Triple-cation low-bandgap perovskite thin-films for high-efficiency four-terminal all-perovskite tandem solar cells

All-perovskite multi-junction photovoltaics, comprised of a wide-bandgap (WBG) and a low-bandgap (LBG) perovskite solar cell (PSC), has opened a new window to cost-effective yet highly efficient solar cells (>33%). However, the poor operational stability of LBG PSCs is a major obstacle to the technological advance of all-perovskite tandem solar cells (all-PTSC). This study demonstrates that introducing minute quantities of Cs (1-10%) into the LBG FA0.8MA0.2Sn0.5Pb0.5I3 perovskite semiconductors (Eg = 1.26 eV) significantly improves the operational photo-stability of the corresponding LBG PSCs, due to a reduction of residual nanosized SnyPb(1-y)I2 aggregates, resulting in a beneficial stoichiometric composition. For an optimal concentration of Cs (2.5%) in the investigated range, the LBG PSCs attain remarkable power conversion efficiency (PCE) as high as 18.2% and maintain up to 92% of their initial power output after two hours under simulated one sun illumination. By mechanically stacking high-performance LBG bottom PSCs with semi-transparent top PSCs (Eg = 1.65 eV), four-terminal all-PTSCs with high PCE of 23.6% are attainable. This journal isWe acknowledge support by the KIT-Publication Fund of the Karlsruhe Institute of Technology. We would like to thank Dirk Hauschild (KIT) and Lothar Weinhardt (KIT) for XPS measurements. S. M. would like to acknowledge the nancial support from DAAD (Deutscher Akademischer Austauschdienst/German academic exchange service) for her doctoral research work under personal reference number 91621525. The nancial support by Alexander von Humboldt (Georg Forster Research Fellowship), German Federal Ministry of Education and Research (BMBF) through PRINTPERO (03SF0557A) project, German Federal Ministry for Economic Affairs and Energy (CAPITANO, funding code: 03EE1038B), the Initiating and Networking funding of Helmholtz Association HYIG of U.W.P. (VH-NG-1148), Helmholtz Energy Materials Foundry (HEMF), PEROSEED (ZT-0024), Science and Technology of Nanostructures (STN), and Karlsruhe School of Optics & Photonics (KSOP) is gratefully acknowledged. T. D. acknowledges the nancial support of a Postdoc Fellowship from the Australian Centre for Advanced Photovoltaics (ACAP). Part of the experiment was performed at the Australian National Fabrication Facility (ANFF) ACT Node

Drying Dynamics of Solution‐Processed Perovskite Thin‐Film Photovoltaics: In Situ Characterization, Modeling, and Process Control

A key challenge for the commercialization of perovskite photovoltaics is the transfer of high‐quality spin coated perovskite thin‐films toward applying industry‐scale thin‐film deposition techniques, such as slot‐die coating, spray coating, screen printing, or inkjet printing. Due to the complexity of the formation of polycrystalline perovskite thin‐films from the precursor solution, efficient strategies for process transfer require advancing the understanding of the involved dynamic processes. This work investigates the fundamental interrelation between the drying dynamics of the precursor solution thin‐film and the quality of the blade coated polycrystalline perovskite thin‐films. Precisely defined drying conditions are established using a temperature‐stabilized drying channel purged with a laminar flow of dry air. The dedicated channel is equipped with laser reflectometry at multiple probing positions, allowing for in situ monitoring of the perovskite solution thin‐film thickness during the drying process. Based on the drying dynamics as measured at varying drying parameters, namely at varying temperature and laminar air flow velocity, a quantitative model on the drying of perovskite thin‐films is derived. This model enables process transfer to industry‐scale deposition systems beyond brute force optimization. Via this approach, homogeneous and pinhole‐free blade coated perovskite thin‐films are fabricated, demonstrating high power conversion efficiencies of up to 19.5% (17.3% stabilized) in perovskite solar cells

