High performance wide bandgap perovskite solar cell with low V_(OC) deficit less than 0.4 V

Wide bandgap perovskite solar cells(PSCs)have attracted significant attention because they can be applied to the top cells of tandem solar cells.However,high open-circuit voltage(V_(OC))deficit(>0.4 V)result from poor crystallization and high non-radiative recombination losses become a serious limitation in the pursuit of high performance.Here,the relevance between different Pbl_(2)proportions and performance parameters are revealed through analysis of surface morphology,residual stress,and photostability.The increase of Pbl_(2)proportion promotes crystal growth and reduces the work function of the perovskite film surface and promotes the energy level alignment with the carrier transport layer,which decreased the V_(OC)deficit.However,residual PbI_(2)exacerbated the stress level of perovskite film,and the resulting lattice disorder deteriorated the photostability of the device.Ultimately,after the synergistic passivation of residual PbI_(2)and PEAI,the V_(OC)achieves 1.266 V and V_(OC)deficit is less than 0.4 V,the record value in wide bandgap PSCs.

Interfacial Modification of NiO_(x)by Self-assembled Monolayer for Efficient and Stable Inverted Perovskite Solar Cells

NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.

Non-destructive buffer enabling near-infrared-transparent inverted inorganic perovskite solar cells toward 1400 h light-soaking stable perovskite/Cu(In,Ga)Se_(2) tandem solar cells

Near-infrared(NIR)transparent inverted all-inorganic perovskite solar cells(PSCs)are excellent top cell candidates in tandem applications.An essential challenge is the replacement of metal contacts with transparent conductive oxide(TCO)electrodes,which requires the introduction of a buffer layer to prevent sputtering damage.In this study,we show that the conventional buffers(i.e.,small organic molecules and atomic layer deposited metal oxides)used for organic-inorganic hybrid perovskites are not applicable to all-inorganic perovskites,due to non-uniform coverage of the vulnerable layers underneath,deterioration upon ion bombardment and moisture induced perovskite phase transition,A thin film of metal oxide nanoparticles by the spin-coating method serves as a non-destructive buffer layer for inorganic PSCs.All-inorganic inverted near-infrared-transparent PSCs deliver a PCE of 17.46%and an average transmittance of 73.7%between 780 and 1200 nm.In combination with an 18.56%Cu(In,Ga)Se_(2) bottom cell,we further demonstrate the first all-inorganic perovskite/CIGS 4-T tandem solar cell with a PCE of 24.75%,which exhibits excellent illumination stability by maintaining 86.7%of its initial efficiency after 1400 h.The non-destructive buffer lays the foundation for efficient and stable NIR-transparent inverted inorganic perovskite solar cells and perovskite-based tandems.

Constructing low-dimensional perovskite network to assist efficient and stable perovskite solar cells

The use of low-dimensional(LD)perovskite materials is crucial for achieving high-performance perovskite solar cells(PSCs).However,LD perovskite films fabricated by conventional approaches give rise to full coverage of the underlying 3D perovskite films,which inevitably hinders the transport of charge carriers at the interface of PSCs.Here,we designed and fabricated LD perovskite structure that forms net-like morphology on top of the underlying three-dimensional(3D)perovskite bulk film.The net-like LD perovskite not only reduced the surface defects of 3D perovskite film,but also provided channels for the vertical transport of charge carriers,effectively enhancing the interfacial charge transfer at the LD/3D hetero-interface.The net-like morphological design comprising LD perovskite effectively resolves the contradiction between interfacial defect passivation and carrier extraction across the hetero-interfaces.Furthermore,the net-like LD perovskite morphology can enhance the stability of the underlying 3D perovskite film,which is attributed to the hydrophobic nature of LD perovskite.As a result,the net-like LD perovskite film morphology assists PSCs in achieving an excellent power conversion efficiency of up to 24.6%with over 1000 h long-term operational stability.

