Long-Range Charge Extraction in Back-Contact Perovskite Architectures via Suppressed Recombination

Metal-halide perovskites are promising solution-processable semiconductors for efficient solar cells and show unexpectedly high diffusion ranges of photogenerated charges. Here, we study charge extraction and recombination in metal-halide perovskite back-contact devices, which provide a powerful experimental platform to resolve electron- or hole-only transport phenomena. We prepare thin films of perovskite semiconductors over laterally-separated electron- and hole-selective materials of SnO¬2 and NiOx, respectively. Upon illumination, electrons (holes) generated over SnO¬2 (NiOx) rapidly transfer to the buried collection electrode, leaving holes (electrons) to diffuse laterally as majority carriers in the perovskite layer. Under these conditions, we find recombination is strongly suppressed. Resulting surface recombination velocities are below 2 cm s-1, an order of magnitude lower than in the presence of both carrier types, and approaching values of high-quality silicon. We find diffusion lengths of electrons and holes exceed 12 µm in our horizontal polycrystalline device, an order of magnitude higher than reported in vertically stacked architectures. We fabricate back-contact solar cells with short-circuit currents as high as 18.4 mA cm-2, reaching 70% external quantum efficiency

Strategy for large???scale monolithic Perovskite/Silicon tandem solar cell: A review of recent progress

For any solar cell technology to reach the final mass-production/commercialization stage, it must meet all technological, economic, and social criteria such as high efficiency, large-area scalability, long-term stability, price competitiveness, and environmental friendliness of constituent materials. Until now, various solar cell technologies have been proposed and investigated, but only crystalline silicon, CdTe, and CIGS technologies have overcome the threshold of mass-production/commercialization. Recently, a perovskite/silicon (PVK/Si) tandem solar cell technology with high efficiency of 29.1% has been reported, which exceeds the theoretical limit of single-junction solar cells as well as the efficiency of stand-alone silicon or perovskite solar cells. The International Technology Roadmap for Photovoltaics (ITRPV) predicts that silicon-based tandem solar cells will account for about 5% market share in 2029 and among various candidates, the combination of silicon and perovskite is the most likely scenario. Here, we classify and review the PVK/Si tandem solar cell technology in terms of homo- and hetero-junction silicon solar cells, the doping type of the bottom silicon cell, and the corresponding so-called normal and inverted structure of the top perovskite cell, along with mechanical and monolithic tandemization schemes. In particular, we review and discuss the recent advances in manufacturing top perovskite cells using solution and vacuum deposition technology for large-area scalability and specific issues of recombination layers and top transparent electrodes for large-area PVK/Si tandem solar cells, which are indispensable for the final commercialization of tandem solar cells

A low viscosity, low boiling point, clean solvent system for the rapid crystallisation of highly specular perovskite films

Perovskite-based photovoltaics have, in recent years, become poised to revolutionise the solar industry. While there have been many approaches taken to the deposition of this material, one-step spin-coating remains the simplest and most widely used method in research laboratories. Although spin-coating is not recognised as the ideal manufacturing methodology, it represents a starting point from which more scalable deposition methods, such as slot-dye coating or ink-jet printing can be developed. Here, we introduce a new, low-boiling point, low viscosity solvent system that enables rapid, room temperature crystallisation of methylammonium lead triiodide perovskite films, without the use of strongly coordinating aprotic solvents. Through the use of this solvent, we produce dense, pinhole free films with uniform coverage, high specularity, and enhanced optoelectronic properties. We fabricate devices and achieve stabilised power conversion efficiencies of over 18% for films which have been annealed at 100 °C, and over 17% for films which have been dried under vacuum and have undergone no thermal processing. This deposition technique allows uniform coating on substrate areas of up to 125 cm2, showing tremendous promise for the fabrication of large area, high efficiency, solution processed devices, and represents a critical step towards industrial upscaling and large area printing of perovskite solar cells

The potential of multijunction perovskite solar cells

Metal halide perovskite semiconductors offer rapid, low-cost deposition of solar cell active layers with a wide range of band gaps, making them ideal candidates for multijunction solar cells. Here, we combine optical and electrical models using experimental inputs to evaluate the feasible performances of all-perovskite double-junction (2PJ), triple-junction (3PJ), and perovskite-perovskite-silicon triple-junction (2PSJ) solar cells. Using parameters and design constraints from the current state-of-the-art generation of perovskite solar cells, we find that 2PJs can feasibly approach 32% power conversion efficiency, 3PJs can reach 33%, and 2PSJs can surpass 35%. We also outline pathways to improve light harvesting and demonstrate that it is possible to raise the performances to 34%, 37%, and 39% for the three architectures. Additionally, we discuss important future directions of research. Finally, we perform energy yield modeling to demonstrate that the multijunction solar cells should not suffer from reduced operational performances due to discrepancies between the AM1.5G and real-world spectrum over the course of a year

The potential of multijunction perovskite solar cells

Metal halide perovskite semiconductors offer rapid, low-cost deposition of solar cell active layers with a wide range of band gaps, making them ideal candidates for multijunction solar cells. Here, we combine optical and electrical models using experimental inputs to evaluate the feasible performances of all-perovskite double-junction (2PJ), triple-junction (3PJ), and perovskite-perovskite-silicon triple-junction (2PSJ) solar cells. Using parameters and design constraints from the current state-of-the-art generation of perovskite solar cells, we find that 2PJs can feasibly approach 32% power conversion efficiency, 3PJs can reach 33%, and 2PSJs can surpass 35%. We also outline pathways to improve light harvesting and demonstrate that it is possible to raise the performances to 34%, 37%, and 39% for the three architectures. Additionally, we discuss important future directions of research. Finally, we perform energy yield modeling to demonstrate that the multijunction solar cells should not suffer from reduced operational performances due to discrepancies between the AM1.5G and real-world spectrum over the course of a year