Nanostructured front electrodes for perovskite/c-Si tandem photovoltaics

The rise in the power conversion efficiency (PCE) of perovskite solar cells has triggered enormous interest in perovskite-based tandem photovoltaics. One key challenge is to achieve high transmission of low energy photons into the bottom cell. Here, nanostructured front electrodes for 4-terminal perovskite/crystalline-silicon (perovskite/c-Si) tandem solar cells are developed by conformal deposition of indium tin oxide (ITO) on self-assembled polystyrene nanopillars. The nanostructured ITO is optimized for reduced reflection and increased transmission with a tradeoff in increased sheet resistance. In the optimum case, the nanostructured ITO electrodes enhance the transmittance by ∼7% (relative) compared to planar references. Perovskite/c-Si tandem devices with nanostructured ITO exhibit enhanced short-circuit current density (2.9 mA/cm2 absolute) and PCE (1.7% absolute) in the bottom c-Si solar cell compared to the reference. The improved light in-coupling is more pronounced for elevated angle of incidence. Energy yield enhancement up to ∼10% (relative) is achieved for perovskite/c-Si tandem architecture with the nanostructured ITO electrodes. It is also shown that these nanostructured ITO electrodes are also compatible with various other perovskite-based tandem architectures and bear the potential to improve the PCE up to 27.0%

In2_{2}O3_{3}:H-Based Hole-Transport-Layer-Free Tin/Lead Perovskite Solar Cells for Efficient Four-Terminal All-Perovskite Tandem Solar Cells

Narrow-band gap (NBG) Sn–Pb perovskites with band gaps of ∼1.2 eV, which correspond to a broad photon absorption range up to ∼1033 nm, are highly promising candidates for bottom solar cells in all-perovskite tandem photovoltaics. To exploit their potential, avoiding optical losses in the top layer stacks of the tandem configuration is essential. This study addresses this challenge in two ways (1) removing the hole-transport layer (HTL) and (2) implementing highly transparent hydrogen-doped indium oxide In2O3:H (IO:H) electrodes instead of the commonly used indium tin oxide (ITO). Removing HTL reduces parasitic absorption loss in shorter wavelengths without compromising the photovoltaic performance. IO:H, with an ultra-low near-infrared optical loss and a high charge carrier mobility, results in a remarkable increase in the photocurrent of the semitransparent top and (HTL-free) NBG bottom perovskite solar cells when substituted for ITO. As a result, an IO:H-based four-terminal all-perovskite tandem solar cell (4T all-PTSCs) with a power conversion efficiency (PCE) as high as 24.8% is demonstrated, outperforming ITO-based 4T all-PTSCs with PCE up to 23.3%

2D/3D Heterostructure for Semitransparent Perovskite Solar Cells with Engineered Bandgap Enables Efficiencies Exceeding 25% in Four‐Terminal Tandems with Silicon and CIGS

Wide-bandgap perovskite solar cells (PSCs) with optimal bandgap (E$_{g}$) and high power conversion efficiency (PCE) are key to high-performance perovskite-based tandem photovoltaics. A 2D/3D perovskite heterostructure passivation is employed for double-cation wide-bandgap PSCs with engineered bandgap (1.65 eV ≤ E$_{g}$ ≤ 1.85 eV), which results in improved stabilized PCEs and a strong enhancement in open-circuit voltages of around 45 mV compared to reference devices for all investigated bandgaps. Making use of this strategy, semitransparent PSCs with engineered bandgap are developed, which show stabilized PCEs of up to 25.7% and 25.0% in fourterminal perovskite/c-Si and perovskite/CIGS tandem solar cells, respectively. Moreover, comparable tandem PCEs are observed for a broad range of perovskite bandgaps. For the first time, the robustness of the four-terminal tandem configuration with respect to variations in the perovskite bandgap for two state-of-the-art bottom solar cells is experimentally validated