Cross-layer all-interface defect passivation with pre-buried additive toward efficient all-inorganic perovskite solar cells

The buried interface in the perovskite solar cell(PSC)has been regarded as a breakthrough to boost the power conversion efficiency and stability.However,a comprehensive manipulation of the buried interface in terms of the transport layer,buried interlayer,and perovskite layer has been largely overlooked.Herein,we propose the use of a volatile heterocyclic compound called 2-thiopheneacetic acid(TPA)as a pre-buried additive in the buried interface to achieve cross-layer all-interface defect passivation through an in situ bottom-up infiltration diffusion strategy.TPA not only suppresses the serious interfacial nonradiative recombination losses by precisely healing the interfacial and underlying defects but also effectively enhances the quality of perovskite film and releases the residual strain of perovskite film.Owing to this versatility,TPA-tailored CsPbBr3 PSCs deliver a record efficiency of 11.23% with enhanced long-term stability.This breakthrough in manipulating the buried interface using TPA opens new avenues for further improving the performance and reliability of PSC.

A short overview of the lead iodide residue impact and regulation strategies in perovskite solar cells

Lead iodide(PbI2) is a vital raw material for preparing perovskite solar cells(PSCs),and it not only takes part in forming the light absorption layer but also remains in the grain boundary as a passivator.In other words,the PbI2 content in the precursor and as formed film will affect the efficiency and stability of the PSCs.With moderate residual PbI2,it passivates the bulk/surface defects of perovskite,reduces the interfacial recombination,promotes the perovskite stability,minimizes the device hysteresis,and so on.Deficient PbI2 residue will reduce the interfacial passivation effect and device performance.In addition to facilitating the non-radiative recombination,over PbI2 residue can also lead to electronic insulation in the grain boundary and deteriorate the device performance.However,the impact and regulation of PbI2 residue on the device performance and stability is still not fully understood.Herein,a comprehensive and detailed review is presented by discussing the PbI2 residue impact and its regulation strategies(i.e., elimination,facilitation and conversion of the residue PbI2) to manipulate the PbI2 content,distribution and forms.Finally,we also show future outlooks in this field,with an aim to help further the progression of high-efficiency and stable PSCs.

Modeling the performance of perovskite solar cells with inserting porous insulating alumina nanoplates

Peng et al.[Science 379683(2023)]reported an effective method to improve the performance of perovskite solar cells by using thicker porous insulator contact(PIC)-alumina nanoplates.This method overcomes the trade-off between the open-circuit voltage and the fill factor through two mechanisms:reduced surface recombination velocity and increased bulk recombination lifetime due to better perovskite crystallinity.From arguments of drift-diffusion simulations,we find that an increase in mobility and carrier recombination lifetime in bulk are the key factors for minimizing the resistance-effect from thicker PICs and achieving a maximum power conversion efficiency(PCE)at approximately 25%reduced contact area.Furthermore,the partially replacement of perovskite films with thicker PICs would result in a reduction in short-current density,but the relative low refractive index of the PICs imbedded into the high refractive index perovskite creates light trapping structures that compensate for this loss.

Stabilizing perovskite precursors with the reductive natural amino acid for printable mesoscopic perovskite solar cells

Solution processability significantly advances the development of highly-efficient perovskite solar cells.However,the precursor solution tends to undergo irreversible degradation reactions,impairing the device performance and reproducibility.Here,we utilize a reductive natural amino acid,Nacetylcysteine(NALC),to stabilize the precursor solution for printable carbon-based hole-conductorfree mesoscopic perovskite solar cells.We find that I_(2) can be generated in the aged solution containing methylammonium iodide(MI) in an inert atmosphere and speed up the MA-FA^(+)(formamidinium) reaction which produces large-size cations and hinders the formation of perovskite phase.NALC effectively stabilizes the precursor via its sulfhydryl group which reduces I_(2) back to I^(-)and provides H^(+).The NALC-stabilized precursor which is aged for 1440 h leads to devices with a power conversion efficiency equivalent to 98% of that for devices prepared with the fresh precursor.Furthermore,NALC improves the device power conversion efficiency from 16.16% to 18.41% along with enhanced stability under atmospheric conditions by modifying grain boundaries in perovskite films and reducing associated defects.

