Piperazine-Assisted Construction of 2D/3D Wide-Bandgap Perovskite for Realizing High-Efficiency Perovskite/Organic Tandem Solar Cells

Monolithic perovskite/organic tandem solar cells(TsCs)have gained significant attention due to their easy device integration and the potential to surpass the Shockley-Queisser limit of single-junction solar cells.However,the surfaces of wide-bandgap perovskite films are densely populated with defects,leading to severe non-radiative recombination and energy loss.As a consequence,the power conversion efficiency(PCE)of perovskite/organic TSCs lags behind that of other TSC counterparts.To address these issues,we designed a functional ammonium salt,4-(2-hydroxyethyl)piperazin-1-ium iodide(Pzol),comprising a piperazine iodide and a terminated hydroxyl group,which was applied for post-treating the perovskite surface.Our findings reveal that Pzol reacts with and consumes residual PbX_(2)(X:I or Br)to form a 2D perovskite component,thereby eliminating Pb^(0)defects,while the terminated hydroxyl group in PZOI can also passivate uncoordinated Pb^(2+).Consequently,the shallow/deep-level defect densities of the 2D/3D perovskite film were significantly reduced,leading to an enhanced PCE of single-junction 2D/3D wide-bandgap perovskite solar cells to 18.18% with a reduced energy loss of 40 mev.Importantly,the corresponding perovskite/organic TSCs achieved a remarkable PCE of 24.05% with enhanced operational stability(T_(90)~500h).

Understanding the role of interconnecting layer on determining monolithic perovskite/organic tandem device carrier recombination properties

As one of the core parts of two-terminal(2 T) monolithic tandem photovoltaics, the interconnecting layers(ICLs) play a critical role in modulating the carrier transport and recombination between the sub-cells,and thus influencing the tandem device performance. Here, for the first time, the relationship between ICLs architecture and 2 T monolithic perovskite/organic tandem device performance has been studied by investigating the change of ICLs composition layer thickness on the ICLs optical and electrical properties, sub-cells EQE properties, and tandem device J-V properties. It is revealed that the ability of ICLs on modulating the sub-cells carrier balance properties is strongly associated with its composited layers thickness, and the tandem device carrier balance properties can be reflected by the relative EQE intensity between the sub-cells. Finally, with a deep understanding of the mechanisms, rational design of ICLs can be made to benefit the tandem device development. Based on the optimized ICL a high PCE of 20.03% is achieved.

Ti_(3)C_(2)T_(x) MXene for organic/perovskite optoelectronic devices

MXenes are emerging two-dimensional(2D)nanomaterials composed of transition metal carbides and/or nitrides and possess unique layered structures with abundant surface functional groups,which enable them with excellent and tunable properties.MXenes films can be solution-processed in polar solvents and are very suitable for optoelectronic device applications.Especially,Ti_(3)C_(2)T_(x) MXene with the clear advantages of facile synthesis,flexible surface controlling,easily tunable work function,high optical transmittance and excellent conductivity shows great potential for applications in organic/perovskite optoelectronic devices.Therefore,this review briefly introduces the mainstream synthesis methods,optical and electrical properties of MXenes,and comprehensively summarizes the versatile applications of Ti_(3)C_(2)T_(x) MXene in different functional layers(electrode,interface layer and active layer)of organic/perovskite optoelectronic devices including solar cells and light-emitting diodes.Finally,the current application characteristics and the future possibilities of MXenes in organic/perovskite optoelectronic devices are concluded and discussed.

Recent progress on advanced transmission electron microscopy characterization for halide perovskite semiconductors

Halide perovskites are strategically important in the field of energy materials. Along with the rapid development of the materials and related devices, there is an urgent need to understand the structure–property relationship from nanoscale to atomic scale. Much effort has been made in the past few years to overcome the difficulty of imaging limited by electron dose,and to further extend the investigation towards operando conditions. This review is dedicated to recent studies of advanced transmission electron microscopy(TEM) characterizations for halide perovskites. The irradiation damage caused by the interaction of electron beams and perovskites under conventional imaging conditions are first summarized and discussed. Low-dose TEM is then discussed, including electron diffraction and emerging techniques for high-resolution TEM(HRTEM) imaging. Atomic-resolution imaging, defects identification and chemical mapping on halide perovskites are reviewed. Cryo-TEM for halide perovskites is discussed, since it can readily suppress irradiation damage and has been rapidly developed in the past few years. Finally, the applications of in-situ TEM in the degradation study of perovskites under environmental conditions such as heating,biasing, light illumination and humidity are reviewed. More applications of emerging TEM characterizations are foreseen in the coming future, unveiling the structural origin of halide perovskite’s unique properties and degradation mechanism under operando conditions, so to assist the design of a more efficient and robust energy material.

