Interface optimization and defects suppression via Na F introduction enable efficient flexible Sb_(2)Se_(3) thin-film solar cells

Sb_(2)Se_(3) with unique one-dimensional(1D) crystal structure exhibits exceptional deformation tolerance,demonstrating great application potential in flexible devices.However,the power conversion efficiency(PCE) of flexible Sb_(2)Se_(3) photovoltaic devices is temporarily limited by the complicated intrinsic defects and the undesirable contact interfaces.Herein,a high-quality Sb_(2)Se_(3) absorber layer with large crystal grains and benign [hkl] growth orientation can be first prepared on a Mo foil substrate.Then NaF intermediate layer is introduced between Mo and Sb_(2)Se_(3),which can further optimize the growth of Sb_(2)Se_(3)thin film.Moreover,positive Na ion diffusion enables it to dramatically lower barrier height at the back contact interface and passivate harmful defects at both bulk and heterojunction.As a result,the champion substrate structured Mo-foil/Mo/NaF/Sb_(2)Se_(3)/CdS/ITO/Ag flexible thin-film solar cell delivers an obviously higher efficiency of 8.03% and a record open-circuit voltage(V_(OC)) of 0.492 V.This flexible Sb_(2)Se_(3) device also exhibits excellent stability and flexibility to stand large bending radius and multiple bending times,as well as superior weak light photo-response with derived efficiency of 12.60%.This work presents an effective strategy to enhance the flexible Sb_(2)Se_(3) device performance and expand its potential photovoltaic applications.

Back contact interfacial modification mechanism in highly-efficient antimony selenide thin-film solar cells

Antimony selenide(Sb_(2)Se_(3))is a potential photovoltaic(PV)material for next-generation solar cells and has achieved great development in the last several years.The properties of Sb_(2)Se_(3)absorber and back contact influence the PV performances of Sb_(2)Se_(3)solar cells.Hence,optimization of back contact characteristics and absorber orientation are crucial steps in raising the power conversion efficiency(PCE)of Sb_(2)Se_(3)solar cells.In this work,MoO2was introduced as an intermediate layer(IL)in Sb_(2)Se_(3)solar cells,and comparative investigations were conducted.The growth of(211)-oriented Sb_(2)Se_(3)with large grains was facilitated by introducing the MoO2IL with suitable thickness.The MoO2IL substantially lowered the back contact barrier and prevented the formation of voids at the back contact,which reduced the thickness of the MoSe2interface layer,inhibited carrier recombination,and minimized bulk and interfacial defects in devices.Subsequently,significant optimization enhanced the open-circuit voltage(VOC)of solar cells from 0.481 V to 0.487 V,short-circuit current density(JSC)from 23.81 m A/cm^(2)to 29.29 m A/cm^(2),and fill factor from 50.28%to 57.10%,which boosted the PCE from 5.75%to 8.14%.

Design of periodic metal-insulator-metal waveguide back structures for the enhancement of light absorption in thin-film solar cells

To increase the absorption in a thin layer of absorbing material （amorphous silicon, a-Si）, a light trapping design is presented. The designed structure incorporates periodic metal-insulator-metal waveguides to enhance the optical path length of light within the solar cells. The new design can result in broadband optical absorption enhancement not only for transverse magnetic （TM）-polarized light, but also for transverse electric （TE）-polarized light. No plasmonic modes can be excited in TE-polarization, but because of the coupling into the a-Si planar waveguide guiding modes and the diffraction of light by the bottom periodic structures into higher diffraction orders, the total absorption in the active region is also increased. The results from rigorous coupled wave analysis show that the overall optical absorption in the active layer can be greatly enhanced by up to 40%. The designed structures presented in this paper can be integrated with back contact technology to potentially produce high-efficiency thin-film solar cell devices.

