Efficient Monolithic Perovskite/Silicon Tandem Photovoltaics

Tunable bandgaps make halide perovskites promising candidates for developing tandem solar cells(TSCs),a strategy to break the radiative limit of 33.7%for single-junction solar cells.Combining perovskites with market-dominant crystalline silicon(c-Si)is particularly attractive;simple estimates based on the bandgap matching indicate that the efficiency limit in such tandem device is as high as 46%.However,state-of-the-art perovskite/c-Si TSCs only achieve an efficiency of~32.5%,implying significant challenges and also rich opportunities.In this review,we start with the operating mechanism and efficiency limit of TSCs,followed by systematical discussions on wide-bandgap perovskite front cells,interface selective contacts,and electrical interconnection layer,as well as photon management for highly efficient perovskite/c-Si TSCs.We highlight the challenges in this field and provide our understanding of future research directions toward highly efficient and stable large-scale wide-bandgap perovskite front cells for the commercialization of perovskite/c-Si TSCs.

Textured Perovskite/Silicon Tandem Solar Cells Achieving Over 30% Efficiency Promoted by 4-Fluorobenzylamine Hydroiodide

Monolithic textured perovskite/silicon tandem solar cells(TSCs)are expected to achieve maximum light capture at the lowest cost,potentially exhibiting the best power conversion efficiency.However,it is challenging to fabricate high-quality perovskite films and preferred crystal orientation on commercially textured silicon substrates with micrometersize pyramids.Here,we introduced a bulky organic molecule(4-fluorobenzylamine hydroiodide(F-PMAI))as a perovskite additive.It is found that F-PMAI can retard the crystallization process of perovskite film through hydrogen bond interaction between F^(−)and FA^(+)and reduce(111)facet surface energy due to enhanced adsorption energy of F-PMAI on the(111)facet.Besides,the bulky molecular is extruded to the bottom and top of perovskite film after crystal growth,which can passivate interface defects through strong interaction between F-PMA+and undercoordinated Pb^(2+)/I^(−).As a result,the additive facilitates the formation of large perovskite grains and(111)preferred orientation with a reduced trap-state density,thereby promoting charge carrier transportation,and enhancing device performance and stability.The perovskite/silicon TSCs achieved a champion efficiency of 30.05%based on a silicon thin film tunneling junction.In addition,the devices exhibit excellent longterm thermal and light stability without encapsulation.This work provides an effective strategy for achieving efficient and stable TSCs.

Efficiency-loss analysis of monolithic perovskite/silicon tandem solar cells by identifying the patterns of a dual two-diode model’s current-voltage curves

In this work,we developed a simple and direct circuit model with a dual two-diode model that can be solved by a SPICE numerical simulation to comprehensively describe the monolithic perovskite/crystalline silicon(PVS/c-Si)tandem solar cells.We are able to reveal the effects of different efficiency-loss mechanisms based on the illuminated current density-voltage(J-V),semi-log dark J-V,and local ideality factor(m-V)curves.The effects of the individual efficiency-loss mechanism on the tandem cell’s efficiency are discussed,including the exp(V/VT)and exp(V/2VT)recombination,the whole cell’s and subcell’s shunts,and the Ohmic-contact or Schottky-contact of the intermediate junction.We can also fit a practical J-V curve and find a specific group of parameters by the trial-and-error method.Although the fitted parameters are not a unique solution,they are valuable clues for identifying the efficiency loss with the aid of the cell’s structure and experimental processes.This method can also serve as an open platform for analyzing other tandem solar cells by substituting the corresponding circuit models.In summary,we developed a simple and effective methodology to diagnose the efficiency-loss source of a monolithic PVS/c-Si tandem cell,which is helpful to researchers who wish to adopt the proper approaches to improve their solar cells.