Defect mediated losses and degradation of perovskite solar cells:Origin impacts and reliable characterization techniques

The rapid advancement of halide-based hybrid perovskite materials has garnered significant research attention,particularly in the domain of photovoltaic technology.Owing to their exceptional optoelec-tronic properties,they demonstrated power conversion efficiency(PcE)of over 25%in single junction solar cells.Despite the notable progress in PCE over the past decade,the inherent high defect density pre-senting in perovskite materials gives rise to several loss mechanisms and associated ion migration in per-ovskite solar cells(PsCs)during operational conditions.These factors collectively contribute to a significant stability challenge in PsCs,placing their longevity far behind for commercialization.While numerous reports have explored defects,ion migration,and their impacts on device performance,a com-prehensive correlation between the types of defects and the degradation kinetics of perovskite materials and PsCs has been lacking.In this context,this review aims to provide a comprehensive overview of the origins of defects and ion migration,emphasizing their correlation with the degradation kinetics of per-ovskite materials and PsCs,leveraging reliable characterization techniques.Furthermore,these charac-terization techniques are intended to comprehend loss mechanisms by different passivation approaches to enhance the durability and PCE of PSCs.

Seed-assisted growth for high-performance perovskite solar cells:A review

The rapid increase in the power conversion efficiency(PCE)of perovskite solar cells(PSCs)is closely related to the development of deposition techinique for perovskite layer.The high-quality perovskite film enables efficient charge transportation and less trap states,which are eventually translated into enhanced device performance.Seed-assisted growth(SAG)is a potential technique for depositing highly-crystallized perovskite films with preferential crystal orientation among the numerous approaches related to crystallization modulation.In this review,we summarize the recent advances in the SAG technique for both one-step and two-step processed perovskite films.Additionally,seeding at the buried interface and on the top surface are also introduced.We present different seeds and their corresponding seeding mechanism in detail,such as inorganic nanomaterials,organic ammoniums,alkali metal halides,and perovskite seeds.Finally,challenges and perspectives are proposed to investigate the potential expansion of seeding engineering in high-performance PSCs,particularly large-area devices.

Surface-functionalized hole-selective monolayer for high efficiency single-junction wide-bandgap and monolithic tandem perovskite solar cells

Carbazole moiety-based 2PACz([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)self-assembled monolayers(SAMs)are excellent hole-selective contact(HSC)materials with abilities to excel the charge-transferdynamics of perovskite solar cells(PSCs).Herein,we report a facile but powerful method to functionalize the surface of 2PACz-SAM,by which reproducible,highly stable,high-efficiency wide-bandgap PSCs can be obtained.The 2PACz surface treatment with various donor number solvents improves assembly of 2PACz-SAM and leave residual surface-bound solvent molecules on 2PACz-SAM,which increases perovskite grain size,retards halide segregation,and accelerates hole extraction.The surface functionalization achieves a high power conversion efficiency(PCE)of 17.62%for a single-junction wide-bandgap(~1.77 e V)PSC.We also demonstrate a monolithic all-perovskite tandem solar cell using surfaceengineered HSC,showing high PCE of 24.66%with large open-circuit voltage of 2.008 V and high fillfactor of 81.45%.Our results suggest this simple approach can further improve the tandem device,when coupled with a high-performance narrow-bandgap sub-cell.