Improvement of the Open Circuit Voltage of CZTSe Thin-Film Solar Cells by Surface Sulfurization Using SnS

The objective of this study is to find an effective method to improve Voc without Jsc loss for Cu2ZnSnSe4 （CZTSe） thin film solar cells, which have been fabricated by the one step co-evaporation technique. Surface sulfurization of CZTSe thin films is carried out by using one technique that does not utilize toxic H2S gas; a sequential evaporation of SnS after CZTSe deposition and the annealing of CZTSe thin films in selenium vapor. A Cu2ZnSn（S, Se）4 （CZTSSe） thin layer is grown on the surface of the CZTSe thin film after the annealing. The conversion efficiency of the completed device is improved due to the enhancement of Voc, which could be attributed to the formation of a hole-recombination barrier at the surface or the passivation of the surface and grain boundary by S incorporation.

β-FeSi_2 as the bottom absorber of triple-junction thin-film solar cells: A numerical study

Using β-FeSi2 as the bottom absorber of triple-junction thin-film solar cells is investigated by a numerical method for widening the long-wave spectral response. The presented results show that the β-FeSi2 subcell can contribute 0.273 V of open-circuit voltage to the a-Si/μc-Si/β-FeSi2 triple-junction thin-film solar cell. The optimized absorber thicknesses for a- Si, μ-Si, and/3-FeSi2 subcells are 260 nm, 900 nm, and 40 nm, respectively. In addition, the temperature coefficient of the conversion efficiency of the a-Si/μc-Si//3-FeSi2 cell is -0.308 %/K, whose absolute value is only greater than that of the a-Si subcell. This result indicates that the a-Si/μc-Si/β-FeSi2 triple-junction solar cell has a good temperature coefficient. As a result, using β-FeSi2 as the bottom absorber can improve the thin-film solar cell performance, and the a-Si/μc-Si/β-FeSi2 triple-junction solar cell is a promising structure configuration for improving the solar cell efficiency.

Non-ionizing energy loss calculations for modeling electron-induced degradation of Cu(In,Ga)Se_2 thin-film solar cells

The lowest energies which make Cu,In,Ga,and Se atoms composing Cu（In,Ga）Se_2（CIGS） material displaced from their lattice sites are evaluated,respectively.The non-ionizing energy loss（NIEL） for electron in CIGS material is calculated analytically using the Mott differential cross section.The relation of the introduction rate（k） of the recombination centers to NIEL is modified,then the values of k at different electron energies are calculated.Degradation modeling of CIGS thin-film solar cells irradiated with various-energy electrons is performed according to the characterization of solar cells and the recombination centers.The validity of the modeling approach is verified by comparison with the experimental data.

Step‑by‑Step Modulation of Crystalline Features and Exciton Kinetics for 19.2%Efficiency Ortho‑Xylene Processed Organic Solar Cells

With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices.However,previous studies are heavily based in chloroform(CF)leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component.Herein,we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy,named BTP-BO-3FO with enlarged bandgap,brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9,processed by CF and ortho-xylene(o-XY).With detailed analyses supported by a series of experiments,the best PCE of 19.24%for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif,which furthermore nourishes a favorable charge generation and recombination behavior.Likewise,over 19%PCE can be achieved by replacing spin-coating with blade coating for active layer deposition.This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance,hence,will be instructive to other ternary OSC works in the future.

Manipulating the Macroscopic and Microscopic Morphology of Large-Area Gravure-Printed ZnO Films for High-Performance Flexible Organic Solar Cells

Gravure printing is a promising large-scale fabrication method for flexible organic solar cells(FOSCs)because it is compatible with two-dimension patternable roll-to-roll fabrication.However,the unsuitable rheological property of ZnO nanoinks resulted in unevenness and looseness of the gravure-printed ZnO interfacial layer.Here we propose a strategy to manipulate the macroscopic and microscopic of the gravure-printed ZnO films through using mixed solvent and poly(vinylpyrrolidone)(PVP)additive.The regulation of drying speed effectively manipulates the droplets fusion and leveling process and eliminates the printing ribbing structure in the macroscopic morphology.The additive of PVP effectively regulates the rheological property and improves the microscopic compactness of the films.Following this method,large-area ZnO∶PVP films(28×9 cm^(2))with excellent uniformity,compactness,conductivity,and bending durability were fabricated.The power conversion efficiencies of FOSCs with gravure-printed AgNWs and ZnO∶PVP films reached 14.34%and 17.07%for the 1 cm^(2)PM6:Y6 and PM6∶L8-BO flexible devices.The efficiency of 17.07%is the highest value to date for the 1 cm^(2)FOSCs.The use of mixed solvent and PVP addition also significantly enlarged the printing window of ZnO ink,ensuring high-quality printed thin films with thicknesses varying from 30 to 100 nm.