Perovskite/Silicon Tandem Solar Cells: From Detailed Balance Limit Calculations to Photon Management

Energy conversion efficiency losses and limits of perovskite/silicon tandem solar cells are investigated by detailed balance calculations and photon management.An extended Shockley-Queisser model is used to identify fundamental loss mechanisms and link the losses to the optics of solar cells.Photon management is used to minimize losses and maximize the energy conversion efficiency.The influence of photon management on the solar cell parameters of a perovskite single-junction solar cell and a perovskite/silicon solar cell is discussed in greater details.An optimized solar cell design of a perovskite/silicon tandem solar cell is presented,which allows for the realization of solar cells with energy conversion efficiencies exceeding 32%.

Composite electron transport layer for efficient N-I-P type monolithic perovskite/silicon tandem solar cells with high open-circuit voltage

Perovskite/silicon tandem solar cells(PSTSCs) have exhibited huge technological potential for breaking the Shockley-Queisser limit of single-junction solar cells. The efficiency of P-I-N type PSTSCs has surpassed the single-junction limit, while the performance of N-I-P type PSTSCs is far below the theoretical value. Here, we developed a composite electron transport layer for N-I-P type monolithic PSTSCs with enhanced open-circuit voltage(VOC) and power conversion efficiency(PCE). Lithium chloride(Li Cl) was added into the tin oxide(SnO_(2)) precursor solution, which simultaneously passivated the defects and increased the electron injection driving force at the electron transfer layer(ETL)/perovskite interface.Eventually, we achieved monolithic PSTSCs with an efficiency of 25.42% and V_(OC) of 1.92 V, which is the highest PCE and VOCin N-I-P type perovskite/Si tandem devices. This work on interface engineering for improving the PCE of monolithic PSTSCs may bring a new hot point about perovskite-based tandem devices.

Stress and Strain in Perovskite/Silicon Tandem Solar Cells

Tandem solar cells based on metal halide perovskites are advancing rapidly during last few years[1–17].The certified power conversion efficiency(PCE)for monolithic perovskite/silicon tandem solar cell reaches 32.5%[18].Since tandem solar cells contain more layers than single-junction solar cells,stress/strain control is an issue during fabrication and further practical operation.The stress can not only affect the stability of the perovskite layer but also change the optoelectronic properties of the films[19–23].

Monolithic perovskite/silicon tandem solar cells offer an efficiency over 29%

Organic-inorganic hybrid perovskite semiconductors pos-sessing superior optoelectronic properties(e.g.long carrier dif-fusion lengths,high optical absorption coefficient,low ex-citon binding energy,and high defect tolerance)are attract-ing serious attention.The certified power conversion effi-ciency(PCE)for single-junction perovskite solar cells have ex-ceeded 25%^([1,2]).As a very promising PCE-enhancement strategy,tandem structure made by stacking a perovskite cell on a market-dominant silicon cell can yield much higher PCEs beyond the Shockley-Queisser limit of single-junction devices without adding substantial cost^([3]).

How to enable highly efficient and large‐area fabrication on specific textures for monolithic perovskite/silicon tandem solar cells?

Perovskite/silicon tandem solar cells(PVSK/Si TSCs)have emerged as a promising photovoltaic technology toward achieving a high power conversion efficiency(PCE)along with cost‐effective manufacturing.The PCE of PVSK/Si TSCs has skyrocketed to a certified 33.9%,surpassing the theoretical limit of any single‐junction solar cell.This achievement is partially attributed to ad-vancements in surface textures for Si bottom cells.In this regard,we present an overview of the recent developments concerning surface textures of Si in monolithic PVSK/Si TSCs,including planar,pyramid texture,and nanotexture.Following,the prevailing perovskite deposition methods on these textures are thoroughly discussed,and the corresponding challenges are evaluated.Addi-tionally,we provide a summary of the advanced morphological,structural,optical,and electrical characterization techniques being utilized for theses textures.Finally,the prospects for further development of PVSK/Si TSCs are outlined,including designing novel textures with industrial compatibility,developing perovskite deposition methods with scalability,and exploring more pertinent characterization techniques for textured PVSK/Si TSCs.

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.