Boosting MA-based two-dimensional Ruddlesden-Popper perovskite solar cells by incorporating a binary spacer

Two-dimensional Ruddlesden-Popper(2DRP)perovskite exhibits excellent stability in perovskite solar cells(PSCs)due to introducing hydrophobic long-chain organic spacers.However,the poor charge transporting property of bulky organic cation spacers limits the performance of 2DRP PSCs.Inspired by the Asite cation alloying strategy in 3D perovskites,2DRP perovskites with a binary spacer can promote charge transporting compared to the unary spacer counterparts.Herein,the superior MA-based 2DRP perovskite films with a binary spacer,including 3-guanidinopropanoic acid(GPA)and 4-fluorophenethylamine(FPEA)are realized.These films(GPA_(0.85)FPEA_(0.15))_(2)MA_(4)Pb_5I_(16)show good morphology,large grain size,decreased trap state density,and preferential orientation of the as-prepared film.Accordingly,the present 2DRP-based PSC with the binary spacer achieves a remarkable efficiency of 18.37%with a V_(OC)of1.15 V,a J_(SC)of 20.13 mA cm^(-2),and an FF of 79.23%.To our knowledge,the PCE value should be the highest for binary spacer MA-based 2DRP(n≤5)PSCs to date.Importantly,owing to the hydrophobic fluorine group of FPEA and the enhanced interlayer interaction by FPEA,the unencapsulated 2DRP PSCs based on binary spacers exhibit much excellent humidity stability and thermal stability than the unary spacer counterparts.

Enhanced performance of solution-processed carbon nanotube transparent electrodes in foldable perovskite solar cells through vertical separation of binders by using eco-friendly parylene substrate

The successful utilization of an eco-friendly and biocompatible parylene-C substrate for high-performance solution-processed double-walled carbon nanotube(CNT)electrode-based perovskite solar cells(PSCs)was demonstrated.Through the use of a novel inversion transfer technique,vertical separation of the binders from the CNTs was induced,rendering a stronger p-doping effect and thereby a higher conductivity of the CNTs.The resulting foldable devices exhibited a power conversion efficiency of 18.11%,which is the highest reported among CNT transparent electrode-based PSCs to date,and withstood more than 10,000 folding cycles at a radius of 0.5 mm,demonstrating unprecedented mechanical stability.Furthermore,solar modules were fabricated using entirely laser scribing processes to assess the potential of the solution-processable nanocarbon electrode.Notably,this is the only one to be processed entirely by the laser scribing process and to be biocompatible as well as eco-friendly among the previously reported nonindium tin oxide-based perovskite solar modules.

Molecular Structure Tailoring of Organic Spacers for High‑Performance Ruddlesden–Popper Perovskite Solar Cells

Layer-structured Ruddlesden–Popper(RP)perovskites(RPPs)with decent stability have captured the imagination of the photovoltaic research community and bring hope for boosting the development of perovskite solar cell(PSC)technology.However,two-dimensional(2D)or quasi-2D RP PSCs are encountered with some challenges of the large exciton binding energy,blocked charge transport and poor film quality,which restrict their photovoltaic performance.Fortunately,these issues can be readily resolved by rationally designing spacer cations of RPPs.This review mainly focuses on how to design the molecular structures of organic spacers and aims to endow RPPs with outstanding photovoltaic applications.We firstly elucidated the important roles of organic spacers in impacting crystallization kinetics,charge transporting ability and stability of RPPs.Then we brought three aspects to attention for designing organic spacers.Finally,we presented the specific molecular structure design strategies for organic spacers of RPPs aiming to improve photovoltaic performance of RP PSCs.These proposed strategies in this review will provide new avenues to develop novel organic spacers for RPPs and advance the development of RPP photovoltaic technology for future applications.

