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  1. Spontaneous formation of robust two-dimensional perovskite phases

    The two-dimensional on three-dimensional (2D/3D) perovskite bilayer heterostructure can improve the stability and performance of perovskite solar cells. Here, we show that the 2D/3D perovskite stack in a device evolves dynamically during its end-of-life decomposition. Initially phase-pure 2D interlayers can evolve differently, resulting in different device stabilities. We show that a robust 2D interlayer can be formed using mixed solvents to regulate its crystallinity and phase purity. The resulting 2D/3D devices achieved 25.9% efficiency and had good durability, retaining 91% of their initial performance after 1074 hours at 85°C using maximum power point tracking.
  2. A 2D/3D Heterostructure Perovskite Solar Cell with a Phase‐Pure and Pristine 2D Layer

    Abstract Interface engineering plays a critical role in advancing the performance of perovskite solar cells. As such, 2D/3D perovskite heterostructures are of particular interest due to their optoelectrical properties and their further potential improvements. However, for conventional solution‐processed 2D perovskites grown on an underlying 3D perovskite, the reaction stoichiometry is normally unbalanced with excess precursors. Moreover, the formed 2D perovskite is impure, leading to unfavorable energy band alignment at the interface. Here a simple method is presented that solves both issues simultaneously. The 2D formation reaction is taken first to completion, fully consuming excess PbI 2 . Then, isopropanol ismore » utilized to remove excess organic ligands, control the 2D perovskite thickness, and obtain a phase‐pure, n = 2, 2D perovskite. The outcome is a pristine (without residual 2D precursors) and phase‐pure 2D perovskite heterostructure with improved surface passivation and charge carrier extraction compared to the conventional solution process. PSCs incorporating this treatment demonstrate a notable improvement in both stability and power conversion efficiency, with negligible hysteresis, compared to the conventional process.« less
  3. Additive‐Free Oxidized Spiro‐MeOTAD Hole Transport Layer Significantly Improves Thermal Solar Cell Stability (in EN)

    Perovskite solar cells are among the most promising new solar technologies, already surpassing polycrystalline silicon solar cell efficiencies. The stability of the highest efficiency devices at elevated temperature is, however, poor. These cells typically use Spiro-MeOTAD as the hole transporting layer. It is generally believed that additives, required for enhancing electrical conductivity and optimizing energy level alignment, are responsible for the reduced stability—inferring that Spiro-MeOTAD based hole transporting layers are intrinsically unstable. Here, a reliable noble metal free synthesis of Spiro-MeOTAD (bis(trifluoromethane)sulfonimide)4 is presented which is used as the oxidizing agent. No additives are added to the partially oxidized Spiro-MeOTADmore » hole-transporting layer. Device efficiencies up to 24.2% are achieved. Electrical conductivity is largely developed by the first 1% oxidation. Further oxidation shifts the energy levels away from the vacuum level, which allows tuning of the energy level alignment without the use of additives—contradicting the current understanding of this system. Without additives, devices demonstrate significant improvement in stability at elevated temperatures up to 85 °C under one sun over 1400 h continuous illumination. The remaining degradation is pinpointed to ion migration and reactions in the perovskite layer which may be further suppressed with compositional engineering and adequate ion barrier layers.« less
  4. Atmospheric Humidity Underlies Irreproducibility of Formamidinium Lead Iodide Perovskites

    Metal halide perovskite solar cells (PSCs) are infamous for their batch-to-batch and lab-to-lab irreproducibility in terms of stability and performance. Reproducible fabrication of PSCs is a critical requirement for market viability and practical commercialization. PSC irreproducibility plagues all levels of the community; from institutional research laboratories, start-up companies, to large established corporations. Here, in this work, the critical function of atmospheric humidity to regulate the crystallization and stabilization of formamidinium lead triiodide (FAPbI3) perovskites is unraveled. It is demonstrated that the humidity content during processing induces profound variations in perovskite stoichiometry, thermodynamic stability, and optoelectronic quality. Almost counterintuitively, it ismore » shown that the presence of humidity is perhaps indispensable to reproduce phase-stable and efficient FAPbI3-based PSCs.« less
  5. Rational Design of A Chemical Bath Deposition Based Tin Oxide Electron Transport Layer for Perovskite Photovoltaics