Exploring Nanoscale Perovskite Materials for Next‑Generation Photodetectors:A Comprehensive Review and Future Directions

The rapid advancement of nanotechnology has sparked much interest in applying nanoscale perovskite materials for photodetection applications.These materials are promising candidates for next-generation photodetectors(PDs)due to their unique optoelectronic properties and flexible synthesis routes.This review explores the approaches used in the development and use of optoelectronic devices made of different nanoscale perovskite architectures,including quantum dots,nanosheets,nanorods,nanowires,and nanocrystals.Through a thorough analysis of recent literature,the review also addresses common issues like the mechanisms underlying the degradation of perovskite PDs and offers perspectives on potential solutions to improve stability and scalability that impede widespread implementation.In addition,it highlights that photodetection encompasses the detection of light fields in dimensions other than light intensity and suggests potential avenues for future research to overcome these obstacles and fully realize the potential of nanoscale perovskite materials in state-of-the-art photodetection systems.This review provides a comprehensive overview of nanoscale perovskite PDs and guides future research efforts towards improved performance and wider applicability,making it a valuable resource for researchers.

Low‑Temperature Fabrication of Stable Black‑Phase CsPbI_(3)Perovskite Flexible Photodetectors Toward Wearable Health Monitoring

Flexible wearable optoelectronic devices fabricated fromorganic–inorganic hybrid perovskites significantly accelerate the developmentof portable energy,biomedicine,and sensing fields,but their poor thermal stabilityhinders further applications.Conversely,all-inorganic perovskites possessexcellent thermal stability,but black-phase all-inorganic perovskite filmusually requires high-temperature annealing steps,which increases energy consumptionand is not conducive to the fabrication of flexible wearable devices.In this work,an unprecedented low-temperature fabrication of stable blackphaseCsPbI3perovskite films is demonstrated by the in situ hydrolysis reactionof diphenylphosphinic chloride additive.The released diphenyl phosphateand chloride ions during the hydrolysis reaction significantly lower the phasetransition temperature and effectively passivate the defects in the perovskitefilms,yielding high-performance photodetectors with a responsivity of 42.1 AW−1 and a detectivity of 1.3×10^(14)Jones.Furthermore,high-fidelity imageand photoplethysmography sensors are demonstrated based on the fabricated flexible wearable photodetectors.This work provides a newperspective for the low-temperature fabrication of large-area all-inorganic perovskite flexible optoelectronic devices.

Graded Heterojunction Improves Wide-Bandgap Perovskite for Highly Efficient 4-Terminal Perovskite/Silicon Tandem Solar Cells

Wide-bandgap(WBG)perovskite solar cells(PSCs)are essential for highly efficient and stable silicon/perovskite tandem solar cells.In this study,we adopted a synthetic strategy with lead thiocyanate(Pb(SCN)_(2))additive and methylammonium chloride(MACl)posttreatment to enhance the crystallinity and improve the interface of WBG perovskite films with a bandgap of 1.68 eV.The excessive PbI_(2)was formed at grain boundaries and converted into MAPbI_(3-x)Cl_(x)perovskites,which are utilized to form the graded heterojunction(GHJ)and compressive strain.This is beneficial for passivating nonradiative recombination defects,suppressing halide phase segregation,and facilitating carrier extraction.Subsequently,the device with GHJ delivered a champion efficiency of 20.30%and superior stability in ambient air and under 85℃.Finally,we achieved a recorded efficiency of 30.91%for 4-terminal WBG perovskite/TOPCon tandem silicon solar cells.Our findings demonstrate a promising approach for fabricating efficient and stable WBG PSCs through the formation of GHJ.

Author Correction: ITO-free silicon-integrated perovskite electrochemical cell for light-emission and light-detection

Correction to:Opto-Electronic Advances https://doi.org/10.29026/oea.2023.220154 published online 26 April 2023 After the publication of this article1,it was brought to our attention that calculations of the PeLEC device elec-troluminescent(EL)efficiency contained a mistake,leading to an inaccurate quantity value.The device’s maxim-um EL efficiency constitutes not‘~120 klm/W’but‘4.3 lm/W’instead.Correction details are listed below.