Dimethylamine oxalate manipulating CsPbI_(3) perovskite film crystallization process for high efficiency carbon electrode based perovskite solar cells

Crystallization process determines the quality of perovskite films and the performances of resultant perovskite solar cells(PSCs).Dimethylamine oxalate has been proven as a multifunctional modulator,and is explored as an efficient additive in manipulating the crystallization process of CsPbI_(3) perovskite films.On one hand,oxalate serves as the precipitator that facilitates the nucleation process of intermediate.The larger size of intermediate is conductive to the larger size and smaller grain boundaries of resultant perovskite.On the other hand,in subsequent annealing process,the phase conversion and growth process of transient perovskite can be decelerated due to the strong interactions of oxalate with both dimethylamine cation(DMA^(+))and Pb^(2+).Due to the optimized crystallization kinetics,the morphology and quality of CsPbI_(3) perovskite films are comprehensively improved with lower defect concentrations,and charge recombination loss is effectively suppressed.Benefiting from the optimized crystal quality of perovskite films,the carbon electrode-based CsPbI_(3) PSCs exhibit a champion efficiency of 18.48%.This represents one of the highest levels among all hole transport layer-free inorganic perovskite solar cells.

Manipulating Crystal Growth and Secondary Phase PbI_(2)to Enable Efficient and Stable Perovskite Solar Cells with Natural Additives

In perovskite solar cells(PSCs),the inherent defects of perovskite film and the random distribution of excess lead iodide(PbI_(2))prevent the improvement of efficiency and stability.Herein,natural cellulose is used as the raw material to design a series of cellulose derivatives for perovskite crystallization engineering.The cationic cellulose derivative C-Im-CN with cyano-imidazolium(Im-CN)cation and chloride anion prominently promotes the crystallization process,grain growth,and directional orientation of perovskite.Meanwhile,excess PbI_(2)is transferred to the surface of perovskite grains or formed plate-like crystallites in local domains.These effects result in suppressing defect formation,decreasing grain boundaries,enhancing carrier extraction,inhibiting non-radiative recombination,and dramatically prolonging carrier lifetimes.Thus,the PSCs exhibit a high power conversion efficiency of 24.71%.Moreover,C-Im-CN has multiple interaction sites and polymer skeleton,so the unencapsulated PSCs maintain above 91.3%of their initial efficiencies after 3000 h of continuous operation in a conventional air atmosphere and have good stability under high humidity conditions.The utilization of biopolymers with excellent structure-designability to manage the perovskite opens a state-of-the-art avenue for manufacturing and improving PSCs.

Interfacial modification using the cross-linkable tannic acid for highly-efficient perovskite solar cells with excellent stability

Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caused by a variety of reasons,including ions diffusion,surface and grain boundary defects,etc.In this work,the cross-linkable tannic acid(TA)is introduced to modify perovskite film through post-treatment method.The numerous organic functional groups(–OH and C=O)in TA can interact with the uncoordinated Pb^(2+)and I^(-)ions in perovskite,thus passivating defects and inhibiting ions diffusion.In addition,the formed TA network can absorb a small amount of the residual moisture inside the device to protect the perovskite layer.Furthermore,TA modification regulates the energy level of perovskite,and reduces interfacial charge recombination.Ultimately,following TA treatment,the device efficiency is increased significantly from 21.31%to 23.11%,with a decreased hysteresis effect.Notably,the treated device shows excellent air,thermal,and operational stability.In light of this,the readily available,inexpensive TA has the potential to operate as a multipurpose interfacial modifier to increase device efficiency while also enhancing device stability.

Multifunctional interfacial molecular bridge enabled by an aggregation-induced emission strategy for enhancing efficiency and UV stability of perovskite solar cells