Reducing surficial and interfacial defects by thiocyanate ionic liquid additive and ammonium formate passivator for efficient and stable perovskite solar cells

Organic–inorganic metal halide perovskites have attained extensive attention owing to their outstanding photovoltaic performances,but the existence of numerous defects in crystalline perovskites is still a serious constraint for the further development of perovskite solar cells(PSCs).In particular,the rapid crystallization guided by anti-solvents leads to plenty of surficial and interfacial defects in perovskite films.Herein,we report the adoption of a pseudo-halide anion based ionic liquid additive,1-butyl-3-methylimidazolium thiocyanate(BMIMSCN)for growing ternary cation(CsFAMA,where FA=formamidinium and MA=methylammonium)perovskites with large-scale crystal grains and strong preferential orientation via the enhanced Ostwald ripening.Meanwhile,a novel halide-free passivator,benzylammonium formate(BAFa),was employed as a buffering layer on the perovskite films to suppress surface-dominated charge recombination.As a result,the cooperative effects of BMIMSCN additive and BAFa passivator lead to significant enhancements on fluorescence lifetime(from 79.41 to 201.01 ns),open-circuit voltage(from 1.13 to 1.19 V),photoelectric conversion efficiency(from 18.90%to 22.33%).Moreover,the BMIMSCN/BAFa-CsFAMA PSCs demonstrated greatly improved stability against moisture and heat.This work suggests a promising strategy to improve the quality of perovskite materials via reducing the surficial and interfacial defects by the synergistic effects of lattice doping and interface engineering.

Recent advances in perovskite/organic integrated solar cells

The integrated perovskite/organic solar cell(IPOSC) is widely concerned as an effective approach to broaden the spectrum of perovskite solar cell(PerSC) by utilizing near-infrared light of lower bandgap organic semiconductor. Compared to tandem solar cells, the IPOSCs eliminate the preparation of the intermediate layer and simplify the manufacturing process, but retain the advantages of wide light harvesting. Meanwhile, the IPOSCs can maintain the open-circuit voltage as high as PerSCs. This review summarizes the recent developments of perovskite materials and low-bandgap organic conjugated materials applied in solar cells. Then, the working mechanism of IPOSCs and the recent developments of IPOSCs based on low-bandgap donor and acceptor materials are highlighted. Besides, the study of charge dynamic in IPOSC is summarized. Finally, the potential of IPOSCs and approach to improve device performance are also envisaged.

Novel broad spectral response perovskite solar cells:A review of the current status and advanced strategies for breaking the theoretical limit efficiency

Perovskite solar cells(PSCs)have revolutionized photovoltaic research.The power conversion efficiency(PCE)of PSCs has now reached 25.7%,which is comparable to current state-of-the-art silicon-based cells.However,PSCs can only utilize light of 300-850 nm,resulting in wasted near-infrared(NIR)light,which occupies 45%-50%of entire solar spectrum,which is one of the main reasons limiting the development of efficiency.Related strategies to broaden NIR spectroscopy to break the theoretical limit efficiency of PSCs have recently attracted extensive attention.This review firstly outlines theoretical basis for improving the NIR spectroscopy,then systematically summarizes some key strategies and research progress to improve NIR spectroscopy of PSCs.We firstly provided a comprehensive overview of historical research experiments on narrow-gap perovskite absorber layers,rare earth up-conversion,tandem devices,and integrated perovskite/organic solar cells and given constructive suggestions for exceeding limit efficiency of PSCs.Finally,based on the development status of PSCs with NIR utilization,the current issues,solutions and future development directions of important aspects to improve NIR utilization of PSCs are systematically discussed.This review lays the foundation for the efficiency of PSCs beyond the Shockley-Queisser limit,and provides a certain development prospect.

Organic functional materials based buffer layers for efficient perovskite solar cells

In this review, we highlight the recent development of organic π-functional materials as buffer layers in constructing efficient perovskite solar cells（PVSCs）. By following a brief introduction on the PVSC development, device architecture and material design features, we exemplified the exciting progresses made in field by exploiting organic π-functional materials based hole and electron transport layers（HTLs and ETLs） to enable high-performance PVSCs.

Porphyrinic Acceptors forFullerene-Free MolecularPhotovoltaics

Over the past few years,the development of nonfullerene acceptors(NFAs)has become a prominent focus in both organic and perovskite solar cell(OSCs and PSCs,respectively)research fields.In this context,porphyrinoids,compounds structurally related to porphyrins,have emerged as promising solar cell candidates.In contrast to the widely used fullerene acceptors,porphyrinoids exhibit strong,broad absorption properties across the UV–vis/NIR spectrum,which can be easily tuned through chemical modifications.Furthermore,they can be prepared and derivatized using cost-effective and straightforward methodologies,allowing for convenient adjustments in thin-film morphology,processability,supramolecular organization,and energy levels.Additionally,these compounds offer higher thermal and photochemical stability,resulting in longer device lifetimes compared to their fullerene-based counterparts.In this review,we outline the utilization of porphyrinoids as NFAs in OSCs and PSCs,discussing essential aspects such as design guidelines,molecular properties,and device configuration.Our goal is to inspire and further promote the development of n-type porphyrinoids,which have not yet fully unleashed their potential.