Review of all-inorganic perovskites and their tandem solar cells with crystalline silicon

In widely studied organic-inorganic hybrid perovskites,the organic component tends to volatilize and decompose under high temperatures,oxygen,and humidity,which adversely affects the performance and longevity of the associated solar cells.In contrast,all-inorganic perovskites demonstrate superior stability under these conditions and offer photoelectric properties comparable to those of their hybrid counterparts.The potential of tandem solar cells(TSCs)made from all-inorganic perovskites is especially promising.This review is the first to address recent advancements in TSCs that use all-inorganic perovskites and crystalline silicon(c-Si),both domestically and internationally.This work provides a systematic and thorough analysis of the current challenges faced by these systems and proposes rational solutions.Additionally,we elucidate the regulatory mechanisms of all-inorganic perovskites and their TSCs when combined with c-Si,summarizing the corresponding patterns.Finally,we outline future research directions for all-inorganic perovskites and their TSCs with c-Si.This work offers valuable insights and references for the continued advancement of perovskitebased TSCs.

Self-polarized RGB device realized by semipolar micro-LEDs and perovskite-in-polymer films for backlight applications

In backlighting systems for liquid crystal displays,conventional red,green,and blue(RGB)light sources that lack polarization properties can result in a significant optical loss of up to 50%when passing through a polarizer.To address this inefficiency and optimize energy utilization,this study presents a high-performance device designed for RGB polarized emissions.The device employs an array of semipolar blueμLEDs with inherent polarization capabilities,coupled with mechanically stretched films of green-emitting CsPbBr3 nanorods and red-emitting CsPbI3-Cs4PbI6 hybrid nanocrystals.The CsPbBr3 nanorods in the polymer film offer intrinsic polarization emission,while the aligned-wire structures formed by the stable CsPbI3-Cs4PbI6 hybrid nanocrystals contribute to substantial anisotropic emissions,due to their high dielectric constant.The resulting device achieved RGB polarization degrees of 0.26,0.48,and 0.38,respectively,and exhibited a broad color gamut,reaching 137.2%of the NTSC standard and 102.5%of the Rec.2020 standard.When compared to a device utilizing c-plane LEDs for excitation,the current approach increased the intensity of light transmitted through the polarizer by 73.6%.This novel fabrication approach for polarized devices containing RGB components holds considerable promise for advancing next-generation display technologies.

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.

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.

Microwave shock motivating the Sr substitution of 2D porous GdFeO_(3) perovskite for highly active oxygen evolution

The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.

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 engineering through lead binding using crown ethers in perovskite solar cells

In the domain of perovskite solar cells(PSCs),the imperative to reconcile impressive photovoltaic performance with lead-related issue and environmental stability has driven innovative solutions.This study pioneers an approach that not only rectifies lead leakage but also places paramount importance on the attainment of rigorous interfacial passivation.Crown ethers,notably benzo-18-crown-6-ether(B18C6),were strategically integrated at the perovskite-hole transport material interface.Crown ethers exhibit a dual role:efficiently sequestering and immobilizing Pb^(2+)ions through host-guest complexation and simultaneously establishing a robust interfacial passivation layer.Selected crown ether candidates,guided by density functional theory(DFT)calculations,demonstrated proficiency in binding Pb2+ions and optimizing interfacial energetics.Photovoltaic devices incorporating these materials achieved exceptional power conversion efficiency(PCE),notably 21.7%for B18C6,underscoring their efficacy in lead binding and interfacial passivation.Analytical techniques,including time-of-flight secondary ion mass spectrometry(ToF-SIMS),ultraviolet photoelectron spectroscopy(UPS),time-resolved photoluminescence(TRPL),and transient absorption spectroscopy(TAS),unequivocally affirmed Pb^(2+)ion capture and suppression of non-radiative recombination.Notably,these PSCs maintained efficiency even after enduring 300 h of exposure to 85%relative humidity.This research underscores the transformative potential of crown ethers,simultaneously addressing lead binding and stringent interfacial passivation for sustainable PSCs poised to commercialize and advance renewable energy applications.