The interface defects between the electron transport layer(ETL)and the perovskite layer,as well as the low ultraviolet(UV)light utilization rate of the perovskite absorption layer,pose significant challenges for the commercialization of perovskite solar cells(PSCs).To address this issue,this paper proposes an innovative multifunctional interface modulation strategy by introducing aggregation-induced emission(AIE)molecule 5-[4-[1,2,2-tri[4-(3,5-dicarboxyphenyl)phenyl]ethylene]phenyl]benzene-1,3-dicarboxylic acid(H_(8)ETTB)at the SnO_(2)ETL/perovskite interface.Firstly,the interaction of H_(8)ETTB with the SnO_(2)surface,facilitated by its carboxyl groups,is effective in passivating surface defects caused by noncoord inated Sn and O vacancies.This interaction enhances the conductivity of the SnO_(2)film and adjusts energy levels,leading to enhanced charge carrier transport.Simultaneously,H_(8)ETTB can passivate noncoord inated Pb^(2+)ions at the perovskite interface,promoting perovskite crystallization and reducing the interface energy barrier,resulting in a perovskite film with low defects and high crystalline quality.More importantly,the H_(8)ETTB molecule,can convert UV light into light absorbable by the perovskite,thereby reducing damage caused by UV light and improving the device's utilization of UV.Consequently,the champion PSC based on SnO_(2)-H_(8)ETTB achieves an impressing efficiency of 23.32%and significantly improved photostability compared with the control device after continuous exposure to intense UV radiation.In addition,the Cs_(0.05)(FA_(0.95)MA_(0.05))_(0.95)Pb(I_(0.95)Br_(0.05))_(3)based device can achieve maximum efficiency of 24.01%,demonstrating the effectiveness and universality of this strategy.Overall,this innovative interface bridging strategy effectively tackles interface defects and low UV light utilization in PSCs,presenting a promising approach for achieving highly efficient and stable PSCs.

Side chain modulated ferrocene derivative as the interstitial conductive medium for high-performance and stable perovskite solar cells

The interfacial nonradiative recombination loss caused by the deep traps and mismatched band alignment restrained the commercial viability of perovskite solar cells(PSCs). Herein, we have constructed ferrocene carboxylic acid(FcA) and octafluoropentyl-ferrocenyl-carboxylate(OFFcA) interstitial conductive mediums to modulate the integral heterointerface properties and the photovoltaic performances of PSCs.By comparing the passivation strengths of the two molecules, we found that the synergistic effects among Fc/Fc^(+)redox shuttle, C=O group, and F substituents realize the optimal elimination of interfacial trap sources. Electron-withdrawing F groups reinforce the capacity of the Fc/Fc^(+)redox shuttle for the healing of metallic Pb defects and provide extensive anchoring sites to stabilize the organic components.Additionally, the homogeneity of the OFFcA layer as well as the humidity stability of perovskite film are facilitated through the introduction of F substituents, which reduce the contact resistance and improve the interfacial charge transfer. The champion OFFcA-modified device delivers an exceptional PCE of 23.62%, exceeding those of the control(PCE=22.32%) and FcA-modified(PCE=23.06%) devices.Moreover, the unencapsulated OFFcA-modified device retains 82.7% of the primary efficiency at 60%RH for more than 50 d and only loses less than 10% of the primary efficiency when stored in a glove box for more than 2000 h.

Chlorofullerene C_(60)Cl_(6) Enables Efficient and Stable Tin-Based Perovskite Solar Cells

Tin-based perovskite solar cells(TPSCs)have received great attention due to their eco-friendly properties and high theoretical efficiencies.However,the fast crystallization feature of tin-based perovskites leads to poor film quality and limits the corresponding device performance.Herein,a chlorofullerene,C_(60)Cl_(6),with six chlorine attached to the C_(60)cage,is applied to modulate the crystallization process and passivate grain boundary defects of the perovskite film.The chemical interactions between C_(60)Cl_(6)and perovskite components retard the transforming process of precursors to perovskite crystals and obtain a high-quality tin-based perovskite film.It is also revealed that the C_(60)Cl_(6)located at the surfaces and grain boundaries can not only passivate the defects but also offer a role in suturing grain boundaries to suppress the detrimental effects of water and oxygen on perovskite films,especially the oxidation of Sn^(2+)to Sn^(4+).As a result,the C_(60)Cl_(6)-based device yields a remarkably improved device efficiency from 10.03%to 13.30%with enhanced stability.This work provides a new strategy to regulate the film quality and stability of TPSCs using functional fullerene materials.