Shunt‐blocking layers for semitransparent perovskite solar cells

Perovskite solar cells have shown phenomenal progress and have great potential to be manufactured as low‐cost large area modules. However, perovskite films often suffer from pinholes and the resulting contact between hole‐ and electron transporting layers provides lower resistance (shunt) pathways, leading to decreased open‐circuit voltage and fill factor. This problem is even more severe in large area cells and especially in the case of neutral color semitransparent cells, where a large absorber‐free area is required to provide the desired transparency. Herein, a simple, inexpensive, and scalable wet chemical method is presented to block these “shunting paths” via deposition of transparent, insulating molecular layers, which preferentially bind to the uncovered surface of the electron collecting oxide, without hindering charge extraction from the perovskite to the charge collection layers. It is shown that this method improves the performance in semitransparent cells, where the enhancement in open‐circuit voltage is up to 30% without negatively impacting the photocurrent. Using this method, we achieved an efficiency of 6.1% for a neutral color semitransparent perovskite cell with 38% average visible transmittance. This simple shunt blocking technique has applications in improving the yield as well as efficiency of large area perovskite solar cells and light emitting devices. </p

Interfacial electron accumulation for efficient homo-junction perovskite solar cells

Here we study perovskite solar cells based on mesoporous alumina scaffold infiltrated and capped with a perovskite absorber layer, which are devoid of a discrete n-type electron collection layer. We employ ethoxylated polyethylenimine (PEIE) to modify the interface between the perovskite absorber layer and the metallic transparent fluorine-doped SnO 2 (FTO) electrode. Surprisingly, the PEIE interlayer obviates the requirement for the conventional dense-TiO 2 (d-TiO 2 ) compact layer (or organic fullerene layer), usually required to selectively extract electrons from the perovskite film. The self-organized PEIE interlayer produced a strong induced dipole moment at the perovskite-FTO interface, with our results indicating that electrons accumulate within the perovskite film at this interface. The resultant “n-type” contact region within the perovskite absorber layer, progressing to an intrinsic (i) region within the bulk of the perovskite layer, represents an n-i homojunction and favorably enables selective electron extraction at the FTO electrode. Resulting solar cells deliver current-voltage measured power conversion efficiencies (η) of over 15.0% and a substantial stabilized efficiency (η) of 9.1%. Although our solar cell performance remains lower than the highest reported efficiencies for perovskite solar cells employing discrete charge selective extraction layers, it indicates significant potential for “homo-junction” perovskite solar cells, once the metallic-to-perovskite contact is fully controlled. Additionally, our work identifies the potential impact of modifying the interface between the perovskite absorber and the subsequent contact materials with dipolar organic compounds, which may be applicable to optimizing contact at perovskite-semiconductor heterojunctions

Shunt‐blocking layers for semitransparent perovskite solar cells

Perovskite solar cells have shown phenomenal progress and have great potential to be manufactured as low‐cost large area modules. However, perovskite films often suffer from pinholes and the resulting contact between hole‐ and electron transporting layers provides lower resistance (shunt) pathways, leading to decreased open‐circuit voltage and fill factor. This problem is even more severe in large area cells and especially in the case of neutral color semitransparent cells, where a large absorber‐free area is required to provide the desired transparency. Herein, a simple, inexpensive, and scalable wet chemical method is presented to block these “shunting paths” via deposition of transparent, insulating molecular layers, which preferentially bind to the uncovered surface of the electron collecting oxide, without hindering charge extraction from the perovskite to the charge collection layers. It is shown that this method improves the performance in semitransparent cells, where the enhancement in open‐circuit voltage is up to 30% without negatively impacting the photocurrent. Using this method, we achieved an efficiency of 6.1% for a neutral color semitransparent perovskite cell with 38% average visible transmittance. This simple shunt blocking technique has applications in improving the yield as well as efficiency of large area perovskite solar cells and light emitting devices. </p

Optical properties and limiting photocurrent of thin-film perovskite solar cells

Metal-halide perovskite light-absorbers have risen to the forefront of photovoltaics research offering the potential to combine low-cost fabrication with high power-conversion efficiency. Much of the development has been driven by empirical optimisation strategies to fully exploit the favourable electronic properties of the absorber layer. To build on this progress, a full understanding of the device operation requires a thorough optical analysis of the device stack, providing a platform for maximising the power conversion efficiency through a precise determination of parasitic losses caused by coherence and absorption in the non-photoactive layers. Here we use an optical model based on the transfer-matrix formalism for analysis of perovskite-based planar heterojunction solar cells using experimentally determined complex refractive index data. We compare the modelled properties to experimentally determined data, and obtain good agreement, revealing that the internal quantum efficiency in the solar cells approaches 100%. The modelled and experimental dependence of the photocurrent on incidence angle exhibits only a weak variation, with very low reflectivity losses at all angles, highlighting the potential for useful power generation over a full daylight cycle