Accelerated Sequential Deposition Reaction via Crystal Orientation Engineering for Low-Temperature,High-Efficiency Carbon-Electrode CsPbBr_(3) Solar Cells

Low-temperature,ambient processing of high-quality CsPbBr_(3)films is demanded for scalable production of efficient,low-cost carbon-electrode perovskite solar cells(PSCs).Herein,we demonstrate a crystal orientation engineering strategy of PbBr_(2)precursor film to accelerate its reaction with CsBr precursor during two-step sequential deposition of CsPbBr_(3)films.Such a novel strategy is proceeded by adding CsBr species into PbBr_(2)precursor,which can tailor the preferred crystal orientation of PbBr_(2)film from[020]into[031],with CsBr additive staying in the film as CsPb_(2)Br_(5)phase.Theoretical calculations show that the reaction energy barrier of(031)planes of PbBr_(2)with CsBr is lower about 2.28 eV than that of(O2O)planes.Therefore,CsPbBr_(3)films with full coverage,high purity,high crystallinity,micro-sized grains can be obtained at a low temperature of 150℃.Carbon-electrode PSCs with these desired CsPbBr_(3)films yield the record-high efficiency of 10.27%coupled with excellent operation stability.Meanwhile,the 1 cm^(2)area one with the superior efficiency of 8.00%as well as the flexible one with the champion efficiency of 8.27%and excellent mechanical bending characteristics are also achieved.

Numerical Study and Optimization of CZTS-Based Thin-Film Solar Cell Structure with Different Novel Buffer-Layer Materials Using SCAPS-1D Software

This study explored the performances of CZTS-based thin-film solar cell with three novel buffer layer materials ZnS, CdS, and CdZnS, as well as with variation in thickness of buffer and absorber-layer, doping concentrations of absorber-layer material and operating temperature. Our aims focused to identify the most optimal thin-film solar cell structure that offers high efficiency and lower toxicity which are desirable for sustainable and eco-friendly energy sources globally. SCAPS-1D, widely used software for modeling and simulating solar cells, has been used and solar cell fundamental performance parameters such as open-circuited voltage (), short-circuited current density (), fill-factor() and efficiency() have been optimized in this study. Based on our simulation results, it was found that CZTS solar cell with Cd0.4Zn0.6S as buffer-layer offers the most optimal combination of high efficiency and lower toxicity in comparison to other structure investigated in our study. Although the efficiency of Cd0.4Zn0.6S, ZnS and CdS are comparable, Cd0.4Zn0.6S is preferable to use as buffer-layer for its non-toxic property. In addition, evaluation of performance as a function of buffer-layer thickness for Cd0.4Zn0.6S, ZnS and CdS showed that optimum buffer-layer thickness for Cd0.4Zn0.6S was in the range from 50 to 150nm while ZnS offered only 50 – 75 nm. Furthermore, the temperature dependence performance parameters evaluation revealed that it is better to operate solar cell at temperature 290K for stable operation with optimum performances. This study would provide valuable insights into design and optimization of nanotechnology-based solar energy technology for minimizing global energy crisis and developing eco-friendly energy sources sustainable and simultaneously.

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.

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.

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.

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.

H-and J-aggregation of conjugated small molecules in organic solar cells

As H-and J-aggregation receive more and more attention in the research of organic solar cells(OSCs),especially in small molecular systems,deep understanding of aggregation behavior is needed to guide the design of conjugated small molecular structure and the fabrication process of OSC device.For this end,this review is written.Here,the review firstly introduced the basic information about H-and J-aggregation of conjugated small molecules in OSCs.Then,the characteristics of H-and J-aggregation and the methods to identify them were summarized.Next,it reviewed the research progress of H-and J-aggregation of conjugated small molecules in OSCs,including the factors influencing H-and J-aggregation in thin film and the effects of H-and J-aggregation on OPV performance.

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.

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.

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.

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.

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.