    Chemical bath deposition is widely used to deposit SnOx as an electron transport layer in perovskite solar cells (PSCs). The conventional recipe uses thioglycolic acid (TGA) to facilitate attachments of SnOx particles onto the substrate. However, nonvolatile TGA has been reported to harm the operational stability of PSCs. In this work, we introduced a volatile oxalic acid (OA) as an alternative to TGA. OA, a dicarboxylic acid, functions as a chemical linker for the nucleation and attachment of particles to the substrate in the chemical bath. Moreover, OA can be readily removed through thermal annealing followed by a mild H2O2more » treatment, as shown by FTIR measurements. Synergistically, the mild H2O2 treatment selectively oxidizes the surface of the SnOx layer, minimizing nonradiative interface carrier recombination. EELS (electron-energy-loss-spectroscopy) confirms that the SnOx surface is dominated by Sn4+, while the bulk is a mixture of Sn2+ and Sn4+. This rational design of a CBD SnOx layer leads to devices with T85~1,500h, a significant improvement over the TGA-based device with T80~250h. Our champion device reached a power conversion efficiency of 24.6%. This work offers a rationale for optimizing the complex parameter space of CBD SnOx to achieve efficient and stable PSCs.« less
  6. Oriented nucleation in formamidinium perovskite for photovoltaics

    The black phase of formamidinium lead iodide (FAPbI3) perovskite shows huge promise as an efficient photovoltaic, but it is not favoured energetically at room temperature, meaning that the undesirable yellow phases are always present alongside it during crystallization. This problem has made it difficult to formulate the fast crystallization process of perovskite and develop guidelines governing the formation of black-phase FAPbI3. Here, we use in situ monitoring of the perovskite crystallization process to report an oriented nucleation mechanism that can help to avoid the presence of undesirable phases and improve the performance of photovoltaic devices in different film-processing scenarios. Themore » resulting device has a demonstrated power-conversion efficiency of 25.4% (certified 25.0%) and the module, which has an area of 27.83 cm2, has achieved an impressive certified aperture efficiency of 21.4%.« less
  7. Suppressing ion migration in metal halide perovskite via interstitial doping with a trace amount of multivalent cations

    Cations with suitable sizes to occupy an interstitial site of perovskite crystals have been widely used to inhibit ion migration and promote the performance and stability of perovskite optoelectronics. However, such interstitial doping inevitably leads to lattice microstrain that impairs the long-range ordering and stability of the crystals, causing a sacrificial trade-off. Here, we unravel the evident influence of the valence states of the interstitial cations on their efficacy to suppress the ion migration. Incorporation of a trivalent neodymium cation (Nd3+) effectively mitigates the ion migration in the perovskite lattice with a reduced dosage (0.08%) compared to a widely usedmore » monovalent cation dopant (Na+, 0.45%). As a result, the photovoltaic performances and operational stability of the prototypical perovskite solar cells are enhanced with a trace amount of Nd3+ doping while minimizing the sacrificial trade-off.« less
  8. Defect passivation of perovskites in high efficiency solar cells

    Abstract Metal halide perovskite solar cells (PSCs) have enormous potential as the next-generation photovoltaic technology. Being solution-processed at relatively low temperatures, it is inevitable that crystallographic defects are formed in abundance during fabrication. Such defects may cause undesirable energy losses by non-radiative recombination to limit the performance of PSCs. More importantly, it has become apparent that defect activity is fundamentally responsible for the operational instability issues hindering the commercialization readiness of PSCs. It is therefore necessary to develop strategies to minimize defect formation and to passivate formed defects. Here, we discuss recent advances on such defect mitigation and passivation strategies.more » We especially emphasize on methodologies that are incorporated into state-of-the-art PSCs that have demonstrated world record efficiencies and long-term stability.« less
  9. Shape-Controlled NaTaO3 by Flux-Mediated Synthesis

    NaTaO3 is a stable and wide bandgap n-type semiconductor material with many different applications. Here, a flux-mediated synthesis method is presented for NaTaO3 resulting in highly distinctive, substrate covering shapes via precursor chemistry variation at comparatively low temperatures. It is found that the microstructure of the resulting NaTaO3 films can be varied from nanocubes to smooth thin films. These shapes and surface chemistries can be correlated by employing density functional theory calculations and surface sensitive X-ray photoemission spectroscopy. This study provides guidance on how to synthesize the material and tailor its shape and surface termination for different applications. Finally, asmore » a proof of concept of one possible application, NaTaO3 is applied to perovskite solar cells as the electron transport layer, resulting in conversion efficiencies of >19%. Further, this study provides a new strategy for designing ternary oxide thin films for renewable energy applications.« less
  10. Material, Phase, and Interface Stability of Photovoltaic Perovskite: A Perspective

    The past decade has witnessed the unprecedented boost of power conversion efficiency (PCE) of photovoltaics based on halide perovskite materials since its early discovery. Despite its remarkably good performance, long-term stability is yet one of the last barriers before commercializing halide perovskite photovoltaics is possible. In this perspective, we discuss the challenges and concurrently the strategies regarding the stability of the perovskite materials, photoactive crystal phases, and the performance as well as stability limiting interfaces. Future perspectives of stable halide perovskite and perovskite solar cells are also proposed to shine light on letting perovskite technology satisfy long-term operation warranty.
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"Tan, Shaun"

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