviewing the development to understand the molecular design strategies, structure–property–performance relationships, and the great potential of NIR NFAs in fabricating ternary and tandem OSCs. Outlooks for future design of NIR NFAs are also provided by considering material stability and production cost based on current knowledges, in hope of aiding the further development of the field.

A strategy for spontaneous construction of a 2D/3D structure is proposed to prepare inorganic CsPbI_{3− x} Br _x perovskite solar cells. The results reveal that the Ruddlesden–Popper 2D-(MOPEA)₂Pb(Br _x I_{4− x} ) perovskite can effectively enhance the hole extraction efficiency and passivate detrimental surface defects. The power conversion efficiency is significantly increased to 20.31%, making it one of the most efficient inorganic perovskite solar cells.

Abstract

CsPbI_{3− x} Br _x -based organic-free perovskite has emerged as a superstar photovoltaic material not only because of its superior photoelectronic properties but also its outstanding thermal and chemical stability. Unfortunately, the significant energy loss resulting from its nonradiative recombination has become a major obstacle to further improvement of device performance. Here, a 2D/3D multidimensional structure formed spontaneously at room temperature is developed. The results reveal that the formed Ruddlesden–Popper 2D (n = 1) perovskite atop CsPbI_{3− x} Br _x plays an active role in mediating carrier transport, maintaining a long-life charge separation state on the nanosecond time scale and promoting the efficiency of carrier injection into the hole transport layer, and thus enhances the hole extraction efficiency, which greatly reduces severe interfacial nonradiative charge recombination. In addition, the undercoordinated Pb²⁺ is effectively passivated, resulting in significantly reduced surface trap density and prolonged charge lifetime within the perovskite films. Consequently, the combination of the above increases the solar cell efficiency from 19.05% to 20.31%, with an open-circuit voltage raised to 1.23 from 1.17 V, which corresponds to an energy loss reduction from 0.54 to 0.49 eV. Also, the optimized solar cells exhibit better long-term and thermal stability.

By incorporating intramolecular S⋅⋅⋅O noncovalent interactions (INIs) for boosting the intrinsic hole mobilities, two simple-structured dopant-free hole-transporting materials (HTMs) were designed and delivered a remarkable efficiency of 21.10 % with decent device stability in inverted perovskite solar cells, demonstrating the great promise of the INI strategy for accessing high-performance dopant-free HTMs.

Abstract

Intramolecular noncovalent interactions (INIs) have served as a powerful strategy for accessing organic semiconductors with enhanced charge transport properties. Herein, we apply the INI strategy for developing dopant-free hole-transporting materials (HTMs) by constructing two small-molecular HTMs featuring an INI-integrated backbone for high-performance perovskite solar cells (PVSCs). Upon incorporating noncovalent S⋅⋅⋅O interaction into their simple-structured backbones, the resulting HTMs, BTORA and BTORCNA, showed self-planarized backbones, tuned energy levels, enhanced thermal properties, appropriate film morphology, and effective defect passivation. More importantly, the high film crystallinity enables the materials with substantial hole mobilities, thus rendering them as promising dopant-free HTMs. Consequently, the BTORCNA-based inverted PVSCs delivered a power conversion efficiency of 21.10 % with encouraging long-term device stability, outperforming the devices based on BTRA without S⋅⋅⋅O interaction (18.40 %). This work offers a practical approach to designing charge transporting layers with high intrinsic mobilities for high-performance PVSCs.